Magnetic metal oxide assisted conducting polymer nanocomposites as eco-friendly electrode materials for supercapacitor applications: a review
-
Mohammad Faraz Ahmer
,
Qasim Ullah
Abstract
Magnetic metallic embedded conducting polymeric nanostructures have demonstrated a pivotal role in high-performance supercapacitors. Numerous research studies have attempted to develop new hybrid electrode materials through the incorporation of electronically conductive polymers into magnetic metallic oxides. To further enhance the electrochemical performance of conducting polymer (CP)–magnetic metal oxide (MMO) hybrid nanocomposites, an additional component (carbon-based material) has been mostly introduced into it. The focus of this review has been on highlighting the electrochemical importance of CP–MMO nanostructured composites in supercapacitor applications. The hybrid nanocomposite materials resulting from embedding conjugated polymers [polyaniline, polypyrrole, and poly (3,4-ethylenedioxythiophene)] and MMO (MnO2, NiO, and Co3O4) have been taken into consideration for discussion from most recent literature covering the period 2018–2024. The concise information presented in this review article will create awareness among researchers about the latest developments in the field of green energy-storing devices, particularly in the case of supercapacitors.
1 Introduction
The expanding global demand for clean energy has become one of the major issues of the current century for sustainable development. Therefore, there is a need for the development of environmentally benign energy storage/conversion systems to meet the ascending demand for energy consumption. Among the various available energy storing/conversion systems, supercapacitors have qualified as the most promising electrochemical energy storing source. An efficient energy storing system should be capable of providing high energy/power density, exceptional cyclic stability, rapid charging/discharging, superior reversibility, cost affordability, high level specific/volumetric capacitance, and clean environment compatibility. 1 In this regard, supercapacitors (SCPs) have attracted favoritism over other energy-storing/conversion electrochemical devices (fuel cells and batteries) because of their unique cyclic stability, higher power density, reasonable energy density, environmental sustainability, and remarkable specific capacitance along with charging – discharging rapidity. As a result, portable flexible solid-state micro-supercapacitors are now gaining popularity, especially for utilization in portable electronic appliances (mobile phones, electronic papers, laptops, etc.), Internet of Things (IoT) devices, biomedical implants, hybrid vehicles, and military equipment. 2 From energy versus power density Ragone plot (Figure 1), 3 it is clear that SCPs with a high power density (PD) and improvable energy density (ED) are ideal energy-storing systems to bridge the gap between batteries (high ED and low PD) and traditional capacitors (high PD and low ED).
Ragone graph of power density versus energy density (ED) for different energy storage devices. 3
The last two decades have witnessed tremendous progress in supercapacitor research leading to innovative technological changes in the development of electrochemical energy-storing devices (EESD). Recently, the generic term “supercapattery” has been coined by a pioneering research group of G. Z. Chen 4 , 5 , 6 to highlight the improved performance of various hybrid devices developed through a combination of merits of rechargeable battery (superior energy density) and supercapacitor (long cyclic life span and excellent power density). The supercapattery involves the approach to merge the electrochemical characteristics of both battery and SCPs into a single device either through a) pairing a supercapacitor electrode with the battery electrode or b) designing the electrodes from active composite materials that possess both capacitive and the Nernstian charge storing capability. Both battery and SCP are electrochemical energy storing devices but in the case of battery the energy produced via chemical reaction is stored as charge whereas in the case of SCP, energy is directly stored in the form of charge. The primary required components to create a full–cell SCP (Figure 2) are:
an electrolyte (aqueous salt solution, ionic liquid, molten salt, etc.) that is electronically non-conductor but acts as an ionic conductor to facilitate ion mobility (or conductivity). The important parameters to consider while selecting an electrolyte include the size of ions and their concentration as well as the ion–solvent interactions. Since, electrolytes have a significant influence on power density, cyclic stability, and specific capacitance, the size of ions/hydrated ions in the electrolyte must not be greater than the pore size of electrode materials. The most commonly used inorganic electrolytes are NaOH, HCl, KCl, H3PO4, and H2SO4. While choosing an electrolyte for use in SCs, the electrolyte should fulfill the following requirements. 7
wider electrochemical potential window
reasonably good ionic conductivity
inertness towards other cell components
safe handling and non-toxicity
high thermal stability
pair of positive and negative electrodes
a separator (polymer membrane, glassy paper, cellulose, etc.) for electrically isolating both electrodes. Among polymer separators, fibrous nanostructured and monolithic networks with specified pores have been widely used.
Current collector (carbon cloth, metal foams/meshes, metallic alloys, etc.) to facilitate unhindered migration of electrons from the electrode surface to the external circuit.
Schematic illustration of working principles of supercapacitor electrolyte furnishing cations (C+) and anions (A−) in solution.
Depending on the active material used and operational energy-storing mechanism, SCPs have been classified as:
EDLCs (electric double-layer capacitors)
PCs (pseudocapacitors) or redox capacitors
HbCs (hybrid capacitors).
The distinct, characteristic features of EDLC and PC are summarized in Table 1.
| EDLC | PC |
|---|---|
| Formation of the double layer at the electrolyte/electrode interface | No such layer formation appeared |
| No involvement of redox reaction, (i.e. non – Faradaic energy storage process) | Involvement of redox reaction (i.e. Faradaic energy storage process) |
| Superior power performance | High energy density |
| High cyclic stability | Superior specific capacitance |
| Mainly use of carbon electrode materials (graphene, activated carbon, nanostructured carbon, carbon aerogel) | Use of transition metal oxides and conducting polymers (CP) as electrode materials |
| Charge accumulation via reversible adsorption/desorption of ions at electrolyte/electrode interface | Charge accumulation via rapid reversible redox reaction of electroactive species onto the surface of the electrode |
The HbCs, categorized as the third group of SCs have been produced through the combination of both EDLC and PC. Thus, HbCs utilize both Faradaic and non-Faradaic charge–transfer mechanisms and display highly improved electrochemical performance in terms of excellent cyclic stability, improved energy/power density, higher specific capacitance, and superb electrical conductivity. For designing HbCs, composite materials comprising of either bi– or tri– components (conducting polymers (CPs), metal oxides (MO), or/and carbon-based matter in appropriate combinations have been generally employed. 11 , 12 CPs as one of the components of electrode material have been used for both EDLCs and PCs. 13 Alternatively, SCs have also been categorized as symmetric and asymmetric depending upon whether both the electrodes used in the device are the same or different. Asymmetric hybrid capacitors combine both Faradaic and non-Faradaic processes due to the linking of pseudo-capacitor electrodes with the EDLC electrodes.
The supercapacitive performance of the electrode composite materials has been assessed by using cyclic voltammetry (CV), galvanostatic charge-discharge (GCD), and electrochemical impedance spectroscopic (EIS) electroanalytical methods. 14 From the electrochemical measurements, some information related to the electrochemical performance of electrode materials such as specific capacity, cyclic stability, energy density, and power density can be obtained. The specific capacity (F/g) of the electrode has been determined from the CV curve using Equation (1).
Here, C is specific capacitance (F/g); m is the mass loading of active material; ΔV is the potential window; dv/dt is the scan rate; and the integration term represents the area under the CV voltammogram. The specific capacitance from the GCD plot can also be calculated with the use of Equation (2).
Here the term I, stands for “current density”, and the integration term represents the inner area of the discharge curve.
Energy and power density are also important performance parameters of supercapacitors. Energy density expresses the quantity of charge/energy stored, whereas power density displays the rate at which a supercapacitor can deliver energy. The specific energy density, E (Wh/kg), and the specific power density, P (W/kg) can be obtained using Equations (3) and (4).
Here Δt (s) represents the discharging time.
Recently, single metal-containing carbon-based hybrid materials have been widely used in supercapacitors due to their admirable porosity, high electrical conductivity, and excellent mechanical/chemical stability. However, the poor charge transfer property and possible disintegration during charging/discharging processes have been their major drawbacks. Therefore, single metal oxides have been replaced by mixed oxides (MnCo2O4, CuCO2O4, NiCo2O4, CoFe2O4, etc.) to develop advanced hybrid electrode materials. 15 To take advantage of the superb electrochemical properties of carbon-based – mixed metal oxide materials, S. S. Raut and co-workers 16 have prepared zinc ferrite (ZFO) anchored CNTs hybrid thin films following “successive ionic layer adsorption and reaction (SILAR) method for use directly as electrode without any binder”. The solid-state symmetric supercapacitor device (ZFO/CNT//ZFO/CNT) displayed excellent electrochemical performance in PVA – LiCl gel electrolyte with delivery of SC (92.20 F/g at 0.35 A/g), specific energy (12.80 Wh/kg), specific power (377.86 W/kg) and good cyclic stability (70 % capacitance retention for 2,000 cycles). The SEM/TEM images of CNT and CNT/ZFO are shown in Figure 3, whereas CV, CD curves, and Ragone plot of symmetric solid state (SSS) device have been presented in Figure 4. The two SSS supercapacitor devices when connected in series were capable to glow an LED (light-emitting diode) for 3 min.
FE-SEM images of (a) CNT and (b) ZFO–CNT films; (c) TEM images of ZFO–CNT film. The yellow dotted circles indicate ZFO particles. 16 Reproduced with permission from John Wiley and Sons, license no. 5864930149224.
Symmetric solid state (SSS) device. (a) CV curves of the ZFO–CNT//ZFO–CNT SSS device in progressively increasing potential windows. (b) CV curves of the ZFO–CNT//ZFO–CNT SSS device at scan rates from 5 to 100 mV s−1. (c) CD curves of the ZFO–CNT//ZFO–CNT SSS device at different current densities. (d) Ragone plot of the ZFO–CNT//ZFO–CNT SSS device (the inset is the variation of the specific capacitance as a function of current density). 16 Reproduced with permission from John Wiley and Sons, license no. 5864930149224.
In an interesting study, B. Pandit et al. 17 have developed a novel binder-free solution–processed technique to prepare nanostructured cerium (IV) oxide (CeO2) materials through air annealing maintaining temperatures between 100 and 300 °C. The CeO2 annealed at 200 °C demonstrated the best electrochemical performance in PVA – LiClO4 gel electrolyte revealing SC (750 F/g) with 95 % cyclic stability and modest potential window (0.6 V vs Ag/AgCl). The assembled CeO2 flexible symmetric (FS) solid-state supercapacitor (SSS) device displayed excellent SC (321.3 F/g) along with broad voltage window (1.2 V), high specific energy (61.4 Wh/kg), marvelous specific power (6.9 kW/kg) and remarkable cyclic stability. This study has paved the way to develop eco-friendly lightweight electronic devices. The interesting electrochemical performance features of fabricated FS-SC are demonstrated in Figures 5–7.
Schematic representation of the fabricated FS-SSS device based on cerium oxide electrode annealed 200 °C and PVA-LiClO4 gel electrolyte. 17 Reproduced with permission from Elsevier, license no. 5864921364855.
Electrochemical performance of FS-SSS device with PVA-LiClO4 gel electrolyte. (a) CV curves at different scan rates ranging from 100 to 2 mV/s with voltage window of 1.2 V, (b) specific capacitance at a function of scan rate, (c) GCD curves at different current densities ranging from 3 to 6 mA/cm2, (d) specific capacitance as a function of current density. 17 Reproduced with permission from Elsevier, license no. 5864921364855.
Electrochemical performance features. (a) Capacitance retention at different bending angles, (b) CV curves with different bending angles at a scan rate of 100 mV/s, (c–e) actual demonstration of FS-SSS device discharging through ‘VNIT’ panel consisting 21 red LEDs for 0, 15, and 30 s, respectively. 17 Reproduced with permission from Elsevier, license no. 5864921364855.
In addition to the use of metal oxide containing binary/ternary nanocomposites in supercapacitors, binary layered chalcogenides have been extensively investigated as next-generation optoelectronic materials. For example, hexagonal 2-D tin selenide (SnSe) synthesized in the form of nanosheets through the one-pot colloidal method has been used as binder-free electrode material for SCs. 18 The fabricated SnSe electrode illustrated remarkable electrochemical performance delivering SC (617 F/g at a scan rate of 2 mV/s), PD (4.3 kW/kg), ED (28.5 Wh/kg), low charge transfer resistance, and promising cyclic stability. The FE – SEM, images demonstrated the large coverage of uniform 2-D hexagonal nanosheets, the average thickness (65 nm) of nanosheets, and hexagonal sheets with smooth surfaces whereas EDS images depicted the presence of Sn and Se purely in elemental form. The electrochemical performance parameters of the SnSe electrode determined in highly basic (1.0 M NaOH) electrolyte revealed its safe applicability in extremely corrosive alkaline aqueous media.
To compensate for the poor conductivity of transition metal oxides, researchers have used metal sulfides in the fabrication of carbon-based nanocomposites for supercapacitor applications. The MWCNT/HgS hybrid nanocomposite synthesized by simple and inexpensive SILAR method in thin film form by 19 has demonstrated exceptional SC (946.43 F/g) at a scan rate of 2 mV/s with maximum ED (42.97 Wh/kg), PD (1.6 kW/kg) and excellent cyclic stability retaining 93 % of initial capacitance over 4,000 cycles for single electrode system (Figure 8). The aqueous symmetric SC device made of MWCNT/HgS nanocomposite displayed SC (301.34 F/g) at 20 mV/s with a potential window (1.2 V). Thus, the development of solid-state device fabrication techniques through the replacement of liquid electrolytes with polymer gel is expected better option for creating high-performance SC devices in the future.
Metal sulfides in the fabrication of carbon-based nanocomposites for supercapacitor applications. (a) CV curves of MWCNTs, HgS, and MWCNT/HgS electrodes at a scan rate of 100 mV/s, (b) CV curves of MWCNT/HgS electrodes at different scan rates ranging from 2 to 100 mV/s, (c) corresponding specific capacitance as a function of scan rate, (d) cycling stability for 4,000 cycles at 100 mV/s scan rate, inset shows CV curves for different cycle numbers. 19 Reproduced with permission from Elsevier, license no. 5864920574867.
2 Electrode materials
The electrochemical performance of SCs is inherently dependent upon the composition and porosity of the materials used in designing electrodes. For achieving outstanding supercapacitor accomplishment, the electrode material must have high capacitance. The capacitance of SCs depends on the availability of effective electrochemically active surface area of electrode material for electrolyte–electrode interaction. The pore size of the electrode material is another factor that influences the capacitance as well as the active surface area. The purity and architectural morphology of electrode material are also important to minimize the undesirable current leakage/self–discharging of SCs.
There are three different types of electrode materials as listed below that have been aggressively pursued in supercapacitors applications.
Carbon materials (CMs)
Metal oxides (MOs)/sulfides or hydroxides
Conducting polymers (CPs)
The electrode materials used in SCs belonging to different categories are displayed in Figure 9.
Electrode materials for supercapacitors.
Among these materials, CMs have shown excellent non–Faradaic capacitance, good conductivity, admirable chemical stability, reasonable power density, and long cyclic life but poor energy density/medium power density and inferior flexibility. On the other hand, MOs possess excellent Faradaic capacitance, medium energy density, and low cyclability. As regards CPs, they have displayed high conductivity, excellent Faradaic capacitance, good flexibility, reasonable chemical stability, and fabrication comfort but poor energy/power densities, and low cycling performance. Thus, none of the individual materials (CM, MO, or CP) is ideal for supercapacitor application. However, their binary or ternary composites have demonstrated superior electrochemical performance due to constructive mutual interactions among the components. It has been observed that CP, CM, and MO can be perfectly integrated to develop anisotropic hybrid composites for electrode fabrication. 20 , 21 , 22 , 23
2.1 Carbon materials
Various carbon-based materials, normally used as electrode materials for EDLCs include activated carbon (AC), carbon aerogels (CAG), graphene (G), graphene oxide (GO), reduced GO, carbon nanotubes (CNTs) carbon dots (CDs) and carbon nanofibres (CNFs). These carbon materials generally display specific capacitance in the following decreasing order: CNTs > GO > G > CNFs > AC. The important nano-structured carbon materials that have been widely used in the fabrication of electrodes for supercapacitors are listed in Table 2.
Carbon nanostructures in different forms used in supercapacitors.
| Dimensional architecture | Carbon nanostructures |
|---|---|
| 3-D |
|
| 2-D |
|
| 1-D |
|
| 0-D |
|
EDLCs involving carbon materials store energy at electrolyte–carbon junction through ion adsorption at the carbon surface where the charge storage mechanism occurs in the absence of redox reaction. AC has been most often used as electrode material in SCs mainly due to its higher surface area and cost-effectiveness. Carbon aerogels with lower equivalent series resistance (ESR) than AC have been popularly used as binder-free electrodes in SCs. Since its discovery in 2004, graphene with a single-atom-thick 2D structure has been a highly attractive material for EDLC energy storage systems. However, its poor dispersibility has been the major drawback.
CNTs as SC electrode materials have received a lot of attention due to their highly accessible surface area, excellent electrical conductivity, unique porous architectural framework, strong thermal resistance, and high mechanical stability. Contrary to other C-based electrodes, interconnected mesopores of CNTs facilitate charge distribution continuity throughout the available exterior surface area. CNTs are classified as SWNTs (single-walled nanotubes) and MWCNTs (multi-walled nanotubes) which can be chemically activated with KOH to enhance specific capacitance. 24 GO containing oxygenated hydrophilic (–OH, –COOH, –CO) functional groups is a chemically modified form of graphene. Unlike GO, rGO which is obtained by deoxygenating GO is a highly conducting material retaining the graphitic structure of carbon – atoms. Carbon-nanofibres have been used to fabricate different types of flexible fibrous structures to achieve enhanced specific capacitance of energy storage devices. 25
CDs are nano-sized carbon particles (zero-dimensional) with sp2 graphitic structure bearing oxidized functionalities. CDs in nanocomposites accelerate the ionic migration which results in high specific capacitance. 26 Accordingly, carbon materials in all three-dimensional nanostructural forms (nanosheets, nanowires, nanoflowers, nanotubes, nanobelts, and nanocoils) have been broadly used in supercapacitor applications. 27 Interestingly, numerous studies have been reported on the use of CP–carbon material nanocomposites for use in supercapacitors. The incorporation of nano-carbon material within the polymer matrix has resulted in enhancement of electrochemical performance. The nanocomposite electrodes fabricated from CP-incorporated carbon nanomaterials have shown improved energy and power densities due to the combination of pseudo – and electrical double-layer capacitive effects. 28
2.2 Magnetic metal oxides
In the recent past, several magnetic redox metal oxides (MnO2, NiO, MoO2, Co3O4, Fe2O3 etc.) have been extensively used for pseudocapacitor electrodes in addition of utilization of mixed ternary metal oxides (Ni/Zn or Cu/Fe2O4 and Mn/Zn or Ni/Co2O4) as electrode materials for PCs. 2 , 28 , 29 Magnetic metallic oxides have been classified as paramagnetic, diamagnetic, and ferromagnetic. Ferromagnetic materials are strongly attracted by magnetic fields due to the alignment of all the unpaired electrons in the same direction. Thus, ferromagnetic substances are easily magnetized by the external magnetic field and capable of retaining magnetism even after the removal of the magnetic field. Ferromagnetic materials have very high positive values of magnetic moment, magnetic susceptibility, relative permeability, and magnetic flux density. The more frequently used ferromagnetic substances are metals like Fe, Co, Ni, Mn, etc., and their alloys. Besides, some compounds of rare earth metals, mixed oxides (iron–cobalt, nickel-cobalt, and manganese–iron) have also been used as ferromagnetic materials. The Curie temperature (Tc), being substance – specific is an important property of magnetic materials. It is defined as the temperature at which ferromagnetic materials lose their permanent magnetic properties and behave like paramagnetic materials. The Curie temperatures (K) of some important ferro – and ferrimagnetic materials (given in parentheses) are: Co (1388), Ni (627), Fe (1043), Fe2O3 (948), NiO.Fe2O3 (858), CrO2 (386) and CuO.Fe2O3 (728). The highest known Tc has been reported for cobalt. Ferromagnetism is very important from a modern technological point–of–view as it is the basis of many electrical and electromechanical devices. As an emerging category of novel materials, ferromagnetic metals/metal oxides alone or in combination with conducting polymers have been widely used in supercapacitors due to their chemical stability, high theoretical capacitance, multiple redox states, structural variance, economical synthesis, excellent electrochemical performance and unique porosity. 30 , 31 , 32
In this review, our emphasis is to highlight the use of Ni, Co, and Mn magnetic oxides and their polymer composites for supercapacitor applications. The main structural features and physical properties of the focused individual MMOs and CPs are briefly mentioned below.
2.2.1 Nickel oxide (NiO)
NiO, a greenish crystalline transition metal oxide with useful ferromagnetic characteristics has been the popular electrochemical performing electrode material for supercapacitors 33 due to high theoretical capacitance (2584 F/g), wide band gap (3.6–4.0 eV), environmentally friendliness, cost-effectiveness, good electrical/heat stability, reasonably good surface area in porous state, availability in different morphologies (nanorods/fibres/wires/tubes/sheets and microspheres), easy natural abundance, intriguing magnetic properties, multifold oxidation states (0, −1, +2, +3 and + 4) and anodic electrochromism. However, the important oxidation state is Ni2+ which is comparatively more stable. Using different synthesizing methods (sol-gel, hydrothermal, solvothermal, electrodeposition, thermal decomposition, and anodic arc plasma, etc.), NiO has been obtained in several morphological nano architectures like tubes, sheets, balls, and wires. In the NiO crystal (Figure 10), Ni is bonded to six O2− ions to form a mixture of corner and edge-sharing NiO6 octahedral in which all Ni–O bonds have the same length (2.09 Ao). It has been reported that nanoporous nickel (np–Ni) prepared under an applied external magnetic field has displayed much better supercapacitor performance in comparison to np – Ni produced in the absence of a magnetic field. 34
Crystal structure of NiO with octahedral Ni2+ and O22− sites.
NiO nanoparticles, in different structural–dimensional forms (0-, 1-, 2- and 3-D), have been prepared using various synthesis (sonochemical, sol-gel, hydrothermal/solvothermal, microwave radiation assisted, precipitation, etc.) methods. 33 The zero-dimensional (0-D) NiO electrode materials in the form of nanoparticles/nanoclusters have been obtained by the use of sonochemical, precipitation, and sol-gel methods 35 , 36 , 37 , 38 whereas hydrothermal and solvothermal methods 39 , 40 , 41 have been generally used to prepare one–dimensional (1-D) mesoporous/microporous NiO materials in nanotube/wires architectural forms. However, electrospinning technique 42 has been used to obtain nanofibres. The two – dimensional (2-D) NiO electrode materials in the form of nanoflakes/sheets/plates/columns and nano slices have been fabricated with the use of microwave/ultrasound assisted synthetic routes 43 , 44 in addition to the use of hydrothermal/chemical precipitation methods. 45 , 46 Y. Wu et al. have examined the effect of calcination temperature on NiO nanoparticles prepared by modified sol-gel method using citric acid and nickel nitrate as ligand and precursor, respectively. 47 The SEM images (Figure 11) indicate the increase in particle size with the increase in calcination temperature from 400 to 550 °C.
![Figure 11:
Effect of increasing calcination temperature [(a) 400, (b) 450, (c) 500, and (d) 550 °C, respectively] on the size of NiO nanostructures.
47
Reproduced with permission from Elsevier, license no. 5877721126065.](/document/doi/10.1515/polyeng-2024-0101/asset/graphic/j_polyeng-2024-0101_fig_011.jpg)
Effect of increasing calcination temperature [(a) 400, (b) 450, (c) 500, and (d) 550 °C, respectively] on the size of NiO nanostructures. 47 Reproduced with permission from Elsevier, license no. 5877721126065.
Furthermore, 3-dimensional (3-D) NiO electrode materials with the unique pleasing appearance as nano–/micro–flowers, nano–/microspheres, nanotube arrays, and hollow–spheres have been synthesized by solvothermal and hydrothermal methods. 48 , 49 , 50 In a unique study, S. Yin et al. have produced flower-like hierarchical 3-D mesoporous NiO for use as electrode material for supercapacitors using an ethanol–assisted hydrothermal method followed by a sintering process. 51 The SEM images (Figure 12) reveals the remarkable changes in morphology of the NiO sample during the progressive increase in hydrothermal time from 20 to 360 min. The most appropriate hydrothermal time was 120 min for obtaining hierarchical NiO which demonstrated excellent SC (678 F/g at 1 A/g) maintaining 94.8 % retention of original capacitance over 5000 cycles.
SEM images of the hydrothermal samples during (a) 10, (b) 30, (c) 60, (d) 120, (e) 240, and (f) 360 min. 51 Reproduced with permission from John Wiley and Sons, license no. 5871420637468.
The obtained 3-D materials have demonstrated higher specific capacitance in comparison to 0-D, 1-D and 2-D structured NiO nanomaterials. Electrochemical performance parameters of 3-D NiO electrode materials listed in Table 3 clearly demonstrate the influence of crystal structure on their supercapacitive efficiency.
Electrochemical performance parameters of 3-D NiO electrode materials prepared in various morphologies.
| Morphology | Surface area (m2/g) | Pore diameter (nm) | Specific capacitance (F/g) | Cyclic stability (% capacitance retention/cycles) | References |
|---|---|---|---|---|---|
| Nanoflower | 159 | 16.7 | 480 | – | 52 |
| Nanospheres | 209.1 | – | 1,201 | 70/500 | 53 |
| Nanotube arrays | 165 | 75–135 | 675 | 93.2/10,000 | 54 |
| Microspheres | 295 | 9.2 | 1,560 | 100/1,000 | 55 |
| Flowers | 135 | 3.4–9.7 | 1,860 | 92/5,000 | 56 |
| Ball-flower | 163.1 | 10.8 | 734 | 82/2,000 | 57 |
| Microspheres | 216 | 64.3 | 710 | 98/2,000 | 58 |
| Nanospheres | 174.1 | – | 982 | 92.6/10,000 | 59 |
| Microflowers | 62.7 | 5–10 | 1,678.4 | 99.7/1,000 | 60 |
| Microstructures | 258.52 | 3.8 | 718 | 94.8/1,000 | 61 |
| Nanospheres | 182 | 2.1 | 603 | 95/1,000 | 62 |
| Hollow spheres | 81 | 5–11 | 600 | 100/1,000 | 63 |
In a few cases, NiO thin films have also been used in supercapacitor applications. 64 , 65 Using the reactive magnetron sputtering technique, A. Kumar et al. have developed NiO nanopyramid thin films on steel substrate 66 for use as binder-free electrode (Figure 13) which displayed high SC (325 F/g at 0.4 mA/cm2) in 1.0 M KOH, efficient ED (19.66 Wh/kg) at PD (2.15 kW/kg), remarkable cyclic stability with 91.4 % capacity retention for 1,000 cycles. The electrochemical performance characteristics of NiO working electrode in three–electrode systems at scan rate (5–100 mV/s) with potential window from −0.3 to +05 versus Ag/AgCl (reference electrode) are presented in Figures 14 and 15.
SEM images of NiO working electrode (a) at 1 μm scale, (b) at 100 nm scale (inset is contact angle image), (c) EDX elemental mapping of NiO working electrode, and (d) AFM image of NiO working electrode (d) at 10 × 10 µm scale, (e) at 2 × 2 µm scale. 66 Reproduced with permission from Elsevier, license no. 5877731116020.
Electrochemical characterization of NiO working electrode: (a) cyclic voltammetry (CV) curves at different scan rates ranging from 5 to 100 mV s¡1, (b) specific and interfacial capacitance calculated from the CV curves as a function of scan rates, (c) galvanostatic charge-discharge (GCD) curves at a different current density ranging from 0.4 to 1.5 mA cm¡2, and (d) specific and interfacial capacitance calculated from the GCD curves as a function of current density. 66 Reproduced with permission from Elsevier, license no. 5877731116020.
(a) Cycling performance at current density 1 mA cm¡2 and corresponding few initial and final GCD cycles, (b) Nyquist plot with a corresponding fitting circuit, and (c) Ragone plot of the NiO working electrode. 66 Reproduced with permission from Elsevier, license no. 5877731116020.
The spray pyrolysis method used by Yadav et al. 67 to fabricate NiO thin film at 450 °C using a suitable substrate exhibited 380 F/g specific capacitance at 1 A/g with residual capacitance retention of 92.1 % for 1,000 cycles. Interestingly, a new film-forming method (known as SILAR) involving successive ionic layer adsorption and reaction has been nicely used by Das et al. to develop NiO nanofilm which exhibited remarkable capacitance (1,341 F/g) at scan rate (2 mV/s). 68 Recently, M. Akhtar et al. 69 have prepared hierarchically porous NiO microspheres and their exfoliated carbon (ExC)-based nanocomposites for supercapacitor applications. The ExC–F/g) at 5 mV/s scan rate with 79 % capacitance retention over 2,000 cycles in comparison to NiO mesoporous particles which displayed specific capacitance (331 F/g) with 50 % capacity retention over 2,000 cycles.
2.2.2 Cobalt oxide (Co3O4)
Cobalt tetraoxide (Co3O4) involving two ionic states (Co2+ and Co3+) has emerged as adorable multifunctional supercapacitor electrode material. The Co3O4 being a mixed oxide has a cubic normal spinal structure with octahedrally coordinated trivalent (Co3+) and tetrahedral coordinated bivalent (Co2+) ions in a 2:1 ratio (Figure 16).
Crystal structure of cobalt (II, III) oxide.
Owing to unique magnetic, electrical, and optical properties, Co3O4 nanoparticles have received a wide range of applicability in nanoscopic electronic and nanosensor fields. Though Co3O4-based electrodes have demonstrated remarkable pseudo–capacitive performance, good reversibility, and high theoretical specific capacitance (over 3,000 F/g), but perishing cyclability and lower ionic conductivity have been their limitations. 70
Cobalt oxide is well well-known antiferromagnetic p-type semiconducting material with direct band gaps extending from 1.48 to 2.19 eV. The simple synthesis routes, strong redox capability, remarkable theoretical capacitance, and high charge storage capacity have made Co3O4 an important electrode material. However, the low conductivity, extensive volume expansion-contraction, strong particle aggregation, and poor cycling performance have been the major drawbacks of Co3O4. Several synthesis methodologies (hydrothermal, solvothermal, co-precipitation, chemical bath deposition, etc.) have been adopted to prepare desired Co3O4 nanostructures. 71 , 72 , 73 Among these, the hydrothermal method has been the most popular to produce nanocomposite with superior electrochemical outputs. According to the report of S. Kalathaya et al. 74 the maximum SC (F/g) delivered by Co3O4 nanocomposite electrode materials synthesized by different methods was in the decreasing order as hydrothermal > chemical – bath deposition > coprecipitation > solvothermal. The Co3O4 synthesized by Zhu et al. 75 in the form of microspheres via hydrothermal route exhibited SC (879 F/g) whereas Co3O4 thin films produced by Tian et al. 76 through the chemical bath deposition method displayed SC (743 F/g). Further, in an interesting study, Jennifer et al. 77 examined the structural, morphological (SEM images), and electrochemical properties of Co3O4 electrode material prepared at different temperatures by use of hydrothermal method (Figure 17). It is evident from Figure 17 that the structural morphology and the electrochemical behavior (area under CV curves at different scan rates) of Co3O4 vary with temperature and the Co3O4 electrode material prepared at 250 °C delivered the highest capacitance (215 F/g) and low series resistance.
Structural morphology and the electrochemical behavior of Co3O4. (A) SEM images of Co3O4 (i) at low temperatures, (ii) 200 °C, (iii) 250 °C, and (iv) 300 °C. Cyclic voltammetry of Co3O4 at (B) 200 °C, (C) 250 °C, and (D) 300 °C under pH = 7, 6, and 11 (E–G). 78
The designed Co3O4 nanostructures used as electrodes so far exist in all zero to 3-dimensional (0-3D) shapes such as mesoporous/nanoporous and nanoclusters (0-D); nanorods/wires/tubes and fibres (1-D); thin films/nanodiscs and nanoplates (2-D) and nano coils/balls/pillars and nanoflowers (3-D). 79 , 80 The 3-D enoki mushroom-like structures of Co3O4 have been reported by F. Luo et al. and investigated for their pseudo-capacitive properties 81 in the form of one – dimensional nanowires which delivered SC (787 F/g) at current density (1 A/g) in 6.0 M KOH electrolyte maintaining 94.5 % of initial capacitance for 1,000 deep cycles. The probable chemical route adopted for the preparation of enoki mushroom-like Co3O4 hierarchitectures is illustrated in Figure 18 whereas the SEM and TEM images showing different morphological architectural shapes are presented in Figures 19 and 20.
Schematic illustration for the formation of 3D enoki mushroom-like cobalt oxide hierarchitecture. 81 Reproduced with permission from Elsevier, license no. 5877750521967.
FE-SEM images of the 3D enoki mushroom-like Co3O4 hierarchitectures. 81 Reproduced with permission from Elsevier, license no. 5877750521967.
TEM images of the 3D enoki mushroom-like Co3O4 hierarchitectures). 81 Reproduced with permission from Elsevier, license no. 5877750521967.
The asymmetric supercapacitor device constructed with the use of Co3O4–electrode as a positive electrode and carbon electrode as a negative electrode displayed excellent electrochemical performance with the delivery of ED (23.9 Wh/kg) and PD (0.375 kW/kg) at 0.5 A/g current density. The discharging curves (Figure 21a) of asymmetric supercapacitors in 6 M KOH at different current densities in the potential range (0–1.5 V) and the corresponding Ragone plot (Figure 21b) support the improved electrochemical features of 3-D enoki mushroom-like Co3O4 hierarchitectures as marvelous electrode material for supercapacitor usage.
Electrochemical performance of 3-D enoki mushroom-like Co3O4 hierarchitectures. (a) Discharge curves of the asymmetric supercapacitor at different current densities and (b) the corresponding Ragone plot. 81 Reproduced with permission from Elsevier, license no. 5877750521967.
The relationship between dimensional morphology and (a) maximum SC, (b) maximum ED, and (c) maximum PD in the case of Co3O4 nanostructures has been reported 74 to be in the following orders:
Thus, 3-D structured Co3O4 nanocomposites have shown the best electrochemical performance probably due to vast accessible surface area, high porosity to provide easy mobility of charged particles, enhanced conductivity, and the variation in structural shapes.
2.2.3 Manganese oxide (MnO2)
Manganese (IV) oxide (MnO2) is a naturally abundant, eco–friendly, and low-cost pseudocapacitive electrode material that possesses excellent energy storage capacity in neutral electrolytes, wide potential range (0.9–1.0 V), long cycling life–span, high power density, effective Faradaic action and adequate theoretical capacitance (1,370 F/g) due to the single electron redox reaction of each Mn atom. The electrochemical efficacy of MnO2 strongly depends upon its micro/nano structural porosity surface, architectural morphology and electroactive surface area. MnO2 82 exists in different crystallographic structural phases (α-, β-, γ-, δ- and ʎ-MnO2) as shown in Figure 22 and displaying the specific capacitances values in the order: α- > δ- > γ- > ʎ- > β-MnO2 as evident from Figures 22 and 23, respectively. 83 , 84
MnO2 (a) 3D structure and top view of MnO2. (b) Morphology of the different crystalline phases of MnO2. 83 Reproduced with permission from Elsevier, license no. 5877751114920.
The specific capacitance of α-, α (m)-, β-, γ-, δ-, and λ-MnO2 electrodes in 0.1 M Na2SO4 at 0.5 mA cm−2 between 0 and 1.0 V versus SCE. 84
While chain-type one-dimensional tunnel structures are demonstrated by α-, β- and γ-MnO2, the sheet/layered two – dimensional structure is exhibited by δ- type MnO2, and the three-dimensional mesh structure is displayed by ʎ- MnO2. 85 In different crystallographic forms, MnO2 is found in various minerals like hollandite (α-MnO2), pyrolusite (β-MnO2), nsutite (γ-MnO2), birnessite (δ-MnO2), and akhtenspite (ʎ-MnO2).
The multiple oxidation states (+2 to +7) of manganese ions influence the specific capacitance of MnO2–based electrodes. Overall, the theoretical specific capacitance trend for NiO, Co3O4, and MnO2 is in the order Co3O4 > NiO > MnO2. 86 The low-ranking cyclability, inferior structural stability, poor ion diffusion capacity, low porosity, electrolyte-mediated dissolution tendency, and ease of agglomeration susceptibility are the main drawbacks of MnO2. 87 To prepare MnO2 magnetic nanoparticles, different synthetic techniques such as chemical precipitation, microemulsion, thermal decomposition, sol-gel, room temperature solid reaction, microwave-assisted synthesis, electrolytic deposition surfactant mediated synthesis and hydrothermal have been successfully utilized. 88 , 89 , 90 , 91 Depending upon the synthesis procedures, MnO2 in various morphologies of MnO2 nanostructure materials have been developed. 92 From Figure 24, the effect of the morphology of nanosized MnO2 particles on their features is evidenced. The synthesis steps involved during the formation of urchin-like MnO2 structures and their TEM images are presented in Figures 25 and 26, respectively.
SEM images of some nanostructured MnO2 materials exhibiting various morphologies. 93
Schematic representation of the synthesis process of α-MnO2 urchin-like structures. 93
TEM images of urchin-shaped α-MnO2 nanoarchitecture (a) and magnification of individual nanoneedles (b). 93
2.3 Conducting polymers
One of the most attractive events of the last two decades is the discovery of conducting polymers (CPs) which are capable of providing considerable electrical conductivity through electrons in their lattice structure. The electrically conducting polymers are attractive due to their reasonable thermal resistance, good mechanical flexibility, easy processability, high electrical conductivity, low toxicity, electrochemical reversibility, and swift switching properties. Since the backbone redox sites of the polymers are not sufficiently stable for manifold repeated charge-discharge processes, CPs exhibit lower cyclic performance. The fascinating feature of CPs is their use as electrode material in both EDLCs and PCs. 94 Compared to conventional polymers, CPs offer superior intrinsic conductivity (up to 500 S/cm) in the doped state, lower band gap (1–3 eV), rapid charging/discharging kinetics, and faster doping/de-doping process but inferior cyclic stability. 95 Among various organic CPs [polyacetylene, polythiophene, para phenylene, polyaniline (PAn), polypyrrole (PPy), and poly (3,4-ethylenedioxythiophene, PEDOT)], the more frequently used polymers for supercapacitors usage have been PAn, PPy, and PEDOT.
These three CPs (PAn, PPy, and PEDOT) have received considerable attention for use in energy storage devices because of their favorable electrochemical properties like facile synthesis, morphological flexibility, affordable cost, chemical endurance, reasonable power density, biocompatibility, high theoretical specific capacitance and useful electronic conductivity in doped state. 96 However, these suffer from low mechanical adaptability and transient cyclic life. To improve mechanical strength, polytetrafluoroethylene (PTFE) and polyvinylidene fluoride (PVDF) as inert thermoplastic polymers have been generally used as binders in polymer technology. These polymers become capable of storing charges after an effective doping process. There are two types (n- and p-) of doped polymers. From a supercapacitor point of view, both n-doping (i.e. reductive doping) and p-doping (i.e. oxidative doping) are important as both types of CPs operate under unidentical potential ranges (Figure 27). Thus, by coupling the positive potential window of p-type polymers with a relatively negative potential window of n-type polymers, the maximum cell working potential window for asymmetric supercapacitors can be achieved.
Illustration of the potential window of hypothetical supercapacitor based on n- and p-conducting polymers. 12 (A) Potential window (p-CPs) (B) Potential window (n-CPs).
The p-doping involves the release of electrons whereas n-doping generates a net negative charge. It has been reported that p-doped polymers exhibit better structural stability against degradation in comparison to n-doped polymers. While PEDOT can undergo both p- and n-doping, PAn and PPy support only p – doping. In this review, the main focus is on the use of PAn, PPy, and PEDOT-embedded binary (CP–magnetic MO) and ternary (CP–CM–magnetic MO) composite electrode materials for supercapacitor applications. Therefore, each conducting polymer is briefly described below.
2.3.1 Polyaniline (PAn)
PAn, first synthesized in 1886 is an important intrinsically conducting polymer with excellent pseudocapacitance. Due to its dark pigment color, it is also referred to as “aniline black”. Oxidative and electro-polymerization methods have been frequently utilized to synthesize PAn. PAn consisting of quinoid and benzenoid rings can exist in three different redox states to achieve considerable surface charge potential during conversion from one oxidation state to an alternate state. The three identified PAn forms are leucoemeraldine base (fully reduced form), pernigraniline base (fully oxidized form), and (emeraldine base/salt half oxidized/half reduced) (Figure 28).
Polyaniline in different oxidation states and their polaronic forms. 21
Among these forms, while leucomeraldine and pernigraniline are non-conducting, emeraldine is conducting. Furthermore, the doped emeraldine salt is highly enriched conductive form of PAn. 97 PAn is very useful pseudocapacitor material for electrochemical energy storing devices due to its nontoxicity, good flexibility, high electrical output, reasonable thermal stability and high theoretical specific capacitance (≈1,200 F/g). However, structural destruction during charging/discharging operations and poor cyclability have been the major drawbacks of PAn. Such demerits of PAn have been addressed through converting PAn into ordered nanostructures like nanorods and nanoparticles. Additionally, nanocomposites with improved electrochemical performance, have been produced through incorporation of metal oxides and/or carbon materials into PAn nanostructured matrix. 98
2.3.2 Polypyrrole (PPy)
It is an important p-type intrinsically conducting polymer for pseudocapacitor application owing to its promising qualities including fantastic conductivity in a doped state. It received popularity as a conductive material after synthesis by electropolymerization of pyrrole monomer in 1979. 99 Due to its considerable conducting nature, PPy has been termed as an organic metal/metallic polymer. 100 According to the literature, PPy exists as conducting salt, and deprotonation reaction is feasible after treatment with base. It has been proposed that the molecular structure of deprotonated PPy could encapsulate both reduced and oxidized forms of pyrrole subunits. The enhancement in pseudocapacitive efficiency of PPy by various chemical doping approaches has been recently reported. 101 PPy in various structural forms (films, wires, sheets, nanospheres, etc.) have been developed following different synthetic strategies. Among various nanostructures, nanosheet architecture exhibited the best specific capacitance. The synthesis of PPy by electropolymerization of pyrrole monomer is represented in Figure 29 12 .
2.3.3 Poly [(3,4-ethylenedioxythiophene), PEDOT]
Out of three main CPs (PAn, PPy and PEDOT), PEDOT: PSS and PEDOT are chronologically youngest CPs. Since the first report on PEDOT in 1988 by Bayer AG, it has been synthesized in different architectural structural designs like nanotubes, flexible fibres, nanospheres, etc. using chemical oxidation, vapor–phase, and electrochemical polymerization techniques. As PEDOT is not conveniently processable, it was paired with an anionic poly (styrene sulfonate) polymeric chain (abbreviated as PSS) in 1990 to obtain PEDOT: PSS dispersion (Figure 30) with conductivity (900–1,000 S/cm). PSS was considered to act both as a stabilizer and dopant. As a versatile polymer, PEDOT has received broad-based applications in capacitors, touch screens, organic solar cells, light-emitting diodes, and printed electronics. 102
Structures of PSS, PEDOT, and PEDOT: PSS.
Like PAn and PPy, the PEDOT and PEDOT: PSS polymers have been well characterized using spectroscopic (FT–IR, UV–Visible) and chromatographic (gel permeation chromatography) techniques. The super capacitive performances (specific capacitance, power density, cyclability, and specific energy) of these polymers and their composites with MOs and/or carbon materials as electrode materials have been extensively investigated by the use of Fourier transform infrared–attenuated total reflection spectroscopy (FTIR–ATR), scanning electron microscopy–energy dispersion X-ray analysis (SEM–EDX), Raman spectroscopy, Brunauer–Emmett–Teller (BET) surface analysis, thermogravimetric (TGA/DTA) analysis, cyclic voltametric (CV), galvanostatic charge/discharge (GCD) and electrochemical impedance spectroscopy (EIS) analysis before utilizing as electrode material. The main advantages and disadvantages of CPs as electrode material are briefly listed in Table 4.
Significant advantages and disadvantages of PAn, PPy, and PEDOT as electrode material for supercapacitors. 97 , 103 , 104 , 105 , 106 , 107
| Polymer | Advantages | Disadvantages |
|---|---|---|
PAn  |
(i) Easy synthesis and processability (ii) High theoretical pseudocapacitance value (1,200 F/g) due to multiple redox states (iii) Thermally stable intrinsic conducting polymer (iv) High conductivity in the doped state due to lowering in the band gap (v) Good electroactivity (vi) Unique structures with enhanced surface area and improved conductivity |
(i) Only p-type conducting polymer (ii) Poor stability due to structural damage of the main chain during long–term charging/discharging (iii) Slow ion–transfer during redox reaction (iv) Poor cyclic stability (v) The necessity of protic ionic solvents for complete charging/discharging |
PPy  |
(i) High electrical conductivity (>103 S/cm) and excellent stability in oxidized form (ii) Prominent energy density and remarkable volumetric capacitance (iii) Fast charging/discharging capability (iv) Marvelous biocompatibility and thermal stability (v) Superb mechanical robustness and chemical resistance (vi) Easy synthesis, fabrication, and favorable redox properties |
(i) Only p-doped polymer (ii) Possible growth of dense/thick PPy layer on current collector leading to the decrease in capacitance value |
PEDOT  |
(i) Both n- and p-type polymers (ii) Admirable stability of p-doped PEDOT against air and humid environment (iii) Exceptional electro-optical properties due to optical transparency in the conducting state (iv) Broad negative potential window (v) Easy conversion into attractive green/blue thin films (vi) Promising electrical conductivity range |
(i) Low specific capacitance (ii) Poor solubility (iii) Requirement of ionic liquid solvents/organic gel electrolyte for better electrochemical performance |
3 Magnetic metal oxide: conducting polymer nanocomposites for supercapacitor application
In this review, our main aim is to epitomize the most recent research developments in the field of supercapacitor technology related to the use of magnetic metal oxide (MMOs) supported conducting polymeric hybrid materials in different nano-structured forms. Magnetic metal oxides, due to their high specific capacitance have been considered useful for use in supercapacitors but their poor energy density has created a major problem for their wide spectrum adoption. However, by introducing MMOs (NiO, MnO2, Co3O4, RuO2, V2O5) into a polymeric matrix, the problem of low energy density has been addressed to a certain extent. The binary MMOs (MnO2, NiO, Co3O4) exhibiting large energy/power density are thus capable of improving energy density and specific capacitance of supercapacitors. Thus, combining the advantageous properties of polymers (flexibility, layer compatibility, and toughness) and MMOs (durability and hardness), MO–CP nanocomposite materials displaying significantly improved electrochemical properties (specific capacitance, cyclic stability, ionic conductivity, energy/power density) have been developed for supercapacitor applications. Further, a third component (carbon substance) has been prominently added into MMO–CP, composites to further improve the electrochemical performance. Thus, the nanocomposites consisting of MMO, CP, and carbon matter have been widely used in supercapacitor applications as electrode materials. The nanocomposites (MMO–CP and MMO–CP– additional component) markedly differ in their properties (melting point, color, surface morphology, interfacial interaction, magnetism, and charge capacity) according to the compositional proportionality of constituting components. According to the literature, CP – MO nanocomposite, prepared by doping MO into CP has shown better photo-sensing and electrochemical performance compared to a single component (MO or CP) alone. 108 In general, the magnitude of specific capacitances delivered by MO, CP, carbon matter and MO – CP nanocomposite have been in the order of MO–CP > MOs > CPs > carbon matter. In fact, CP – MO composites (CP–MnO2, CP–Co3O4, CP–NiO) have shown much better capacitance compared to individual MO or CP. 12 In ternary composites, CNTs, porous/mesoporous carbon, carbon nanofibers, activated carbon, rGO/GO, graphene in the form of nanoribbons, sheets/platelets, carbon paper, and sulfonated graphene have been generally used as a third component along with CP and MMO. 103 , 109 , 110 , 111 , 112 , 113 Despite the superiority of ternary nanocomposites, numerous binary nanocomposites consisting of MMO (NiO, MnO2, or Co3O4) and different forms of carbon have been synthesized in the recent past to use as promising magnetic materials for fabricating high-performance supercapacitors 3 , 9 , 114 , 115 , 116 , 117 which have demonstrated excellent electrochemical behavior due to fast redox reactions between ions and electrons in association with the synergistic affinity between both components. B. R. Sankpal et al. 118 have used a novel cost-effective “SILAR” method for anchoring Co3O4 nanoparticles onto the surface of MWCNTs. The resulting Co3O4/MWCNTs nanocomposite electrode displayed remarkable electrochemical performance in 2.0 M KOH electrolyte at scan rate (5 mV/s) revealing SC (685 F/g), cyclic stability (73 % for 5,000) cycles, specific energy (16.41 Wh/kg) and specific power (300 W/kg).
The scattered research work reported during the last seven years on the development of CPs (PAn, PPy, and PEDOT) – MMO (MnO2, NiO, and Co3O4) composite materials and their applications in supercapacitors has been succinctly summarized in Tables 5–7. The electrochemical performance data presented in these tables on CPs–MMOs composite electrode materials with/without the use of a third additional component admirably provide a succinct account of their technological utility in green energy storing/conversion systems.
PPy containing MMO-based nanocomposite electrode materials.
| Composition | Performance parameters SC (F/g)/ED (Wh/kg)/PD (W/kg) | Electrolyte | Remarks | References |
|---|---|---|---|---|
| PPy/Functionalized carbon nanofibres (F-CNFs)/MnO2 | SC (409.88) at current density (1 A/g) with capacitance retention of 86.3 % over 3,000 cycles at 2 A/g current density displaying ED (42.53) and PD (297.35) | 1.0 M KCl | The developed ternary functionalized carbon nanofibres (CNFs)/PPy/MnO2 nanocomposite has been utilized for fabricating high-performance supercapacitor electrode which exhibited very low resistance of charge transfer (RCT) value due to its unique structure involving randomly distributed PPy granular particles and spherical MnO2 nanoparticles on the surface of F-CNFs. The results indicated the super hydrophilic nature of F-CNFs | 133 |
| MnO2@MoS2/PPy | SC (490) at a current density of 1.0 A/g with excellent 90 % cyclic stability for 1,000 cycles | – | Development of MnO2@MoS2/PPy ternary composite through a combination of simple oxidation and hydrothermal methods using MnO2@MoS2 sheet as the substrate and PPy as conducting binder material. The as-prepared ternary composite used as an electrode for pseudocapacitor delivered superior performance due to the synergistic effect of all three constituting components leading to enhanced redox reactivity | 134 |
| NiO@N-MWCNT/PPy | SC (395) at a current density of 0.5 A/g with capacitance retention of 90 % after 5,000 cycles | 2.0 M KOH | Synthesized NiO@N-MWCNT/PPy composite by thermal reduction approach displayed remarkable electrochemical performance due to efficient synergistic effect between hexagonal crystal structured NiO and N-MWCNT/PPy composite | 135 |
| Co3O4@PPy/Ag | The fabricated supercapattery delivered ED (24.79) and corresponding PD (554.4) at a current density of 0.7 A/g with capacity retention (153.67 %) over 3,000 cycles | 1.0 M KOH | The oxidative chemical polymerization and hydrothermal methods in combination were used for the synthesis of ternary Co3O4@PPy/Ag nano-composites through incorporating PPy with hydrothermally produced Co3O4 nanograins and Ag nanoparticles for use as positive electrode material in the fabrication of supercapattery | 136 |
| MnO2 / rGO/PPy | Superior capacitance conservation (94.7 %) for rGO/MnO2/PPy after 1,000 cycles than other synthesized composites like rGO/MnO2*/PPy (50 %), rGO/MnO2* (74.01 %) and rGO/MnO2 (68 %) | 1.0 M H2SO4 | Out of different synthesized binary (rGO/MnO2, rGO/MnO2*), and ternary (MnO2/rGO/PPy and MnO2*/rGO/PPy) electrode materials using activated (MnO2*) and non-activated (MnO2), the SC value (285.91 F/g at 1 mV/s) of rGO/MnO2/PPy in two – electrode system was 7.67, 9.53, 7.34 and 21.22 times higher than rGO/MnO2, rGO/MnO2*, rGO/MnO2*/PPy and Ppy, respectively. The cyclic voltammetric behavior of symmetric supercapacitor fabricated using binary nanocomposite as positive electrode and ternary-composite as negative electrode was examined at different scan rates (10–100 mV/s) in the potential range (0.0–0.8 V). The spectroscopic studies showed that all composites have compact surfaces with uniform distribution of rGO and accumulation of MnO2 and PPy along the edges of rGO nanosheets | 137 |
| NiO/PPy-6 | SC (3,648.6 at 3 A/g) with a high rate capability of 1,783 F/g at 30 A/g current density | – | Synthesis of NiO/PPy – 6 (NiO: PPy molar ratio, 6) via embedding NiO microspheres with fish-scale type structured PPy and use as electrode material for symmetric supercapacitor applications. Further, the NiO/PPy – 6 was also used as a positive electrode in combination with activated carbon as a negative electrode to construct an asymmetric supercapacitor (NiO/PPy – 6//AC) which displayed excellent specific capacitance (937.5 F/g), high power (2,399.99 W/kg) and energy (333.3 Wh/kg) densities at 3 A/g | 138 |
| MnO2/PPy/CB (carbon black) | SC (273.2)/ED (0.5513)/PD (91.556) | LiCl/PVA | The ternary composite comprising of CB, Mn (IV) oxide (MnO2), and PPy (1:1:3 ratio) showed the highest values of specific capacitance, (273.2 F/g at 1 mV/s), energy (0.5513 Wh/kg) and power (91.556 W/kg) densities at 6 mV/s. The composite (composition 1:1:5) displayed maximum cyclic stability with 86 % capacity retention for 5,000 cycles in LiCl/PVA electrolyte | 139 |
| MnO2/PPy//Ti3C2Tx | Areal capacitance (61.5 mF/cm2) and ED (6.73 µ Wh/cm2) displayed by AMSC | – | A flexible asymmetric micro supercapacitor (AMSC) based on Ti3C2Tx (titanium carbide)//PPy/MnO2 revealing very high energy density was developed using Ti3C2Tx coated graphitic paper (GP) as negative electrode and successively deposited MnO2 and PPy on GP as positive electrode | 140 |
| Co3O4 nanowires @ PPy-MnO2 | SC (215 at 0.5 A/g)/ED (41.3)/PD (4,348) with 96.8 % capacitance retention for 1,000 bending and twisting cycles | – | Fabrication of flexible solid-state supercapacitor (FSSC) using well – architectured 3D Co3O4 nanowires @ MnO2 – PPy hybrid nanoflake electrode for practical application in wearable and portable electronics. The PPy – MnO2 nanoflakes grown – up on Co3O4 nanowires (vertically matured on carbon fibres) facilitated fast ion/electron transfer through active electrode material resulting in high specific capacitance of developed FSSC | 141 |
| MnO2/PPy/C3N4 | SC (509.4)/ED (63.9)/PD (2,000) | 1 M aqueous Na2SO4 | An asymmetric supercapacitor constructed with the use of cyanide nitrogen (C3N4)/PPy/MnO2 as a cathode and AC as anode exhibited high energy density (63.9 Wh/kg), power density (2,000 W/kg) and excellent cycling performance with capacity retention of 95.7 % after 5,000 charge-discharge cycles | 142 |
| MnO2/PPy/CC (carbon cloth) | SC (270 at 1 A/g)/ED (165.3)/PD (21.0 at an energy density of 86.4 Wh/kg) | – | Development of PPy/MnO2/CC flexible supercapacitor demonstrating remarkable energy density, extended operating voltage range (0–2.1 V), improved cyclability with 92.1 % capacity retention after 3,000 cycles, and outstanding rate capability (141 F/g at 20 A/g) | 143 |
| NiO/PPy/graphene (G) | SC (970.85)/ED (33.71)/PD | 6 M KOH | Hybrid NiO/G/PPy ternary nanocomposite synthesized through the combination of co-precipitation, heat treatment, and in-situ chemical polymerization methods was used to assemble a fully symmetric cell. The electrochemical performance data of the cell, within 0–2 V potential window showed high specific capacitance (66.17 F/g) and energy density (36.76 Wh/kg) | 144 |
| Co3O4/PPy@N-doped MWCNT | SC (872 at 0.5 A/g) with 96.8 % original capacitance retention over 10,000 cycles | KOH | The hexagonally structured nanocomposite (Co3O4/PPy @ N – MWCNT) prepared by the ultrasonication-mediated solvothermal method was used as a promising material for the fabrication of supercapacitors and glucose sensing devices | 145 |
| MnO2/PPy @ Ni foam | Areal capacitance (59.29 mF/cm2)/ED (42.99–77.94 µWh/cm2)/PD (0.272–6.818 mW/cm2) performance parameters displayed by asymmetric supercapacitor (Ni foam –PPy//Ni foam – MnO2) | LiClO4 | Development of a novel method for fabrication of Ni-foam based hybrid asymmetric planar micro – supercapacitor (Ni-foam/MnO2//Ni foam/PPy) for use as energy storing device which demonstrated excellent cyclic stability (95.6 % initial capacitance retention over 10,000 charge/discharge cycles) | 146 |
| NiO/PPy | SC (679 at 1 A/g)/ED (94.4)/PD (500.74) | 0.1 M LiClO4 | Preparation of highly porous NiO/Ppy nanocomposite following electrochemical deposition method for use as the electrode material to develop efficient supercapacitors exhibiting high cyclability with capacitance retention of 83 % for 1,000 cycles at 1 A/g | 147 |
| NiO-CoO/PPy | SC (1,123 at 1 A/g) with cyclic stability (90.1 % for 5,000 cycles) | 2 M KOH | Synthesis of NiO–CoO/Ppy composite nanosheets onto carbon cloth to use as a supercapacitor. As a cathode in asymmetric supercapacitor assembly in combination with AC as anode, it demonstrated excellent performance displaying energy (35.9 Wh/kg) and power (801 W/kg) densities | 148 |
| MnO2@ PPy @ N – doped porous carbon nanofibres (NPCNFs) | SC (595.77) with excellent cyclic stability (96.2 % capacitance retention for 1,000 cycles)/ED (9.36)/PD (1,000) | 6.0 M KOH | Synthesis of multicore-shell ternary nanocomposite (MnO2 @ PPy @ NPCNFs) possessing excellent electrochemical properties for fabrication of high-performance supercapacitors. The unique structural morphology revealed the appearance of a large number of beautiful flowers-like spherically shaped MnO2 nanoparticles onto the outer layer of the synthesized multicore-shell ternary composite | 149 |
| PPy@ MnO2 – 3 (KMnO4 loading of 300 g) | SC (713 at 1 A/g) with 92 % retention after 5,000 cycles at current density (4 A/g)/ED (40.8)/PD (720) | 3.0 M KOH | The PPy @ MnO2 in the form of hollow mesoporous nanocomposite was synthesized by low – temperature redox reactions and used as a positive electrode in a combination of activated carbon (AC) as a negative electrode to construct PPy @ MnO2//AC asymmetric supercapacitor device which exhibited high energy density (40.8 Wh/kg) at a power density of 720 W/kg | 150 |
| PPy/Ni – foam (NiF)/C – Co3O4 | SC (1,176 at 20 mV/s) and (695 at 0.5 A/g)/ED (34.44) at PD (1,100) with 93.88 % retention of original capacitance over 8,000 cycles | 4.0 M KOH | A green pseudo-sol-gel method involving the use of the aqueous extract of plant leaves was developed for the synthesis of microporous carbon – film coated Co3O4 (C – Co3O4) nanoparticles followed by electro polymerization of conducting PPy polymer on Ni – foam/C – Co3O4 to obtain PPy/NiF/C – Co3O4 electrode material for fabricating symmetric supercapacitor which exhibited high rate capability with potential window 1.1 V. The deposition of a thin PPy monolayer onto NiF/C – Co3O4 resulted in the enhancement of specific capacitance (221 F/g) of C – Co3O4 @ NiF composite to the specific capacitance (695 F/g) for PPy/NiF/C–Co3O4) composite at 0.5 A/g | 151 |
| MnO2/PPy @ MnOOH nanowire arrays (NWAs) | Areal capacitance (1.62 F/cm2 at 2 mA/cm2) in voltage window (0–1 V) with a retention rate of 92.1 % for 8,000 cycles, better than that of MnOOH (63.3 %) | CMC – Na2SO4 gel | Development of MnO2/PPy @ MnOOH NWAs nanocomposite with core-shell hierarchical one-dimensional (1D) structural configuration and its use as a cathode in the combination of Fe2O3/PPy hybrid nanosheets (3-D porous network) as the anode (areal capacitance, 1.68 F/cm2 at 2 mA/cm2 in negative voltage window) to fabricate flexible all – pseudo capacitive asymmetric (MnO2/PPy @ MnOOH NWAs//Fe2O3/PPy) supercapacitor. The assembled ASC demonstrated maximum volume energy density (2.66 m Wh/cm3) at power density (19.72 mW/cm3) with volumetric capacitance (4.92 F/cm3) in a stable voltage window of 2 V and 90.6 % capacitance retention over 10,000 cycles in CMC-sodium (CMC-Na2SO4) gel electrolyte. This study utilized the better conductivity of MnOOH (10−4 – 10−5 S/cm) compared to MnO2 (10−5 – 10−6 S/cm) | 152 |
PAn containing MMO-based nanocomposite materials.
| Composition | Performance parameters SC (F/g)/ED (Wh/kg)/PD (W/kg) | Electrolyte | Remarks | References |
|---|---|---|---|---|
| PAn/NiO | SC (362 F/g), ED (50.2 Wh/kg), PD (0.5 kW/kg) and Coulombic efficiency (70.8 %) at current density (1 A/g) | 1.0 M H2SO4 | Preparation of microporous structured PAn/NiO core/shell multifunctional binary nanocomposite consisting of PAn shell on NiO core where each core/shell particle has a single NiO particle and the PAn shell evenly encapsulated the core. CV – GCD studies between −0.6 and 1 V at different scan rates (20–100 mV/s) and the experiments at current densities (1–4 A/g) between 0 and 1 V were performed | 153 |
| MnO2/graphene (G)/PAn | Areal SC (3.5 F/cm2 at 5 mA/cm2) with capacity retention (90 %) for 1,000 bending (from 0o to 180o) cycles/volumetric ED (5.2 mWh/cm3)/PD (8.4 mW/cm3) | 1.0 M H2SO4 | Synthesis of flexible three-dimensional hierarchical structure PAn/G/MnO2 composite paper through layer-by-layer in-situ growth method using printing paper as the scaffold to fabricate free-standing hybrid electrode which exhibited high mass loading (11.75 mg/cm2) of active material. The all-solid-state supercapacitor based on the as-prepared electrode had an excellent electrochemical performance. Fortunately, eight supercapacitors when connected in series were capable of lighting – up a green light emitting diode of 3 V | 154 |
| Co3O4/PAn NCs | SC (1,301 at 1 A/g) with superior cyclic stability (90 % capacitance retention capability over 2,000 cycles) | – | Development of a new method for synthesis of hierarchically cavern Co3O4/PAn nanocages (NCs) electrode materials for fabricating symmetric as well as asymmetric supercapacitors. Compared to Co3O4 NCs, Co3O4/PAn NCs electrode demonstrated better electrochemical performance with enhanced electrical conductivity and cyclability. The asymmetric supercapacitor assembly consisting of Co3O4/PAn NCs as positive electrode and AC as negative electrode has demonstrated remarkable supercapacitive properties (energy density, 41.5 Wh/kg at 0.8 kw/kg; power density, 15.9 kw/kg at 18.4 Wh/kg) | 155 |
| NiO/PAn: PSS | SC (834 at 1 A/g) with remarkable cycling stability (88.9 % capacitance retention over 3,000 cycles) | – | The hierarchically structured binary nanocomposite (NiO/PAn: PSS) was prepared by dry-spraying method using highly porous NiO nanosheets and PAn: PSS as starting materials. The prepared nanocomposite where PAn acted as conductor and spacer between NiO sheets and cross-linked PAn: PSS as binder exhibited admirable performance in supercapacitor application. Additionally, NiO/PAn: PSS (positive electrode) and activated carbon (negative electrode) combination used to fabricate asymmetric supercapacitors displayed exceptional performance with high energy density (32.84 Wh/kg), excellent power density (375 W/kg) and remarkable cyclic life – span | 156 |
| MnO2/PAn/MWCNT | Display of specific energy (190 Wh/kg at 1 mA/cm2) and 78 % capacitance retention by ASC device for 2,000 cycles | Synthesis of highly porous coaxial MWCNT/PAn-MnO2 ternary nanocomposite through wrapping of MWCNT by a layer of MnO2 dispersed in PAn for use as positive electrode in combination with MWCNT as negative electrode to construct an asymmetric supercapacitor (ASC). The resulting ASC device exhibited excellent cyclability, rate capability, and specific energy | 157 | |
| MnO2/PAn/hollow mesoporous silica | SC (428.6 at 4 A/g), reaching to 485 F/g after 3,000 cycles | 6 M KOH | Synthesis of flower-like structured ternary nanocomposite comprising of PAn, hollow mesoporous silica, and MnO2 for use as electrode material to fabricate an all-solid-state asymmetric supercapacitor which exhibited high specific capacitance (248.5 F/g at 1 A/g), improved energy density (88.4 Wh/kg at 800 W/kg power density) and remarkable cyclability with 97.7 % capacitance conservation for 5,000 cycles | 158 |
| PAn@MnO2 @ PCNF | SC (289) with good cycling stability (91 % capacitance retention for 1,000 cycles) | 1 M H2SO4 | Development of binder-free PAn @ MnO2 @ porous carbon nanofibres (PCNF) nanocomposite via chemical polymerization of PAn on MnO2 @ PCNF composite for use as electrode material in supercapacitors. The fabricated asymmetric cell configuration (PAn @ MnO2 @ PCNF//PCNF) demonstrated excellent cyclic stability (86 % capacity retention for 5,000 cycles and improved densities of energy (119 Wh/kg) as well as power (322 W/kg) | 159 |
| NiO/PAn/Sulfonated graphene | SC (1,350 at 1 A/g) with conservation of 92.23 % original capacitance over 5,000 cycles | 6 M KOH | Synthesis of core-shell structured electrode material consisting of PAn, sulfonated graphene (as substrate), and uniformly – dispersed NiO particles using hydrothermal and chemical oxidation polymerization processes and its use in developing all solid–states asymmetric PAn/NiO/sulfonated graphene//AC supercapacitor which demonstrated admirable specific capacitance (308.8 F/g), superior energy density (109.8 Wh/kg), excellent power density (0.8 kW/kg) and high cyclability, retaining 91.15 % initial capacitance for 10,000 cycles | 160 |
| Co3O4 – PAn@ ZIF-8NPC (nanoporous carbons) | SC (1,407 at 1 A/g) with excellent cycling performance and rate efficiency | KOH | Synthesis of Co3O4-PAn @ zeolitic imidazolate framework – 8 (ZIF – 8) nanocomposite for use as positive electrode with ZIF-8 nanoporous carbon as negative electrode to construct asymmetric supercapacitor which exhibited exceptional electrochemical activities (energy density = 52.81 Wh/kg at 751.51 W/kg power density) and cycling performance of retaining 88.43 % original capacitance over 10,000 cycles at 10 A/g) | 161 |
| NiO/PAn | SC (480 at 10 mV/s) | – | Synthesis of NiO nanoparticles filled PAn nanocomposites using chemical oxidative polymerization process, characterization, and examination of their electrochemical performance | 162 |
| MnO2/PAn | PAn-grafted MnO2: SC (417 at 5 mV/s scan rate) with ED (11.4) at PD (875) and PAn – coated MnO2; SC (271 at 5 mV/s scan rate) with ED (7.2) at PD (280) | 1 M H2SO4 | Out of two different types of nanocomposites (a) PAn-coated MnO2 and (b) PAn-grafted MnO2 developed for supercapacitor applications, PAn-grafted MnO2 composite demonstrated better performance with the retention of 96.4 % of initial capacitance after 2,000 cycles in high-performance energy storing devices | 163 |
| CF@ ˠ -MnO2/PAn | SC (654.3 at 1 A/g) with retaining about 76 % over 4,000 cycles | 0.2 M H2SO4 | The ternary nanocomposite material (CF@ ˠ -MnO2/PAn) prepared under hydrothermal conditions via in-situ polymerization of PAn onto carbon fiber @ ˠ – MnO2 surface was used to fabricate asymmetric supercapacitor which displayed remarkable cyclability (73.2 % initial capacitance retention for 5,000 cycles), high energy density (30.9 Wh/kg at power density of 750 W/kg) and good specific capacitance (260 F/g) | 164 |
| PAn/MnO2/MoS2 | SC (479 at 5 mV/s scan rate) | 1.0 M H2SO4 | The PAn/MoS2 – MnO2 composite on a glassy carbon electrode was used for supercapacitor applications. The two-electrode device comprising of PAn-MoS2 – MnO2//PAn – MoS2–MnO2 electrode configuration exhibited excellent electrochemical performance parameters (specific capacitance, 259 F/g at 1 A/g, specific energy, 35.97 Wh/kg at power density of 500 W/kg and cyclic stability with capacity retention of 94.1 % over 4,000 cycles at 16 A/g) | 165 |
| ˠ-MnO2/PAn/CP | SC (642.5 at 1 A/g)/ED (114.2)/PD (798.6) | Development of ˠ-MnO2/PAn/carbon fiber paper substrate (CP) nanocomposite for use as an electrode in supercapacitor. The designed flexible electrode material showed remarkable cyclic charge/discharge performance with retention of 81.3 % original capacitance for 5,000 cycles | 166 | |
| Ag@MnO2/PAn | SC (1,028.66 at 1 A/g) with 88.4 % cyclic stability for 5,000 cycles | 2.0 M KOH | The synthesized PAn wrapped Ag decorated MnO2 (PAn/Ag @MnO2) nanorods were used as a positive electrode to develop PAn/Ag@MnO2//AC asymmetric supercapacitor which exhibited excellent energy density (49.77 Wh/kg) at power density (1,599.75 W/kg) with long cyclic life – span | 167 |
| Co3O4/PAn | SC (3,105.46 at 1 A/g) and ED (250) with excellent cyclic stability retaining 74.81 % original capacitance for 3,000 cycles | 6.0 M KOH | The PAn/Co3O4 nanocomposite comprising of a uniform coating of PANi on Co3O4 nanorods was synthesized by the combination of hydrothermal and in-situ polymerization techniques and used as electrode material for supercapacitor applications. Additionally, PAn/Co3O4 as a positive electrode coupled with activated carbon (AC) negative electrode was used to fabricate PAn/Co3O4//AC asymmetric supercapacitor which showed remarkable energy density (58.84 Wh/kg) at 0.16 kW/kg power density | 168 |
| PAn @ FNCO (Fe–Ni co-doped Co3O4) |
SC (1,171)/ED (144) at a current density of 1 A/g with good cyclic stability, retaining 84 % initial capacitance for 2,000 cycles | 1 M H2SO4 | PAn @ Fe – Ni codoped Co3O4 nanocomposite consisting of 10 % Fe – Ni codoped Co3O4 as filler in PAn matrix was synthesized in the form of nanowires for use as electrode material in supercapacitors applications | 169 |
| PAn@MnO2/CC | SC (1,105 mF/cm2) with remarkable cyclic stability (86.35 % capacitance retention for 2,000 cycles) at current density of 1 mA/cm2 in aqueous H2SO4 | 0.5 M H2SO4 | Use of hydrothermal and in-situ electrochemical polymerization techniques for producing PAn@ˠ-MnO2/CC ternary composite for utilization in flexible supercapacitor applications. The assembled highly flexible asymmetric supercapacitor device based on PAn@ˠ-MnO2/CC and polyvinylalcohol – H2SO4 gel electrolyte showed remarkable energy density (10.4 mW/cm3 at a power density of 1.5 m Wh/cm3) | 170 |
| MnO2/PAn/CC | SC (634 at 1 A/g) | – | Synthesis of PAn–MnO2/carbon cloth (CC) electrode material and its use as positive electrode in combination with MXene/CC (negative electrode) to fabricate flexible asymmetric supercapacitor (FASC) for achieving broadened potential range. The resulting FASC device exhibited excellent electrochemical performance (capacitance, 21.1 F/g at 0.5 A/g, cyclic stability, 83 % initial capacitance retention over 4,000 cycles, energy density, 47.25 µ Wh/cm2 at a power density of 2.4 m W/cm2 | 130 |
| Co3O4/PAn | SC (1,308 at 10 mV/s)/ED (250)/PD (6400) | 1 M H2SO4 | A novel low-temperature synthetic method was developed to prepare mesoporous structured Co3O4 anchored PAn binary nanocomposite exhibiting exceptionally higher PD among PAn nanocomposites for fabricating symmetric supercapacitors of enhanced electrochemical performance | 171 |
| MnO2/PAn activated CC | SC (620.2 at 2 A/g) with retaining 87 % of it for 2,000 cycles at 1 A/g | – | A highly porous nanofibrous layer-structured ternary nanocomposite (activated carbon cloth/MnO2/polyaniline-30) produced by the electrodeposition method was successfully utilized to fabricate symmetric supercapacitor which exhibited high specific capacitance (128.2 F/g) at 2 A/g | 172 |
PEDOT/PEDOT: PSS containing MMO-based nanocomposite electrode materials.
| Composition | Performance parameters SC (F/g)/ED (Wh/kg)/PD (W/kg) | Electrolyte | Remarks | References |
|---|---|---|---|---|
| Mn–Ni oxides/PEDOT and Mn–Ni–Ru oxides/PEDOT | SC (300 mC/cm2) and SC (328 mC/cm2) | 0.5 M Na2SO4 | Development of a lucid single electrodeposition procedure for fabrication of mixed metal oxides (Mn – Ni and Mn – Ni – Ru)/PEDOT/hybrid electrodes for use in an electro – osmotic pump (EOP) where Mn – Ni oxide/PEDOT electrodes exhibited better performance compared to Mn – Ni – Ru/PEDOT electrodes in water | 173 |
| MnO2 / C-black/CNT/PEDOT: PSS | SC (351) | PVA/H3PO4 gel electrolyte | The synthesis of ternary fibrous nanocomposite involves the preparation of CNT/C-black fibres by wet-spinning followed by modification by KMnO4 to produce MnO2/CNT/C-black fibres which were – dip-coated with 0.1 % PEDOT: PSS solution to obtain MnO2/C-black/CNT/PEDOT: PSS. The two ternary composite fiber electrodes assembled in a parallel solid-state device exhibited specific capacitance (51.3 F/g) with 84.2 % capacitance retention over 1,000 cycles in PVA/H3PO4 gel which was used both as separator and electrolyte | 174 |
| MnO2/P–F-CNFs (porous functionalized carbon nanofibers)/PEDOT | SC (776.7) at scan rate (25 V/s) | 1.0 M KCl | Development of MnO2/P–F-CNFs/PEDOT nanocomposite through potentiostatic deposition of PEDOT onto porous functionalized carbon fibres for use as positive electrode in combination with porous carbon nanofibers as negative electrode for developing asymmetric supercapacitor (ASC) which displayed high specific capacitance (1,061 F/g)), excellent specific energy (60.5 Wh/kg), remarkable cyclic stability (104.6 % capacity retention) over 5,000 cycles. The ASC provided a specious working potential window up to 1.6 V and was capable of lighting up around 25 (LEDs) | 175 |
| ZnO/MnO2/PEDOT core shell | Areal capacitance (1090)/ED (37.9) with energy density (37.9 Wh/kg) | - | The fabricated vertically aligned ZnO/MnO2/PEDOT core-shell nanostructured electrode was found highly beneficial for high energy storage applications due to synergistic advantages of nano MnO2 and molecularly integrated microporous PEDOT onto ZnO nanorods in three-dimensional architecture | 176 |
| MnO2/rGO/PEDOT: PSS | SC (2.9 F/m2 or 194 F/cm3) at current density (5 mA/cm2) with 95 % initial capacity retention for 5,000 cycles | 1.0 M Na2SO4 | Synthesis of binder-free ternary – nanocomposite (MnO2/rGO/PEDOT: PSS) on carbon fiber substrate for use as electrode material in the fabrication of fiber-shaped micro-supercapacitors. An ASC (MnO2/rGO/PEDOT: PSS//rGO) constructed by use of the resulted ternary composite delivered high energy density (295 µWh/cm2) at power density (14 mW/cm2) within an operating voltage window (0–2.0 V) in solid state Na2SO4 – CMC electrolyte. Interestingly, the use of super-concentrated potassium acetate – based water – in – salt electrolyte, enabled a cell voltage of 2.8 V for the asymmetric microdevice | 177 |
| MnO2/PEDOT:PSS | SC (365.5 at 1 A/g) with excellent cycling life-span retaining 80 % initial capacitance without a loss for 2,000 cycles at 5 A/g current density | 6.0 M KOH | The solvothermal and oxidative polymerization processes used to prepare binary PEDOT: PSS/MnO2 nanocomposites in nanorod structures showed unparalleled electrochemical super capacitive accomplishment | 178 |
| MnO2/PEDOT; PSS/CNT | SC (105.2 mF/cm2)/ED (13.2 µWh/cm2)/PD (162 μW/cm2) | 1.0 M Na2SO4 | The ternary nanocomposite (MnO2/PEDOT: PSS/CNT) was successfully used as an anode for the development of light-driven bio-super capacitors or supercapacitive bio-photovoltaics. The as-prepared nanocomposite on carbon – cloth displayed excellent SC (261 F/g) and unchanging charge/discharge reversibility for 14,000 cycles. In association with cyanobacterial biofilm, the anode unveiled elevated areal capacitance (294 mF/cm2) under illumination | 179 |
| MnO2/PEDOT/NCC (nanocrystalline (cellulose) | SC (144.69 at 25 mV/s)/ED (10.3)/PD (494.9) | 1.0 M aqueous KCl | A cauliflower structured ternary nanocomposite (PEDOT + NCC + MnO2) synthesized following the one-step electro-polymerization technique showed superb electrochemical performance at optimized MnO2 concentration level allowing 83 % retention of original capacitance over 2,000 cycles | 180 |
| MnO2/PEDOT/NBC | SC (76.6 F/g at 0.1 A/g of current density)/ED (14.0) at PD (53.1) | – | The nanocomposite comprising MnO2, nitric acid pretreated biochar (NBC), and PEDOT was used to develop a micro-supercapacitor (MSC) using pen lithography. The supercapacitive capacitance of the fabricated MSC remained unchanged over 500 bending cycles | 181 |
| Co3O4/PEDOT/CNFs | SC (849.65)/ED (14.54)/PD (1,726.96) | – | Development of flower-like ternary nanocomposite comprising of PEDOT functionalized porous carbon nanofibers (fpCNFs), and Co3O4 using hydrothermal coupled with annealing technique for use as the positive electrode in supercapattery coupling with nitrogen-doped graphene (NDG) as a negative electrode. The supercapattery system (FpCNFs/PEDOT/Co3O4//NDG) demonstrated remarkable performance at 2 A/g (energy density, 14.54 Wh/kg, power density, 1,726.96 W/kg and cyclic stability, 106.26 % capacitance retention for 2,000 cycles) | 182 |
| MnO2@PEDOT nanospheres | Areal SC (116.9 mF/cm2 at 0.1 mA/cm2) | – | Synthesis of nano spherical shaped MnO2@PEDOT composite by electrodeposition of PEDOT on MnO2 nanoparticles to use as cathode electrode (working window range, 0–1.0 V vs Ag/AgCl) in combination of urchin-like V2O5 electrode (voltage working range, −0.8 to 0.0 V) for fabricating a planar ASC (MnO2@PEDOT//V2O5) by use of a combination of screen printing and electro-coating methods. The assembled ASC displayed remarkable electrochemical characteristics including high energy density (15.1 µWh/cm2), stable operating voltage (1.8 V), superb power density (1.8 mW/cm2), and conservation of excellent cyclic stability (87.2 % capacitance for 10,000 cycles). Furthermore, the successful integration of ASC with solar cells has created a new field for the use of high-performance pseudocapacitor planar ASCs in wearable and integrated systems | 183 |
| PEDOT – Ni2+/NiO – CC | SC (236.0) at 1 A/g with outstanding cyclic stability (99 % initial capacitance retention over 2,500 cycles) | – | Preparation of PEDOT – Ni2+/NiO – CC composite by depositing traces of NiO on the intermediate layer between PEDOT and carbon cloth (CC) conducing substate as positive electrode for subsequent use in combination of PEDOT deposited on CC (PEDOT–CC) as the negative electrode to fabricate flexible all-solid-state asymmetric (Ni2+/NiO/PEDOT//PEDOT) supercapacitor. The assembled ASC revealed admirable SC (32.524 F/g), specific energy (40.15 mWh/g), and power density (1.32 kW/kg) | 184 |
Some interesting examples of CP–MMO composite electrode materials (not covered in Tables 5–7) include PAn–MnO2 (specific capacitance, 497 F/g) exhibiting 88.2 % capacity retention over 5,000 cycles at 10 A/g, 119 PAn–NiO– activated carbon nano fibres (specific capacitance, 1,157 F/g) with capacitance retention of 93.89 % for 5,000 cycles, 120 PEDOT/NiO/NiOH (specific capacitance 404 mF/cm2 at 4 mA/cm2) with capacitance retention (82.2 %) for 1,000 cycles, 121 PEDOT/Co3O4 displaying admirable cyclic stability with 93 % original capacitance retention over 20,000 cycles, 122 PAn/porous graphene/Co3O4 hybrid aerogels (specific capacitance, 1,247 F/g) at 1 A/g exhibiting no loss in original capacitance for 3,500 cycles, 123 hierarchical Co3O4 @ PPy core–shell composite nanowires retaining about 78 % of original capacitance for 5,000 cycles, 124 Co3O4/GO/PEDOT demonstrating excellent cycling performance with 92.7 % capacitance retention over 2,000 cycles 125 and the core – shell PANI–Co3O4 nanocomposite displaying specific capacitance of 1,184 F/g at 1.25 A/g along with capacitance retention of 84.9 % after 1,000 charge/discharge cycles. 126 .
Regarding PEDOT-based nanocomposite supercapacitors, highest PD (12,920 W/kg) with 69.7 % retention of original capacitance (805.3 F/g) even after 10,000 charging/discharging cycles was achieved for NiO/Ni@C//PEDOT–AC asymmetric SC whereas the Ni foam–MnO2//Ni-foam PPy supercapacitor exhibited very low specific capacitance (59.29 mF/cm2). 127 Wet-spinning technique integrated with electrodeposition has been successfully used to prepare MnO2/CNT and PPy/CNT nanocomposites for use in developing wire-shaped supercapacitors (WSC). The ASC (MnO2/CNT//PPy CNT) fabricated by twisting the MnO2/CNT fibers (cathode) and PPy/CNT (anode) using LiCl/PVA electrolyte delivered SC (10.7 F/g), ED (4.82 Wh/kg) and PD (1,382 W/kg) with retention of 86 % initial capacitance and 96 % Coulombic efficiency for 5,000 cycles. 128 The synthesized nanostructured NiO/CS (chitosan) – pyrrole nanotube (PNT) composite was found most favorable for supercapacitors due to its excellent capacitance (934.11 F/g at 1 A/g). The as-prepared NiO/CS–PNT nanocomposite was used both as positive and negative electrodes to construct a symmetric supercapacitor which demonstrated excellent electrochemical performance with the delivery of 4,045.69 W/kg (PD) at an ED (27.80 Wh/kg) with initial capacity retention of 84.9 % over 10,000 cycles. 129 The PAn–MnO2/CC composite produced through the synthesis of PAn and MnO2 on carbon cloth (CC) by electropolymerization in the presence of LiClO4 showed good electrochemical performance with delivery of 634.0 F/g SC at 1 A/g. The flexible ASC device assembled with the use of PAn–MnO2/CC as positive electrode and MXene/CC as negative electrode showed SC (21.1 F/g at 0.5 A/g) with capacitance retention (83 %) over 4,000 cycles, voltage window of 1.5 V, ED (47.25 µWh/cm2 and PD (2.40 mW/cm2). The selection of CC as substrate was due to its good ductility, large surface area, and high electrical conductivity. Two devices connected in series after bending 500 times greater than 90° were successful in powering 1.8 V LED. 130 The PPy–MOF (metal-organic framework) composite has been used as electrode material in supercapacitor applications but compared to PPy–MOF, nickel foam-modified PPy–MOF displayed better electrochemical performance with SC (715.6 F/g at 0.3 A/g current density) in 3.0 M KOH. However, the ASC (PPy–MoF//AC) delivered high ED (40.1 Wh/kg) at PD (1,500.6 W/kg). 131 Nanostructured PPy composites with CoOx, NiOx, MnOx, and FeOx were prepared by E. Karaca et al. 132 using the galvanostatic method on their metal-intercalated graphite surface in the presence of Na–CMC and TX100 (surfactant). The resulting composites (PPy/CoOx/Na–CMC, PPy/NiOx/Na–CMC, and PPy/FeOx/Na–CMC) showed marvelous SC and cycling stability. The symmetric SC fabricated with the use of PPy/MnO2/Na–CMC composite exhibited 0.290 kW/kg (PD)and 15.0 Wh/kg (ED) at 0.5 A/g maintaining good cyclic stability for 5,000 cycles.
From above-reviewed literature, it is clear that compared to PAn and PPy, lesser work has been reported on PEDOT-based MMO composites probably due to its poor solubility and low specific capacitance. Furthermore, even though MOF-based electrode materials possess enlarged surface area and tunable structures, their use in SCPs is lacking. Among 2-D materials, MXene is gaining popularity as a promising candidate for use in supercapacitor electrodes. It is hoped that further research on hybrid composites will uncover the latent potential applications of CPs/MMOs composites consisting of binary, ternary, or even quaternary phases of various constituting materials. It is heartening to note that compared to PAn and PPy, lesser work has been reported on PEDOT/MMO composites.
4 Conclusions
This review unfolds the recent developments and electrochemical applications of CPs–MMOs nanocomposite electrode materials in supercapacitors. In fact, the need for an ideal electrode material (binary or ternary) comprising of CP, MO, and C-matter has been always felt despite lots of studies that have previously reported. Therefore, tremendous efforts are continuing in search of advanced CP/MO-based electrode materials to widen the scope of supercapacitors in compressible energy storage devices and tiny portable electronic systems (i.e. smart mobile phones and digital cameras). In this review, the developments in CP/MMO-based nanocomposites have been highlighted and their use in energy storage devices has been summarized. To be concise, the three most useful CPs (PAN, PPy and PEDOT) along with three prominent MMOs (MnO2, NiO, and Co3O4) were selected to evaluate their super capacitive performance in the form of CP/MMO nanocomposites. The reported work on MMO nanoparticles embedded polymeric composites supercapacitors has been complied covering the period of last seven years.
In the future, intensive research is expected on the development of:
Integrated multi-component supercapacitor electrode materials,
Ecofriendly renewable energy devices,
Recyclable super capacitive materials,
Binder-free nanostructured composites,
High-capacity nano-architectured composites for use as current devices,
Mixed – magnetic metal oxides – CPs composites,
Nanostructured current collectors that facilitate unhindered transfer of both electron and ion through the entire electrode configuration.
5 Future challenges
Because of certain advantages (high PD, rapid charging, and long cycling lifespan) over traditional batteries, SCPs have been attractive choices for several energy storage and power delivery applications. However, some core issues/challenges related to SCPs include:
Lower energy storage capacity which needs to be improved without compromising power density,
Self-discharging with time leading to the loss of stored energy is a very important issue to be addressed in future research,
Broadening of operating voltage window without disturbing the initial stability of electrode material,
Developing novel composites with excellent electrochemical performance (improved ED/PD, high cyclic stability and enhanced electrical conductivity, etc.) through modification in currently used synthesis techniques such as microwave-assisted thermal decomposition as an industrially scalable method, non-aqueous synthesis methods to produce nanocomposites of controlled shape and size and anodic arc plasma method to generate nano-composites of high purity in ultra-fine particle size,
The selection of appropriate electrolytes has been a vital challenge in SCPs because it influences PD/ED, cyclic life, rate capability, specific capacitance, and charge balance between the electrodes in a cell. The high electrical conductivity, low internal resistance, and compatibility with electrode materials have been essential parameters for selecting an electrolyte. While aqueous electrolytes have high conductivity but small operating voltage windows and low ED, organic electrolytes are suitable for use at higher operational potential windows but have lower ionic conductivity. In this scenario, gel electrolytes, ionic liquids, and deep eutectic solvents (DES) seem to be alternative future electrolytes.
In addition to above mentioned main challenges, the improvement in rate capability at high voltage and enhancement in cyclic life with minimal capacity loss of SCPs are also challenging issues to deal with. Further, it is expected that future research on the use of SCPs will be focused on developing hybrid energy storage systems through combination with other energy storage technologies and portable electronic devices. It is believed that futuristic SCPs may be useful in addressing the intermittent nature of renewable energy sources (wind/solar) by storing energy during short demand periods and releasing it at high demand, opening the door to a more reliable and stable renewable energy grid.
Abbreviations
- AC
-
Activated carbon
- ASC
-
Asymmetric supercapacitor
- BET
-
Brunauer – Emmett – Teller
- C3N4
-
Cyanide nitrogen
- CAG
-
Carbon aerogels
- CB
-
Carbon black
- CC
-
Carbon cloth
- CDs
-
Carbon dots
- CF
-
Carbon fiber
- CMC
-
Carboxy methyl cellulose
- CMs
-
Carbon materials
- CNFs
-
Carbon nanofibers
- CNT
-
Carbon nanotubes
- CP
-
Conducting polymers
- CS
-
Chitosan
- CV
-
Cyclic voltammetry
- ED
-
Energy density
- EDLC
-
Electric double layer capacitor
- EDX
-
Energy dispersion X-ray analysis
- EESD
-
Electrochemical energy storing devices
- EIs
-
Electrochemical impedance spectroscopy
- ESR
-
Equivalent series resistance
- ExC
-
Exfoliated carbon
- FE – SEM
-
Field emission scanning electron microscopy
- FNCO
-
Fe–Ni co-doped Co3O4
- FS – SSS
-
Flexible symmetric solid-state supercapacitor
- FTIR – ATR
-
Fourier transform infrared – attenuated total reflection spectroscopy
- G
-
Graphene
- GCD
-
Galvanostatic charge – discharge
- Go
-
Graphene oxide
- HbCs
-
Hybrid capacitors
- LED
-
Light-emitting diode
- MC
-
Mesoporous carbon
- MMO
-
Magnetic metal oxides
- MO
-
Metal oxide
- MOF
-
Metal-organic framework
- MWCNT
-
Multiwalled carbon nanotubes
- NCC
-
Nanocrystalline cellulose
- NCs
-
Nanocages
- PAn
-
Polyaniline
- PC
-
Pseudocapacitor
- PD
-
Power density
- PEDOT
-
Poly (3,4 ethylene dioxythiophene)
- PfCNF
-
Porousfunctionalized carbon nanofibre
- PNT
-
Pyrrole nanotube
- PPy
-
Polypyrrole
- PSS
-
Polystyrene sulphonate
- PTFE
-
Polytetrafluoroethylene
- PVA
-
Polyvinyl alcohol
- PVDF
-
Polyvinylidene fluoride
- RCT
-
Resistance of charge transfer
- rGO
-
Reduced graphene oxide
- SC
-
Specific capacitance
- SCPs
-
Supercapacitors
- SILAR
-
Successive ionic layer adsorption and reaction
- SSS
-
Symmetric solid–state
- SWCNTs
-
Single-walled nanotubes
- TEM
-
Transmission electron microscopy
- TGA
-
Thermogravimetric analysis
- Ti3C2Tx
-
Titanium carbide (A maxene)
- ZFO
-
Zinc ferrite
- ZIF-8-CC
-
Zeolitic imidazolate framework-carbon cloth
-
Research ethics: Not applicable.
-
Informed consent: Not applicable.
-
Author contributions: MFA: Design and Implementation, Writing, and Supervision. QU: A literature survey. MKU: Revision, Editing
-
Use of Large Language Models, AI and Machine Learning Tools: None declared.
-
Conflict of interest: The authors state no conflict of interest.
-
Research funding: None declared.
-
Data availability: Not applicable.
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Artikel in diesem Heft
- Frontmatter
- Material Properties
- Magnetic metal oxide assisted conducting polymer nanocomposites as eco-friendly electrode materials for supercapacitor applications: a review
- Effects of different ratios of soft and rigid segment on the properties of soil and sand fixing materials of polyacrylate
- Research on the impact of active calcium carbonate on the performance of degradable composite films
- Research and functionalization of konjac glucomannan and its hydrogel in wound dressing
- Preparation and Assembly
- Acryloyl starch/carboxymethyl cellulose grafting copolymerization composite hydrogel for efficient adsorption of methylene blue
- Preparation and anti-fouling behavior of conductive and hydrophilic polypyrrole modified PVDF composite membrane
- Engineering and Processing
- Gas assisted fused deposition modeling: effects of assist gas parameters on print quality and properties
- Remediation of Ni2+ and Sr2+ ions from aqueous solutions by acacia gum/polyacrylic acid hydrogel reinforced with TiO2 nanoparticles
Artikel in diesem Heft
- Frontmatter
- Material Properties
- Magnetic metal oxide assisted conducting polymer nanocomposites as eco-friendly electrode materials for supercapacitor applications: a review
- Effects of different ratios of soft and rigid segment on the properties of soil and sand fixing materials of polyacrylate
- Research on the impact of active calcium carbonate on the performance of degradable composite films
- Research and functionalization of konjac glucomannan and its hydrogel in wound dressing
- Preparation and Assembly
- Acryloyl starch/carboxymethyl cellulose grafting copolymerization composite hydrogel for efficient adsorption of methylene blue
- Preparation and anti-fouling behavior of conductive and hydrophilic polypyrrole modified PVDF composite membrane
- Engineering and Processing
- Gas assisted fused deposition modeling: effects of assist gas parameters on print quality and properties
- Remediation of Ni2+ and Sr2+ ions from aqueous solutions by acacia gum/polyacrylic acid hydrogel reinforced with TiO2 nanoparticles
