In this critical review, metal oxides-based materials for electrochemical supercapacitor (ES) electrodes are reviewed in detail together with a brief review of carbon materials and conducting polymers. Their advantages, disadvantages, and performance in ES electrodes are discussed through extensive analysis of the literature, and new trends in material development are also reviewed. Two important future research directions are indicated and summarized, based on results published in the literature: the development of composite and nanostructured ES materials to overcome the major challenge posed by the low energy density of ES (476 references).

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A review of electrode materials for electrochemical supercapacitors

The science and technology of ultracapacitors are reviewed for a number of electrode materials, including carbon, mixed metal oxides, and conducting polymers. More work has been done using microporous carbons than with the other materials and most of the commercially available devices use carbon electrodes and an organic electrolytes. The energy density of these devices is 3¯5 Wh/kg with a power density of 300¯500 W/kg for high efficiency (90¯95%) charge/discharges. Projections of future developments using carbon indicate that energy densities of 10 Wh/kg or higher are likely with power densities of 1¯2 kW/kg. A key problem in the fabrication of these advanced devices is the bonding of the thin electrodes to a current collector such the contact resistance is less than 0.1 cm2. Special attention is given in the paper to comparing the power density characteristics of ultracapacitors and batteries. The comparisons should be made at the same charge/discharge efficiency.

Ultracapacitors: Why, How, and Where is the Technology

A promising family of mixed transition-metal oxides (MTMOs) (designated as Ax B3-x O4 ; A, B=Co, Ni, Zn, Mn, Fe, etc.) with stoichiometric or even non-stoichiometric compositions, typically in a spinel structure, has recently attracted increasing research interest worldwide. Benefiting from their remarkable electrochemical properties, these MTMOs will play significant roles for low-cost and environmentally friendly energy storage/conversion technologies. In this Review, we summarize recent research advances in the rational design and efficient synthesis of MTMOs with controlled shapes, sizes, compositions, and micro-/nanostructures, along with their applications as electrode materials for lithium-ion batteries and electrochemical capacitors, and efficient electrocatalysts for the oxygen reduction reaction in metal-air batteries and fuel cells. Some future trends and prospects to further develop advanced MTMOs for next-generation electrochemical energy storage/conversion systems are also presented.

Mixed transition-metal oxides: design, synthesis, and energy-related applications.

This Review focuses on noncovalent functionalization of graphene and graphene oxide with various species involving biomolecules, polymers, drugs, metals and metal oxide-based nanoparticles, quantum dots, magnetic nanostructures, other carbon allotropes (fullerenes, nanodiamonds, and carbon nanotubes), and graphene analogues (MoS2, WS2). A brief description of π–π interactions, van der Waals forces, ionic interactions, and hydrogen bonding allowing noncovalent modification of graphene and graphene oxide is first given. The main part of this Review is devoted to tailored functionalization for applications in drug delivery, energy materials, solar cells, water splitting, biosensing, bioimaging, environmental, catalytic, photocatalytic, and biomedical technologies. A significant part of this Review explores the possibilities of graphene/graphene oxide-based 3D superstructures and their use in lithium-ion batteries. This Review ends with a look at challenges and future prospects of noncovalently modified graph...

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Noncovalent Functionalization of Graphene and Graphene Oxide for Energy Materials, Biosensing, Catalytic, and Biomedical Applications

A facile two-step method is developed for large-scale growth of ultrathin mesoporous nickel cobaltite (NiCo2O4) nanosheets on conductive nickel foam with robust adhesion as a high-performance electrode for electrochemical capacitors. The synthesis involves the co-electrodeposition of a bimetallic (Ni, Co) hydroxide precursor on a Ni foam support and subsequent thermal transformation to spinel mesoporous NiCo2O4. The as-prepared ultrathin NiCo2O4 nanosheets with the thickness of a few nanometers possess many interparticle mesopores with a size range from 2 to 5 nm. The nickel foam supported ultrathin mesoporous NiCo2O4 nanosheets promise fast electron and ion transport, large electroactive surface area, and excellent structural stability. As a result, superior pseudocapacitive performance is achieved with an ultrahigh specific capacitance of 1450 F g−1, even at a very high current density of 20 A g−1, and excellent cycling performance at high rates, suggesting its promising application as an efficient electrode for electrochemical capacitors.

Ultrathin mesoporous NiCo2O4 nanosheets supported on Ni foam as advanced electrodes for supercapacitors

ZnO/reduced graphite oxide composites were synthesized using a two-step method in which KOH reacts with Zn(NO3)2 in the aqueous dispersions of graphite oxide (GO) to form a Zn(OH)2/graphite oxide precursor, followed by thermal treatment in air. It was found that the dispersion of reduced graphene oxide (rGO) sheets within composites was key for achieving an excellent capacitive performance of the samples. However, the mass ratio of ZnO to rGO determined whether rGO sheets within composites were dispersed or agglomerated. The composite achieved homogeneous incorporation of rGO sheets within the ZnO matrix when the mass ratio of ZnO to rGO was equal to 93.3:6.7. This composite, in which the weight percent of rGO was only 6.7%, appeared in the SEM images to be almost entirely filled with rGO sheets coated by ZnO and exhibited high specific capacitance and excellent cycling ability. Furthermore, the sheets overlapped to form a three-dimensional network structure, through which electrolyte ions easily access t...

Zinc Oxide/Reduced Graphene Oxide Composites and Electrochemical Capacitance Enhanced by Homogeneous Incorporation of Reduced Graphene Oxide Sheets in Zinc Oxide Matrix

In the present work, we used charge-bearing nanosheets as building blocks to construct a binary composite composed of NiCo2O4 and reduced graphene oxide (RGO). Co–Ni hydroxides intercalated by p-aminobenzoate (PABA) ion and graphite oxide (GO) were exfoliated into positively charged hydroxide nanosheets and negatively charged graphene oxide nanosheets in water, respectively, and then these oppositely charged nanosheets were assembled to form heterostructured nanohybrids through electrostatic interactions. The subsequent thermal treatment led to the transformation of the hydroxide nanosheets into spinel NiCo2O4 and also to the reduction of graphene oxide. The as-obtained NiCo2O4–RGO composite exhibits an initial specific capacitance of 835 F g−1 at a specific current of 1 A g−1 and 615 F g−1 at 20 A g−1. More interestingly, the specific capacitance of the composite increases with cycling numbers, reaches 1050 F g−1 at 450 cycles and remains at 908 F g−1 (higher than the initial value) after 4000 cycles. The high specific capacitance, remarkable rate capability and excellent cycling ability of the composites mean that they show promise for application in supercapacitors. Comparison with the capacitive behavior of pure NiCo2O4 and NiCo2O4 mechanically mixed with RGO displays the importance of the self-assembly of the nanosheets in making a wide range of graphene-based composite materials for applications in electrochemical energy storage.

Design and synthesis of NiCo2O4–reduced graphene oxide composites for high performance supercapacitors

Polyaniline/SnO2 nanocomposite for supercapacitor applications

The four α-cobalt hydroxides (green or blue) with different intercalated anions were synthesized by a chemical precipitation route in which polyethylene glycol was used as the structure-directing reagent for application in the electrode materials of electrochemical capacitors. Every one among the four samples displays an interesting and distinctive morphology although the synthesis conditions were the same except for the anions. The intercalated anions have a critical effect on the basal plane spacing, morphologies, and capacitive properties of the products. Structural and morphological characterizations were performed by using power X-ray diffraction (XRD) and field emission scanning electron microscopy (FESEM). The component and thermal stability of the sample were respectively measured by FT-IR and thermal analyses, including thermogravimetry (TG) and differential thermogravimetry (DTG). The electrochemical behaviors were measured by cyclic voltammogram and galvanostatic charge−discharge. The specific ...

Synthesis of α-Cobalt Hydroxides with Different Intercalated Anions and Effects of Intercalated Anions on Their Morphology, Basal Plane Spacing, and Capacitive Property

Zhongai Hu

Papers

Zinc Oxide/Reduced Graphene Oxide Composites and Electrochemical Capacitance Enhanced by Homogeneous Incorporation of Reduced Graphene Oxide Sheets in Zinc Oxide Matrix

Design and synthesis of NiCo2O4–reduced graphene oxide composites for high performance supercapacitors

Polyaniline/SnO2 nanocomposite for supercapacitor applications

Synthesis of α-Cobalt Hydroxides with Different Intercalated Anions and Effects of Intercalated Anions on Their Morphology, Basal Plane Spacing, and Capacitive Property

Synthesis and electrochemical characterization of mesoporous CoxNi1−x layered double hydroxides as electrode materials for supercapacitors