Citation: Chen Yao, Chen George Zheng. New Precursors Derived Activated Carbon and Graphene for Aqueous Supercapacitors with Unequal Electrode Capacitances[J]. Acta Physico-Chimica Sinica, ;2020, 36(2): 190402. doi: 10.3866/PKU.WHXB201904025 shu

New Precursors Derived Activated Carbon and Graphene for Aqueous Supercapacitors with Unequal Electrode Capacitances

Chen Yao ^1,, ,
Chen George Zheng ^1,2,3,,

1.
The State Key Laboratory of Refractories and Metallurgy, College of Materials and Metallurgy, Wuhan University of Science and Technology, Wuhan 430081, P. R. China
2.
Department of Chemical and Environmental Engineering, Faculty of Science and Engineering, University of Nottingham Ningbo China, Ningbo 315100, Zhejiang Province, P. R. China
3.
Department of Chemical and Environmental Engineering, Faculty of Engineering, University of Nottingham, Nottingham NG2 7RD, UK

Author Bio: Yao Chen (ORCID: 0000-0003-0147-8156) obtained his PhD degree from Institute of Electrical Engineering, Chinese Academy of Sciences under Prof. Yanwei Ma's supervision in 2012. He then completed his postdoc research in IFW Dresden, Germany, together with Prof. Oliver Schmidt and in AIST Kansai, Japan with Prof. Qiang Xu. Since 2015, as an instructor, he had joined Wuhan University of Science and Technology where he was mainly engaged in research on carbon based electrochemical energy storage devices and heterogeneous catalysis
George Z. Chen (ORCID: 0000-0002-5589-5767) graduated from Jiujiang Teachers Training College with a Diploma in 1981, Fujian Normal University with the MSc in 1985, and the University of London with the PhD and DIC in 1992. After contracted work in the Universities of Oxford, Leeds and Cambridge, he joined the University of Nottingham in 2003, and has been Professor since 2009. He is Li Dak Sam Chair Professor of the University of Nottingham Ningbo China, and Specially Invited Professor of Wuhan University of Science and Technology. His research aims at electrochemical and liquid salts innovations for materials, energy and environment
Corresponding author: Chen Yao, y.chen@wust.edu.cn Chen George Zheng, george.chen@nottingham.ac.uk
Received Date: 3 April 2019
Revised Date: 17 May 2019
Accepted Date: 7 June 2019
Available Online: 17 February 2019
Fund Project: the Ningbo Municipal Government, China 2014A35001-1The project was supported by State Key Laboratory of Materials Processing and the Die & Mould Technology, Huazhong University of Science and Technology, China (P2019-014) and the Ningbo Municipal Government, China (3315 Plan, and 2014A35001-1)State Key Laboratory of Materials Processing and the Die & Mould Technology, Huazhong University of Science and Technology, China P2019-014the Ningbo Municipal Government, China 3315计划

Carbon materials can offer various micro- and nanostructures as well as bulk and surface functionalities; hence, they remain the most popular for manufacturing supercapacitors. This article critically reviews recent developments in the preparation of carbon materials from new precursors for supercapacitors. Typical examples are activated carbon (AC) and graphene, which can be prepared from various conventional and new precursors such as biomass, polymers, graphite oxide, CH₄, and even CO₂ via innovative processes to achieve low-cost and/or high specific capacitance. Specifically, when producing AC from natural biomasses or synthetic polymers, either new, spent, or waste, popular activation agents, such as KOH and ZnCl₂, are often used to process the ACs derived from these new precursors while the respective activation mechanisms always attract interest. The traditional two-step calcination process at high temperatures is widely employed to achieve high performance, with or without retaining the morphology of the precursors. The three-step calcination, including a post-vacuum treatment, is also the preferred choice in many cases, but it can increase the cost per capacity (kWh∙g⁻¹). More recently, one-step molecular activation promises a better and more economical approach to the commercial application of AC, although further increase of the yield is necessary. In addition to activation, graphitization, N doping, and template control can further improve ACs in terms of the charging and discharging rates, or pseudocapacitance, or both. Considerations are also given to material structure design, and carbon regeneration during activation. Metal-organic frameworks, which were initially used as templates, have been found to be good direct carbon precursors. Various graphene structures, including powders, films, aerogels, foams, and fibers, can be produced from graphite oxide, CO₂, and CH₄. Similar to AC, graphene can possess micropores by activation. Self-propagating high-temperature synthesis and molten salt processing are newly-reported methods for fabrication of mesoporous graphene. Macroporous graphene hydrogels can be produced by hydrothermal treatment of graphite oxide suspension, which can also be transferred into films. Hierarchically porous structures can be achieved by H₂O₂ etching or ZnCl₂ activation of the macroporous graphene precursor. Sponges as templates combined with KOH activation are applied to create both micro- and macropores in graphene foams. Graphene can grow on fibers and textiles by electrodeposition, dip-coating, or filtration, which can be woven into clothes with a large area or thick loading, illuminating the potential application in flexible and wearable supercapacitors. The key obstacles in AC and graphene production are high cost, low yield, low packing density, and low working potential range. Most Carbon materials derived from new precursors work very well with aqueous electrolytes. Charge storage occurs not only in the electric double layer (i.e., the "carbon | electrolyte" interface), but also via redox activity in association with the bulk and surface functionalities, and the resulting partial delocalization of valence electrons. The analysis of the capacitive electrode has shown a design defect that prevents the working voltage of a symmetrical supercapacitor from reaching the full potential window of the carbon material. This defect can be avoided in AC-based supercapacitors with unequal electrode capacitances, leading to higher cell voltages and hence higher specific energy than their symmetrical counterparts. There are also emerging ways to raise the energy capacity of AC supercapacitors, such as the use of redox electrolytes to enable the Nernstian charge storage mechanism, and of the three dimensional printing method for a desirable electrode structure. All these developments are promising carbon materials from various precursors of new and waste sources for a more affordable and sustainable supercapacitor technology.
- New precursor,
- Activated carbon,
- Graphene,
- Aqueous supercapacitor,
- Unequal electrode capacitance
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