Affiliation: | 1. College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang, 325035 China These authors contributed equally to this work.;2. School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, 710072 China These authors contributed equally to this work.;3. College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang, 325035 China;4. Department of Materials Science and Engineering, University of North Texas, Denton, TX, 76203 USA;5. Center of Advanced Science and Engineering for Carbon, School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052 Australia;6. Fachgebiet Angewandte Nanophysik, Institut für Physik & IMN MacroNano (ZIK), Technische Universität Ilmenau, Ilmenau, 98693 Germany;7. Department of Chemistry and Biochemistry, University of Windsor, Windsor, ON, N9B3P4 Canada |
Abstract: | Although tremendous efforts have been devoted to understanding the origin of boosted charge storage on heteroatom-doped carbons, none of the present studies has shown a whole landscape. Herein, by both experimental evidence and theoretical simulation, it is demonstrated that heteroatom doping not only results in a broadened operating voltage, but also successfully promotes the specific capacitance in aqueous supercapacitors. In particular, the electrolyte cations adsorbed on heteroatom-doped carbon can effectively inhibit hydrogen evolution reaction, a key step of water decomposition during the charging process, which broadens the voltage window of aqueous electrolytes even beyond the thermodynamic limit of water (1.23 V). Furthermore, the reduced adsorption energy of heteroatom-doped carbon consequently leads to more stored cations on the heteroatom-doped carbon surface, thus yielding a boosted charge storage performance. |