Origins of Boosted Charge Storage on Heteroatom‐Doped Carbons
Origins of Boosted Charge Storage on Heteroatom‐Doped Carbons
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杂原子掺杂碳增强电荷存储的起源
DOI：
10.1002/ange.202000319
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发表时间：
2020
期刊：
影响因子：
--
通讯作者：
Shun Wang
中科院分区：
文献类型：
--
作者：
Cuixia Cui;Yong Gao;Jun Li;Chongyin Yang;Min Liu;Huile Jin;Zhenhai Xia;Liming Dai;Yong Lei;Jichang Wang;Shun Wang
尽管人们已经付出了巨大的努力来理解杂原子掺杂碳上增强电荷储存的起源，但目前的研究还没有显示出一个完整的图景。本文通过实验证据和理论模拟证明，杂原子掺杂不仅使工作电压变宽，而且成功地提高了水性超级电容器的比电容。特别是，电解质阳离子吸附在杂原子掺杂碳上，可以有效抑制析氢反应，这是充电过程中水分解的关键步骤，从而拓宽了含水电解质的电压窗口，甚至超出了水的热力学极限（1.23 V）。此外，杂原子掺杂碳的吸附能降低，导致更多的阳离子存储在杂原子掺杂碳表面，从而提高电荷存储性能。
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.