Rational design of phosphorus-doped cobalt sulfides electrocatalysts for hydrogen evolution
Rational design of phosphorus-doped cobalt sulfides electrocatalysts for hydrogen evolution
复制标题
磷掺杂硫化钴析氢电催化剂的合理设计
DOI：
10.1007/s12274-019-2538-x
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发表时间：
2019-10-17
期刊：
影响因子：
9.9
通讯作者：
Yue, Qin
中科院分区：
文献类型：
--
作者：
Qu, Guoxing;Wu, Tianli;Yue, Qin
适量的阴离子掺杂可以调节电催化剂的电子结构、活性位和相态，是提高电催化剂析氢性能的有效途径。报道的研究主要集中在设计P掺杂的CoS2，而很少研究其他相的硫化钴，如Co1-xS和Co9S8掺杂P作为HER电催化剂。在此，掺杂有P的各种钴硫化物（包括CoS2/Co1-xS、Co1-xS和Co9S8）通过容易的水热方法锚定在碳布上。在测试的电催化剂中，P掺杂的Co1-xS表现出优异的电催化性能，在电流密度为10和100 mA·cm-2时，过电位分别为110和165 mV（相对于RHE）。密度泛函理论计算表明，P掺杂的Co1 − xS具有比原始Co1 − xS更小的带隙和更优的氢吸附位点。本工作初步研究了P掺杂的各种钴硫化物，并进一步深入了解P掺杂的活性改善机制，这可以指导用于"氢经济"的地球丰富的HER电催化剂的设计。
Moderate anionic doping is an effective approach to improve the performance of electrocatalysts toward hydrogen evolution reaction (HER) since it can adjust the electronic structure, active site, and phase. The reported studies mainly focus on designing P doped CoS2, while other phases of cobalt sulfide, such as Co1−xS and Co9S8doped with P are rarely investigated for HER electrocatalysts. Herein, various cobalt sulfides (including CoS2/Co1−xS, Co1−xS, and Co9S8) doped with P are anchored on carbon cloth through a facile hydrothermal method. Among tested electrocatalysts, P doped Co1−xS exhibits excellent electrocatalytic performance with an overpotential of 110 and 165 mV (vs. RHE) for current densities of 10 and 100 mA·cm−2, respectively. Density functional theory calculations reveal that P doped Co1−xS possesses a smaller bandgap and more optimal hydrogen adsorption sites than pristine Co1−xS. This work initially investigates various cobalt sulfides doped with P and further gets insight into the activity improvement mechanism of P doping, which could guide the design of earth-abundant HER electrocatalysts for the “hydrogen economy”.