Boosting Electrocatalytic HER Activity of 3D Interconnected CoSP via Metal Doping: Active and Stable Electrocatalysts for pH-Universal Hydrogen Generation,Chemistry of Materials

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Boosting Electrocatalytic HER Activity of 3D Interconnected CoSP via Metal Doping: Active and Stable Electrocatalysts for pH-Universal Hydrogen Generation
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-10-19 , DOI: 10.1021/acs.chemmater.0c03052
Viet Q. Bui _{1,

2} , Ashwani Kumar _{1,

2} , Huong T. D. Bui _{1,

2} , Jinsun Lee _{1,

2} , Yosep Hwang _{1,

2} , Hung M. Le ₃ , Yoshiyuki Kawazoe ₄ , Hyoyoung Lee _{1,

2,

5}

Affiliation

Recently, many research studies have been focused on anion or cation substitution into the lattice of pyrite-type cobalt disulfide (CoS₂) for enhancing the hydrogen evolution reaction (HER) performance. Nonetheless, finding the correct pair of anion–cation dual substitution with added synergistic effect for boosting pH-universal HER activity remains an ongoing challenge. Additionally, a generalized activity descriptor and the HER mechanism in alkaline media remain elusive. Herein, to elucidate the HER mechanism and obtain the suitable anion–cation pair, we investigated the codoping of metal cations (Ti/V/Cr/Mn/Fe) and phosphorus anions into the CoS₂ moiety. Our theoretical prediction revealed that Ti and P codoping into CoS₂ exhibits superior HER performance at both pH 0 and 14, which is ascribed to the weak hydrogen binding energy in acid and fast water dissociation kinetics in alkaline media, thereby promoting HER. Remarkably, a follow-up experiment confirmed that Ti-CoSP showed astonishing HER activity inducing low overpotentials of 44 and 132 mV at −10 mA cm^–2 in acidic and alkaline media, respectively, with superior stability for 40 h.

中文翻译：

通过金属掺杂提高3D互连CoSP的电催化HER活性：用于产生pH值通用氢的活性和稳定电催化剂

近来，许多研究集中在阴离子或阳离子取代成黄铁矿型二硫化钴（CoS ₂）的晶格中，以增强氢释放反应（HER）的性能。尽管如此，找到正确的一对阴离子-阳离子双重取代并增加协同作用以增强pH值通用的HER活性仍然是一个挑战。另外，在碱性介质中的广义活性描述符和HER机制仍然难以捉摸。在本文中，为了阐明HER机理并获得合适的阴离子阳离子对，我们研究了将金属阳离子（Ti / V / Cr / Mn / Fe）和磷阴离子共掺杂到CoS ₂部分中。我们的理论预测表明，Ti和P共掺杂到CoS _2中在pH 0和14时均显示出优异的HER性能，这归因于酸中弱的氢结合能和碱性介质中快速的水离解动力学，从而促进了HER。值得注意的是，一项后续实验证实，Ti-CoSP表现出惊人的HER活性，在-10 mA cm ^–2的酸性和碱性介质中分别诱导44和132 mV的低过电势，并具有出色的40 h稳定性。

更新日期：2020-11-25

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