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

被引:48
作者
Bui, Viet Q. [1 ,2 ]
Kumar, Ashwani [1 ,2 ]
Bui, Huong T. D. [1 ,2 ]
Lee, Jinsun [1 ,2 ]
Hwang, Yosep [1 ,2 ]
Le, Hung M. [3 ]
Kawazoe, Yoshiyuki [4 ]
Lee, Hyoyoung [1 ,2 ,5 ]
机构
[1] Sungkyunkwan Univ, Inst Basic Sci IBS, Ctr Integrated Nanostruct Phys CINAP, Suwon 16419, South Korea
[2] Sungkyunkwan Univ SKKU, Dept Chem, Suwon 16419, South Korea
[3] Washington State Univ, Dept Chem, Pullman, WA 99164 USA
[4] Tohoku Univ, New Ind Creat Hatchery Ctr, Sendai, Miyagi 9808579, Japan
[5] Sungkyunkwan Univ SKKU, Dept Biophys, Suwon 16419, South Korea
关键词
Cobalt compounds - Electrocatalysts - Pyrites - Alkalinity - Hydrogen production - Negative ions - Positive ions - Binding energy;
D O I
10.1021/acs.chemmater.0c03052
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:9591 / 9601
页数:11
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