Dynamic evolution and reversibility of single-atom Ni(II) active site in 1T-MoS2 electrocatalysts for hydrogen evolution

Brian Pattengale, Yichao Huang, Xingxu Yan, Sizhuo Yang, Sabrina Younan, Wenhui Hu, Zhida Li, Sungsik Lee, Xiaoqing Pan, Jing Gu () and Jier Huang ()
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Brian Pattengale: Marquette University
Yichao Huang: San Diego State University
Xingxu Yan: University of California
Sizhuo Yang: Marquette University
Sabrina Younan: San Diego State University
Wenhui Hu: Marquette University
Zhida Li: San Diego State University
Sungsik Lee: Argonne National Laboratory
Xiaoqing Pan: University of California
Jing Gu: San Diego State University
Jier Huang: Marquette University

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract 1T-MoS2 and single-atom modified analogues represent a highly promising class of low-cost catalysts for hydrogen evolution reaction (HER). However, the role of single atoms, either as active species or promoters, remains vague despite its essentiality toward more efficient HER. In this work, we report the unambiguous identification of Ni single atom as key active sites in the basal plane of 1T-MoS2 (Ni@1T-MoS2) that result in efficient HER performance. The intermediate structure of this Ni active site under catalytic conditions was captured by in situ X-ray absorption spectroscopy, where a reversible metallic Ni species (Ni0) is observed in alkaline conditions whereas Ni remains in its local structure under acidic conditions. These insights provide crucial mechanistic understanding of Ni@1T-MoS2 HER electrocatalysts and suggest that the understanding gained from such in situ studies is necessary toward the development of highly efficient single-atom decorated 1T-MoS2 electrocatalysts.

Date: 2020
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DOI: 10.1038/s41467-020-17904-z

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