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Surface and bulk reconstruction of CoW sulfides during pH-universal electrocatalytic hydrogen evolution

Fan, Ke (author)
State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Centre on Molecular Devices, Institute for Energy Science and Technology, Dalian University of Technology, Dalian, 116024, China
Zou, H. (author)
Dharanipragada, N. V. R. Aditya (author)
Stockholms universitet,Institutionen för material- och miljökemi (MMK)
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Fan, L. (author)
Inge, A. Ken (author)
Stockholms universitet,Institutionen för material- och miljökemi (MMK)
Duan, L. (author)
Zhang, Biaobiao (author)
KTH,Organisk kemi
Sun, Licheng, 1962- (author)
KTH,Organisk kemi,State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Centre on Molecular Devices, Institute for Energy Science and Technology, Dalian University of Technology, Dalian, 116024, China; Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, 310024, China
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 (creator_code:org_t)
2021
2021
English.
In: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 9:18, s. 11359-11369
  • Journal article (peer-reviewed)
Abstract Subject headings
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  • Electrocatalytic water splitting is an efficient means of producing energy carriers, such as H2. The hydrogen evolution reaction (HER) requires high-efficiency electrocatalysts. Understanding the active site structures of the HER electrocatalysts is essential for the rational design and development of water splitting devices. In this study, porous CoW sulfides were employed as model electrocatalysts for pH-universal HER. Multiple characterization studies, such as X-ray photoelectron spectroscopy, X-ray absorption spectroscopy and operando X-ray diffraction, were systematically used to investigate the reconstruction of the active species at the surface and in the bulk. The results show that during the HER, the structural transformation of the species CoW sulfides is strongly dependent on the pH of the electrolyte. Electrolytes of varying pH lead to varied reconstruction and influence the true catalytically active species responsible for the HER. The surface and the bulk of the electrocatalysts transform to different oxides/hydroxides when subjected to the HER. This is the first time that the pH-dependent bulk and surface structural evolution in the HER has been revealed. This study reveals the reconstruction and potential active site evolution of mixed-metal sulfides for the HER. We believe that the present study not only provides an idealized "pre-catalyst"for pH-universal highly-efficient HER, but also provides a thorough understanding about the identification of the real active sites and the mechanism of the structural evolution of the electrocatalysts during hydrogen evolution.

Subject headings

NATURVETENSKAP  -- Kemi -- Materialkemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Materials Chemistry (hsv//eng)
NATURVETENSKAP  -- Kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)

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