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Title: MoOxSy/Ni3S2 Microspheres on Ni Foam as Highly Efficient, Durable Electrocatalysts for Hydrogen Evolution Reaction

Abstract

Hydrogen energy derived from water splitting is the cleanest renewable energy source, but it is also very challenging to achieve because the hydrogen evolution reaction (HER) requires highly efficient and low-cost electrocatalysts. Here, we have fabricated a novel hierarchical system of amorphous molybdenum oxy/sulfide microspheres with crystalline Ni3S2 intergrown in situ on Ni foam (MoOxSy/Ni3S2/NF) as an outstanding electrocatalyst for HER. The MoOxSy/Ni3S2/NF demonstrates an ultra-low overpotential of 58 mV at a current density of 10 mA cm-2 and extremely durable stability (>200 h), suggesting superior performance comparable to that of Pt-C/NF under acidic conditions. The X-ray absorption fine structure (XAFS) determines the average valence state of Mo to be +(5 + δ), with a coordination motif by O and S. To explain such high HER activity, a [Mo2O2(S,O)4] dimer-based periodic model structure with the average composition of [Mo4O8S4] interfaced with the Ni3S2(101) surface is proposed. The interactions between the Ni of Ni3S2 and bridging S/O of [Mo4O8S4] result in an average formal Mo charge state between +5 and +6, and significant charge transfer from Ni3S2 to [Mo4O8S4] activates the Mo = O bonds. The calculated |ΔGH*| of less than 50 meV suggests that the double-bonded O is the mostmore » active site. This work points to the importance of oxy/sulfides with Mon+ (+5 < n < +6) as exceptional electrochemical catalysts for HER.« less

Authors:
 [1]; ORCiD logo [2];  [3];  [1];  [4]; ORCiD logo [5];  [6];  [1]; ORCiD logo [1]; ORCiD logo [7]; ORCiD logo [8]
+ Show Author Affiliations
  1. Beijing Normal University (China)
  2. Ningxia Medical Univ., Yinchuan (China)
  3. Beijing Normal University (China); Northwestern Univ., Evanston, IL (United States)
  4. Chinese Academy of Sciences (CAS), Shanghai (China)
  5. Valparaiso Univ., IN (United States)
  6. National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
  7. Argonne National Lab. (ANL), Argonne, IL (United States)
  8. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NSFC); Ministry of Science and Technology, Taiwan
OSTI Identifier:
1868890
Grant/Contract Number:  
AC02-06CH11357; 22176017; U1832152; 11805261; 21665021; MOST 108-2113-M-213-006
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 34; Journal Issue: 2; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemical structure; Electrical energy; Electrical properties; Electrocatalysts; Evolution reactions

Citation Formats

Yu, Zihuan, Yao, Huiqin, Yang, Yan, Yuan, Mengwei, Li, Cheng, He, Haiying, Chan, Ting-Shan, Yan, Dongpeng, Ma, Shulan, Zapol, Peter, and Kanatzidis, Mercouri G. MoOxSy/Ni3S2 Microspheres on Ni Foam as Highly Efficient, Durable Electrocatalysts for Hydrogen Evolution Reaction. United States: N. p., 2022. Web. doi:10.1021/acs.chemmater.1c03682.
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Yu, Zihuan, Yao, Huiqin, Yang, Yan, Yuan, Mengwei, Li, Cheng, He, Haiying, Chan, Ting-Shan, Yan, Dongpeng, Ma, Shulan, Zapol, Peter, & Kanatzidis, Mercouri G. MoOxSy/Ni3S2 Microspheres on Ni Foam as Highly Efficient, Durable Electrocatalysts for Hydrogen Evolution Reaction. United States. https://doi.org/10.1021/acs.chemmater.1c03682
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Yu, Zihuan, Yao, Huiqin, Yang, Yan, Yuan, Mengwei, Li, Cheng, He, Haiying, Chan, Ting-Shan, Yan, Dongpeng, Ma, Shulan, Zapol, Peter, and Kanatzidis, Mercouri G. Tue . "MoOxSy/Ni3S2 Microspheres on Ni Foam as Highly Efficient, Durable Electrocatalysts for Hydrogen Evolution Reaction". United States. https://doi.org/10.1021/acs.chemmater.1c03682. https://www.osti.gov/servlets/purl/1868890.
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@article{osti_1868890,
title = {MoOxSy/Ni3S2 Microspheres on Ni Foam as Highly Efficient, Durable Electrocatalysts for Hydrogen Evolution Reaction},
author = {Yu, Zihuan and Yao, Huiqin and Yang, Yan and Yuan, Mengwei and Li, Cheng and He, Haiying and Chan, Ting-Shan and Yan, Dongpeng and Ma, Shulan and Zapol, Peter and Kanatzidis, Mercouri G.},
abstractNote = {Hydrogen energy derived from water splitting is the cleanest renewable energy source, but it is also very challenging to achieve because the hydrogen evolution reaction (HER) requires highly efficient and low-cost electrocatalysts. Here, we have fabricated a novel hierarchical system of amorphous molybdenum oxy/sulfide microspheres with crystalline Ni3S2 intergrown in situ on Ni foam (MoOxSy/Ni3S2/NF) as an outstanding electrocatalyst for HER. The MoOxSy/Ni3S2/NF demonstrates an ultra-low overpotential of 58 mV at a current density of 10 mA cm-2 and extremely durable stability (>200 h), suggesting superior performance comparable to that of Pt-C/NF under acidic conditions. The X-ray absorption fine structure (XAFS) determines the average valence state of Mo to be +(5 + δ), with a coordination motif by O and S. To explain such high HER activity, a [Mo2O2(S,O)4] dimer-based periodic model structure with the average composition of [Mo4O8S4] interfaced with the Ni3S2(101) surface is proposed. The interactions between the Ni of Ni3S2 and bridging S/O of [Mo4O8S4] result in an average formal Mo charge state between +5 and +6, and significant charge transfer from Ni3S2 to [Mo4O8S4] activates the Mo = O bonds. The calculated |ΔGH*| of less than 50 meV suggests that the double-bonded O is the most active site. This work points to the importance of oxy/sulfides with Mon+ (+5 < n < +6) as exceptional electrochemical catalysts for HER.},
doi = {10.1021/acs.chemmater.1c03682},
journal = {Chemistry of Materials},
number = 2,
volume = 34,
place = {United States},
year = {Tue Jan 04 00:00:00 EST 2022},
month = {Tue Jan 04 00:00:00 EST 2022}
}
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