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Title: Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis

Abstract

The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. In this work, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co2P (Pt–Co2P) to introduce a stronger dopant–host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H–H bond formation. As a proof-of-concept, the interior-modified Pt–Co2P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm–2, and excellent durability for long-term utilization. The interior-modified Pt–Co2P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [1];  [3];  [4];  [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [1]
  1. Univ. of Central Florida, Orlando, FL (United States)
  2. Physical and Computational Sciences Directorate;Pacific Northwest National Laboratory;Richland;USA
  3. Southern Univ. of Science and Technology, Shenzhen (China)
  4. Oregon State Univ., Corvallis, OR (United States)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1714368
Alternate Identifier(s):
OSTI ID: 1661739
Report Number(s):
PNNL-SA-150276
Journal ID: ISSN 1754-5692
Grant/Contract Number:  
AC05-76RL01830; FG02-11ER16243; AC02-06CH11357; 68278; CMMI-1851674; ECCS-1726636; 21802065
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 13; Journal Issue: 9; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; interior modification; alkaline hydrogren evolution; water dissociation; near-zero onset potential; dopant-host interaction

Citation Formats

Li, Zhao, Niu, Wenhan, Yang, Zhenzhong, Kara, Abdelkader, Wang, Qi, Wang, Maoyu, Gu, Meng, Feng, Zhenxing, Du, Yingge, and Yang, Yang. Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis. United States: N. p., 2020. Web. doi:10.1039/D0EE01750G.
Li, Zhao, Niu, Wenhan, Yang, Zhenzhong, Kara, Abdelkader, Wang, Qi, Wang, Maoyu, Gu, Meng, Feng, Zhenxing, Du, Yingge, & Yang, Yang. Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis. United States. https://doi.org/10.1039/D0EE01750G
Li, Zhao, Niu, Wenhan, Yang, Zhenzhong, Kara, Abdelkader, Wang, Qi, Wang, Maoyu, Gu, Meng, Feng, Zhenxing, Du, Yingge, and Yang, Yang. Fri . "Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis". United States. https://doi.org/10.1039/D0EE01750G. https://www.osti.gov/servlets/purl/1714368.
@article{osti_1714368,
title = {Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis},
author = {Li, Zhao and Niu, Wenhan and Yang, Zhenzhong and Kara, Abdelkader and Wang, Qi and Wang, Maoyu and Gu, Meng and Feng, Zhenxing and Du, Yingge and Yang, Yang},
abstractNote = {The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. In this work, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co2P (Pt–Co2P) to introduce a stronger dopant–host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H–H bond formation. As a proof-of-concept, the interior-modified Pt–Co2P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm–2, and excellent durability for long-term utilization. The interior-modified Pt–Co2P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design.},
doi = {10.1039/D0EE01750G},
journal = {Energy & Environmental Science},
number = 9,
volume = 13,
place = {United States},
year = {Fri Jul 31 00:00:00 EDT 2020},
month = {Fri Jul 31 00:00:00 EDT 2020}
}

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