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Simultaneously enhancing adsorbed hydrogen and dinitrogen to enable efficient electrochemical NH3 synthesis on Sm(OH)3
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Lv, Zengxiang, Li, Zexu, Liu, Honghong, Li, Weixiang, Wu, Tai-Sing, Hong, Song, Ruan, Yukun, Soo, Yun-Liang, Hao, Leiduan, Xu, Liang, Robertson, Alex W., Xiong, Pei, Li, Molly Meng-Jung, Ding, Liang-Xin and Sun, Zhenyu (2023) Simultaneously enhancing adsorbed hydrogen and dinitrogen to enable efficient electrochemical NH3 synthesis on Sm(OH)3. Small Structures, 4 (11). 2300158. doi:10.1002/sstr.202300158 ISSN 2688-4062.
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Official URL: http://doi.org/10.1002/sstr.202300158
Abstract
The electrochemical N2 reduction reaction (ENRR), driven by renewable electricity and run under ambient conditions, offers a promising sustainable avenue for carbon-neutral NH3 production. Yet, to efficiently bind and activate the inert N2 remains challenge. Herein, effective and stable electrochemical NH3 synthesis on Sm(OH)3 via enhanced adsorption of hydrogen and dinitrogen by dual integration of sulfur dopants and oxygen vacancies (VO) is reported. The resulting S-doped lanthanide electrocatalyst attains both a good NH3 yield rate, exceeding 21 μgNH3 h−1 mgcat.−1, and an NH3 faradaic efficiency of over 29% at −0.3 V (vs reversible hydrogen electrode) in an H-type cell using a neutral electrolyte, figures of merit that are largely maintained after 2 days of consecutive polarization. Density functional theory calculations show that the adsorption energy barrier of N2 on S-Sm(OH)3(VO) is greatly lowered by the introduction of VO. In addition, the S sites improve the adsorption of hydrogen produced via the Volmer reaction, which is conducive to the formation of the *N–NH intermediate (i.e., the potential determining step, PDS) on adjacent Sm sites, and thereby significantly promotes the reaction kinetics of ENRR. The PDS free energy for the catalyst is comparable with the values at the peak of the ENRR volcano plots of leading transition metal catalyst surfaces.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QD Chemistry T Technology > TP Chemical technology |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||||||
Library of Congress Subject Headings (LCSH): | Ammonia -- Synthesis, Electrolytic reduction, Electrochemistry, Ammonia industry -- Environmental aspects | ||||||||||||
Journal or Publication Title: | Small Structures | ||||||||||||
Publisher: | Wiley-Blackwell Publishing Ltd. | ||||||||||||
ISSN: | 2688-4062 | ||||||||||||
Official Date: | November 2023 | ||||||||||||
Dates: |
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Volume: | 4 | ||||||||||||
Number: | 11 | ||||||||||||
Article Number: | 2300158 | ||||||||||||
DOI: | 10.1002/sstr.202300158 | ||||||||||||
Status: | Peer Reviewed | ||||||||||||
Publication Status: | Published | ||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | ||||||||||||
Copyright Holders: | © 2023 The Authors. Small Structures published by Wiley-VCH GmbH | ||||||||||||
Date of first compliant deposit: | 30 August 2023 | ||||||||||||
Date of first compliant Open Access: | 30 August 2023 | ||||||||||||
RIOXX Funder/Project Grant: |
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