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Oxygen-Bridged Vanadium Single-Atom Dimer Catalysts Promoting High Faradaic Efficiency of Ammonia Electrosynthesis

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Title
Oxygen-Bridged Vanadium Single-Atom Dimer Catalysts Promoting High Faradaic Efficiency of Ammonia Electrosynthesis
Author(s)
Wang, Lingling; Liu, Yang; Wang, Hongdan; Yang, Taehun; Luo, Yongguang; Lee, Seungeun; Kim, Min Gyu; Nga, Ta Thi Thuy; Dong, Chung-Li; Lee, Hyoyoung
Publication Date
2023-04
Journal
ACS Nano, v.17, no.8, pp.7406 - 7416
Publisher
American Chemical Society
Abstract
Copyright © 2023 American Chemical Society. Single-atom catalysts have already been widely investigated for the nitrogen reduction reaction (NRR). However, the simplicity of a single atom as an active center encounters the challenge of modulating the multiple reaction intermediates during the NRR process. Moving toward the single-atom-dimer (SAD) structures can not only buffer the multiple reaction intermediates but also provide a strategy to modify the electronic structure and environment of the catalysts. Here, a structure of a vanadium SAD (V-O-V) catalyst on N-doped carbon (O-V2-NC) is proposed for the electrochemical nitrogen reduction reaction, in which the vanadium dimer is coordinated with nitrogen and simultaneously bridged by one oxygen. The oxygen-bridged metal atom dimer that has more electron deficiency is perceived to be the active center for nitrogen reduction. A loop evolution of the intermediate structure was found during the theoretical process simulated by density functional theory (DFT) calculation. The active center V-O-V breaks down to V-O and V during the protonation process and regenerates to the original V-O-V structure after releasing all the nitrogen species. Thus, the O-V2-NC structure presents excellent activity toward the electrochemical NRR, achieving an outstanding faradaic efficiency (77%) along with the yield of 9.97 μg h-1 mg-1 at 0 V (vs RHE) and comparably high ammonia yield (26 μg h-1 mg-1) with the FE of 4.6% at −0.4 V (vs RHE). This report synthesizes and proves the peculiar V-O-V dimer structure experimentally, which also contributes to the library of SAD catalysts with superior performance.
URI
https://pr.ibs.re.kr/handle/8788114/13584
DOI
10.1021/acsnano.2c11954
ISSN
1936-0851
Appears in Collections:
Center for Integrated Nanostructure Physics(나노구조물리 연구단) > 1. Journal Papers (저널논문)
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