Oxygen-Bridged Vanadium Single-Atom Dimer Catalysts Promoting High Faradaic Efficiency of Ammonia Electrosynthesis
學年 111
學期 2
出版（發表）日期 2023-04-12
作品名稱 Oxygen-Bridged Vanadium Single-Atom Dimer Catalysts Promoting High Faradaic Efficiency of Ammonia Electrosynthesis
作品名稱（其他語言）
著者 L. Wang, Y. Liu, H. Wang, T. Yang, Y. Luo, S. Lee, M. G. Kim, T. T. T. Nga, C. L. Dong, and H. Lee
單位
出版者
著錄名稱、卷期、頁數 ACS Nano 17(8), 7406-7416
摘要 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.
關鍵字 Electrocatalyst; Nitrogen Reduction Reaction; Single-Atom Dimer; Oxygen-Bridged Vanadium; Ammonia
語言 en_US
ISSN 1936-0851; 1936-086X
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度 否
國別 USA
公開徵稿
出版型式 ,電子版
相關連結

機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/125748 )