期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 48, 页码 25263-25268出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202110879
关键词
density functional theory; electrocatalysis; MoS2; NH3 synthesis; NO reduction reaction
资金
- National Natural Science Foundation of China [22072015, 20A20145, 21878195, 21805198]
- Program for Science & Technology Innovation Talents in Universities of Henan Province [20HASTIT028]
MoS2/GF nanosheet on graphite felt shows promising catalytic performance in electrochemical reduction of NO for NH3 production, offering a potential environmentally friendly and efficient approach for nitrogen cycle restoration.
Electrochemical reduction of NO not only offers an attractive alternative to the Haber-Bosch process for ambient NH3 production but mitigates the human-caused unbalance of nitrogen cycle. Herein, we report that MoS2 nanosheet on graphite felt (MoS2/GF) acts as an efficient and robust 3D electrocatalyst for NO-to-NH3 conversion. In acidic electrolyte, such MoS2/GF attains a maximal Faradaic efficiency of 76.6 % and a large NH3 yield of up to 99.6 mu mol cm(-2) h(-1). Using MoS2 nanosheet-loaded carbon paper as the cathode, a proof-of-concept device of Zn-NO battery was assembled to deliver a discharge power density of 1.04 mW cm(-2) and an NH3 yield of 411.8 mu g h(-1) mg(cat.)(-1). Calculations reveal that the positively charged Mo-edge sites facilitate NO adsorption/activation via an acceptance-donation mechanism and disfavor the binding of protons and the coupling of N-N bond.
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