期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 27, 页码 10888-10893出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202003518
关键词
electrochemistry; Fe-SnO2; N-2 fixation; nitrogen oxidation; nitrogen reduction
资金
- National Natural Science Foundation of China [21908120, 21875030]
- Natural Science Foundation of Shandong Province [ZR2018BB037]
- Youth Innovation Team Project of Shandong Provincial Education Department [2019KJC023]
- project of Qingdao Applied Basic Research Programs of Science and Technology [18-2-2-10-jch, 18-2-2-35-jch]
Electrochemical N-2 reduction reactions (NRR) and the N-2 oxidation reaction (NOR), using H2O and N-2, are a sustainable approach to N-2 fixation. To date, owing to the chemical inertness of nitrogen, emerging electrocatalysts for the electrochemical NRR and NOR at room temperature and atmospheric pressure remain largely underexplored. Herein, a new-type Fe-SnO2 was designed as a Janus electrocatalyst for achieving highly efficient NRR and NOR catalysis. A high NH3 yield of 82.7 mu g h(-1) mg(cat.)(-1) and a Faraday efficiency (FE) of 20.4 % were obtained for NRR. This catalyst can also serve as an excellent NOR electrocatalyst with a NO3- yields of 42.9 mu g h(-1) mg(cat.)(-1) and a FE of 0.84 %. By means of experiments and DFT calculations, it is revealed that the oxygen vacancy-anchored single-atom Fe can effectively adsorb and activate chemical inert N-2 molecules, lowering the energy barrier for the vital breakage of N equivalent to N and resulting in the enhanced N-2 fixation performance.
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