期刊
CHEMICAL ENGINEERING JOURNAL
卷 431, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133383
关键词
Fe doping; Oxygen vacancies; Electrocatalysis; Nitrogen reduction reaction; InVO4 nanosheets
资金
- National Key R & D Program of China [2017YFA0207203]
- National Natural Science Foundation of China [21773050, 21929401, 21871066]
- Natural Science Foundation of Heilongjiang Province in China [LH2021B010]
- State Key Laboratory of Urban Water Resource and Environment (Har-bin Institute of Technology) [2020DX03]
This research demonstrates the effective modulation of the electronic structure of InVO4 nanosheets through Fe doping, which generates abundant oxygen vacancies and significantly enhances the electrochemical N-2 reduction performance with high selectivity.
Electrocatalytic nitrogen fixation shows a promising possibility for converting nitrogen to ammonia. We demonstrate Fe as an effective dopant for modulating the electronic structure of InVO4 nanosheets to generate abundant oxygen vacancies, which significantly boost the electrochemical N-2 reduction performance with high selectivity. Benefiting from the optimal Fe content, the catalyst achieves a high NH3 yield of 17.23 mu gh(-1)mg(cat)(-1). with a Faradaic efficiency up to 14.27% at-0.4 V versus reversible hydrogen electrode in 0.1 M HCl with electrochemical and structural stability. The catalytic mechanism is explored by theorical calculations. Density functional theory (DFT) calculations elucidate that N-2 is preferentially adsorbed on Fe sites doped in InVO4 (110) surface and reduced to ammonia via the distal pathway. The oxygen vacancies generated by the introduction of Fe synergistically activate N-2.
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