催化作用
电化学
氧化还原
析氧
无机化学
氨生产
材料科学
可逆氢电极
分子
化学
电极
物理化学
有机化学
工作电极
作者
Ying Guo,Shaoce Zhang,Rong Zhang,Donghong Wang,Daming Zhu,Xuewan Wang,Diwen Xiao,Na Li,Yuwei Zhao,Zhaodong Huang,Wenjie Xu,Shuangming Chen,Li Song,Jun Fan,Qing Chen,Chunyi Zhi
出处
期刊:ACS Nano
[American Chemical Society]
日期:2021-12-22
卷期号:16 (1): 655-663
被引量:115
标识
DOI:10.1021/acsnano.1c08109
摘要
Electrocatalytic N 2 oxidation (NOR) into nitrate is a potential alternative to the emerging electrochemical N 2 reduction (NRR) into ammonia to achieve a higher efficiency and selectivity of artificial N 2 fixation, as O 2 from the competing oxygen evolution reaction (OER) potentially favors the oxygenation of NOR, which is different from the parasitic hydrogen evolution reaction (HER) for NRR. Here, we develop an atomically dispersed Fe-based catalyst on N-doped carbon nanosheets (AD-Fe NS) which exhibits an exceptional catalytic NOR capability with a record-high nitrate yield of 6.12 μ mol mg –1 h –1 (2.45 μ mol cm –2 h –1 ) and Faraday efficiency of 35.63%, outperforming all reported NOR catalysts and most well-developed NRR catalysts. The isotopic labeling NOR test validates the N source of the resultant nitrate from the N 2 electro-oxidation catalyzed by AD-Fe NS. Experimental and theoretical investigations identify Fe atoms in AD-Fe NS as active centers for NOR, which can effectively capture N 2 molecules and elongate the N≡N bond by the hybridization between Fe 3d orbitals and N 2p orbitals. This hybridization activates N 2 molecules and triggers the subsequent NOR. In addition, a NOR-related pathway has been proposed that reveals the positive effect of O 2 derived from the parasitic OER on the NO 3 – formation.
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