期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 18, 页码 7203-7208出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c03427
关键词
-
资金
- NSF [CHE-1900020, DMR MRI1126394]
- DOE [DE-AC02-06CH11357]
This work presents a graphite-conjugated diimine macrocyclic Co catalyst that efficiently reduces nitrite to ammonium on graphitic carbon electrodes. Compared to the molecular analogue, this catalyst exhibits a higher reaction rate and may involve a different reaction mechanism.
This work reports on the generation of a graphite-conjugated diimine macrocyclic Co catalyst (GCC-CoDIM) that is assembled at o-quinone edge defects on graphitic carbon electrodes. X-ray photoelectron spectroscopy and X-ray absorption spectroscopy confirm the existence of a new Co surface species with a coordination environment that is the same as that of the molecular analogue, [Co(DIM)Br-2](+). GCC-CoDIM selectively reduces nitrite to ammonium with quantitative Faradaic efficiency and at a rate that approaches enzymatic catalysis. Preliminary mechanistic investigations suggest that the increased rate is accompanied by a change in mechanism from the molecular analogue. These results provide a template for creating macrocycle-based electrocatalysts based on first-row transition metals conjugated to an extreme redox-active ligand.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据