电极
石墨氮化碳
纳米技术
电化学储能
电催化剂
阴极
作者
Chuhao Liu,Yue Wu,Kaian Sun,Jinjie Fang,Aijian Huang,Yuan Pan,Weng-Chon Cheong,Zewen Zhuang,Zhongbin Zhuang,Qiuhua Yuan,Huolin L. Xin,Chao Zhang,Jiangwei Zhang,Hai Xiao,Chen Chen,Yadong Li
出处
期刊:Chem
[Elsevier]
日期:2021-05-13
卷期号:7 (5): 1297-1307
被引量:18
标识
DOI:10.1016/j.chempr.2021.02.001
摘要
Summary Atomically dispersed Fe–N–C catalyst has shown great performance in the CO2-to-CO conversion, yet the high CO selectivity is achieved only within a rather narrow potential range, which cannot well meet the requirements for the following CO dimerization or hydrogenation. Here, we developed a hydrogen-pyrolysis etching strategy to precisely manipulate the uncoordinated N dopants in the Fe–N–C catalyst. This strategy could preferentially eliminate pyridinic and pyrrolic N atoms while leaving graphitic N. The resulting catalyst gave a CO faradaic efficiency (FECO) above 90% over a broad window from −0.3 to −0.8 V (versus RHE) (in particular, FECO > 97% at −0.6 V). In situ ATR-SEIRAS and first-principle calculations further revealed that this strategy can not only suppress the parasitic H2 generation but also promote CO2 activation and protonation with the assistance of co-adsorbed H2O on the “atomic interface” of “FeN4/graphitic N.”
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