法拉第效率
催化作用
拉曼光谱
碳纳米管
材料科学
可逆氢电极
原位
Atom(片上系统)
电极
纳米技术
化学工程
碳纤维
电化学
电子转移
化学
光化学
物理化学
工作电极
有机化学
嵌入式系统
复合材料
工程类
物理
光学
计算机科学
复合数
作者
Fubin Yang,Haoming Yu,Yun Su,Jingwen Chen,Shixia Chen,Zheling Zeng,Shuguang Deng,Jun Wang
出处
期刊:Nano Research
[Springer Nature]
日期:2022-06-30
卷期号:16 (1): 146-154
被引量:12
标识
DOI:10.1007/s12274-022-4623-9
摘要
Low-coordinated single atom catalysts compared to M−N4 are appealing in optimized electronic structure for CO2 electro-reduction, but the preparation is still very challenging. Herein, a novel single Ni atom catalyst with Ni−N1−C3 configuration is in-situ evolved on curved carbon nanotubes. The obtained Ni−N1−C3 catalyst exhibits a superior CO Faradaic efficiency of 97% and turnover frequency of 2,890 h−1 at −0.9 V versus the reversible hydrogen electrode, as well as long-term stability over 45 h. High current densities exceeding 200 mA·cm−2 and CO Faradaic efficiency of 99% are achieved in flow-cell. Moreover, in-situ potential-and time-dependent Raman spectra identify the key intermediates of *COOH and *CO during CO2-to-CO conversion. Theoretical calculations reveal that the upward-shifted d-band center and charge-rich Ni sites of Ni−N1−C3 facilitate the electron transfer to *COOH and thus reduce the *COOH formation energy barrier. This work demonstrates a strategy for modulating the coordination environment for efficient CO2 reduction.
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