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FeN/FeN 界面内置电场可有效电化学还原 CO 为 CO。

The built-in electric field across FeN/FeN interface for efficient electrochemical reduction of CO to CO.

机构信息

State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, China.

Department of Chemistry, Brown University, Providence, RI, USA.

出版信息

Nat Commun. 2023 Mar 28;14(1):1724. doi: 10.1038/s41467-023-37360-9.

Abstract

Nanostructured metal-nitrides have attracted tremendous interest as a new generation of catalysts for electroreduction of CO, but these structures have limited activity and stability in the reduction condition. Herein, we report a method of fabricating FeN/FeN nanoparticles with FeN/FeN interface exposed on the NP surface for efficient electrochemical CO reduction reaction (CORR). The FeN/FeN interface is populated with Fe-N and Fe-N coordination sites respectively that show the desired catalysis synergy to enhance the reduction of CO to CO. The CO Faraday efficiency reaches 98% at -0.4 V vs. reversible hydrogen electrode, and the FE stays stable from -0.4 to -0.9 V during the 100 h electrolysis time period. This FeN/FeN synergy arises from electron transfer from FeN to FeN and the preferred CO adsorption and reduction to *COOH on FeN. Our study demonstrates a reliable interface control strategy to improve catalytic efficiency of the Fe-N structure for CORR.

摘要

纳米结构金属氮化物作为新一代电还原 CO 的催化剂引起了极大的关注,但这些结构在还原条件下的活性和稳定性有限。在此,我们报告了一种在 NP 表面上暴露 FeN/FeN 界面的 FeN/FeN 纳米颗粒的制备方法,用于高效电化学 CO 还原反应 (CORR)。FeN/FeN 界面分别含有 Fe-N 和 Fe-N 配位位,显示出所需的催化协同作用,以增强 CO 的还原为 CO。在相对于可逆氢电极的-0.4 V 下,CO 的法拉第效率达到 98%,并且在 100 h 的电解时间段内,FE 从-0.4 到-0.9 V 保持稳定。这种 FeN/FeN 协同作用源于从 FeN 到 FeN 的电子转移,以及对 FeN 上*COOH 的 CO 吸附和还原的偏好。我们的研究表明,一种可靠的界面控制策略可以提高 CORR 中 Fe-N 结构的催化效率。

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