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