Статья

Atomic Tuning of Single-Atom Fe–N–C Catalysts with Phosphorus for Robust Electrochemical CO<sub>2</sub> Reduction

Ke LiDepartment of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, ChinaShengbo ZhangKey Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, ChinaXiuli ZhangSchool of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, ChinaShuang LiuDepartment of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, ChinaHaosong JiangDepartment of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, ChinaTaoli JiangDepartment of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, ChinaChunyue ShenDepartment of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, ChinaYi YuSchool of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, ChinaWei ChenDepartment of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China

2022en

ABI

Аннотация

The electrochemical reduction of CO2 to produce carbon-based fuels and chemicals possesses huge potentials to alleviate current environmental problems. However, it is confronted by great challenges in the design of active electrocatalysts with low overpotentials and high product selectivity. Here we report the atomic tuning of a single-Fe-atom catalyst with phosphorus (Fe–N/P–C) on commercial carbon black as a robust electrocatalyst for CO2 reduction. The Fe–N/P–C catalyst exhibits impressive performance in the electrochemical reduction of CO2 to CO, with a high Faradaic efficiency of 98% and a high mass-normalized turnover frequency of 508.8 h–1 at a low overpotential of 0.34 V. On the basis of ex-situ X-ray absorption spectroscopy measurements and DFT calculations, we reveal that the tuning of P in single-Fe-atom catalysts reduces the oxidation state of the Fe center and decreases the free-energy barrier of *CO intermediate formation, consequently maintaining the electrocatalytic activity and stability of single-Fe-atom catalysts.

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Идентификаторы

DOI: 10.1021/acs.nanolett.1c04382

Цитирования и источники

Цитирований: 2Использованных источников: 0

Показатели — AkademScholar