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journal article·2025-03

Modulation of Single‐Iron‐Atom Coordination Environment Toward Three‐Electron Oxygen Reduction for Photocatalytic CH 4 Conversion to CH 3 OH

Laiquan Li, Xiuwen Shi, Lingyue Liu, Ying Tu, Yuhang Liu, Yuhang Zhang, Hong Bin Yang, Shixue Dou, Bin Liu

Small· Volume 21· Issue 11
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Source abstract

Abstract

Abstract By modifying the coordination environment of single‐Fe‐atom active site, effective regulation of the photocatalytic oxygen reduction pathway can be achieved to attain high activity for photocatalytic oxidation of CH 4 to CH 3 OH in an aqueous solution. A comprehensive investigation is conducted to study the impact of different coordination numbers of single Fe atoms on photocatalytic CH 4 oxidation reaction over carbon nitride. Among which, Fe 1 /C 3‐x N 4 with a Fe‐N3 coordination exhibit an exceptional photocatalytic performance in CH 4 oxidation, reaching a remarkable methanol yield of 928.27 µmol g cat −1 , much higher than Fe 1 /C 3 N 4 and Fe 1 /C 3 N 4‐x (308.47 and 473.26 µmol g cat −1 , respectively). Based on a collection of in situ characterizations and time‐dependent density functional theory calculations, it is determined that Fe 1 /C 3‐x N 4 with an optimal coordination number possesses the optimized electronic configuration that enables three‐electron oxygen reduction to generate hydroxyl radicals for photocatalytic conversion of CH 4 to CH 3 OH.
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Research context

Catalysis & surfaces

OpenAlex topics: Catalytic Processes in Materials Science · Advanced Photocatalysis Techniques · Electrocatalysts for Energy Conversion

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Energy Materials Science University of Shanghai for Science and Technology Shanghai 200093 China

School of Materials Science and Engineering Suzhou University of Science and Technology Suzhou 215009 China

Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong SAR 100872 China

International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale Optoelectronics Shenzhen University Shenzhen 518060 China

Department of Materials Science and Engineering Department of Chemistry Hong Kong Institute of Clean Energy (HKICE) & Center of Super‐Diamond and Advanced Films (COSDAF) City University of Hong Kong Hong Kong SAR 999077 China

Funding

National Natural Science Foundation of China · Natural Science Foundation of Jiangsu Province · City University of Hong Kong

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