Dual-Fluorinated Ni Single Atom Catalyst for Efficient Artificial Photosynthetic Diluted CO2 Reduction
Qimeng Sun1, Lujie Jin2, Weijie He1, Xiaoyong Xia1, Youyong Li2,3, Dongyun Chen1（陈冬赟）*, Qingfeng Xu1（徐庆锋）*, Jianmei Lu1,4（路建美）*
1College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123, P. R. China
2Institute of Functional Nano & Soft Materials (FUNSOM)Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University Suzhou 215123, P. R. China
3Macao Institute of Materials Science and Engineering Macau University of Science and Technology Taipa, Macau SAR 999078, P. R. China
4Suzhou Laboratory Suzhou 215123, P. R. China
Adv. Mater. 2025, 37, 2503414
Abstract: The development of efficient photocatalysts to convert dilute CO2 from flue gas into high value-added products is a promising approach to achieving carbon neutrality. In this work, a dual-fluorinated Ni single atom photocatalyst is reported for the photoreduction of diluted CO2 to CO. Under a dilute CO2 (10%) atmosphere, TPB-SA2F-Ni achieves the highest reported CO yield (30344.4 µmol g−1 h−1) among heterogeneous catalytic systems with a CO selectivity of 98%. Kevin probe force microscopy and photoelectrochemical characterizations indicate that dual-fluorination strategy enhances photoexcited electron transfer between the photosensitizer and photocatalyst by optimizing the conjugated electronic structure. Pore size distribution and CO2 adsorption experiments show that the uniform microporous structure induced by the dual-F site further enhanced the ability of the Ni-N2O2 active site to capture CO2 molecules. Density functional theory calculations indicate that the high CO yield of TPB-SA2F-Ni stems from a lowered energy barrier for *COOH intermediate formation.
Article information: //doi.org/10.1002/adma.202503414
