A nickel gallium oxide chlorophyll mimic for green methanol synthesis

Rui Song, Zhiwen Chen (), Chenyue Qiu, Yang-fan Xu, Andrew Wang, Xiaoliang Yan, Yubin Fu, Paul N. Duchesne, Emerson MacNeil, Jigang Zhou, Chaoqian Ai, Jiuli Guo, Chaoran Li, Xingda An, Zhijie Chen, Jiajun Han, Dengwei Jing, Athanasios A. Tountas, Jessica Ye, Guangming Cai, Joel Y. Y. Loh, Abhinav Mohan, Wenqiang Qu, Zhihao Zhu, Camilo J. Viasus, Lu Wang, Chang Xu, Zhao Li, Xiaohong Zhang, Alán Aspuru-Guzik, Chandra Veer Singh (), Le He () and Geoffrey A. Ozin ()
Additional contact information
Rui Song: Soochow University, Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Zhiwen Chen: Jilin University, Key Laboratory of Automobile Materials, Ministry of Education, and School of Materials Science and Engineering
Chenyue Qiu: University of Toronto, Department of Materials Science and Engineering
Yang-fan Xu: Soochow University, Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Andrew Wang: University of Toronto, Solar Fuels Group, Department of Chemistry
Xiaoliang Yan: Taiyuan University of Technology, College of Chemistry and Chemical Engineering and State Key Laboratory of Clean and Efficient Coal Utilization
Yubin Fu: Max Planck Institute of Microstructure Physics
Paul N. Duchesne: Queen’s University, Department of Chemistry
Emerson MacNeil: Queen’s University, Department of Chemistry
Jigang Zhou: Canadian Light Source Inc
Chaoqian Ai: Xi’an International University, College of Engineering
Jiuli Guo: Anyang Normal University, School of Chemistry and Chemical Engineering
Chaoran Li: Soochow University, Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Xingda An: Soochow University, Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Zhijie Chen: Soochow University, Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Jiajun Han: China Agricultural University, Department of Applied Chemistry, College of Science
Dengwei Jing: Xi’an Jiaotong University, International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering
Athanasios A. Tountas: University of Toronto, Solar Fuels Group, Department of Chemistry
Jessica Ye: University of Toronto, Solar Fuels Group, Department of Chemistry
Guangming Cai: University of Toronto, Department of Chemical Engineering and Applied Chemistry
Joel Y. Y. Loh: University of Manchester, Department of Electrical and Electronic Engineering, Photon Science Institute
Abhinav Mohan: University of Toronto, Solar Fuels Group, Department of Chemistry
Wenqiang Qu: University of Toronto, Solar Fuels Group, Department of Chemistry
Zhihao Zhu: University of Toronto, Solar Fuels Group, Department of Chemistry
Camilo J. Viasus: University of Toronto, Solar Fuels Group, Department of Chemistry
Lu Wang: Shenzhen, School of Science and Engineering, The Chinese University of Hong Kong
Chang Xu: Shenzhen, School of Science and Engineering, The Chinese University of Hong Kong
Zhao Li: University of Toronto, Solar Fuels Group, Department of Chemistry
Xiaohong Zhang: Soochow University, Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Alán Aspuru-Guzik: University of Toronto, Department of Materials Science and Engineering
Chandra Veer Singh: University of Toronto, Department of Materials Science and Engineering
Le He: Soochow University, Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Geoffrey A. Ozin: University of Toronto, Solar Fuels Group, Department of Chemistry

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Light-driven methanol synthesis from CO2 provides a sustainable fuel source and approach to carbon neutralization. Mimicking natural photosynthesis could improve gas-solid photocatalytic efficiency, but it remains highly challenging due to the absence of well-organized mass and charge transfer networks in artificial materials. Herein, we report a chlorophyll-mimicking, nano-pigment nickel gallium oxide, which facilitates discrete light/dark reactions and proton-mediated charge transfer for efficient photocatalytic hydrogenation of CO2 to methanol. This nano-pigment features surface frustrated Lewis pairs, enabling heterolytic hydrogen splitting into H- and H+. The H- acts analogously to nicotinamide adenine dinucleotide phosphate in natural photosynthesis, with Ni(II)/Ni(III) and OH(-I) respectively serving as conduits for ion transport of H- and H+ to the Ni site, where they subsequently react with CO2, mimicking natural carbon fixation. This approach establishes a chlorophyll-mimetic structure for photocatalytic stepwise CO2 hydrogenation, achieving 3.0% quantum efficiency, 3.20 mmol·h-1·g-1 methanol activity, and 79.6% selectivity.

Date: 2025
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DOI: 10.1038/s41467-025-65560-y

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