A nickel gallium oxide chlorophyll mimic for green methanol synthesis

Light-driven methanol synthesis from CO<sub>2</sub> 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 CO<sub>2</sub> to methanol. This nano-pigment features surface frustrated Lewis pairs, enabling heterolytic hydrogen splitting into H<sup>-</sup> and H<sup>+</sup>. The H<sup>-</sup> 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<sup>-</sup> and H<sup>+</sup> to the Ni site, where they subsequently react with CO<sub>2</sub>, mimicking natural carbon fixation. This approach establishes a chlorophyll-mimetic structure for photocatalytic stepwise CO<sub>2</sub> hydrogenation, achieving 3.0% quantum efficiency, 3.20 mmol·h<sup>-1</sup>·g<sup>-1</sup> methanol activity, and 79.6% selectivity.

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Journal
Nature Communications
Published
2025-11-26
DOI
https://doi.org/10.1038/s41467-025-65560-y
Citations
1
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
0.36

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article

A nickel gallium oxide chlorophyll mimic for green methanol synthesis

Camilo J. Viasus, Yubin Fu, Joel Y. Y. Loh, Chenyue Qiu et al.
1 citations
Nature Communications
CO2 Reduction Techniques and Catalysts
0.36
article

A nickel gallium oxide chlorophyll mimic for green methanol synthesis

Camilo J. Viasus, Yubin Fu, Joel Y. Y. Loh, Chenyue Qiu, Yangfan Xu, Jigang Zhou, Xingda An, Athanasios A. Tountas, Zhiwen Chen, Wenqiang Qu, Paul N. Duchesne, Le He, Jessica Ye, Jiuli Guo, Dengwei Jing, Guangming Cai, Alán Aspuru‐Guzik, Xiaoliang Yan, Chandra Veer Singh, Rui Song, Abhinav Mohan, Zhihao Zhu, Chaoqian Ai, Geoffrey A. Ozin, Emerson M. MacNeil, Xiaohong Zhang, Lu Wang, Zhao Li, Andrew Wang, Chang Xu, Zhijie Chen, Chaoran Li, Jiajun Han
article en
1 citations

Abstract

Light-driven methanol synthesis from CO<sub>2</sub> 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 CO<sub>2</sub> to methanol. This nano-pigment features surface frustrated Lewis pairs, enabling heterolytic hydrogen splitting into H<sup>-</sup> and H<sup>+</sup>. The H<sup>-</sup> 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<sup>-</sup> and H<sup>+</sup> to the Ni site, where they subsequently react with CO<sub>2</sub>, mimicking natural carbon fixation. This approach establishes a chlorophyll-mimetic structure for photocatalytic stepwise CO<sub>2</sub> hydrogenation, achieving 3.0% quantum efficiency, 3.20 mmol·h<sup>-1</sup>·g<sup>-1</sup> methanol activity, and 79.6% selectivity.

Nature CommunicationsVol. 16(1)
Fleming College (CA), University of Toronto (CA), Jilin University (CN), Queen's University (CA), University of Manchester (GB), Soochow University (CN), Max Planck Institute of Microstructure Physics (DE), Chinese University of Hong Kong, Shenzhen (CN), Anyang Normal University (CN), Xi’an International University (CN), China Agricultural University (CN), Canadian Light Source (Canada) (CA), Xi'an Jiaotong University (CN), Taiyuan University of Technology (CN)
Alexander von Humboldt-Stiftung, National Natural Science Foundation of China, Government of Jiangsu Province, University of Toronto, Natural Science Foundation of Jiangsu Province, Ministero dello Sviluppo Economico, Natural Sciences and Engineering Research Council of Canada, Ontario Ministry of Research and Innovation
Openalex Percentile: Top 36%
CO2 Reduction Techniques and Catalysts
0.36
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