Coupling photocatalytic CO2 reduction and CH3OH oxidation for selective dimethoxymethane production

Yixuan Wang, Yang Liu, Lingling Wang, Silambarasan Perumal, Hongdan Wang, Hyun Ko, Chung-Li Dong, Panpan Zhang, Shuaijun Wang, Ta Thi Thuy Nga, Young Dok Kim, Yujing Ji, Shufang Zhao, Ji-Hee Kim, Dong-Yub Yee, Yosep Hwang, Jinqiang Zhang, Min Gyu Kim and Hyoyoung Lee ()
Additional contact information
Yixuan Wang: Sungkyunkwan University
Yang Liu: Sungkyunkwan University
Lingling Wang: Sungkyunkwan University
Silambarasan Perumal: Sungkyunkwan University
Hongdan Wang: Sungkyunkwan University
Hyun Ko: Sungkyunkwan University
Chung-Li Dong: Tamkang University
Panpan Zhang: Jiangsu University
Shuaijun Wang: Jiangsu University
Ta Thi Thuy Nga: Tamkang University
Young Dok Kim: Sungkyunkwan University
Yujing Ji: Sungkyunkwan University
Shufang Zhao: Sungkyunkwan University
Ji-Hee Kim: Sungkyunkwan University
Dong-Yub Yee: Sungkyunkwan University
Yosep Hwang: Sungkyunkwan University
Jinqiang Zhang: The University of Adelaide
Min Gyu Kim: Pohang University of Science and Technology
Hyoyoung Lee: Sungkyunkwan University

Nature Communications, 2024, vol. 15, issue 1, 1-15

Abstract: Abstract Currently, conventional dimethoxymethane synthesis methods are environmentally unfriendly. Here, we report a photo-redox catalysis system to generate dimethoxymethane using a silver and tungsten co-modified blue titanium dioxide catalyst (Ag.W-BTO) by coupling CO2 reduction and CH3OH oxidation under mild conditions. The Ag.W-BTO structure and its electron and hole transfer are comprehensively investigated by combining advanced characterizations and theoretical studies. Strikingly, Ag.W-BTO achieve a record photocatalytic activity of 5702.49 µmol g−1 with 92.08% dimethoxymethane selectivity in 9 h of ultraviolet-visible irradiation without sacrificial agents. Systematic isotope labeling experiments, in-situ diffuse reflectance infrared Fourier-transform analysis, and theoretical calculations reveal that the Ag and W species respectively catalyze CO2 conversion to *CH2O and CH3OH oxidation to *CH3O. Subsequently, an asymmetric carbon-oxygen coupling process between these two crucial intermediates produces dimethoxymethane. This work presents a CO2 photocatalytic reduction system for multi-carbon production to meet the objectives of sustainable economic development and carbon neutrality.

Date: 2024
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DOI: 10.1038/s41467-024-49927-1

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