Coupling photocatalytic CO2 reduction and CH3OH oxidation for selective dimethoxymethane production

被引：16

作者：

Wang, Yixuan ^{[1
,2
,3
]}

Liu, Yang ^{[1
,2
]}

Wang, Lingling ^{[1
,2
]}

Perumal, Silambarasan ^{[1
,2
,3
]}

Wang, Hongdan ^{[1
,2
]}

Ko, Hyun ^{[4
]}

Dong, Chung-Li ^{[5
]}

Zhang, Panpan ^{[6
]}

Wang, Shuaijun ^{[7
]}

Nga, Ta Thi Thuy ^{[5
]}

Kim, Young Dok ^{[1
]}

Ji, Yujing ^{[1
]}

Zhao, Shufang ^{[1
]}

Kim, Ji-Hee ^{[8
]}

Yee, Dong-Yub ^{[8
]}

Hwang, Yosep ^{[1
,2
]}

Zhang, Jinqiang ^{[9
]}

Kim, Min Gyu ^{[10
]}

Lee, Hyoyoung ^{[1
,2
,3
,4
]}

机构：

[1] Sungkyunkwan Univ, Dept Chem, 2066 Seobu Ro, Suwon 16419, South Korea

[2] Sungkyunkwan Univ, Creat Res Inst, 2066 Seobu Ro, Suwon 16419, South Korea

[3] Sungkyunkwan Univ, Multicarbon Prod Ctr CO2, 2066 Seobu Ro, Suwon 16419, South Korea

[4] Sungkyunkwan Univ, Inst Quantum Biophys, 2066 Seobu Ro, Suwon 16419, South Korea

[5] Tamkang Univ, Dept Phys, New Taipei City 25137, Taiwan

[6] Jiangsu Univ, Sch Mat Sci & Engn, Zhenjiang 212013, Peoples R China

[7] Jiangsu Univ, Sch Energy & Power Engn, Zhenjiang 212013, Peoples R China

[8] Sungkyunkwan Univ, Dept Energy Sci, 2066 Seobu Ro, Suwon 16419, South Korea

[9] Univ Adelaide, Sch Chem Engn, Adelaide, SA 5005, Australia

[10] Pohang Univ Sci & Technol, Beamline Res Div, Pohang Accelerator Lab, Pohang 37673, South Korea

来源：

NATURE COMMUNICATIONS | 2024年 / 15卷 / 01期

基金：

新加坡国家研究基金会;

关键词：

METHANOL; CONVERSION; CATALYSTS;

D O I：

10.1038/s41467-024-49927-1

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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 mu mol 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.

引用

页数：15

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