Coupling photocatalytic CO<sub>2</sub> reduction and CH<sub>3</sub>OH oxidation for selective dimethoxymethane production.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 39025876.
- Also identified by DOI 10.1038/s41467-024-49927-1 and PMC identifier 11258228.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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 CO<sub>2</sub> reduction and CH<sub>3</sub>OH 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<sup>-1</sup> 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 CO<sub>2</sub> conversion to *CH<sub>2</sub>O and CH<sub>3</sub>OH oxidation to *CH<sub>3</sub>O. Subsequently, an asymmetric carbon-oxygen coupling process between these two crucial intermediates produces dimethoxymethane. This work presents a CO<sub>2</sub> photocatalytic reduction system for multi-carbon production to meet the objectives of sustainable economic development and carbon neutrality.