Photosynthesis of CH<sub>3</sub>OH via oxygen-atom-grafting from CO<sub>2</sub> to CH<sub>4</sub> enabled by AuPd/GaN.

Su, Hui; Han, Jing-Tan; Miao, Botong; Salehi, Mahdi; Li, Chao-Jun · Nat Commun · 2024

basic_science · Level V

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Abstract

The direct co-conversion of methane and carbon dioxide into valuable chemicals has been a longstanding scientific pursuit for carbon neutrality and combating climate change. Herein, we present a photo-driven chemical process that reforms these two major greenhouse gases together to generate green methanol and CO, two high-valued industrial chemicals. Isotopic labeling and control experiments indicate an oxygen-atom-graft occurs, wherein CO<sub>2</sub> transfers one O into the C-H bond of CH<sub>4</sub> via photo-activated interfacial catalysis with AuPd nanoparticles supported on GaN. The photoexcited AuPd/GaN interface effectively orchestrates the CH<sub>4</sub> oxidation and the CO<sub>2</sub> reduction producing 13.66 mmol g<sup>-1</sup> of CH<sub>3</sub>OH yield over 10 h. This design provides a solid scientific basis for the photo-driven oxygen-atom-grafting process to be further extended to visible light region.