Photosynthesis of CH3OH via oxygen-atom-grafting from CO2 to CH4 enabled by AuPd/GaN

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 CO2 transfers one O into the C–H bond of CH4 via photo-activated interfacial catalysis with AuPd nanoparticles supported on GaN. The photoexcited AuPd/GaN interface effectively orchestrates the CH4 oxidation and the CO2 reduction producing 13.66 mmol g−1 of CH3OH 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.