Journal
NATURE COMMUNICATIONS
Volume 9, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-018-03543-y
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Funding
- Ministry of Science and Technology of China [2017YFB0602201, 2016YFA0204100, 2016YFA0200200]
- National Natural Science Foundation of China [21690082, 91545203, 21373166, 21503176]
- Chinese Academy of Sciences [QYZDB-SSW-JSC020]
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The development of new methods for the direct transformation of methanol into two or multi-carbon compounds via controlled carbon-carbon coupling is a highly attractive but challenging goal. Here, we report the first visible-light-driven dehydrogenative coupling of methanol into ethylene glycol, an important chemical currently produced from petroleum. Ethylene glycol is formed with 90% selectivity and high efficiency, together with hydrogen over a molybdenum disulfide nanofoam-modified cadmium sulfide nanorod catalyst. Mechanistic studies reveal a preferential activation of C-H bond instead of O-H bond in methanol by photoexcited holes on CdS via a concerted proton-electron transfer mechanism, forming a hydroxymethyl radical (center dot CH2OH) that can readily desorb from catalyst surfaces for subsequent coupling. This work not only offers an alternative nonpetroleum route for the synthesis of EG but also presents a unique visible-light-driven catalytic C-H activation with the hydroxyl group in the same molecule keeping intact.
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