期刊
NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-020-20684-1
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资金
- National Natural Science Foundation of China [31971607, 21776020]
- Natural Science Foundation of Liaoning Province [2019MS-019]
- Science Foundation of Dalian Polytechnic University [61010201]
An atomically dispersed Ru catalyst has been developed for efficient cleavage of C-O bonds in C-lignin without hydrogenation of C=C bonds, resulting in high yields of propenylcatechol with high TONs.
C-lignin is a homo-biopolymer, being made up of caffeyl alcohol exclusively. There is significant interest in developing efficient and selective catalyst for depolymerization of C-lignin, as it represents an ideal feedstock for producing catechol derivatives. Here we report an atomically dispersed Ru catalyst, which can serve as an efficient catalyst for the hydrogenolysis of C-lignin via the cleavage of C-O bonds in benzodioxane linkages, giving catechols in high yields with TONs up to 345. A unique selectivity to propenylcatechol (77%) is obtained, which is otherwise hard to achieve, because this catalyst is capable of hydrogenolysis rather than hydrogenation. This catalyst also demonstrates good reusability in C-lignin depolymerization. Detailed investigations by model compounds concluded that the pathways involving dehydration and/or dehydrogenation reactions are incompatible routes; we deduced that caffeyl alcohol generated via concurrent C-O bonds cleavage of benzodioxane unit may act as an intermediate in the C-lignin hydrogenolysis. Current demonstration validates that atomically dispersed metals can not only catalyze small molecules reactions, but also drive the transformation of abundant and renewable biopolymer. C-lignin represents an ideal feedstock for producing catechol derivatives. Here, the authors engineered an atomically dispersed Ru catalyst, which can cleave C-O bonds efficiently and circumvent C=C bonds hydrogenation selectively, thus leading to propenylcatechol in high yields with high TONs.
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