Journal
ACS CATALYSIS
Volume 9, Issue 5, Pages 4441-4447Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b00669
Keywords
lignin depolymerization; redox-neutral; rhodium complex; lignin-first biorefinery; aqueous reaction
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Funding
- 2017 Royal Society International Collaboration Award [IC170044]
- National Natural Science Foundation of China [21773145, 21473109, 21690080, 21690083, 21878288]
- Science and Technology Program of Shaanxi Province [2016KJXX-26]
- Projects for the Academic Leaders and Academic Backbones, Shaanxi Normal University [16QNGG008]
- 111 project [B14041]
- Fundamental Research Funds for the Central Universities [GK201803079]
- DNL cooperation fund CAS [DNL180302]
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A mild redox-neutral lignin depolymerization system featuring a water-soluble binuclear Rh complex has been developed. The catalytic system could be successfully applied to the depolymerization of a lignin-like polymer, alkaline lignin, as well as raw lignocellulose samples to produce aromatic ketones, providing a homogeneous catalytic system for lignin-first biorefinery in water. Mechanistic studies on the model substrate suggest that the reaction proceeds via a metal-catalyzed dehydrogenation step to afford a carbonyl intermediate, followed by C-O bond cleavage to afford ketone and phenol products. Deuterium labeling study shows that the hydrogen used for cleavage of the C-O bond originates from the alcohol moiety in the substrate.
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