Synergy of Single Atoms and Lewis Acid Sites for Efficient and Selective Lignin Disassembly into Monolignol Derivatives

Authors：Meng, Ge; Lan, Wu; Zhang, Lilong; Wang, Shibin; Zhang, Tanhao; Zhang, Shuo; Xu, Ming; Wang, Yu; Zhang, Jian; Yue, Fengxia^*; Wu, Yulong^*; Wang, Dingsheng^*

Source：Journal of the American Chemical Society, 2023, 145(23): 12884-12893.

DOI：10.1021/jacs.3c04028

• CATALYTIC FRACTIONATION
• DEPOLYMERIZATION
• INSIGHTS
• ALLOY
• HYDROGENOLYSIS
• LIGNOCELLULOSE
• CLEAVAGE
• MONOMERS
• BIOMASS

Lignin is the most abundant aromatic polymer from thenatural andrenewable lignocellulosic biomass resource. Developing highly efficientcatalysts for lignin depolymerization to produce valuable monophenolswith high yield and selectivity remains a desirable but challengingtarget in this field. Here, we design a synergistic catalyst combiningatomically dispersed Mo centers and Al Lewis acid sites on a MgO substrate(Mo1Al/MgO) for the depolymerization of Eucalyptus lignin via the beta-aryl ether bond cleavage. A near-theoreticalmonophenol yield of 46% with an ultrahigh selectivity of 92% for coniferyland sinapyl methyl ether, as well as good cycling durability, wasachieved simultaneously by Mo1Al/MgO in an inert N-2 atmosphere. First-principles calculations and control catalyticexperiments confirmed the synergistic catalysis mechanism betweenMo(1)-O-5 single-atom centers and the neighboringAl Lewis acid sites with the participation of a methanol solvent.This study validates the feasibility of designing better-performingcatalysts with synergistic multiactive sites for the efficient andselective disassembly of complex renewable biopolymers into highlyvalue-added products with lower cost and greater security.

• Institution
  北京化工大学; 中国科学院; 浙江工业大学; 清华大学