Cooperative catalysis of Co single atoms and nanoparticles enables selective CAr-OCH_(3) cleavage for sustainable production of lignin-based cyclohexanols

查看全文 作　　者：Baoyu [1,3]Wang;Peng [2]Zhou;Ximing [3]Yan;Hu [1]Li;Hongguo [1,4]Wu;Zehui [2]Zhang

机构地区：[1]National Key Laboratory of Green Pesticide,Key Laboratory of Green Pesticide&Agricultural Bioengineering,Ministry of Education,State-Local Joint Laboratory for Comprehensive Utilization of Biomass,Center for R&D of Fine Chemicals,Guizhou University,Guiyang 550025,Guizhou,China;[2]Key Laboratory of Catalysis and Material Sciences of the State Ethnic Affairs Commission&Ministry of Education,College of Chemistry and Material Sciences,South-Central University for Nationalities,Wuhan 430074,Hubei,China;[3]Guangxi Key Laboratory of Green Chemical Materials and Safety Technology,Beibu Gulf University,Qinzhou 535011,Guangxi,China;[4]College of Pharmacy,Guizhou University,Guiyang 550025,Guizhou,China

出　　处：《Journal of Energy Chemistry》索引2023年第4期,共15页

基　　金：the Guizhou Provincial S&T Project(ZK[2022]011);the National Natural Science Foundation of China(21908033,21922513);the Natural Science Foundation of Guangxi Zhuang Autonomous Region(2020GXNSFAA297072);the Fok Ying-Tong Education Foundation(161030)。 摘　　要：In this work,a dual-size MOF-derived Co catalyst(0.2Co_(1-NPs)@NC)composed of single atoms(Co_(1))and highly dispersed nanoparticles(Co NPs)was prepared by in-situ Zn evaporation for the highperformance conversion of lignin-derived o-methoxyphenols(lignin oil)to cyclohexanols(up to 97%yield)via cascade demethoxylation and dearomatization.Theoretical calculations elaborated that the dual-size Co catalyst exhibited a cooperative effect in the selective demethoxylation process,in which the Co NPs could initially dissociate hydrogen at lower energies while Co1remarkably facilitated the cleavage of the C_(Ar)-OCH_(3)bond.Moreover,the intramolecular hydrogen bonds formed in the omethoxy-containing phenols were found to result in a decrease in the bond energy of the C_(Ar)-OCH_(3)bond,which was more prone to be activated by the dual-size Co sites.Notably,the pre-hydrogenated intermediate(e.g.,2-methoxycyclohexanol from guaiacol)is difficult to undergo demethoxylation,indicating that the selective C_(Ar)-OCH_(3)bond cleavage is a prerequisite for the synthesis of cyclohexanols.The 0.2Co_(1-NPs)@NC catalyst was highly recyclable with a neglect decline in activity during five consecutive cycles.This cooperative catalytic strategy based on the metal size effect opens new avenues for biomass upgrading via enhanced C-O bond cleavage of high selectivity. 关键词：Biomass conversion Heterogeneous catalysis C-O bond cleavage Lignin valorization CYCLOHEXANOLS

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Cooperative catalysis of Co single atoms and nanoparticles enables selective CAr-OCH_(3) cleavage for sustainable production of lignin-based cyclohexanols

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