Integrating Zeolite and Layered Double Hydroxide for Highly Selective Catalytic Production ofγ-Valerolactone  

作　　者：Mingkun Gao Guoju Yang Guangyuan He Risheng Bai Jialiang Li Yinghao Liu Qiang Zhang Guangrui Chen Donghai Mei Jihong Yu 

机构地区：[1]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,College of Chemistry,International Center of Future Science,Jilin University,Changchun 130012 [2]School of Materials Science and Engineering,Tiangong University,Tianjin 300387

出　　处：《CCS Chemistry》2024年第3期652-662,共11页中国化学会会刊（英文）

基　　金：the National Natural Science Foundation of China(grant nos.22288101,21920102005,and 21835002);the National Key Research and Development Program of China(grant nos.2021YFA1501202 and 2022YFA1503600);the 111 Project(grant no.B17020)for their financial support of this work.

摘　　要：The production ofγ-valerolactone(GVL)from biomass derivatives levulinic acid(LA)based on acidbase metallic catalysts offers a sustainable pathway to the synthesis of valuable chemicals and biofuels.However,the development of efficient metallic catalysts with tunable Lewis acid–base and Brønsted acid sites remains a challenge.Herein,for the first time,we integrated zeolite and layered double hydroxide(LDH),in a core–shell structure,wherein zeolite and CoFe-LDH provided the Brønsted acidic sites and Lewis acid sites,respectively.Meanwhile,oxygen vacancies(OV_(x))acting as Lewis bases were generated on the surface of LDH via Ga doping.An efficient cascade catalytic reaction from LA to GVL was successfully achieved over the designed Beta@LDH-OVx catalyst,affording a superior conversion of LA(>99.9%)and an impressive selectivity to GVL(89.18%).Importantly,the“memory effect”of LDH endowed the catalyst with excellent regeneration of metal active sites.Density functional theory calculations revealed that the introduced OVx facilitated the adsorption of carbonyl oxygen in LA and boosted the production of GVL through the synergistic effect of acid/base sites in the composite catalyst.This work presents a rational design route for the construction of multifunctional catalysts by coupling zeolites and LDHs for highly selective catalytic conversion of biomass.

关 键 词：ZEOLITE layered double hydroxide oxygen vacancies BIOMASS γ-valerolactone 

分 类 号：O64[理学—物理化学]