低碳化学与化工2025，Vol.50Issue(11)：52-63,12.DOI:10.12434/j.issn.2097-2547.20250305
Ru@ZSM-5催化纤维素和甲醇耦合转化制γ-戊内酯
Integrated conversion of cellulose and methanol to γ-valerolactone catalyzed by Ru@ZSM-5
摘要
Abstract
γ-valerolactone(GVL)is an important biomass derivative,which is produced by"hydrolysis-hydrogenation"route of cellulose.However,at present,liquid acid and supported metal mixed catalysts are mainly used,which have the problem of low GVL yield.Therefore,a new route of"alcoholysis-hydrogenation"of cellulose and methanol was proposed.ZSM-5 molecular sieve pore confined Ru catalyst(Ru@ZSM-5)was designed with dual functional active sites of metal and acid by"ligand protection strategy"in-situ hydrothermal method,and Ru nanoclusters were encapsulated within the pore channels of ZSM-5 molecular sieve.TEM characterization and encapsulation degree test confirm that the average diameter of Ru clusters is only 0.57 nm,and a large number of Ru clusters(92.7%)are confined within the ten-membered ring cross pore channels of ZSM-5 molecular sieve.The results show that Ru@ZSM-5 exhibits excellent catalytic performance in the integrated conversion of cellulose and methanol to γ-valerolactone.Under the conditions of 230 ℃,3 MPa H2 and volume ratio of water to methanol of 10%,the GVL yield is 51.1%(reaction for six hours),far superior to traditional supported Ru/ZSM-5,Ru/SiO2+ZSM-5,and Ru/Al2O3+ZSM-5 catalysts.Due to the confinement effect of ZSM-5 molecular sieve pores,Ru@ZSM-5 shows high stability,with the GVL yield of 51.5%and the particle size of Ru clusters remains 0.59 nm after five reaction cycles.However,Ru/ZSM-5 undergoes severe deactivation,and the Ru nanoparticles dispersed on the outer surface of ZSM-5 molecular sieve suffer from significant sintering,with the average particle size of 6.57 nm.关键词
纤维素/甲醇/γ-戊内酯/Ru@ZSM-5/生物质Key words
cellulose/methanol/γ-valerolactone/Ru@ZSM-5/biomass分类
化学工程引用本文复制引用
高晓庆,朱善辉,郑洪岩..Ru@ZSM-5催化纤维素和甲醇耦合转化制γ-戊内酯[J].低碳化学与化工,2025,50(11):52-63,12.基金项目
国家自然科学基金(22202148,22278416) （22202148,22278416）
山西省基础研究计划(202203021212326) （202203021212326）
太原工业学院引进人才科研资助项目(2022KJ051,2022LJ030) （2022KJ051,2022LJ030）
中国科学院山西煤炭化学研究所自主创新基金(SCIC-DT-2023-02). （SCIC-DT-2023-02）
