甲酸为氢源的甘油催化选择氢解  

Efficient catalytic hydrogenolysis of glycerol using formic acid as hydrogen source

作　　者：袁静[1] 李舒爽 于磊[1] 刘永梅[1] 曹勇[1] 

机构地区：[1]复旦大学化学系上海市分子催化和功能材料重点实验室,上海200433

出　　处：《催化学报》2013年第11期2066-2074,共9页

基　　金：国家自然科学基金(21273044)~~

摘　　要：以甲酸作为氢源,采用铜基复合金属氧化物催化剂,催化氢解甘油制备1,2-丙二醇,其中液相甲酸的高选择性分解是实现甘油氢解的必要和关键步骤.活性测试表明,高分散的铜和ZrO2载体间的协同作用对甲酸分解和甘油到1,2-丙二醇的转化至关重要,20%Cu/ZrO2催化剂的活性最佳.由于避免使用相对昂贵的化石燃料氢,因而该催化体系在生物质的高值利用方面具有潜在的应用前景.We describe a sustainable,cost-effective,and highly efficient H2 -free protocol for catalytic hydro- genolysis of glycerol to 1,2-propanediol(1,2-PDO) using formic acid(FA) as the H2 source.The pro- cess is catalyzed by an earth-abundant and robust Cu-based metal oxide catalyst,in which the high performance of the Cu catalyst for the in situ generation of H2 gas in the system by highly selective decomposition of FA in an aqueous medium is essential.The activity test results showed that a syn- ergy effect of well-dispersed Cu and amphoteric ZrO2 is essential for FA decomposition as well as for glycerol conversion to 1,2-PDO.The Cu content of the Cu/ZrO2 catalyst prepared by the oxalate gel method has a significant role in the FA-mediated glycerol conversion to 1,2-PDO,and a Cu content of 20 wt% on ZrO2 was identified as the optimum Cu content.Moreover,the creation and maintenance of high component dispersion is essential for high glycerol hydrogenolysis activity of the Cu/ZrO2 system.Because selective hydrogenolysis with minimum use of external fossil-fuel H2 is a critical issue in the realization of biorefinery concepts,the procedure described here is expected to be of broad applicability in biomass use.

关 键 词：铜 二氧化锆 氢解 甘油 甲酸 

分 类 号：O643.32[理学—物理化学]