炭载钌催化剂的微波制备及其水相乙酰丙酸加氢性能（英文）  

Aqueous phase hydrogenation of levulinic acid to γ-valerolactone on supported Ru catalysts prepared by microwave-assisted thermolytic method

作　　者：李闯[1] 倪晓娟[1] 邸鑫[1] 梁长海[1] LI Chuang;NI Xiao-juan;DI Xin;LIANG Chang-hai(Laboratory of Advanced Materials and Catalytic Engineering,Dalian University of Technology,Dalian 116024,China)

机构地区：[1]大连理工大学化工学院先进材料和催化工程实验室,辽宁大连116024

出　　处：《燃料化学学报》2018年第2期161-170,共10页Journal of Fuel Chemistry and Technology

基　　金：supported by the National Key Research&Development Program of the Ministry of Science and Technology of China(2016YFB0600305)

摘　　要：生物质衍生物乙酰丙酸是生物质转化过程中重要的平台分子,对其进行催化加氢可以得到高附加值的产物,是连接生物质转化和石油化工的重要途径。本实验研究了无溶剂微波辅助热解法绿色制备负载型钌基催化剂,以Ru3(CO)12为金属前体,碳纳米管、椰壳活性炭和活性氧化铝为催化剂载体,该制备方法简单易操作,环保高效低能耗,不使用溶剂,避免了杂质的引入和对催化剂的污染,是一种新型负载型贵金属催化剂的制备方法。同样采取传统浸渍法制备Ru/γ-Al2O3-IM。在乙酰丙酸水相催化加氢反应中的催化活性顺序为Ru/AC>Ru/CNT≈Ru/FCNT>Ru/γ-Al2O3-M W≈Ru/γ-Al2O3-IM。比较不同反应溶液水、甲醇、乙醇、苯甲醚、环己烷和丙酮等对于乙酰丙酸催化加氢反应的影响,并通过考察反应温度、反应压力和反应物初始浓度等因素对加氢反应的影响,确定最佳实验条件为:反应温度为90℃,反应压力2.0 MPa,适宜反应物浓度为0.10 g/m L,产品GVL收率大于99%。γ-Valerolactone(GVL),as a sustainable platform chemical,were produced through an aqueous phase hydrogenation of biomass-derived levulinic acid(LA)in the presence of supported ruthenium catalysts,in which the catalysts were prepared by solvent-free microwave-assisted thermolytic method.The effects of catalyst support,reaction media,pressure,temperature and LA initial concentration were investigated to obtain the optimum conditions for highγ-valerolactone yield.5%Ru/AC catalyst exhibits a more superior catalytic performance compared with Ru/CNT,Ru/FCNT,Ru/γ-Al2 O3-MW and Ru/γ-Al2 O3-IM at 100℃and 2.0 MPa of 0.10 g/mL LA concentration in water solution.This superior performance is attributed to the higher dispersion of metallic Ru over coconut shell activated carbon.GVL can be produced with a good yield of>99%under optimum conditions,and has the potential to provide a green,renewable platform for biotransformation.

关 键 词：钌催化剂 微波绿色合成 乙酰丙酸 水相加氢 Γ-丁内酯 

分 类 号：TQ426.6[化学工程]