摘要
羰基是有机化学中重要的含氧官能团,许多有机化工原料含有羰基官能团(包括醛、酮、酸等).C-C键和C-H键选择氧化断裂反应是生成羰基官能团的重要途径之一.本文以分子氧为氧化剂,以四氢糠醇为底物选择氧化制备γ-丁内酯(GBL),开发了催化氧化制备羰基化合物的新体系.探讨了反应温度、反应压力、反应时间对催化活性的影响及催化剂循环使用的稳定性;在V/MCN催化剂作用下,四氢糠醇的转化率和GBL的选择性分别达到84.6%和92.8%;循环使用20次,催化剂活性未见明显降低.测试结果表明催化剂活性中心是分散的氧化钒物种,介孔氮化碳(MCN)材料作为一种碱性载体可以有效地抑制GBL的深度氧化.
Abstract
Carbonyl groups are important oxygen-containing functional groups in organic chemistry,and many organic chemical raw materials contain carbonyl functional groups(in-cluding aldehydes,ketones,acids,etc.).The selective oxidative cleavage reaction of C-C and C-H bonds is one of the important pathways for generating carbonyl functional groups.In this paper,molecular oxygen was used as oxidant,and tetrahydrofurfuryl alcohol was used as substrate for selective oxidation to prepare γ-butyrolactone(GBL),a new system for catalytic oxidation of butyrolactone to prepare carbonyl compounds has been developed.Ex-plored the effects of reaction temperature,reaction pressure,and reaction time on catalytic activity and the cyclic stability of catalyst use.Under the action of V/MCN catalyst,the con-version rate of tetrahydrofurfuryl alcohol and the selectivity of GBL reached 84.6%and 92.8%,respectively.After 20 cycles of use,there was no significant decrease in catalyst ac-tivity.The test results indicate that the active center of the catalyst is a dispersed vanadium oxide species,and MCN material as an alkaline carrier can effectively inhibit the deep oxi-dation of GBL.
维普
万方数据