分子筛改性铜硅催化剂对顺酐选择性加氢反应性能的影响  

EFFECT OF ZEOLITE-MODIFIED COPPER-SILICON CATALYST ONSELECTIVE HYDROGENATION OF MALEIC ANHYDRIDE

作　　者：刘天意 黄卫国 邢闯 伞晓广 Liu Tianyi;Huang Weiguo;Xing Chuang;San Xiaoguang(School of Chemical Engineering,Shenyang University of Chemical Technology,Shenyang 110142;Zhejiang Liansheng Chemical Co.,Ltd.;School of Biological and Chemical Engineering,Zhejiang University of Science and Technology)

机构地区：[1]沈阳化工大学化学工程学院,沈阳110142 [2]浙江联盛化学股份有限公司 [3]浙江科技大学生物与化学工程学院

出　　处：《石油炼制与化工》2024年第5期58-66,共9页Petroleum Processing and Petrochemicals

基　　金：浙江省自然科学基金项目探索项目(LY23B060002,LY23B060001);国家自然科学基金面上项目(22278376);浙江科技学院研究生教学改革研究项目(2021yjsjg04)。

摘　　要：采用蒸氨法将不同分子筛掺杂在CuSi催化剂中,考察了ZSM-5,MOR,4A,5A分子筛对Cu基催化剂顺酐(MA)选择性加氢反应性能的影响。相比于未经分子筛掺杂的CuSi催化剂,分子筛掺杂催化剂的活性明显提高。CuSi-4A催化剂中Cu粒子的分散较差,导致其比表面积小,H 2在催化剂上的吸附能力最弱,CuSi-4A活性明显低于CuSi-MOR,CuSi-ZSM-5,CuSi-5A催化剂。而CuSi-MOR催化剂有丰富的Cu+,Cu粒子更小,表现出最佳的催化性能,在反应温度为280℃、氢酐摩尔比为79、质量空速为0.12 h-1的反应条件下,MA转化率高达99.6%,γ-丁内酯选择性为47.9%。在蒸氨法制备CuSi催化剂过程中掺杂分子筛,可提高金属分散度,为催化剂设计提供一定的借鉴。In this paper,the effects of ZSM-5,MOR,4A and 5A zeolites on the selective hydrogenation of maleic anhydride over copper-based catalysts were investigated by using ammonia evaporation method to treat CuSi catalysts.The results showed that the dispersion of copper particles in CuSi-4A catalyst was poor,which resulted in a small specific surface area;the adsorption capacity of H 2 on CuSi-4A catalyst was the weakest,and the activity of CuSi-4A was significantly lower than that of CuSi-MOR,CuSi-ZSM-5 and CuSi-5A catalysts.The CuSi-MOR catalyst was rich in Cu+,and the copper particles were smaller.Under the reaction conditions of a temperature of 280℃,a molar ratio of hydrogen to anhydride of 79 and a WHSV of 0.12 h-1,the maleic anhydride conversion rate was as high as 99.6%,and the selectivity ofγ-butyrolactone anhydride was 47.9%.Compared with CuSi catalysts without zeolite doping,the catalytic activity was significantly lower than that of the zeolite doped catalysts.Therefore,the use of zeolite as part of the silicon source in the process of preparing catalyst by ammonia evaporation can provide certain reference for improving metal dispersion and catalyst design.

关 键 词：顺酐 CuSi催化剂 选择性加氢 分子筛 丁二酸酐 γ -丁内酯 

分 类 号：O643.36[理学—物理化学] TQ235[理学—化学]