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煅烧温度对Cu/HMOR催化剂结构及其催化二甲醚羰基化反应性能影响
张雪,李宇萍,仇松柏,王铁军*,马隆龙,张琦,定明月
作者单位E-mail
张雪 中国科学院广州能源研究所可再生能源与天然气水合物重点实验室广州510640中国科学院大学北京100049  
李宇萍 中国科学院广州能源研究所可再生能源与天然气水合物重点实验室广州510640  
仇松柏 中国科学院广州能源研究所可再生能源与天然气水合物重点实验室广州510640  
王铁军* 中国科学院广州能源研究所可再生能源与天然气水合物重点实验室广州510640 wangtj@ms.giec.ac.cn 
马隆龙 中国科学院广州能源研究所可再生能源与天然气水合物重点实验室广州510640  
张琦 中国科学院广州能源研究所可再生能源与天然气水合物重点实验室广州510640  
定明月 中国科学院广州能源研究所可再生能源与天然气水合物重点实验室广州510640  
摘要:
采用离子交换法在不同煅烧温度下制备HMOR负载Cu(Cu/HMOR)催化剂,用于催化二甲醚(DME)羰基化合成乙酸甲酯(MA)反应. 活性测试结果表明430 oC煅烧制得Cu/HMOR具有较好催化活性,在210 oC、1.5 MPa、空速4883 h-1下DME转化率为97.2%,MA选择性为97.9%. 对催化剂进行X射线衍射、N2物理吸附、NH3程序升温脱附、CO程序升温脱附及拉曼方法表征. 催化剂经一定的煅烧温度有利于Cu离子迁移及扩散和硝酸铜完全分解,从而使HMOR载体具有较多的酸性活性位、大比表面、适宜的微孔结构以及更多的CO吸附位.
关键词:  二甲醚,乙酸甲酯,催化,羰基化,丝光沸石
DOI:10.1063/1674-0068/26/02/220-224
分类号:
基金项目:
Effect of Calcination Temperature on Catalytic Activity and Textual Property of Cu/HMOR Catalysts in Dimethyl Ether Carbonylation Reaction
Xue Zhang,Yu-ping Li,Song-bai Qiu,Tie-jun Wang*,Long-long Ma,Qi Zhang,Ming-yue Ding
Abstract:
The effect of calcination temperature on the catalytic activity for the dimethyl ether (DME) carbonylation into methyl acetate (MA) was investigated over mordenite supported copper (Cu/HMOR) prepared by ion-exchange process. The results showed that the catalytic activ-ity was obviously affected by the calcination temperature. The maximal DME conversion of 97.2% and the MA selectivity of 97.9% were obtained over the Cu/HMOR calcined at 430 oC under conditions of 210 oC, 1.5 MPa, and GSHV of 4883 h-1. The obtained Cu/HMOR catalysts were characterized by powder X-ray diffraction, N2 absorption, NH3 temperature program desorption, CO temperature program desorption, and Raman techniques. Proper calcination temperature was effective to promote copper ions migration and diffusion, and led the support HMOR to possess more acid activity sites, which exhibited the complete decomposing of copper nitrate, large surface area and optimum micropore structure, more amount of CO adsorption site and proper amount of weak acid centers.
Key words:  Dimethyl ether, Methyl acetate, Calcination temperature, Carbonylation, HMOR