CuCl/SiO_2-TiO_2催化剂的结构及其催化甲醇氧化羰基化反应性能  

Structure of CuCl/SiO_2-TiO_2 Catalyst and Its Catalytic Properties for Oxidative Carbonylation of Methanol

作　　者：李忠[1] 刘树森[1] 任军[1] 牛燕燕[1] 郑华艳[1] 赵强[1] 崔丽萍[1] 

机构地区：[1]太原理工大学煤科学与技术教育部和山西省重点实验室,山西太原030024

出　　处：《催化学报》2010年第6期683-688,共6页

基　　金：国家自然科学基金(20606022和20976113);国家自然科学基金重点项目(20936003);国家重点基础研究发展计划(973计划;2005CB221204);山西省研究生优秀创新项目(20093044)

摘　　要：在微波辐射条件下,将CuCl快速分散到载体表面制得CuCl/SiO2-TiO2催化剂,利用X射线衍射、透射电镜、N2吸附-脱附、热重、H2程序升温还原和CO程序升温脱附对催化剂进行了表征.结果表明,微波辐射制备的催化剂中CuCl和载体发生了强相互作用,比传统加热制备的催化剂中形成更多的易还原铜物种,吸附CO的能力更强.在甲醇液相氧化羰基化反应中,微波辐射制备的催化剂上甲醇转化率为11.7%,碳酸二甲酯选择性达96.5%,高于相同条件下传统加热制备催化剂的活性.Microwave heating for a mixture of CuCl and SiO2-TiO2 support was used to prepare a CuCl/SiO2-TiO2 catalyst with high dispersion of CuCl on the support surface in a short time.X-ray diffraction,transmission electron microscopy,N2 adsorption-desorption,thermal gravimetric analysis,H2 temperature-programmed reduction,and CO temperature-programmed desorption were carried out to examine the bulk and surface properties of the CuCl/SiO2-TiO2 catalyst.The characterization results showed that in the CuCl/SiO2-TiO2 catalyst prepared by microwave heating,a great amount of CuCl particles strongly attached to the SiO2-TiO2 support as compared with that prepared by conventional heating,resulting in a lower reduction temperature of copper species and a stronger adsorption to CO.Microwave heating also caused that the mass loss temperature of part CuCl was higher than 1200℃,which could be attributed to the formation of a strong Cu–O coordinate bond between CuCl and the SiO2-TiO2 support.Catalytic test results showed that the CuCl/SiO2-TiO2 catalyst prepared by microwave heating exhibited methanol conversion of 11.7% and dimethyl carbonate selectivity of 96.5%,higher than that prepared by conventional heating in liquid-phase oxidative carbonylation of methanol.

关 键 词：微波辐射 氯化亚铜 二氧化硅 二氧化钛 负载型催化剂 甲醇 氧化羰基化 碳酸二甲酯 

分 类 号：O643.32[理学—物理化学]