CuCl_2和HY分子筛的表面反应及Cu/Y分子筛的制备及其催化甲醇氧化羰基化（英文）  

Surface reactions of CuCl_2 and HY zeolite during the preparation of CuY catalyst for the oxidative carbonylation of methanol

作　　者：王瑞玉[1] 李忠[2] 

机构地区：[1]中国矿业大学江苏省煤基CO2捕集与地质储存重点实验室,江苏徐州221116 [2]太原理工大学煤科学与技术教育部与山西省重点实验室,山西太原030024

出　　处：《催化学报》2014年第1期134-139,共6页

基　　金：supported by the National Natural Science Foundation of China(20936003);the Fundamental Research Funds for the Central Universities(China University of Mining and Technology,2010QNA11);the Innovation Funds for China University of Mining and Technology and High Tech Insititute of Lianyungang Xuwei new district(2011KDGXYJJ06)~~

摘　　要：以CuCl2为前驱物与HY分子筛进行固相离子交换制备了Cu/Y催化剂,采用热重方法研究了CuCl2与HY分子筛的表面固相离子交换反应,结合活性测试表明催化剂中高度分散的CuCl和离子交换形式的Cu+物种是甲醇氧化羰基化合成碳酸二甲酯的催化活性中心.X射线光电子能谱表征和元素分析结果表明,活性金属Cu主要以CuCl形式存在于分子筛外表面,而在分子筛笼内则以交换的Cu+和少量吸附的CuCl形式存在.与以CuCl为交换铜源所制催化剂相比,以CuCl2为铜源制备的催化剂Cu含量低,催化活性更高.A Cu1/Y catalyst was prepared for the vapor phase oxidative carbonylation of methanol to dimethyl carbonate （DMC）.The surface solid-state interactions of CuCl2 with HY zeolite were studied using thermogravimetry.The surface properties and morphologies of catalyst samples were analyzed by thermogravimetry,X-ray photoelectron spectroscopy,and elemental analysis,and their catalytic performance was assessed in a fixed-bed reactor.Both CuCl and CuCl2 were found to co-exist on the external surface of the catalyst,while ion-exchanged Cu1 along with small amounts of adsorbed CuCl were contained in the internal Y zeolite cage structures.Both the CuCl and CuCl2 were active species during the DMC synthesis.Compared with a conventional Cu1/Y catalyst prepared by heating a mixture of CuCl and HY zeolite,the Cu1/Y catalyst prepared by heating a mixture of CuCl2 and HY zeolite showed increased catalytic activity for the oxidative carbonylation of methanol,even though it had lower Cu and Cl contents.

关 键 词：氯化铜 固相离子交换 催化剂 氧化羰基化 甲醇 碳酸二甲酯 

分 类 号：O643.32[理学—物理化学]