铜丝光沸石上甲醇羰基化反应的固体核磁共振研究

波谱学杂志

铜丝光沸石上甲醇羰基化反应的固体核磁共振研究

李博解，徐君*，王强，王秀梅，齐国栋，邓风*

波谱与原子分子物理国家重点实验室，武汉磁共振中心（中国科学院武汉物理与数学研究所），湖北武汉 430071

收稿日期:2013-11-28 修回日期:2014-07-17 出版日期:2014-09-05 发布日期:2014-09-05
作者简介:李博解(1985-)，男，湖北孝感人，博士研究生，主要从事羰基化反应机理的固体NMR 研究． *通讯联系人：徐君，E-mail: xujun@wipm.ac.cn；邓风，电话：027-87198820；E-mail: dengf@wipm.ac.cn.
基金资助:
国家自然科学基金资助项目(21210005，21173254，21221064)；武汉市晨光计划资助项目(201271031383)．

Carbonylation of Methanol on Cu-H-MOR Zeolites: Insights from Solid-State NMR Spectroscopy

LI Bo-jie，XU Jun*，WANG Qiang，WANG Xiu-mei，QI Guo-dong，DENG Feng*

State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan (Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences), Wuhan 430071, China

Received:2013-11-28 Revised:2014-07-17 Online:2014-09-05 Published:2014-09-05
About author:XU Jun, E-mail: xujun@wipm.ac.cn; DENG Feng, Tel: 027-87198820; E-mail: dengf@wipm.ac.cn.
Supported by:
国家自然科学基金资助项目(21210005，21173254，21221064)；武汉市晨光计划资助项目(201271031383)．

摘要/Abstract

摘要：

利用固体核磁共振方法，研究了铜修饰丝光沸石(Cu-H-MOR)分子筛催化甲醇(CH₃OH)与一氧化碳(CO)羰基化反应过程．通过研究反应过程中生成的各吸附物种与Cu²⁺的相互作用，分别对这些吸附物种进行了归属，确定了铜甲氧基(Cu-OCH₃)和铜乙酰基(Cu-(CO)-CH₃)为羰基化反应过程的中间产物，讨论了可能的反应机理．

关键词: 固体核磁共振(solid-state NMR), 丝光沸石, 羰基化反应, 多相催化, 反应机理

Abstract:

Carbonylation of methanol with CO on Cu-H-mordenite (Cu-H-MOR) zeolites was studied by ¹³C solid-state NMR spectroscopy. By characterizing the interaction between adsorbed species and Cu²⁺ cations, we determined copper methoxy group (Cu-OCH₃) and copper acetyl group (Cu-(CO)-CH₃) as the intermediates of this reaction. The possible mechanisms of carbonylation reaction of methanol with CO on Cu-H-MOR zeolites were discussed.

Key words: solid-state NMR spectroscopy, mordenite zeolite, carbonylation reaction, heterogeneous catalysis, reaction mechanism

中图分类号:

O482.53

李博解，徐君*，王强，王秀梅，齐国栋，邓风*. 铜丝光沸石上甲醇羰基化反应的固体核磁共振研究[J]. 波谱学杂志.

LI Bo-jie，XU Jun*，WANG Qiang，WANG Xiu-mei，QI Guo-dong，DENG Feng*. Carbonylation of Methanol on Cu-H-MOR Zeolites: Insights from Solid-State NMR Spectroscopy[J]. Chinese Journal of Magnetic Resonance.

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