固体核磁共振技术在固体酸催化剂表征及催化反应机理研究之应用进展

doi:10.1016/S1872-2067(12)60528-2

催化学报 ›› 2013, Vol. 34 ›› Issue (3): 436-491.DOI: 10.1016/S1872-2067(12)60528-2

• 专栏：中国催化三十年进展回顾 • 上一篇下一篇

固体核磁共振技术在固体酸催化剂表征及催化反应机理研究之应用进展

郑安民^a, 黄信炅^b, 王强^a, 张海禄^c, 邓风^a, 刘尚斌^d,e

a 中国科学院武汉物理与数学研究所, 波谱与原子分子国家重点实验室, 武汉磁共振中心, 湖北武汉 430071;
b 台湾大学化学系, 台湾台北 10617;
c 中国科学院苏州纳米技术与纳米仿生研究所, 江苏苏州 215123;
d “中央”研究院原子与分子科学研究所, 台湾台北 10617;
e 台湾师范大学化学系, 台湾台北 11677

收稿日期:2012-06-30 修回日期:2012-09-10 出版日期:2013-04-02 发布日期:2013-04-03
通讯作者: 邓风,刘尚斌
基金资助:
国家自然科学基金(20933009, 21073228, 21210005, 21103223, 21173255);台湾国科会(NSC98-2113-M-001-017-MY3, NSC101-2113-M-001-020-MY3).

Progress in development and application of solid-state NMR for solid acid catalysis

ZHENG Anmin^a, HUANG Shing-Jong^b, WANG Qiang^a, ZHANG Hailu^c, DENG Feng^a, LIU Shang-Bin^d,e

a State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Center for Magnetic Resonance, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, Hubei, China;
b Departmentof Chemistry, National Taiwan University, Taipei 10617, Taiwan, China;
c Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, Jiangsu, China;
d Institute of Atomic and Molecular Sciences, “Academia Sinica”, Taipei 10617, Taiwan, China;
e Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan, China

Received:2012-06-30 Revised:2012-09-10 Online:2013-04-02 Published:2013-04-03
Supported by:
This work was supported by the National Natural Science Foundation of China (20933009, 21073228, 21210005, 21103223, 21173255) and the National Science Council (NSC98-2113-M-001-017-MY3, NSC101-2113-M-001-020-MY3), Taiwan, China.

摘要/Abstract

摘要：

固体酸催化剂广泛应用于现代石油与化学工业中,其反应活性与其酸性密切相关.与传统的酸性表征方法(红外光谱、程序升温脱附、滴定等)相比,利用先进的探针分子技术、双共振和二维相关谱等核磁共振(NMR)技术可以获取固体催化剂酸种类、酸分布、酸浓度和酸强度等完整信息.同时,原位固体NMR实验可跟踪反应分子在催化剂活性中心吸附状态和转换的中间体物种,为揭示反应机理提供了最直接的实验证据.本文详细介绍了固体NMR的原理和一系列相关新技术,着重综述了固体NMR技术在酸催化剂结构、活性中心特性以及催化反应机理方面的应用进展.

关键词: 固体核磁共振波谱, 固体酸催化剂, 探针分子, 酸性, 催化反应机理

Abstract:

Solid acid catalysts have been widely used in petrochemical industry and their catalytic activities are normally dictated by their acidities. Unlike conventional acidity characterization techniques such as titration, infrared, or temperature-programmed desorption, detailed acid features of solid acids, such as type, distribution, concentration, and strength of acid sites may be attained by advanced methods involving pertinent probe molecules and state-of-the-art solid-state nuclear magnetic resonance (SSNMR) techniques,i.e. double resonance and two-dimensional correlation spectroscopies. In addition, in situ solid-state NMR method is capable of probing the guest/host properties of the reactant at the active centers of the catalystsas well as the intermediate species formed during conversion. Itprovides direct experimental evidence for exploring the mechanism of catalytic reaction. In this report, the fundamental theory and the recent developments in solid-state NMR are reviewed with specific focus on relevant applications in structure and acidity characterization of solid acid catalysts and catalytic mechanisms.

Key words: Solid-state NMR spectroscopy, Solid acid catalyst, Probe molecule, Acidity, Catalytic reaction mechanism

郑安民, 黄信炅, 王强, 张海禄, 邓风, 刘尚斌. 固体核磁共振技术在固体酸催化剂表征及催化反应机理研究之应用进展[J]. 催化学报, 2013, 34(3): 436-491.

ZHENG Anmin, HUANG Shing-Jong, WANG Qiang, ZHANG Hailu, DENG Feng, LIU Shang-Bin. Progress in development and application of solid-state NMR for solid acid catalysis[J]. Chinese Journal of Catalysis, 2013, 34(3): 436-491.

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固体核磁共振技术在固体酸催化剂表征及催化反应机理研究之应用进展

Progress in development and application of solid-state NMR for solid acid catalysis

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