固体酸催化剂结构和催化反应机理核磁共振研究.PDFVIP

物理化学学报(Wuli Huaxue Xuebao) 270 Acta Phys. -Chim. Sin. 2017, 33 (2), 270－282 February [Feature Article] doi: 10.3866/PKU.WHXB201611022 固体酸催化剂结构与催化反应机理的核磁共振研究 李申慧 李 静 郑安民 邓 风* ( 中国科学院武汉物理与数学研究所，波谱与原子分子物理国家重点实验室，武汉磁共振中心，武汉430071) 摘要：固体酸催化剂因具有环境友好、高产物选择性和易于分离等优点而广泛应用于现代石油化工领域的各 种催化过程。固体核磁共振是一种研究功能材料结构和动力学性质的有力工具。本文将主要介绍固体核磁共 振在表征固体酸催化剂的表面酸性以及多相催化反应机理方面的应用。具体来说，可以通过一系列探针分子 (如吡啶、丙酮、三烷基氧磷和三甲基磷)的NMR 化学位移实验观测值来定量测量酸强度；二维双量子魔角旋 转(DQ MAS)固体核磁共振技术能够揭示催化剂上酸中心的空间临近性及协同效应。另外，原位固体核磁共 振可以揭示多相催化反应过程中反应物、中间体、反应产物的演化，阐明催化反应机理。 关键词：固体核磁共振；酸表征；固体酸催化剂；催化反应机理；主客体相互作用 中图分类号：O643 Solid-State NMR Characterization of the Structure and Catalytic Reaction Mechanism of Solid Acid Catalysts LI Shen-Hui LI Jing ZHENG An-Min 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, P. R. China) Abstract: Solid acid catalysts have been widely used in advanced petrochemical processes because of their environmental friendliness, high product selectivity, and easy product separation. Solid-state nuclear magnetic resonance (NMR) spectroscopy is a well-established tool for structure determination and dynamic study of various functional materials. In this review, we focus mainly on our research using solid-state NMR to characterize the acid properties and elucidate the catalytic reaction mechanism of solid acid catalysts. The acid strength of solid acids can be quantitatively measured from the ch