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中文摘要：
本项目针对固体酸催化反应中催化剂的结构与性能这一基本物理化学问题开展研究工作。发展用于固体酸表面酸性位（活性中心）结构及相互作用研究的固体核磁共振新方法，利用固体核磁共振（NMR）实验技术并结合量化计算，揭示固体酸催化剂的结构与反应性能的关系。采用原位固体NMR结合GC-MS重点考察固体酸的酸强度、酸种类对催化活性的影响，揭示表面酸性与催化活性及选择性的内在关系；捕捉反应过程中的活性中间体，考察催化剂骨架及孔道的限域效应对中间体的形成与性能的影响；阐明一些在固体酸上进行的重要催化反应（低碳烷烃活化、烷基化、异构化等）的机理以及固体酸催化剂的失活机理，为高性能固体酸催化剂的合成、改性和应用提供依据。
英文摘要：
solid acid catalysts；solid state NMR；theoretical calculations；reaction mechanism；structure-property relationshi
结论摘要：
固体酸催化剂（如沸石分子筛、氧化物、杂多酸等）由于具有环境友好、产物选择性高等优点而被广泛应用于石油化工的各种催化过程。本项目针对固体酸催化剂结构与反应性能关系这一科学问题，发展固体NMR表征方法，用NMR实验结合量化计算研究了催化剂酸中心结构效应和孔道限域效应对反应性能的影响。主要成果如下（1）建立了用丙酮和三甲基磷两种探针分子的化学位移测量固体酸催化剂酸强度的方法；（2）建立了研究固体酸催化剂酸中心协同作用的27Al-27Al双量子魔角旋转NMR实验技术；（3）揭示了固体酸催化剂酸强度及孔道限域效应对催化反应的影响; （4）揭示了在Zn改性H-ZSM-5沸石分子筛催化剂上甲烷的低温活化与转化、CO的室温氧化以及甲烷与CO、甲烷与CO2共转化的反应机理。
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期刊论文
Bronsted/Lewis Acid Sites Synergy in H-MCM-22 Zeolite Studied by H-1 and Al-27 DQ-MAS NMR Spectrosco
Extra-framework aluminium species in hydrated faujasite zeolite as investigated by two-dimensional s
Breaking the T-1 Constraint for Quantitative Measurement in Magic Angle Spinning Solid-State NMR Spe
NMR-Spectroscopic Evidence of Intermediate-Dependent Pathways for Acetic Acid Formation from Methane
Influence of acid strength on the reactivity of alkane activation on solid acid catalysts: A theoret
A solid-state NMR study of structure and segmental dynamics of poly(propylmethacryl-heptaisobutyl-ps
Pore Selectivity for Olefin Protonation Reactions Confined inside Mordenite Zeolite: A Theoretical C
Acidity characterization of heterogeneous catalysts by solid-state NMR spectroscopy using probe mole
Insight into Dimethyl Ether Carbonylation Reaction over Mordenite Zeolite from in-Situ Solid-State N
Construction of Covalent Organic Framework for Catalysis: Pd/COF-LZU1 in Suzuki-Miyaura Coupling Rea
Insights into the Dealumination of Zeolite HY Revealed by Sensitivity-Enhanced Al-27 DQ-MAS NMR Spec
Combined Solid-State NMR and Theoretical Calculation Studies of Bronsted Acid Properties in Anhydrou
C-13 Chemical Shift of Adsorbed Acetone for Measuring the Acid Strength of Solid Acids: A Theoretica
New Insights into the Effects of Acid Strength on the Solid Acid-Catalyzed Reaction: Theoretical Cal
Intactness and spatial proximity of acid-base groups in bifunctional SBA-15 as revealed by solid-sta
Insights into the Dual Activation Mechanism Involving Bifunctional Cinchona Alkaloid Thiourea Organo
Bronsted/Lewis Acid Synergy in H-ZSM-5 and H-MOR Zeolites Studied by H-1 and Al-27 DQ-MAS Solid-Stat
Measurement of C-13-H-1 dipolar couplings in solids by using ultra-fast magic-angle spinning NMR spe
Distance measurement between a spin-1/2 and a half-integer quadrupolar nuclei by solid-state NMR usi
Boron Environments in B-Doped and (B, N)-Codoped TiO2 Photocatalysts: A Combined Solid-State NMR and
Enhancement of Bronsted acidity in zeolitic catalysts due to an intermolecular solvent effect in con
Low-Temperature Reactivity of Zn+ Ions Confined in ZSM-5 Zeolite toward Carbon Monoxide Oxidation: I
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