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沸石硅铝比和铝分布的调控及其对性能的影响。

Regulation of the Si/Al ratios and Al distributions of zeolites and their impact on properties.

作者信息

Li Jialiang, Gao Mingkun, Yan Wenfu, Yu Jihong

机构信息

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University 2699 Qianjin Street Changchun 130012 China

International Center of Future Science, Jilin University 2699 Qianjin Street Changchun 130012 China.

出版信息

Chem Sci. 2022 Dec 28;14(8):1935-1959. doi: 10.1039/d2sc06010h. eCollection 2023 Feb 22.

DOI:10.1039/d2sc06010h
PMID:36845940
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9945477/
Abstract

Zeolites are typically a class of crystalline microporous aluminosilicates that are constructed by SiO and AlO tetrahedra. Because of their unique porous structures, strong Brönsted acidity, molecular-level shape selectivity, exchangeable cations, and high thermal/hydrothermal stability, zeolites are widely used as catalysts, adsorbents, and ion-exchangers in industry. The activity, selectivity, and stability/durability of zeolites in applications are closely related to their Si/Al ratios and Al distributions in the framework. In this review, we discussed the basic principles and the state-of-the-art methodologies for regulating the Si/Al ratios and Al distributions of zeolites, including seed-assisted recipe modification, interzeolite transformation, fluoride media, and usage of organic structure-directing agents (OSDAs), The conventional and newly developed characterization methods for determining the Si/Al ratios and Al distributions were summarized, which include X-ray fluorescence spectroscopy (XRF), solid state Si/Al magic-angle-spinning nuclear magnetic resonance spectroscopy (Si/Al MAS NMR), Fourier-transform infrared spectroscopy (FT-IR), The impact of Si/Al ratios and Al distributions on the catalysis, adsorption/separation, and ion-exchange performance of zeolites were subsequently demonstrated. Finally, we presented a perspective on the precise control of the Si/Al ratios and Al distributions of zeolites and the corresponding challenges.

摘要

沸石通常是一类由SiO和AlO四面体构成的结晶微孔铝硅酸盐。由于其独特的多孔结构、较强的布朗斯台德酸度、分子水平的形状选择性、可交换阳离子以及高热/水热稳定性，沸石在工业中被广泛用作催化剂、吸附剂和离子交换剂。沸石在应用中的活性、选择性和稳定性/耐久性与其骨架中的硅铝比和铝分布密切相关。在本综述中，我们讨论了调节沸石硅铝比和铝分布的基本原理和最新方法，包括种子辅助配方改性、沸石间转化、氟化物介质以及有机结构导向剂（OSDAs）的使用。总结了用于测定硅铝比和铝分布的传统及新开发的表征方法，包括X射线荧光光谱法（XRF）、固态硅铝魔角旋转核磁共振光谱法（Si/Al MAS NMR）、傅里叶变换红外光谱法（FT-IR）。随后展示了硅铝比和铝分布对沸石催化、吸附/分离及离子交换性能的影响。最后，我们对精确控制沸石的硅铝比和铝分布以及相应挑战提出了展望。

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