沸石分子筛结构内配位不饱和位点:构筑与催化应用（英文）
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摘要
具有规则微孔结构的沸石分子筛是目前广泛应用的吸附剂和催化剂,而它的框架结构还可作为承载配位不饱和位点的理想平台.近年来,沸石分子筛结构内配位不饱和位点的构建、表征和催化应用方面已经取得重要进展,本文将从配位催化的视角对其进行总结与讨论.配位催化的概念由Natta在讨论Ziegler-Natta催化剂的性质时提出,已被广泛用于一系列重要反应,如加氢、氧化、羰基化、氢甲酰化和C-C键偶联中.配位催化尽管表现出高活性、高选择性和反应机理清晰等优点,但通常的过渡金属配合物催化剂在分离与回收方面也存在明显缺陷.沸石分子筛具有分子尺寸的规则孔道结构,其骨架、孔道内与离子交换位均可以引入过渡金属离子构筑配位不饱和位点.这一策略可以将配位化学与沸石化学的相关概念结合起来,并在多相催化反应过程中充分利用配位催化的优点.本文首先介绍了沸石分子筛骨架内与骨架外配位不饱和位点不同构筑策略,即离子交换-焙烧、扩散浸渍-焙烧、直接水热合成、过渡金属配合物封装以及骨架脱铝补位修饰,并对其特点进行了比较.随后讨论了用于检测阳离子落位、存在状态及其在沸石分子筛结构中动态变化的光谱技术,包括振动光谱(傅里叶变换红外光谱、拉曼光谱)、电子光谱(紫外-可见漫反射光谱、X射线光电子能谱)、共振波谱(固体核磁共振、电子自旋共振)以及X射线吸收谱(X射线近边吸收、X射线吸收精细结构).最后一部分总结了含配位不饱和位点的沸石分子筛在代表性重要催化反应中的应用,从氮氧化物转化、C-H键活化(甲烷羟基化、苯羟基化、丙烷氧化脱氢)、烯烃功能化(聚合、环氧化)、环氧化物开环(水合、氨解)和羰基活化(Baeyer-Villiger氧化重排、Meerwein-Ponndorf-Verley还原)等几类反应展开讨论.对反应机理与构效关系的认识一直以来是催化领域研究的挑战,而对于含配位不饱和位点的沸石分子筛这样复杂的体系来说更是如此.如果能够在沸石分子筛结构内构筑均一且结构明确的孤立金属离子位点,则可以将沸石分子筛骨架作为中心金属离子的配体,从而将含配位不饱和位点的沸石分子筛整体作为一类金属无机配合物,有助于更好地理解催化反应过程与本质.
Zeolites with ordered porous structure of molecular size are widely employed as commercial adsorbents and catalysts. On the other hand, the zeolite matrix is regarded as an ideal scaffold for hosting coordinatively unsaturated sites. Remarkable achievements have been made dealing with the construction, characterization and catalytic applications of coordinatively unsaturated sites in zeolite matrix. Herein, a literature overview of recent progresses on this important topic is presented from the specific view of coordination chemistry. Different strategies to construction coordinatively unsaturated sites in zeolite matrix, in zeolite framework or extraframework positions, are first introduced and their characteristics are compared. Then, spectroscopic techniques to determine the existing states of cation sites and their transformations in zeolite matrix are discussed. In the last section, the catalytic applications of coordinatively unsaturated sites in zeolite matrix for various important chemical transformations are summarized.
Zeolites with ordered porous structure of molecular size are widely employed as commercial adsorbents and catalysts. On the other hand, the zeolite matrix is regarded as an ideal scaffold for hosting coordinatively unsaturated sites. Remarkable achievements have been made dealing with the construction, characterization and catalytic applications of coordinatively unsaturated sites in zeolite matrix. Herein, a literature overview of recent progresses on this important topic is presented from the specific view of coordination chemistry. Different strategies to construction coordinatively unsaturated sites in zeolite matrix, in zeolite framework or extraframework positions, are first introduced and their characteristics are compared. Then, spectroscopic techniques to determine the existing states of cation sites and their transformations in zeolite matrix are discussed. In the last section, the catalytic applications of coordinatively unsaturated sites in zeolite matrix for various important chemical transformations are summarized.
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