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分级沸石:通过材料设计的进展提高微孔晶体在催化中的利用率。

Hierarchical zeolites: enhanced utilisation of microporous crystals in catalysis by advances in materials design.

作者信息

Pérez-Ramírez Javier, Christensen Claus H, Egeblad Kresten, Christensen Christina H, Groen Johan C

机构信息

Institute of Chemical Research of Catalonia (ICIQ), Tarragona, Spain.

出版信息

Chem Soc Rev. 2008 Nov;37(11):2530-42. doi: 10.1039/b809030k. Epub 2008 Sep 18.

Abstract

The introduction of synthetic zeolites has led to a paradigm shift in catalysis, separations, and adsorption processes, due to their unique properties such as crystallinity, high-surface area, acidity, ion-exchange capacity, and shape-selective character. However, the sole presence of micropores in these materials often imposes intracrystalline diffusion limitations, rendering low utilisation of the zeolite active volume in catalysed reactions. This critical review examines recent advances in the rapidly evolving area of zeolites with improved accessibility and molecular transport. Strategies to enhance catalyst effectiveness essentially comprise the synthesis of zeolites with wide pores and/or with short diffusion length. Available approaches are reviewed according to the principle, versatility, effectiveness, and degree of reality for practical implementation, establishing a firm link between the properties of the resulting materials and the catalytic function. We particularly dwell on the exciting field of hierarchical zeolites, which couple in a single material the catalytic power of micropores and the facilitated access and improved transport consequence of a complementary mesopore network. The carbon templating and desilication routes as examples of bottom-up and top-down methods, respectively, are reviewed in more detail to illustrate the benefits of hierarchical zeolites. Despite encircling the zeolite field, this review stimulates intuition into the design of related porous solids (116 references).

摘要

合成沸石的引入引发了催化、分离和吸附过程的范式转变,这归因于其诸如结晶度、高比表面积、酸性、离子交换能力和择形性等独特性质。然而,这些材料中仅存在微孔往往会造成晶内扩散限制,导致催化反应中沸石活性体积的利用率较低。这篇批判性综述考察了在具有改善的可及性和分子传输的沸石快速发展领域中的最新进展。提高催化剂效率的策略主要包括合成具有宽孔和/或短扩散长度的沸石。根据原理、通用性、有效性和实际实施的现实程度对现有方法进行了综述,在所得材料的性质与催化功能之间建立了紧密联系。我们特别关注分级沸石这一令人兴奋的领域,它在单一材料中兼具微孔的催化能力以及互补介孔网络带来的便利可及性和改善的传输效果。分别以碳模板法和脱硅法为例,详细综述了自下而上和自上而下的方法,以说明分级沸石的优势。尽管围绕着沸石领域,但这篇综述激发了对相关多孔固体设计的直观认识(参考文献116篇)。

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