Maximizing the Accessibility of Acid Sites Within Zeolite Catalysts for Syngas Conversion

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-02-16 DOI:10.1002/anie.202424946
Haodi Wang, Prof. Feng Jiao, Jingyao Feng, Yinchan Zhang, Prof. Zhaochao Xu, Prof. Xiulian Pan, Prof. Xinhe Bao
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Abstract

Mass transport within zeolites is pivotal in determining the accessibility of active sites to reactants and hence the catalytic performance. However, there lacks of quantitative guidance for synthesis of desired zeolites with reduced diffusion limitation. Herein, we take mordenite (MOR) zeolite as a model, which is characterized by 12-membered rings (MR) channels as transport path towards the active sites within the 8MR side pockets for syngas conversion to light olefins. By correlating the effective diffusion lengths ( ) with the Thiele modulus and the effectiveness factors of reaction rates over a composite catalyst ZnAlOx-MOR, we determine that the shortest 12MR channel length ( ) of 60 nm in this study is close to the threshold length necessary for full access to the 8MR acid sites. As a result, it exhibits excellent catalytic performance with CO conversion reaching 33 % and ethylene selectivity 69 %. Furthermore, the methodology is general and essential for further development of efficient zeolite catalysts with fully accessible active sites.

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合成气转化沸石催化剂中酸位的可及性最大化
沸石内部的质量传输是决定活性位点对反应物的可及性和催化性能的关键。然而,缺乏定量指导,以合成所需的沸石,可以忽略扩散限制。本文以丝光沸石(MOR)分子筛为模型,其特征是12元环(MR)通道作为通往8MR侧袋内活性位点的运输路径,用于合成气转化为轻烯烃。通过将有效扩散长度(2l)与Thiele模量和复合催化剂ZnAlOx - MOR上反应速率的有效因子相关联,我们确定本研究中最短的12MR通道长度(2l)为60 nm,接近完全进入8MR酸位所需的阈值长度。结果表明,该催化剂具有优异的催化性能,CO转化率达到33%,乙烯选择性达到69%。此外,该方法对于进一步开发具有完全可达活性位点的高效沸石催化剂具有普遍性和必要性。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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