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将铂簇限制在铟改性的ZSM-5沸石中以促进丙烷脱氢。

Confining platinum clusters in indium-modified ZSM-5 zeolite to promote propane dehydrogenation.

作者信息

Yuan Yong, Huang Erwei, Hwang Sooyeon, Liu Ping, Chen Jingguang G

机构信息

Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA.

Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, USA.

出版信息

Nat Commun. 2024 Aug 2;15(1):6529. doi: 10.1038/s41467-024-50709-y.

DOI:10.1038/s41467-024-50709-y
PMID:39095363
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11297129/
Abstract

Designing highly active and stable catalytic sites is often challenging due to the complex synthesis procedure and the agglomeration of active sites during high-temperature reactions. Here, we report a facile two-step method to synthesize Pt clusters confined by In-modified ZSM-5 zeolite. In-situ characterization confirms that In is located at the extra-framework position of ZSM-5 as In, and the Pt clusters are stabilized by the In-ZSM-5 zeolite. The resulting Pt clusters confined in In-ZSM-5 show excellent propane conversion, propylene selectivity, and catalytic stability, outperforming monometallic Pt, In, and bimetallic PtIn alloys. The incorporation of In in ZSM-5 neutralizes Brønsted acid sites to inhibit side reactions, as well as tunes the electronic properties of Pt clusters to facilitate propane activation and propylene desorption. The strategy of combining precious metal clusters with metal cation-exchanged zeolites opens the avenue to develop stable heterogeneous catalysts for other reaction systems.

摘要

由于合成过程复杂且高温反应过程中活性位点会发生团聚,设计高活性和稳定的催化位点通常具有挑战性。在此,我们报道了一种简便的两步法来合成由铟改性的ZSM-5沸石限制的铂簇。原位表征证实铟以In的形式位于ZSM-5的骨架外位置,并且铂簇被In-ZSM-5沸石稳定。所得限制在In-ZSM-5中的铂簇表现出优异的丙烷转化率、丙烯选择性和催化稳定性,优于单金属铂、铟和双金属铂铟合金。在ZSM-5中引入铟可中和布朗斯台德酸位点以抑制副反应,同时调节铂簇的电子性质以促进丙烷活化和丙烯脱附。将贵金属簇与金属阳离子交换沸石相结合的策略为开发用于其他反应体系的稳定多相催化剂开辟了道路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5d8/11297129/5e4d9818cb0a/41467_2024_50709_Fig7_HTML.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5d8/11297129/7aa7939e04bc/41467_2024_50709_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5d8/11297129/5e4d9818cb0a/41467_2024_50709_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5d8/11297129/64ca18b1c541/41467_2024_50709_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5d8/11297129/ffeda6471e32/41467_2024_50709_Fig2_HTML.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5d8/11297129/e3cbeefe261c/41467_2024_50709_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5d8/11297129/7aa7939e04bc/41467_2024_50709_Fig6_HTML.jpg
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