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通过沸石中骨架铟(III)位点的存在提高亚纳米铂催化剂的稳定性

Boosting the Stability of Subnanometer Pt Catalysts by the Presence of Framework Indium(III) Sites in Zeolite.

作者信息

Zhu Chaofeng, Li Wenying, Chen Tianxiang, He Zhe, Villalobos Eduardo, Marini Carlo, Zhou Jian, Woon Lo Benedict Tsz, Xiao Hai, Liu Lichen

机构信息

Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing, 100084, China.

Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hunghom, Hong Kong, China.

出版信息

Angew Chem Int Ed Engl. 2024 Oct 7;63(41):e202409784. doi: 10.1002/anie.202409784. Epub 2024 Sep 3.

Abstract

Subnanometer metal clusters show advantages over conventional metal nanoparticles in numerous catalytic reactions owing to their high percentage of exposed surface sites, abundance of under-coordinated metal sites and unique electronic structures. However, the applications of subnanometer metal clusters in high-temperature catalytic reactions (>600 °C) are still hindered, because of their low stability under harsh reaction conditions. In this work, we have developed a zeolite-confined bimetallic PtIn catalyst with exceptionally high stability against sintering. A combination of experimental and theoretical studies shows that the isolated framework In(III) species serve as the anchoring sites for Pt species, precluding the migration and sintering of Pt species in the oxidative atmosphere at ≥650 °C. The catalyst comprising subnanometer PtIn clusters exhibits long-term stability of >1000 h during a cyclic reaction-regeneration test for ethane dehydrogenation reaction.

摘要

亚纳米金属簇在众多催化反应中比传统金属纳米颗粒具有优势,这归因于其高比例的表面暴露位点、大量配位不足的金属位点以及独特的电子结构。然而,亚纳米金属簇在高温催化反应(>600 °C)中的应用仍然受到阻碍,因为它们在苛刻的反应条件下稳定性较低。在这项工作中,我们开发了一种对烧结具有极高稳定性的沸石限域双金属PtIn催化剂。实验和理论研究相结合表明,孤立的骨架In(III)物种作为Pt物种的锚定位点,可防止Pt物种在≥650 °C的氧化气氛中迁移和烧结。在乙烷脱氢反应的循环反应 - 再生测试中,包含亚纳米PtIn簇的催化剂表现出超过1000小时的长期稳定性。

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