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一种用于丙烷脱氢的具有高耐久性的自再生Pt/Ge-MFI沸石。

A self-regenerating Pt/Ge-MFI zeolite for propane dehydrogenation with high endurance.

作者信息

Hong Huizhen, Xu Zhikang, Mei Bingbao, Hu Wende, Fornasiero Paolo, Wang Chuanming, Wang Tinghai, Yue Yuanyuan, Li Tiesen, Yang Chen, Cui Qingyan, Zhu Haibo, Bao Xiaojun

机构信息

State Key Laboratory of Fluorine & Nitrogen Chemicals, College of Chemical Engineering, Fuzhou University, Fuzhou, China.

Qingyuan Innovation Laboratory, Quanzhou, China.

出版信息

Science. 2025 May;388(6746):497-502. doi: 10.1126/science.adu6907. Epub 2025 Apr 10.

Abstract

Supported noble metal cluster catalysts are typically operated under severe conditions involving switching between reducing and oxidizing atmospheres, causing irreversible transformation of the catalyst structure and thereby leading to permanent deactivation. We discovered that various platinum (Pt) precursors spontaneously disperse in a germanium-MFI (Ge-MFI) zeolite, which opposes the Ostwald ripening phenomenon, producing self-regenerating Pt/Ge-MFI catalysts for propane dehydrogenation. These catalysts reversibly switch between Pt clusters and Pt single atoms in response to reducing reaction and oxidizing regeneration conditions. This environmental adaptability allows them to completely self-regenerate over 110 reaction and regeneration cycles in propane dehydrogenation, and they exhibited unprecedented sintering resistance when exposed to air at 800°C for 10 days. Such spontaneous metal dispersion in a Ge-MFI zeolite is a robust and versatile methodology for fabricating various rhodium, ruthenium, iridium, and palladium cluster catalysts.

摘要

负载型贵金属簇催化剂通常在苛刻条件下运行,涉及在还原和氧化气氛之间切换,这会导致催化剂结构发生不可逆转变,从而导致永久性失活。我们发现,各种铂(Pt)前驱体在锗-MFI(Ge-MFI)沸石中自发分散,这与奥斯特瓦尔德熟化现象相反,从而制备出用于丙烷脱氢的自再生Pt/Ge-MFI催化剂。这些催化剂会根据还原反应和氧化再生条件在Pt簇和Pt单原子之间可逆切换。这种环境适应性使它们在丙烷脱氢的110个反应和再生循环中能够完全自再生,并且在800°C下暴露于空气中10天时表现出前所未有的抗烧结性。在Ge-MFI沸石中这种自发的金属分散是一种用于制备各种铑、钌、铱和钯簇催化剂的强大且通用的方法。

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