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

• 成果类型: Article
• 署名作者: 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
• 署名单位: Fuzhou University; Qingyuan Innovation Laboratory; Chinese Academy of Sciences; Shanghai Advanced Research Institute, CAS; University of Trieste
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-12385
• DOI: 10.1126/science.adu6907
• 发表日期: 2025-05-01
• 页码: 497-502
• 关键词: supported pt-sn; sinter-resistant; nanoparticle catalysts; silicalite-1 zeolite; mesoporous zeolite; light alkanes; in-situ; clusters; efficient; chemistry

摘要

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 degrees 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.