Germanium-enriched double-four-membered-ring units inducing zeolite-confined subnanometric Pt clusters for efficient propane dehydrogenation

作者：Ma, Yue; Song, Shaojia; Liu, Changcheng; Liu, Lingmei; Zhang, Longkang; Zhao, Yuhong; Wang, Xin; Xu, Hao^*; Guan, Yejun^*; Jiang, Jingang; Song, Weiyu^*; Han, Yu^*; Zhang, Jiangwei^*; Wu, Peng^*

来源：Nature Catalysis, 2023, 6(6): 506-518.

DOI：10.1038/s41929-023-00968-7

• PREFERENTIAL LOCATION
• SILICALITE-1 ZEOLITE
• METAL-CLUSTERS
• TRANSFORMATION
• NANOPARTICLES
• GE
• CO
• ENCAPSULATION
• CONSEQUENCES
• CATALYSIS

It is a great challenge to regulate the precise placement of confined metal species and assemble specific structures at the atomic level. Here we report the design and synthesis of a durable supported-metal-cluster catalyst, Pt@Ge-UTL, that features subnanometric Pt clusters encapsulated inside the extra-large pores of a stabilized UTL-type germanosilicate. Integrated differential phase contrast scanning transmission electron microscopy, in situ X-ray absorption fine structure, F-19 magic-angle-spinning NMR, full-range synchrotron pair distribution function G(r) analysis and density functional theory calculations revealed that Pt clusters with an average of four atoms are firmly segregated within 14-membered-ring channels. This is achieved by selectively and directionally anchoring Pt, via Pt-O-Ge bonding, to the UTL zeolite's unique secondary building units that feature a double-four-membered-ring (d4r) configuration and a Ge-enriched composition. The host-guest bimetallic structure (Pt-4-Ge-2-d4r@UTL) promotes propane dehydrogenation with high activity, high propylene selectivity and long-term stability. This research demonstrates the use of germanosilicates in the designed synthesis of high-performance propane dehydrogenation catalysts.

• 单位
  重庆大学; y