4.8 Article

Propane Dehydrogenation Catalyzed by Isolated Pt Atoms in SiOZn-OH Nests in Dealuminated Zeolite Beta

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 50, 页码 21364-21378

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c10261

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  1. Office of Science, Office of Basic Energy Sciences (BES), of the U.S. Department of Energy (DOE) [DE-AC02-05CH11231, DESC0012702, DEFG02-04ER15513]
  2. Dalian Institute of Chemical Physics, Chinese Academy of Sciences, People's Republic of China
  3. DOE BES [DE-AC02-76SF00515]
  4. Consortium for Operando and Advanced Catalyst Characterization via Electronic Spectroscopy and Structure (CoACCESS) at SLAC
  5. DOE, BES, Chemical Sciences, Geosciences and Biosciences [DE-AC02-76SF00515]

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This study presents a novel strategy for the design, synthesis, and characterization of a zeolite-supported propane dehydrogenation catalyst with predominantly isolated Pt atoms stably bonded within nests of Zn atoms. The catalyst exhibits high activity and selectivity to propene, and atomic resolution images confirm the predominantly atomic dispersion of Pt in the nests.
Atomically dispersed noble metal catalysts have drawn wide attention as candidates to replace supported metal clusters and metal nanoparticles. Atomic dispersion can offer unique chemical properties as well as maximum utilization of the expensive metals. Addition of a second metal has been found to help reduce the size of Pt ensembles in bimetallic clusters; however, the stabilization of isolated Pt atoms in small nests of nonprecious metal atoms remains challenging. We now report a novel strategy for the design, synthesis, and characterization of a zeolite-supported propane dehydrogenation catalyst that incorporates predominantly isolated Pt atoms stably bonded within nests of Zn atoms located within the nanoscale pores of dealuminated zeolite Beta. The catalyst is stable in long-term operation and exhibits high activity and high selectivity to propene. Atomic resolution images, bolstered by X-ray absorption spectra, demonstrate predominantly atomic dispersion of the Pt in the nests and, with complementary infrared and nuclear magnetic resonance spectra, determine a structural model of the nested Pt.

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