Propane Dehydrogenation Catalyzed by Isolated Pt Atoms in ≡SiOZn–OH Nests in Dealuminated Zeolite Beta
Hoffman, Adam S.
Bare, Simon R.
Gates, Bruce C.
Bell, Alexis T.
KAUST DepartmentAdvanced Membranes and Porous Materials Research Center
Chemical Science Program
Nanostructured Functional Materials (NFM) laboratory
Physical Science and Engineering (PSE) Division
Embargo End Date2022-12-09
Permanent link to this recordhttp://hdl.handle.net/10754/673994
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AbstractAtomically 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.
CitationQi, L., Babucci, M., Zhang, Y., Lund, A., Liu, L., Li, J., … Bell, A. T. (2021). Propane Dehydrogenation Catalyzed by Isolated Pt Atoms in ≡SiOZn–OH Nests in Dealuminated Zeolite Beta. Journal of the American Chemical Society. doi:10.1021/jacs.1c10261
SponsorsThis work was supported by the Office of Science, Office of Basic Energy Sciences (BES), of the U.S. Department of Energy (DOE) under Contract Nos. DE-AC02-05CH11231, DE-SC0012702 (an Energy Frontier Research Center, the Inorganometallic Catalyst Design Center, MB), and DE-FG02-04ER15513. L.Q. also acknowledges support from the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, People’s Republic of China. Use of the Stanford Synchrotron Radiation Light Source (SSRL), SLAC National Accelerator Laboratory, is supported by the DOE BES, under Contract No. DE-AC02-76SF00515. Additional support by the Consortium for Operando and Advanced Catalyst Characterization via Electronic Spectroscopy and Structure (Co-ACCESS) at SLAC is acknowledged. Co-ACCESS is supported by DOE, BES, Chemical Sciences, Geosciences and Biosciences, under Contract DE-AC02-76SF00515. We thank Dr. Hasan Celik and UC Berkeley’s NMR facility in the College of Chemistry (CoC-NMR) for spectroscopic assistance. We thank Dr. Xinglong Dong of KAUST and Jia Lv of Chongqing University for assistance with STEM.
PublisherAmerican Chemical Society (ACS)