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Structural evolution of an intermetallic Pd–Zn catalyst selective for propane dehydrogenation

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/c5cp00222b· OSTI ID:1210837
 [1];  [2];  [3];  [3];  [2];  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Univ. of Illinois, Chicago, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
We report the structural evolution of Pd–Zn alloys in a 3.6% Pd–12% Zn/Al2O3 catalyst which is selective for propane dehydrogenation. In this work, high signal-to-noise, in situ synchrotron X-ray diffraction (XRD) was used quantitatively, in addition to in situ diffuse-reflectance infrared Fourier transform spectroscopy (DRIFTS) and extended X-ray absorption fine structure (EXAFS) to follow the structural changes in the catalyst as a function of reduction temperature. XRD in conjunction with DRIFTS of adsorbed CO indicated that the β1-PdZn intermetallic alloy structure formed at reduction temperatures as low as 230 °C, likely first at the surface, but did not form extensively throughout the bulk until 500 °C which was supported by in situ EXAFS. DRIFTS results suggested there was little change in the surfaces of the nanoparticles above 325 °C. The intermetallic alloy which formed was Pd-rich at all temperatures but became less Pd-rich with increasing reduction temperature as more Zn incorporated into the structure. In addition to the β1-PdZn alloy, a solid solution phase with face-center cubic structure (α-PdZn) was present in the catalyst, also becoming more Zn-rich with increasing reduction temperature.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Energy Frontier Research Centers (EFRC) (United States). Institute for Atom-efficient Chemical Transformations (IACT)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1210837
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 42 Vol. 17; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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