Promotion of Pd nanoparticles by Fe and formation of a Pd3Fe intermetallic alloy for propane dehydrogenation

Yang, Ce; Wu, Zhenwei; Zhang, Guanghui; Sheng, Huaping; Tian, Jun; Duan, Zhengli; Sohn, Hyuntae; Kropf, A. Jeremy; Wu, Tianpin; Krause, Theodore R.; Miller, Jeffrey T.

doi:10.1016/j.cattod.2018.07.043

Promotion of Pd nanoparticles by Fe and formation of a Pd₃Fe intermetallic alloy for propane dehydrogenation

Journal Article · Tue Jul 17 04:00:00 EDT 2018 · Catalysis Today

DOI:https://doi.org/10.1016/j.cattod.2018.07.043· OSTI ID:1650346

Yang, Ce ^[1]; Wu, Zhenwei ^[2]; ^[2]; Sheng, Huaping ^[3]; Tian, Jun ^[3]; Duan, Zhengli ^[3]; Sohn, Hyuntae ^[1]; Kropf, A. Jeremy ^[1]; Wu, Tianpin ^[4]; Krause, Theodore R. ^[1]; ^[5]

Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Purdue Univ., West Lafayette, IN (United States). Davidson School of Chemical Engineering
Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Purdue Univ., West Lafayette, IN (United States). Davidson School of Chemical Engineering

In this study, silica supported Pd (~2 nm), Pd₃Fe (~2 nm) and Pd₃Fe_large (~12 nm) catalysts were synthesized and tested for propane dehydrogenation at 510 °C. At the 10% conversion, Pd and Pd₃Fe catalysts exhibited propylene selectivity of 45% and 94%, respectively. Moreover, the latter showed a turnover rate (TOR) of 0.2 s^-1, which is five times higher than that of the Pd catalyst (0.04 s^-1). Pd K edge XAS, XRD, and CO adsorbed IR were used to characterize the geometric structure of the catalysts. By combined comparison of XRD and XAS spectra of Pd₃Fe and Pd₃Fe_large catalysts, we successfully identified the crystalline phase in the 2 nm Pd₃Fe catalyst. The CO adsorbed IR suggests that the formation of Pd₃Fe breaks the ensemble of Pd, which is responsible for the increase of selectivity. The Pd L edge XAS was used to characterize the electronic structure of the catalysts. The Pd₃Fe catalyst exhibits an increase of the edge energy compared with the Pd catalyst, which indicates the change of d-band structure in the bimetallic catalyst. The change in the electronic structure is likely the reason for the increase in TOR.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1650346

Alternate ID(s):: OSTI ID: 1874719

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Vol. 323; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Two-dimensional transition metal carbides as supports for tuning the chemistry of catalytic nanoparticles Li, Zhe; Yu, Liang; Milligan, Cory Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-07502-5	journal	December 2018

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Pd3Fe nanoparticles
Propane dehydrogenation
X-ray absorption
X-ray diffraction