Sulfur Tolerant Subnanometer Fe/Alumina Catalysts for Propane Dehydrogenation

Sharma, Lohit; Purdy, Stephen C.; Page, Katharine; Rangarajan, Srinivas; Pham, Hien; Datye, Abhaya; Baltrusaitis, Jonas

doi:10.1021/acsanm.1c01366

Sulfur Tolerant Subnanometer Fe/Alumina Catalysts for Propane Dehydrogenation

Journal Article · Fri Sep 17 00:00:00 EDT 2021 · ACS Applied Nano Materials

DOI:https://doi.org/10.1021/acsanm.1c01366· OSTI ID:1831624

^[1]; ^[2]; ^[3]; ^[1]; Pham, Hien ^[4]; ^[4]; ^[1]

Lehigh Univ., Bethlehem, PA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Univ. of New Mexico, Albuquerque, NM (United States)

A series of Al₂O₃-supported Fe-containing catalysts were synthesized by incipient wetness impregnation. The iron surface density was varied from 1 to 13 Fe atoms/nm² spanning submonolayer to above-monolayer coverage. Here, the resulting supported Fe-catalysts were characterized by N₂ physisorption, ex situ X-ray diffraction (XRD), X-ray pair distribution function (PDF), X-ray absorption spectroscopy (XAS), aberration corrected scanning transmission electron microscopy (AC-STEM) and chemically probed by hydrogen temperature-programmed reduction (H₂-TPR). The results suggest that over this entire range of loadings, Fe was present as dispersed species, with only a very small fraction of Fe₂O₃ aggregates, at the highest Fe loading in oxide phase. The in situ sulfidation of Fe/Al₂O₃ resulted in the formation of a highly active and selective PDH catalyst. The highest activity with 52% propane conversion and ~99% propylene selectivity at 560 °C was obtained for the 6.4 Fe/Al₂O₃-S catalyst, suggesting that this is the highest amount of Fe that could be fully dispersed on the support in sulfided form. XRD and AC-STEM indicated the absence of any crystalline iron sulfide aggregates after sulfidation and reaction. H₂-TPR results indicated that the amount of the reducible Fe sites in the sulfided catalyst remained constant above monolayer coverage, and increasing loading did not increase the number of reducible Fe sites. Consistent with these results, the reactivity per gram of catalyst showed no increase with Fe loading above monolayer coverage, suggesting that additional Fe remains conformal to the alumina surface.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1831624

Alternate ID(s):: OSTI ID: 1841207

Journal Information:: ACS Applied Nano Materials, Journal Name: ACS Applied Nano Materials Journal Issue: 10 Vol. 4; ISSN 2574-0970

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
H2S
alumina
catalyst
diffraction
iron
oxides
propane dehydrogenation
redox reactions
sulfidation

Sulfur Tolerant Subnanometer Fe/Alumina Catalysts for Propane Dehydrogenation

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