Single-Atom Manganese-Based Catalysts for the Oxidative Dehydrogenation of Propane

Byron, Carly; Ignacio-de Leon, Patricia Anne; Bryant, Jacob; Langeslay, Ryan; Savereide, Louisa; Wen, Jianguo; Camacho-Bunquin, Jeffrey; Notestein, Justin M.; Delferro, Massimiliano; Ferrandon, Magali

doi:10.1021/acscatal.4c06021

Single-Atom Manganese-Based Catalysts for the Oxidative Dehydrogenation of Propane

Journal Article · Tue Oct 29 00:00:00 EDT 2024 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.4c06021· OSTI ID:2574298

Byron, Carly ^[1]; Ignacio-de Leon, Patricia Anne ^[1]; ^[1]; ^[1]; Savereide, Louisa ^[2]; ^[3]; ^[1]; ^[2]; ^[1]; ^[1]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Combinatorial screening of 150 supported metal oxide (manganese and additives) catalysts was carried out via a high-throughput synthesis platform and parallel reactors for the oxidative dehydrogenation (ODH) of propane to propylene. Specifically, an organomanganese (0.05-2.5 Mn atoms/nm²) complex was grafted on metal oxide supports (Al₂O₃, SiO₂, TiO₂, and ZrO₂) premodified with either Lewis acid (Al, Ti, Zn, and Zr) or redox-active (Cu, Cr, Ga Ni, V) additives at various surface coverages (25, 50, and 75%). Catalysts were characterized by high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), Raman spectroscopy, and UV-vis spectroscopy. Catalysts 0.05 Mn/V(50%)/Al₂O₃ and 0.05 Mn/Ni(50%)/ZrO₂ showed the highest combined propane conversion and propylene selectivities (31/41% and 15/85%), with excellent stability at 500 degrees C for 25 h. The presence of Ni in Mn/Ni/ZrO₂ resulted in a 6-fold increase in turnover frequency (TOF) over the Mn/ZrO₂. HRTEM identified single Mn atoms after 500 degrees C heat treatment. For the Mn/Ni/ZrO₂ system, Mn was incorporated into the support lattice due to the similar ionic radius of Mn²⁺ and Zr⁴⁺, which was also enhanced by the presence of Ni. For the Mn/V/Al₂O₃ system, highly active MnO was prevalent as observed by Raman. Both V and Mn contributed to an increase in mutual dispersion, but both species remained on the surface. Finally, it is proposed that the highly dispersed atom and interactions between Mn with either Ni or V are responsible for the ODH performance and stability.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2574298

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 22 Vol. 14; ISSN 2155-5435

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
combinatorial screening
manganese
nickel
propane dehydrogenation
single atom
vanadium

Single-Atom Manganese-Based Catalysts for the Oxidative Dehydrogenation of Propane

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