Experimental and computational investigation of acetic acid deoxygenation over oxophilic molybdenum carbide: Surface chemistry and active site identity

Schaidle, Joshua A.; Blackburn, Jeffrey; Farberow, Carrie A.; Nash, Connor; Steirer, K. Xerxes; Clark, Jared; Robichaud, David J.; Ruddy, Daniel A.

doi:10.1021/acscatal.5b01930

Experimental and computational investigation of acetic acid deoxygenation over oxophilic molybdenum carbide: Surface chemistry and active site identity

Journal Article · Thu Jan 21 00:00:00 EST 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b01930· OSTI ID:1239059

Schaidle, Joshua A. ^[1]; Blackburn, Jeffrey ^[1]; Farberow, Carrie A. ^[1]; Nash, Connor ^[1]; Steirer, K. Xerxes ^[1]; Clark, Jared ^[1]; Robichaud, David J. ^[1]; Ruddy, Daniel A. ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)

Ex situ catalytic fast pyrolysis (CFP) is a promising route for producing fungible biofuels; however, this process requires bifunctional catalysts that favor C–O bond cleavage, activate hydrogen at near atmospheric pressure and high temperature (350–500 °C), and are stable under high-steam, low hydrogen-to-carbon environments. Recently, early transition-metal carbides have been reported to selectively cleave C–O bonds of alcohols, aldehydes, and oxygenated aromatics, yet there is limited understanding of the metal carbide surface chemistry under reaction conditions and the identity of the active sites for deoxygenation. In this study, we evaluated molybdenum carbide (Mo₂C) for the deoxygenation of acetic acid, an abundant component of biomass pyrolysis vapors, under ex situ CFP conditions, and we probed the Mo₂C surface chemistry, identity of the active sites, and deoxygenation pathways using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations.

View Accepted Manuscript (DOE)

Research Organization:: NREL (National Renewable Energy Laboratory (NREL), Golden, CO (United States))

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1239059

Report Number(s):: NREL/JA--5100-64755

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 2 Vol. 6; ISSN 2155-5435

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Experimental and computational investigation of acetic acid deoxygenation over oxophilic molybdenum carbide: Surface chemistry and active site identity

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