Activation and Conversion of Methane to Syngas over ZrO2/Cu(111) Catalysts near Room Temperature

Huang, Erwei; Rui, Ning; Rosales, Rina; Liu, Ping; Rodriguez, José A.

doi:10.1021/jacs.3c01980

Title: Activation and Conversion of Methane to Syngas over ZrO₂/Cu(111) Catalysts near Room Temperature

Journal Article · Wed Apr 05 00:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c01980· OSTI ID:1975249

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Brookhaven National Laboratory (BNL), Upton, NY (United States). Chemistry Division; Stony Brook Univ., NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Chemistry Division
Stony Brook Univ., NY (United States)

Enzymatic systems achieve the catalytic conversion of methane at room temperature under mild conditions. Here, in this study, varying thermodynamic and kinetic parameters, we show that the reforming of methane by water (MWR, CH₄ + H₂O → CO + 3H₂) and the water-gas shift reaction (WGS, CO + H₂O → H₂ + CO₂), two essential processes to integrate fossil fuels toward a H2 energy loop, can be achieved on ZrO₂/Cu(111) catalysts near room temperature. Measurements of ambient-pressure X-ray photoelectron spectroscopy and mass spectrometry, combined with density functional calculations and kinetic Monte Carlo simulations, were used to study the behavior of the inverse oxide/metal catalysts. The superior performance is associated with a unique zirconia-copper interface, where multifunctional sites involving zirconium, oxygen, and copper work coordinatively to dissociate methane and water at 300 K and move forward the MWR and WGS processes.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704; AC02-05CH11231

OSTI ID:: 1975249

Report Number(s):: BNL-224437-2023-JAAM

Journal Information:: Journal of the American Chemical Society, Vol. 145, Issue 15; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Activation and Conversion of Methane to Syngas over ZrO2/Cu(111) Catalysts near Room Temperature

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Title: Activation and Conversion of Methane to Syngas over ZrO₂/Cu(111) Catalysts near Room Temperature