Engineering metal-oxide interface by depositing ZrO2 overcoating on Ni/Al2O3 for dry reforming of methane

Jin, Baitang; Li, Shiguang; Liu, Yuzi; Liang, Xinhua

doi:10.1016/j.cej.2022.135195

Title: Engineering metal-oxide interface by depositing ZrO₂ overcoating on Ni/Al₂O₃ for dry reforming of methane

Journal Article · 10 February 2022 · Chemical Engineering Journal

DOI: https://doi.org/10.1016/j.cej.2022.135195 · OSTI ID:1960732

Jin, Baitang ^[1]; Li, Shiguang ^[2]; Liu, Yuzi ^[3]; Liang, Xinhua ^[1]

Missouri Univ. of Science and Technology, Rolla, MO (United States)
Gas Technology Institute, Des Plaines, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials

Zirconium oxide (ZrO₂) was deposited onto Ni/Al₂O₃ catalyst as overcoating by atomic layer deposition (ALD) for dry reforming of methane (DRM). High-temperature heating during H-2-reduction could transform the ALD-prepared ZrO₂ thin film to tetragonal phase and crack the encapsulating layer on Ni sites, which constructed a beneficial Ni-ZrO_x interface. Here, interfacial surface oxygen vacancies on ZrO₂ overcoating were induced by the partial reduction of ZrO₂ surface during high-temperature H₂ reduction, with the assistance of Ni. During DRM, the interfacial oxygen vacancies enhanced CO₂ activation by dissociating CO₂ and releasing active O, thereby limiting carbon formation. For DRM at 700 °C and 800 °C, Ni/Al₂O₃ with 5 cycles of ZrO₂ ALD overcoating enhanced both activity and stability significantly. For a 100-h DRM test at 600 °C, no deactivation was observed for the Ni/Al₂O₃ catalyst with 10 cycles of ZrO₂ ALD overcoating, as compared to 59% relative activity loss of Ni/Al₂O₃.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Gas Technology Institute, Des Plaines, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357; FE0029760

OSTI ID:: 1960732

Journal Information:: Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Vol. 436; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Atomic layer deposition (ALD)
Dry reforming of methane (DRM)
Metal-oxide interface
Oxygen vacancy
ZrO2 overcoating

Title: Engineering metal-oxide interface by depositing ZrO2 overcoating on Ni/Al2O3 for dry reforming of methane

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Title: Engineering metal-oxide interface by depositing ZrO₂ overcoating on Ni/Al₂O₃ for dry reforming of methane