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

Abstract

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 H2-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-ZrOx interface. 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 800 °C and 700 °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.

Authors:
 [1];  [2];  [3];  [1]
  1. Missouri Univ. of Science and Technology, Rolla, MO (United States)
  2. Gas Technology Institute, Des Plaines, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States); Gas Technology Institute, Des Plaines, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1960732
Alternate Identifier(s):
OSTI ID: 1846207; OSTI ID: 1968723
Grant/Contract Number:  
AC02-06CH11357; FE0029760
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Engineering Journal
Additional Journal Information:
Journal Volume: 436; Journal ID: ISSN 1385-8947
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ZrO2 overcoating; Atomic layer deposition (ALD); Dry reforming of methane (DRM); Metal-oxide interface; Oxygen vacancy

Citation Formats

Jin, Baitang, Li, Shiguang, Liu, Yuzi, and Liang, Xinhua. Engineering metal-oxide interface by depositing ZrO2 overcoating on Ni/Al2O3 for dry reforming of methane. United States: N. p., 2022. Web. doi:10.1016/j.cej.2022.135195.
Jin, Baitang, Li, Shiguang, Liu, Yuzi, & Liang, Xinhua. Engineering metal-oxide interface by depositing ZrO2 overcoating on Ni/Al2O3 for dry reforming of methane. United States. https://doi.org/10.1016/j.cej.2022.135195
Jin, Baitang, Li, Shiguang, Liu, Yuzi, and Liang, Xinhua. Thu . "Engineering metal-oxide interface by depositing ZrO2 overcoating on Ni/Al2O3 for dry reforming of methane". United States. https://doi.org/10.1016/j.cej.2022.135195. https://www.osti.gov/servlets/purl/1960732.
@article{osti_1960732,
title = {Engineering metal-oxide interface by depositing ZrO2 overcoating on Ni/Al2O3 for dry reforming of methane},
author = {Jin, Baitang and Li, Shiguang and Liu, Yuzi and Liang, Xinhua},
abstractNote = {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 H2-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-ZrOx interface. 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 800 °C and 700 °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.},
doi = {10.1016/j.cej.2022.135195},
journal = {Chemical Engineering Journal},
number = ,
volume = 436,
place = {United States},
year = {Thu Feb 10 00:00:00 EST 2022},
month = {Thu Feb 10 00:00:00 EST 2022}
}

Works referenced in this record:

Influence of growth temperature on properties of zirconium dioxide films grown by atomic layer deposition
journal, August 2002

  • Kukli, Kaupo; Ritala, Mikko; Aarik, Jaan
  • Journal of Applied Physics, Vol. 92, Issue 4
  • DOI: 10.1063/1.1493657

Dry reforming of methane by stable Ni–Mo nanocatalysts on single-crystalline MgO
journal, February 2020


Controlling the rate of change of Ni dispersion in commercial catalyst by ALD overcoat during dry reforming of methane
journal, April 2020


Promotion effects of Ga2O3 on CO2 adsorption and conversion over a SiO2-supported Ni catalyst
journal, January 2010

  • Pan, Yun-xiang; Kuai, Pingyu; Liu, Yuan
  • Energy & Environmental Science, Vol. 3, Issue 9
  • DOI: 10.1039/c0ee00149j

Insight into the effects of the oxygen species over Ni/ZrO2 catalyst surface on methane reforming with carbon dioxide
journal, May 2019


Structural effect of Ni/ZrO2 catalyst on CO2 methanation with enhanced activity
journal, May 2019


Tandem In 2 O 3 -Pt/Al 2 O 3 catalyst for coupling of propane dehydrogenation to selective H 2 combustion
journal, March 2021


A Tandem Catalyst with Multiple Metal Oxide Interfaces Produced by Atomic Layer Deposition
journal, April 2016

  • Ge, Huibin; Zhang, Bin; Gu, Xiaomin
  • Angewandte Chemie International Edition, Vol. 55, Issue 25
  • DOI: 10.1002/anie.201600799

Dry reforming of methane over La2O2CO3-modified Ni/Al2O3 catalysts with moderate metal support interaction
journal, May 2020


Tuning Selectivity of CO 2 Hydrogenation Reactions at the Metal/Oxide Interface
journal, July 2017

  • Kattel, Shyam; Liu, Ping; Chen, Jingguang G.
  • Journal of the American Chemical Society, Vol. 139, Issue 29
  • DOI: 10.1021/jacs.7b05362

Highly active and stable alumina supported nickel nanoparticle catalysts for dry reforming of methane
journal, February 2017


Structure evolution of atomic layer deposition grown ZrO2 films by deep-ultra-violet Raman and far-infrared spectroscopies
journal, July 2003


Effects of the surface adsorbed oxygen species tuned by rare-earth metal doping on dry reforming of methane over Ni/ZrO2 catalyst
journal, May 2020


Reducibility of ZrO 2 /Pt 3 Zr and ZrO 2 /Pt 2D films compared to bulk zirconia: a DFT+U study of oxygen removal and H 2 adsorption
journal, January 2017

  • Ruiz Puigdollers, Antonio; Pacchioni, Gianfranco
  • Nanoscale, Vol. 9, Issue 20
  • DOI: 10.1039/C7NR01904A

Effect of ceria and zirconia promotors on Ni/SBA-15 catalysts for coking and sintering resistant steam reforming of propylene glycol in microreactors
journal, April 2017


Design of an active and stable catalyst for dry reforming of methane via molecular layer deposition
journal, February 2021


Organic acid-assisted preparation of highly dispersed Co/ZrO2 catalysts with superior activity for CO2 methanation
journal, October 2019


Contrasting the Role of Ni/Al 2 O 3 Interfaces in Water–Gas Shift and Dry Reforming of Methane
journal, November 2017

  • Foppa, Lucas; Margossian, Tigran; Kim, Sung Min
  • Journal of the American Chemical Society, Vol. 139, Issue 47
  • DOI: 10.1021/jacs.7b08984

High carbon-resistance Ni/CeAlO3-Al2O3 catalyst for CH4/CO2 reforming
journal, June 2013


Vacancy engineering of the nickel-based catalysts for enhanced CO2 methanation
journal, March 2021


Activity and stability of NiCe@SiO multi–yolk–shell nanotube catalyst for tri-reforming of methane
journal, December 2019


Stabilizing Ni Catalysts by Molecular Layer Deposition for Harsh, Dry Reforming Conditions
journal, July 2014

  • Gould, Troy D.; Izar, Alan; Weimer, Alan W.
  • ACS Catalysis, Vol. 4, Issue 8
  • DOI: 10.1021/cs500809w

ZrO 2 -Based Alternatives to Conventional Propane Dehydrogenation Catalysts: Active Sites, Design, and Performance
journal, November 2015

  • Otroshchenko, Tatyana; Sokolov, Sergey; Stoyanova, Mariana
  • Angewandte Chemie International Edition, Vol. 54, Issue 52
  • DOI: 10.1002/anie.201508731

High-performance of nanostructured Ni/CeO2 catalyst on CO2 methanation
journal, July 2020


Interpretation of Measurements in Experimental Catalysis
book, January 1954


Fabrication of highly dispersed nickel in nanoconfined spaces of as-made SBA-15 for dry reforming of methane with carbon dioxide
journal, June 2020


Improved Thermal Stability and Methane-Oxidation Activity of Pd/Al 2 O 3 Catalysts by Atomic Layer Deposition of ZrO 2
journal, August 2015


Structure–Activity–Selectivity Relationships in Propane Dehydrogenation over Rh/ZrO 2 Catalysts
journal, May 2020


Sintering and Coke Resistant Core/Yolk Shell Catalyst for Hydrocarbon Reforming
journal, October 2018


Promotional effect of La2O3 and CeO2 on Ni/γ-Al2O3 catalysts for CO2 reforming of CH4
journal, September 2010


Approaches for Understanding and Controlling Interfacial Effects in Oxide-Supported Metal Catalysts
journal, July 2018


Novel Processing to Produce Polymer/Ceramic Nanocomposites by Atomic Layer Deposition
journal, January 2007


Comparative study at low and medium reaction temperatures of syngas production by methane reforming with carbon dioxide over silica and alumina supported catalysts
journal, May 1998

  • Ferreira-Aparicio, P.; Guerrero-Ruiz, A.; Rodrı́guez-Ramos, I.
  • Applied Catalysis A: General, Vol. 170, Issue 1
  • DOI: 10.1016/S0926-860X(98)00048-9

Design of stable Ni/ZrO2 catalysts for dry reforming of methane
journal, December 2017


Tests for Transport Limitations in Experimental Catalytic Reactors
journal, October 1971

  • Mears, D. E.
  • Industrial & Engineering Chemistry Process Design and Development, Vol. 10, Issue 4
  • DOI: 10.1021/i260040a020

Comprehensive study on the effect of magnesium loading over nickel-ordered mesoporous alumina for dry reforming of methane
journal, December 2020


Effect of oxide additives on the hydrotalcite derived Ni catalysts for CO2 reforming of methane
journal, December 2019


Coking- and Sintering-Resistant Palladium Catalysts Achieved Through Atomic Layer Deposition
journal, March 2012


Surface Spectroscopy on UHV-Grown and Technological Ni–ZrO2 Reforming Catalysts: From UHV to Operando Conditions
journal, August 2016


Kinetic analysis of supported Ni-catalyzed CO2/CH4 reactions using photoacoustic spectroscopy
journal, January 2007

  • Kim, Ji-Woong; Ha, Jae-Au; Jung, Hun
  • Physical Chemistry Chemical Physics, Vol. 9, Issue 43
  • DOI: 10.1039/b709102h

CO 2 conversion to synthesis gas via DRM on the durable Al 2 O 3 /Ni/Al 2 O 3 sandwich catalyst with high activity and stability
journal, January 2018

  • Zhao, Yu; Kang, Yunqing; Li, Hui
  • Green Chemistry, Vol. 20, Issue 12
  • DOI: 10.1039/C8GC00743H

Increasing Oxide Reducibility: The Role of Metal/Oxide Interfaces in the Formation of Oxygen Vacancies
journal, August 2017

  • Ruiz Puigdollers, Antonio; Schlexer, Philomena; Tosoni, Sergio
  • ACS Catalysis, Vol. 7, Issue 10
  • DOI: 10.1021/acscatal.7b01913

Nano-engineered nickel catalysts supported on 4-channel α-Al 2 O 3 hollow fibers for dry reforming of methane
journal, March 2018

  • Shang, Zeyu; Li, Shiguang; Wang, Qingfa
  • AIChE Journal, Vol. 64, Issue 7
  • DOI: 10.1002/aic.16160

Ni-alumina dry reforming catalysts: Atomic layer deposition and the issue of Ni aluminate
journal, March 2020


CO 2 reforming with methane over small-sized Ni@SiO 2 catalysts with unique features of sintering-free and low carbon
journal, November 2018


Tuning electron density of metal nickel by support defects in Ni/ZrO2 for selective hydrogenation of fatty acids to alkanes and alcohols
journal, September 2019