DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Enhanced activity and stability of MgO-promoted Ni/Al2O3 catalyst for dry reforming of methane: Role of MgO

Abstract

Highly dispersed nickel nanoparticles (NPs) were deposited on Al2O3 NPs by atomic layer deposition (ALD). Various amounts of MgO were loaded on Ni/Al2O3 catalysts by the incipient wetness (IW) method for dry reforming of methane. Fresh and used catalysts were systematically characterized to reveal the effects of MgO on the catalytic performance. MgO was found to increase the basic amount and basic strength of catalyst surfaces, which provided additional surface oxygen species and assisted the adsorption and activation of CO2. Although the formation of NiO-MgO solid solution, during the calcination of incipient wetness, did not improve the overall reducibility, the Ni NPs from NiO-MgO solid solution after reduction formed an intimate interaction with MgO, which could inhibit Ni NPs from sintering and provide sufficient metal-support interface for CO2 activation. The MgO-promoted Ni/Al2O3 reached a methane reforming rate of 1780 LCH4gNi-1 h-1 at 850 °C, which is 26% more than that of the pristine Ni/Al2O3. The higher CO2 activity enhanced the oxidation rate of the surface carbon generated from side-reactions, thereby resulting in a higher reforming rate and inhibiting coke formation, especially the detrimental graphitic encapsulating carbon on an active nickel surface.

Authors:
 [1];  [2]; ORCiD logo [1]
  1. Missouri Univ. of Science and Technology, Rolla, MO (United States). Dept. of Chemical and Biochemical Engineering
  2. Gas Technology Inst., Des Plaines, IL (United States)
Publication Date:
Research Org.:
Gas Technology Institute, Des Plaines, IL (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1849228
Alternate Identifier(s):
OSTI ID: 1775782; OSTI ID: 1968721
Grant/Contract Number:  
FE0029760
Resource Type:
Accepted Manuscript
Journal Name:
Fuel
Additional Journal Information:
Journal Volume: 284; Journal Issue: C; Journal ID: ISSN 0016-2361
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Energy & fuels; Engineering; Dry reforming of methane; MgO; Ni; Atomic layer deposition

Citation Formats

Jin, Baitang, Li, Shiguang, and Liang, Xinhua. Enhanced activity and stability of MgO-promoted Ni/Al2O3 catalyst for dry reforming of methane: Role of MgO. United States: N. p., 2020. Web. doi:10.1016/j.fuel.2020.119082.
Jin, Baitang, Li, Shiguang, & Liang, Xinhua. Enhanced activity and stability of MgO-promoted Ni/Al2O3 catalyst for dry reforming of methane: Role of MgO. United States. https://doi.org/10.1016/j.fuel.2020.119082
Jin, Baitang, Li, Shiguang, and Liang, Xinhua. Thu . "Enhanced activity and stability of MgO-promoted Ni/Al2O3 catalyst for dry reforming of methane: Role of MgO". United States. https://doi.org/10.1016/j.fuel.2020.119082. https://www.osti.gov/servlets/purl/1849228.
@article{osti_1849228,
title = {Enhanced activity and stability of MgO-promoted Ni/Al2O3 catalyst for dry reforming of methane: Role of MgO},
author = {Jin, Baitang and Li, Shiguang and Liang, Xinhua},
abstractNote = {Highly dispersed nickel nanoparticles (NPs) were deposited on Al2O3 NPs by atomic layer deposition (ALD). Various amounts of MgO were loaded on Ni/Al2O3 catalysts by the incipient wetness (IW) method for dry reforming of methane. Fresh and used catalysts were systematically characterized to reveal the effects of MgO on the catalytic performance. MgO was found to increase the basic amount and basic strength of catalyst surfaces, which provided additional surface oxygen species and assisted the adsorption and activation of CO2. Although the formation of NiO-MgO solid solution, during the calcination of incipient wetness, did not improve the overall reducibility, the Ni NPs from NiO-MgO solid solution after reduction formed an intimate interaction with MgO, which could inhibit Ni NPs from sintering and provide sufficient metal-support interface for CO2 activation. The MgO-promoted Ni/Al2O3 reached a methane reforming rate of 1780 LCH4gNi-1 h-1 at 850 °C, which is 26% more than that of the pristine Ni/Al2O3. The higher CO2 activity enhanced the oxidation rate of the surface carbon generated from side-reactions, thereby resulting in a higher reforming rate and inhibiting coke formation, especially the detrimental graphitic encapsulating carbon on an active nickel surface.},
doi = {10.1016/j.fuel.2020.119082},
journal = {Fuel},
number = C,
volume = 284,
place = {United States},
year = {Thu Sep 03 00:00:00 EDT 2020},
month = {Thu Sep 03 00:00:00 EDT 2020}
}

Works referenced in this record:

Elevated temperature CO2 capture on nano-structured MgO–Al2O3 aerogel: Effect of Mg/Al molar ratio
journal, April 2014


The effect of synthesis gas composition on the Fischer–Tropsch synthesis over Co/γ-Al2O3 and Co–Re/γ-Al2O3 catalysts
journal, July 2007


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


Effects of CeO2 addition on Ni/Al2O3 catalysts for the reaction of ammonia decomposition to hydrogen
journal, April 2008


Dry reforming of methane to synthesis gas on NiO–MgO nanocrystalline solid solution catalysts
journal, March 2013


One-Pot Synthesis of Ordered Mesoporous NiO–CaO–Al 2 O 3 Composite Oxides for Catalyzing CO 2 Reforming of CH 4
journal, May 2012

  • Xu, Leilei; Song, Huanling; Chou, Lingjun
  • ACS Catalysis, Vol. 2, Issue 7
  • DOI: 10.1021/cs3001072

Dry reforming of methane over CeO2-ZnAl2O4 supported Ni and Ni-Co nano-catalysts
journal, January 2019


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

Carbon Dioxide Reforming of Methane over Nickel Catalyst Supported on MgO(111) Nanosheets
journal, November 2013


High-performing and durable MgO/Ni catalysts via atomic layer deposition for CO 2 reforming of methane (CRM)
journal, April 2016


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


Cooperativity and Dynamics Increase the Performance of NiFe Dry Reforming Catalysts
journal, January 2017

  • Kim, Sung Min; Abdala, Paula Macarena; Margossian, Tigran
  • Journal of the American Chemical Society, Vol. 139, Issue 5
  • DOI: 10.1021/jacs.6b11487

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


Transient studies of low-temperature dry reforming of methane over Ni-CaO/ZrO2-La2O3
journal, January 2013


Dry Reforming of Shale Gas and Carbon Dioxide with Ni-Ce-Al 2 O 3 Catalyst: Syngas Production Enhanced over Ni-CeO x Formation
journal, September 2018


Atomically dispersed nickel as coke-resistant active sites for methane dry reforming
journal, November 2019


CO2 hydrogenation to methanol over Pd/In2O3: effects of Pd and oxygen vacancy
journal, December 2017


Insight into the reaction mechanism of CO 2 activation for CH 4 reforming over NiO-MgO: A combination of DRIFTS and DFT study
journal, September 2017


Remarkable activity and stability of Ni catalyst supported on CeO2-Al2O3 via CeAlO3 perovskite towards glycerol steam reforming for hydrogen production
journal, December 2017

  • Kamonsuangkasem, Krongthong; Therdthianwong, Supaporn; Therdthianwong, Apichai
  • Applied Catalysis B: Environmental, Vol. 218
  • DOI: 10.1016/j.apcatb.2017.06.073

Reforming of methane with carbon dioxide over cerium oxide promoted nickel nanoparticles deposited on 4-channel hollow fibers by atomic layer deposition
journal, January 2020

  • Jin, Baitang; Shang, Zeyu; Li, Shiguang
  • Catalysis Science & Technology, Vol. 10, Issue 10
  • DOI: 10.1039/D0CY00039F

Dynamic Behavior of Carbonate Species on Metal Oxide Surface:  Oxygen Scrambling between Adsorbed Carbon Dioxide and Oxide Surface
journal, October 2003

  • Tsuji, Hideto; Okamura-Yoshida, Akie; Shishido, Tetsuya
  • Langmuir, Vol. 19, Issue 21
  • DOI: 10.1021/la0342666

Comparison of Nanoscaled and Bulk NiO Structural and Environmental Characteristics by XRD, XAFS, and XPS
journal, November 2012

  • Peck, Matthea A.; Langell, Marjorie A.
  • Chemistry of Materials, Vol. 24, Issue 23
  • DOI: 10.1021/cm300739y

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

The role of carbonaceous deposits in the activity and stability of Ni-based catalysts applied in the dry reforming of methane
journal, January 2014

  • Düdder, Hendrik; Kähler, Kevin; Krause, Bastian
  • Catal. Sci. Technol., Vol. 4, Issue 9
  • DOI: 10.1039/C4CY00409D

La-promoted Ni-hydrotalcite-derived catalysts for dry reforming of methane at low temperatures
journal, October 2016


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


Adsorption of carbon dioxide at high temperature—a review
journal, March 2002


Catalytic partial oxidation of methane to syngas over Ca-decorated-Al2O3-supported Ni and NiB catalysts
journal, September 2005


Identification of active sites in CO2 activation on MgO supported Ni cluster
journal, April 2020


Nanostructured Pt- and Ni-based catalysts for CO2-reforming of methane
journal, March 2010


Durable Ni/MgO catalysts for CO2 reforming of methane: Activity and metal–support interaction
journal, February 2009


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

The catalytic methanation of coke oven gas over Ni-Ce/Al2O3 catalysts prepared by microwave heating: Effect of amorphous NiO formation
journal, March 2015


A review of dry (CO 2 ) reforming of methane over noble metal catalysts
journal, January 2014

  • Pakhare, Devendra; Spivey, James
  • Chem. Soc. Rev., Vol. 43, Issue 22
  • DOI: 10.1039/C3CS60395D

The effect of CeO2 on the surface and catalytic properties of Pt/CeO2–ZrO2 catalysts for methane dry reforming
journal, July 2009


Ordered mesoporous “one-pot” synthesized Ni-Mg(Ca)-Al2O3 as effective and remarkably stable catalysts for combined steam and dry reforming of methane (CSDRM)
journal, February 2017


Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst
journal, August 2018


Dry reforming of methane on Ni-Fe-MgO catalysts: Influence of Fe on carbon-resistant property and kinetics
journal, May 2020