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Title: Improved Coking Resistance of “Intelligent” Ni Catalysts Prepared by Atomic Layer Deposition

Conformal CaTiO 3 films were deposited onto MgAl 2O 4 by atomic layer deposition (ALD) and then examined as “intelligent” catalyst supports for Ni in the steam and CO 2 reforming of methane. CaTiO 3 films (1 nm) were characterized by scanning transmission electron microscopy and XRD and shown to be stable to at least 1073 K. Catalysts with 1 and 20 wt % Ni were studied, and it was found that, following calcination at 1073 K, the Ni-CaTiO 3/MgAl 2O 4 catalysts required high-temperature reduction to achieve activities comparable to that of their Ni/MgAl 2O 4 counterparts. However, the Ni-CaTiO 3/MgAl 2O 4 catalysts exhibited dramatically improved tolerance toward carbon-whisker formation. The carbon content on the 1 wt % Ni catalyst on CaTiO 3/MgAl 2O 4 was small even after heating the catalyst in a dry, 10% CH 4–90% He mixture at 1073 K for 12 h. As a result, possible mechanisms for the high carbon tolerance of the perovskite-containing catalysts are discussed.
Authors:
ORCiD logo [1] ;  [1] ;  [2] ; ORCiD logo [1] ;  [1]
  1. Univ. of Pennsylvania, Philadelphia, PA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Grant/Contract Number:
SC0009440
Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Research Org:
Univ. of Pennsylvania, Philadelphia, PA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; atomic layer feposition (ALD); CaTiO3; coking resistance; dry methane reforming; Ni catalyst; steam methane reforming; “intelligent” catalyst
OSTI Identifier:
1461634

Lin, Chao, Jang, Joon Baek, Zhang, Lihua, Stach, Eric A., and Gorte, Raymond J.. Improved Coking Resistance of “Intelligent” Ni Catalysts Prepared by Atomic Layer Deposition. United States: N. p., Web. doi:10.1021/acscatal.8b01598.
Lin, Chao, Jang, Joon Baek, Zhang, Lihua, Stach, Eric A., & Gorte, Raymond J.. Improved Coking Resistance of “Intelligent” Ni Catalysts Prepared by Atomic Layer Deposition. United States. doi:10.1021/acscatal.8b01598.
Lin, Chao, Jang, Joon Baek, Zhang, Lihua, Stach, Eric A., and Gorte, Raymond J.. 2018. "Improved Coking Resistance of “Intelligent” Ni Catalysts Prepared by Atomic Layer Deposition". United States. doi:10.1021/acscatal.8b01598.
@article{osti_1461634,
title = {Improved Coking Resistance of “Intelligent” Ni Catalysts Prepared by Atomic Layer Deposition},
author = {Lin, Chao and Jang, Joon Baek and Zhang, Lihua and Stach, Eric A. and Gorte, Raymond J.},
abstractNote = {Conformal CaTiO3 films were deposited onto MgAl2O4 by atomic layer deposition (ALD) and then examined as “intelligent” catalyst supports for Ni in the steam and CO2 reforming of methane. CaTiO3 films (1 nm) were characterized by scanning transmission electron microscopy and XRD and shown to be stable to at least 1073 K. Catalysts with 1 and 20 wt % Ni were studied, and it was found that, following calcination at 1073 K, the Ni-CaTiO3/MgAl2O4 catalysts required high-temperature reduction to achieve activities comparable to that of their Ni/MgAl2O4 counterparts. However, the Ni-CaTiO3/MgAl2O4 catalysts exhibited dramatically improved tolerance toward carbon-whisker formation. The carbon content on the 1 wt % Ni catalyst on CaTiO3/MgAl2O4 was small even after heating the catalyst in a dry, 10% CH4–90% He mixture at 1073 K for 12 h. As a result, possible mechanisms for the high carbon tolerance of the perovskite-containing catalysts are discussed.},
doi = {10.1021/acscatal.8b01598},
journal = {ACS Catalysis},
number = ,
volume = 8,
place = {United States},
year = {2018},
month = {7}
}