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Title: Low Temperature Propane Oxidation over Co3O4 based Nano-array Catalysts. Ni Dopant Effect, Reaction Mechanism and Structural Stability

Abstract

Low temperature propane oxidation has been achieved by Co3O4-based nano-array catalysts featuring low catalytic materials loading. The Ni doping into the Co3O4 lattice has led to enhanced reaction kinetics at low temperature by promoting the surface lattice oxygen activity. In situ DRIFTS investigation in tandem with isotopic oxygen exchange reveals that the propane oxidation proceeds via Mars-van Krevelen mechanism where surface lattice oxygen acts as the active site whereas O2 in the reaction feed does not directly participate in CO2 formation. The Ni doping promotes the formation of less stable carbonates on the surface to facilitate the CO2 desorption. The thermal stability of Ni doped Co3O4 decreases with increased Ni concentration while catalytic activity increases. A balance between enhanced activity and compromised thermal stability shall be considered in the Ni doped Co3O4 nano-array catalysts for low temperature hydrocarbon oxidation. This study provides useful and timely guidance for rational catalyst design toward low temperature catalytic oxidation.

Authors:
 [1];  [2];  [1];  [1];  [3];  [1];  [3];  [1];  [1]
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. National Univ. of Singapore (Singapore)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1213987
Alternate Identifier(s):
OSTI ID: 1398071
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Catalysis B: Environmental
Additional Journal Information:
Journal Volume: 180; Journal Issue: 1; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ren, Zheng, Wu, Zili, Gao, Puxian, Song, Wenqiao, Xiao, Wen, Guo, Yanbing, Ding, Jun, Suib, Steven L., and Gao, Pu-Xian. Low Temperature Propane Oxidation over Co3O4 based Nano-array Catalysts. Ni Dopant Effect, Reaction Mechanism and Structural Stability. United States: N. p., 2015. Web. doi:10.1016/j.apcatb.2015.04.021.
Ren, Zheng, Wu, Zili, Gao, Puxian, Song, Wenqiao, Xiao, Wen, Guo, Yanbing, Ding, Jun, Suib, Steven L., & Gao, Pu-Xian. Low Temperature Propane Oxidation over Co3O4 based Nano-array Catalysts. Ni Dopant Effect, Reaction Mechanism and Structural Stability. United States. https://doi.org/10.1016/j.apcatb.2015.04.021
Ren, Zheng, Wu, Zili, Gao, Puxian, Song, Wenqiao, Xiao, Wen, Guo, Yanbing, Ding, Jun, Suib, Steven L., and Gao, Pu-Xian. 2015. "Low Temperature Propane Oxidation over Co3O4 based Nano-array Catalysts. Ni Dopant Effect, Reaction Mechanism and Structural Stability". United States. https://doi.org/10.1016/j.apcatb.2015.04.021. https://www.osti.gov/servlets/purl/1213987.
@article{osti_1213987,
title = {Low Temperature Propane Oxidation over Co3O4 based Nano-array Catalysts. Ni Dopant Effect, Reaction Mechanism and Structural Stability},
author = {Ren, Zheng and Wu, Zili and Gao, Puxian and Song, Wenqiao and Xiao, Wen and Guo, Yanbing and Ding, Jun and Suib, Steven L. and Gao, Pu-Xian},
abstractNote = {Low temperature propane oxidation has been achieved by Co3O4-based nano-array catalysts featuring low catalytic materials loading. The Ni doping into the Co3O4 lattice has led to enhanced reaction kinetics at low temperature by promoting the surface lattice oxygen activity. In situ DRIFTS investigation in tandem with isotopic oxygen exchange reveals that the propane oxidation proceeds via Mars-van Krevelen mechanism where surface lattice oxygen acts as the active site whereas O2 in the reaction feed does not directly participate in CO2 formation. The Ni doping promotes the formation of less stable carbonates on the surface to facilitate the CO2 desorption. The thermal stability of Ni doped Co3O4 decreases with increased Ni concentration while catalytic activity increases. A balance between enhanced activity and compromised thermal stability shall be considered in the Ni doped Co3O4 nano-array catalysts for low temperature hydrocarbon oxidation. This study provides useful and timely guidance for rational catalyst design toward low temperature catalytic oxidation.},
doi = {10.1016/j.apcatb.2015.04.021},
url = {https://www.osti.gov/biblio/1213987}, journal = {Applied Catalysis B: Environmental},
issn = {0926-3373},
number = 1,
volume = 180,
place = {United States},
year = {Tue Jun 09 00:00:00 EDT 2015},
month = {Tue Jun 09 00:00:00 EDT 2015}
}

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Cited by: 144 works
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Highly stable Co3O4 nanoparticles-assembled microrods derived from MOF for efficient total propane oxidation
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Facet‐Dependent Activity of Co 3 O 4 Catalyst for C 3 H 8 Combustion
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Decreasing Co3O4 Particle Sizes by Ammonia-Etching and Catalytic Oxidation of Propane
journal, January 2017


Copper manganese oxide enhanced nanoarray-based monolithic catalysts for hydrocarbon oxidation
journal, January 2018


Catalytic Glycolysis of Poly(ethylene terephthalate) Using Zinc and Cobalt Oxides Recycled from Spent Batteries
journal, September 2019


Gaseous CO and toluene co-oxidation over monolithic core–shell Co 3 O 4 -based hetero-structured catalysts
journal, January 2019


NaCl-induced nickel–cobalt inverse spinel structure for boosting hydrogen evolution from ethyl acetate and water
journal, January 2019


Catalytic oxidation of propane over palladium alloyed with gold: an assessment of the chemical and intermediate species
journal, January 2018


Oxidant free conversion of alcohols to nitriles over Ni-based catalysts
journal, January 2019


Effect of Ce and La dopants in Co 3 O 4 nanorods on the catalytic activity of CO and C 3 H 6 oxidation
journal, January 2019


Oxidant free conversion of alcohols to nitriles over Ni-based catalysts
text, January 2019