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Title: Understanding the Impact of Surface Reconstruction of Perovskite Catalysts on CH4 Activation and Combustion

Journal Article · · ACS Catalysis
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [3];  [4];  [5];  [6];  [7]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of California, Riverside, CA (United States)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  4. Tennessee Technological Univ., Cookeville, TN (United States); Purdue Univ., West Lafayette, IN (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); West Virginia Univ., Morgantown, WV (United States)
  6. West Virginia Univ., Morgantown, WV (United States)
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); W. L. Gore and Assoc., Newark, DE (United States)
+ Show Author Affiliations

Methane conversion has received renewed interest due to the rapid growth in production of shale gas. Methane combustion for power generation and transportation is one of the alternatives for methane utilization. However, complete conversion of methane is critical to minimize negative environmental effects from unburned methane, whose noxious effect is 25 times greater than that of CO2. Although perovskite catalysts have high thermal stability, their low activities for methane combustion prevent them from being utilized on a commercial basis. In this work, we show the impact from reconstruction of surface and subsurface monolayers of perovskite catalysts on methane combustion, using SrTiO3 (STO) as a model perovskite. Several STO samples obtained through different synthetic methods and subjected to different postsynthetic treatments were tested for methane combustion. Through top surface characterization, kinetic experiments (including isotope labeling experiments) and density functional theory calculations, it is shown that both surface segregation of Sr and creation of step surfaces of STO can impact the rate of methane combustion over an order of magnitude. Here, this work highlights the role of surface reconstruction in tuning perovskite catalysts for methane activation.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1486951
Journal Information:
ACS Catalysis, Vol. 8, Issue 11; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 44 works
Citation information provided by
Web of Science

References (42)

Recent Advances in Catalysts for Methane Combustion journal August 2015
Complete oxidation of methane at low temperature over noble metal based catalysts: a review journal November 2002
Catalysts for combustion of methane and lower alkanes journal August 2002
Perovskites as Substitutes of Noble Metals for Heterogeneous Catalysis: Dream or Reality journal September 2014
Perovskite Oxides: Preparation, Characterizations, and Applications in Heterogeneous Catalysis journal August 2014
Synergistic Oxygen Evolving Activity of a TiO 2 -Rich Reconstructed SrTiO 3 (001) Surface journal February 2015
A highly active and stable IrO x /SrIrO 3 catalyst for the oxygen evolution reaction journal September 2016
Dynamic surface self-reconstruction is the key of highly active perovskite nano-electrocatalysts for water splitting journal July 2017
Theoretical Model of Oxidative Adsorption of Water on a Highly Reduced Reconstructed Oxide Surface journal September 2014
Surface Tuning of La 0.5 Sr 0.5 CoO 3 Perovskite Catalysts by Acetic Acid for NO x Storage and Reduction journal June 2016
Enhanced CO catalytic oxidation by Sr reconstruction on the surface of La x Sr 1− x CoO 3− δ journal May 2017
Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts journal July 2017
Shape Effect Undermined by Surface Reconstruction: Ethanol Dehydrogenation over Shape-Controlled SrTiO 3 Nanocrystals journal December 2017
Achieving A-Site Termination on La0.18Sr0.82Al0.59Ta0.41O3 Substrates journal April 2010
Surface termination and subsurface restructuring of perovskite-based solid oxide electrode materials journal January 2014
Interaction of nanostructured metal overlayers with oxide surfaces journal November 2007
Surface phase, morphology, and charge distribution transitions on vacuum and ambient annealed SrTi O 3 (100) journal May 2016
Structure change of TiO2-terminated SrTiO3(001) surfaces by annealing in O2 atmosphere and ultrahigh vacuum journal February 1999
c(6×2) and c(4×2) reconstruction of SrTiO 3 (001) journal April 1999
Surface Structures of SrTiO 3 (001):  A TiO 2 -rich Reconstruction with a c(4 × 2) Unit Cell journal August 2003
The structure and chemistry of the TiO2-rich surface of SrTiO3 (001) journal September 2002
Electronic structure and thermodynamic stability of double-layered Sr Ti O 3 ( 001 ) surfaces: Ab initio simulations journal March 2007
Transition from Reconstruction toward Thin Film on the (110) Surface of Strontium Titanate journal March 2016
Synthesis-Dependent Atomic Surface Structures of Oxide Nanoparticles journal October 2013
Sites for Methane Activation on Lithium-Doped Magnesium Oxide Surfaces journal April 2014
Oxidative Coupling of Methane over SrO Deposited on Different Commercial Supports Precoated with La 2 O 3 journal June 1998
Basicities of alumina-supported alkaline earth metal oxides journal September 1998
Shape-controlled growth of SrTiO3 polyhedral submicro/nanocrystals journal August 2014
Enhancing charge separation on high symmetry SrTiO 3 exposed with anisotropic facets for photocatalytic water splitting journal January 2016
Facet-Specific Assembly of Proteins on SrTiO3 Polyhedral Nanocrystals journal May 2014
Adsorption of Gases in Multimolecular Layers journal February 1938
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Generalized Gradient Approximation Made Simple journal October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Projector augmented-wave method journal December 1994
Special points for Brillouin-zone integrations journal June 1976
A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal December 2000
Direct Conversion of Methane to Value-Added Chemicals over Heterogeneous Catalysts: Challenges and Prospects journal March 2017
FT-IR Spectroscopic Studies of Methane Adsorption on Magnesium Oxide journal February 1994
Interaction of methane with surface of alumina studied by FT-IR spectroscopy journal January 1994
Characterisation of the basicity of modified MgO-catalysts journal May 1999

Cited By (4)

Impact of Surface Composition of SrTiO 3 Catalysts for Oxidative Coupling of Methane journal April 2019
Enhancement of the SrTiO 3 Surface Reactivity by Exposure to Electric Fields journal May 2019
Redox oxidative cracking of n -hexane with Fe-substituted barium hexaaluminates as redox catalysts journal January 2019
Surface phase diagrams of La-based perovskites towards the O-rich limit from first principles journal January 2019

Figures / Tables (8)

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Figure 3(p. 5)figure Figure 3
Table 1(p. 5)table Table 1
Figure 4(p. 6)figure Figure 4
Table 2(p. 7)table Table 2
Figure 5(p. 8)figure Figure 5
Figure 6(p. 8)figure Figure 6

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
methane activation
methane combustion
perovskite catalysts
step-sites
surface reconstruction