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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)

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) (SC-22)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1486951
Journal Information:
ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 11 Vol. 8; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (4)

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