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

Polo-Garzon, Felipe; Fung, Victor; Liu, Xiaoming; Hood, Zachary D.; Bickel, Elizabeth E.; Bai, Lei; Tian, Hanjing; Foo, Guo Shiou; Chi, Miaofang; Jiang, De-en; Wu, Zili

doi:10.1021/acscatal.8b02307

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

Journal Article · 23 September 2018 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.8b02307 · OSTI ID:1486951

^[1]; Fung, Victor ^[2];

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^[3]; Bickel, Elizabeth E. ^[4]; Bai, Lei ^[5]; Tian, Hanjing ^[6]; Foo, Guo Shiou ^[7];

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^[2];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of California, Riverside, CA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Tennessee Technological Univ., Cookeville, TN (United States); Purdue Univ., West Lafayette, IN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); West Virginia Univ., Morgantown, WV (United States)
West Virginia Univ., Morgantown, WV (United States)
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.

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