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 · Mon Sep 24 00:00:00 EDT 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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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 Lab. (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

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Cited by: 34 works

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Impact of Surface Composition of SrTiO ₃ Catalysts for Oxidative Coupling of Methane Bai, Lei; Polo‐Garzon, Felipe; Bao, Zhenghong ChemCatChem, Vol. 11, Issue 8 https://doi.org/10.1002/cctc.201900159	journal	April 2019
Enhancement of the SrTiO ₃ Surface Reactivity by Exposure to Electric Fields Klauke, Kurt; Kayaalp, Buğra; Biesuz, Mattia ChemNanoMat, Vol. 5, Issue 7 https://doi.org/10.1002/cnma.201900201	journal	May 2019
Redox oxidative cracking of n -hexane with Fe-substituted barium hexaaluminates as redox catalysts Tian, Xin; Dudek, Ryan B.; Gao, Yunfei Catalysis Science & Technology, Vol. 9, Issue 9 https://doi.org/10.1039/c8cy02530d	journal	January 2019
Surface phase diagrams of La-based perovskites towards the O-rich limit from first principles Li, Yang; Yang, Jie; Zhu, Yi-An Physical Chemistry Chemical Physics, Vol. 21, Issue 24 https://doi.org/10.1039/c9cp02288k	journal	January 2019

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Understanding the Impact of Surface Reconstruction of Perovskite Catalysts on CH4 Activation and Combustion

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