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Title: Understanding the Impact of Surface Reconstruction of Perovskite Catalysts on CH 4 Activation and Combustion

Abstract

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 CO 2. 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 SrTiO 3 (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.

Authors:
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)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1486951
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal Issue: 11; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; methane activation; methane combustion; perovskite catalysts; step-sites; surface reconstruction

Citation Formats

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, and Wu, Zili. Understanding the Impact of Surface Reconstruction of Perovskite Catalysts on CH4 Activation and Combustion. United States: N. p., 2018. Web. doi:10.1021/acscatal.8b02307.
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. Understanding the Impact of Surface Reconstruction of Perovskite Catalysts on CH4 Activation and Combustion. United States. doi:10.1021/acscatal.8b02307.
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, and Wu, Zili. Mon . "Understanding the Impact of Surface Reconstruction of Perovskite Catalysts on CH4 Activation and Combustion". United States. doi:10.1021/acscatal.8b02307. https://www.osti.gov/servlets/purl/1486951.
@article{osti_1486951,
title = {Understanding the Impact of Surface Reconstruction of Perovskite Catalysts on CH4 Activation and Combustion},
author = {Polo-Garzon, Felipe and Fung, Victor and Liu, Xiaoming and Hood, Zachary D. and Bickel, Elizabeth E. and Bai, Lei and Tian, Hanjing and Foo, Guo Shiou and Chi, Miaofang and Jiang, De-en and Wu, Zili},
abstractNote = {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.},
doi = {10.1021/acscatal.8b02307},
journal = {ACS Catalysis},
number = 11,
volume = 8,
place = {United States},
year = {2018},
month = {9}
}

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