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Title: Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework

Abstract

The catalyzed conversion of shale gas-derived light hydrocarbons, e.g. methane to methanol, for further application as automotive fuels and/or bulk chemicals is especially attractive in light of improved methods of hydrocarbon extraction. MOF based catalysts have previously been demonstrated to be active for a range of catalytic reactions. In this work we used Cu-NU1000 as a methane-to-methanol oxidation catalyst. In addition to product studies, in-situ X-ray Absorption Spectroscopic (XAS) experiments are performed under catalytic conditions in order to follow the modification of the Cu-species and directly probe the structure/activity properties of the Cu-NU1000 system. The insights reported herein serve as a first look at metal-organic framework materials as catalysts for methane oxidation and be the basis for development of the subsequent generations of materials.

Authors:
 [1]; ORCiD logo [2];  [2];  [1]; ORCiD logo [3];  [3];  [2]; ORCiD logo [2]; ORCiD logo [4];  [3];  [2];  [5]; ORCiD logo [6]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [7]
  1. Department of Chemistry and Catalysis Research Institute, Technische Universität München, 85748 Garching, Germany
  2. Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
  3. Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota, Minneapolis, Minnesota 55455, United States
  4. Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
  5. Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Materials Science and Engineering, University of Washington, Seattle, Washington 98195, United States
  6. Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States; Department of Chemistry, Faculty of Science, King Abdulaziz University, Jeddah 21589, Saudi Arabia
  7. Department of Chemistry and Catalysis Research Institute, Technische Universität München, 85748 Garching, Germany; Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1378015
Report Number(s):
PNNL-SA-122186
Journal ID: ISSN 0002-7863; KC0307010
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 30; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; methane oxidation; methanol production; metal-organic framework; Cu XAFS spectroscopy

Citation Formats

Ikuno, Takaaki, Zheng, Jian, Vjunov, Aleksei, Sanchez-Sanchez, Maricruz, Ortuño, Manuel A., Pahls, Dale R., Fulton, John L., Camaioni, Donald M., Li, Zhanyong, Ray, Debmalya, Mehdi, B. Layla, Browning, Nigel D., Farha, Omar K., Hupp, Joseph T., Cramer, Christopher J., Gagliardi, Laura, and Lercher, Johannes A. Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework. United States: N. p., 2017. Web. doi:10.1021/jacs.7b02936.
Ikuno, Takaaki, Zheng, Jian, Vjunov, Aleksei, Sanchez-Sanchez, Maricruz, Ortuño, Manuel A., Pahls, Dale R., Fulton, John L., Camaioni, Donald M., Li, Zhanyong, Ray, Debmalya, Mehdi, B. Layla, Browning, Nigel D., Farha, Omar K., Hupp, Joseph T., Cramer, Christopher J., Gagliardi, Laura, & Lercher, Johannes A. Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework. United States. doi:10.1021/jacs.7b02936.
Ikuno, Takaaki, Zheng, Jian, Vjunov, Aleksei, Sanchez-Sanchez, Maricruz, Ortuño, Manuel A., Pahls, Dale R., Fulton, John L., Camaioni, Donald M., Li, Zhanyong, Ray, Debmalya, Mehdi, B. Layla, Browning, Nigel D., Farha, Omar K., Hupp, Joseph T., Cramer, Christopher J., Gagliardi, Laura, and Lercher, Johannes A. Mon . "Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework". United States. doi:10.1021/jacs.7b02936.
@article{osti_1378015,
title = {Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework},
author = {Ikuno, Takaaki and Zheng, Jian and Vjunov, Aleksei and Sanchez-Sanchez, Maricruz and Ortuño, Manuel A. and Pahls, Dale R. and Fulton, John L. and Camaioni, Donald M. and Li, Zhanyong and Ray, Debmalya and Mehdi, B. Layla and Browning, Nigel D. and Farha, Omar K. and Hupp, Joseph T. and Cramer, Christopher J. and Gagliardi, Laura and Lercher, Johannes A.},
abstractNote = {The catalyzed conversion of shale gas-derived light hydrocarbons, e.g. methane to methanol, for further application as automotive fuels and/or bulk chemicals is especially attractive in light of improved methods of hydrocarbon extraction. MOF based catalysts have previously been demonstrated to be active for a range of catalytic reactions. In this work we used Cu-NU1000 as a methane-to-methanol oxidation catalyst. In addition to product studies, in-situ X-ray Absorption Spectroscopic (XAS) experiments are performed under catalytic conditions in order to follow the modification of the Cu-species and directly probe the structure/activity properties of the Cu-NU1000 system. The insights reported herein serve as a first look at metal-organic framework materials as catalysts for methane oxidation and be the basis for development of the subsequent generations of materials.},
doi = {10.1021/jacs.7b02936},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 30,
volume = 139,
place = {United States},
year = {2017},
month = {7}
}