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Title: Active sites for tandem reactions of CO 2 reduction and ethane dehydrogenation

We present that ethylene (C 2H 4) is one of the most important raw materials for chemical industry. The tandem reactions of CO 2-assisted dehydrogenation of ethane (C 2H 6) to ethylene creates an opportunity to effectively use the underutilized ethane from shale gas while mitigating anthropogenic CO 2 emissions. Here we identify the most likely active sites over CeO 2-supported NiFe catalysts by using combined in situ characterization with density-functional theory (DFT) calculations. The experimental and theoretical results reveal that the Ni–FeO x interfacial sites can selectively break the C–H bonds and preserve the C–C bond of C 2H 6 to produce ethylene, while the Ni–CeO x interfacial sites efficiently cleave all of the C–H and C–C bonds to produce synthesis gas. Lastly, controlled synthesis of the two distinct active sites enables rational enhancement of the ethylene selectivity for the CO 2-assisted dehydrogenation of ethane.
Authors:
 [1] ;  [2] ;  [2] ;  [3] ;  [4] ;  [4] ;  [2] ;  [5] ;  [6]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department; Tsinghua Univ., Beijing (China). Department of Chemical Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
  3. Stony Brook Univ., NY (United States). Department of Materials Science and Chemical Engineering
  4. Columbia Univ., New York, NY (United States). Department of Chemical Engineering
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department; Columbia Univ., New York, NY (United States). Department of Chemical Engineering
Publication Date:
Report Number(s):
BNL-209055-2018-JAAM
Journal ID: ISSN 0027-8424
Grant/Contract Number:
SC0012704; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 115; Journal Issue: 33; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CO2 reduction; ethane dehydrogenation; metal–oxide interfaces; selectivity; heterogeneous catalysis
OSTI Identifier:
1473652
Alternate Identifier(s):
OSTI ID: 1462157

Yan, Binhang, Yao, Siyu, Kattel, Shyam, Wu, Qiyuan, Xie, Zhenhua, Gomez, Elaine, Liu, Ping, Su, Dong, and Chen, Jingguang G. Active sites for tandem reactions of CO 2 reduction and ethane dehydrogenation. United States: N. p., Web. doi:10.1073/pnas.1806950115.
Yan, Binhang, Yao, Siyu, Kattel, Shyam, Wu, Qiyuan, Xie, Zhenhua, Gomez, Elaine, Liu, Ping, Su, Dong, & Chen, Jingguang G. Active sites for tandem reactions of CO 2 reduction and ethane dehydrogenation. United States. doi:10.1073/pnas.1806950115.
Yan, Binhang, Yao, Siyu, Kattel, Shyam, Wu, Qiyuan, Xie, Zhenhua, Gomez, Elaine, Liu, Ping, Su, Dong, and Chen, Jingguang G. 2018. "Active sites for tandem reactions of CO 2 reduction and ethane dehydrogenation". United States. doi:10.1073/pnas.1806950115.
@article{osti_1473652,
title = {Active sites for tandem reactions of CO 2 reduction and ethane dehydrogenation},
author = {Yan, Binhang and Yao, Siyu and Kattel, Shyam and Wu, Qiyuan and Xie, Zhenhua and Gomez, Elaine and Liu, Ping and Su, Dong and Chen, Jingguang G.},
abstractNote = {We present that ethylene (C2H4) is one of the most important raw materials for chemical industry. The tandem reactions of CO2-assisted dehydrogenation of ethane (C2H6) to ethylene creates an opportunity to effectively use the underutilized ethane from shale gas while mitigating anthropogenic CO2 emissions. Here we identify the most likely active sites over CeO2-supported NiFe catalysts by using combined in situ characterization with density-functional theory (DFT) calculations. The experimental and theoretical results reveal that the Ni–FeOx interfacial sites can selectively break the C–H bonds and preserve the C–C bond of C2H6 to produce ethylene, while the Ni–CeOx interfacial sites efficiently cleave all of the C–H and C–C bonds to produce synthesis gas. Lastly, controlled synthesis of the two distinct active sites enables rational enhancement of the ethylene selectivity for the CO2-assisted dehydrogenation of ethane.},
doi = {10.1073/pnas.1806950115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 33,
volume = 115,
place = {United States},
year = {2018},
month = {7}
}

Works referenced in this record:

Oxidative dehydrogenation of ethane and propane: How far from commercial implementation?
journal, September 2007