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

Abstract

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–FeO_x interfacial sites can selectively break the C–H bonds and preserve the C–C bond of C₂H₆ 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 CO₂-assisted dehydrogenation of ethane.

Authors:

Yan, Binhang ^[1]; Yao, Siyu ^[2]; Kattel, Shyam ^[2]; Wu, Qiyuan ^[3]; Xie, Zhenhua ^[4]; Gomez, Elaine ^[4]; Liu, Ping ^[2]; Su, Dong ^[5]; Chen, Jingguang G. ^[6]

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+ Show Author Affiliations

1. Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973,, Department of Chemical Engineering, Tsinghua University, 100084 Beijing, China,
2. Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973,
3. Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794,
4. Department of Chemical Engineering, Columbia University, New York, NY 10027,
5. Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973
6. Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973,, Department of Chemical Engineering, Columbia University, New York, NY 10027,

Publication Date:

Mon Jul 30 00:00:00 EDT 2018

Research Org.:

Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1462157

Alternate Identifier(s):

OSTI ID: 1473652

Report Number(s):

BNL-209055-2018-JAAM
Journal ID: ISSN 0027-8424

Grant/Contract Number:  

SC0012704; AC02-05CH11231

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 33; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

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