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Title: Carbon dioxide reduction in tandem with light-alkane dehydrogenation

Abstract

A greenhouse gas and mild oxidant, CO2 can effect the oxidative dehydrogenation (CO2-ODH) of light alkanes over heterogeneous catalysts. These catalysts are bifunctional in that they mediate CO2 reduction while oxidizing the alkanes, most notably the C2–C4 components in shale gas. In this way, one obtains CO and alkenes as value-added products. Although desirable, this transformation has proven challenging in terms of catalyst design, with most catalysts for the CO2-ODH being metal oxides that typically undergo rapid deactivation. More recently, bimetallic catalysts have been identified as promising systems to activate alkanes by either selectively cleaving C–H bonds to produce alkenes or breaking all the C–C and C–H bonds to produce the dry reforming products CO and H2. This Review describes general trends in the CO2-ODH of light alkanes. Furthermore, we will outline how to use a combined approach involving flow reactor experiments, in operando characterization and density functional theory to determine whether a catalyst is intrinsically active for CO2-ODH or dry reforming.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]
  1. Columbia Univ., New York, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States); Tsinghua Univ., Beijing (China)
  3. Columbia Univ., New York, NY (United States); Florida A & M University, Tallahassee, FL (United States)
  4. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1580234
Report Number(s):
BNL-212449-2019-JAAM
Journal ID: ISSN 2397-3358
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Reviews Chemistry
Additional Journal Information:
Journal Volume: 3; Journal Issue: 11; Journal ID: ISSN 2397-3358
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Gomez, Elaine, Yan, Binhang, Kattel, Shyam, and Chen, Jingguang G. Carbon dioxide reduction in tandem with light-alkane dehydrogenation. United States: N. p., 2019. Web. doi:10.1038/s41570-019-0128-9.
Gomez, Elaine, Yan, Binhang, Kattel, Shyam, & Chen, Jingguang G. Carbon dioxide reduction in tandem with light-alkane dehydrogenation. United States. doi:10.1038/s41570-019-0128-9.
Gomez, Elaine, Yan, Binhang, Kattel, Shyam, and Chen, Jingguang G. Tue . "Carbon dioxide reduction in tandem with light-alkane dehydrogenation". United States. doi:10.1038/s41570-019-0128-9. https://www.osti.gov/servlets/purl/1580234.
@article{osti_1580234,
title = {Carbon dioxide reduction in tandem with light-alkane dehydrogenation},
author = {Gomez, Elaine and Yan, Binhang and Kattel, Shyam and Chen, Jingguang G.},
abstractNote = {A greenhouse gas and mild oxidant, CO2 can effect the oxidative dehydrogenation (CO2-ODH) of light alkanes over heterogeneous catalysts. These catalysts are bifunctional in that they mediate CO2 reduction while oxidizing the alkanes, most notably the C2–C4 components in shale gas. In this way, one obtains CO and alkenes as value-added products. Although desirable, this transformation has proven challenging in terms of catalyst design, with most catalysts for the CO2-ODH being metal oxides that typically undergo rapid deactivation. More recently, bimetallic catalysts have been identified as promising systems to activate alkanes by either selectively cleaving C–H bonds to produce alkenes or breaking all the C–C and C–H bonds to produce the dry reforming products CO and H2. This Review describes general trends in the CO2-ODH of light alkanes. Furthermore, we will outline how to use a combined approach involving flow reactor experiments, in operando characterization and density functional theory to determine whether a catalyst is intrinsically active for CO2-ODH or dry reforming.},
doi = {10.1038/s41570-019-0128-9},
journal = {Nature Reviews Chemistry},
number = 11,
volume = 3,
place = {United States},
year = {2019},
month = {9}
}

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