skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts

Abstract

In this paper, the inherent variability and insufficiencies in the co-production of propylene from steam crackers has raised concerns regarding the global propylene production gap and has directed industry to develop more on-purpose propylene technologies. The oxidative dehydrogenation of propane by CO2 (CO2-ODHP) can potentially fill this gap while consuming a greenhouse gas. Non-precious FeNi and precious NiPt catalysts supported on CeO2 have been identified as promising catalysts for CO2-ODHP and dry reforming, respectively, in flow reactor studies conducted at 823 K. In-situ X-ray absorption spectroscopy measurements revealed the oxidation states of metals under reaction conditions and density functional theory calculations were utilized to identify the most favorable reaction pathways over the two types of catalysts.

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [2]; ORCiD logo [3]
  1. Columbia Univ., New York, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. 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)
OSTI Identifier:
1439297
Report Number(s):
BNL-205709-2018-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Gomez, Elaine, Kattel, Shyam, Yan, Binhang, Yao, Siyu, Liu, Ping, and Chen, Jingguang G. Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts. United States: N. p., 2018. Web. doi:10.1038/s41467-018-03793-w.
Gomez, Elaine, Kattel, Shyam, Yan, Binhang, Yao, Siyu, Liu, Ping, & Chen, Jingguang G. Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts. United States. doi:10.1038/s41467-018-03793-w.
Gomez, Elaine, Kattel, Shyam, Yan, Binhang, Yao, Siyu, Liu, Ping, and Chen, Jingguang G. Wed . "Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts". United States. doi:10.1038/s41467-018-03793-w. https://www.osti.gov/servlets/purl/1439297.
@article{osti_1439297,
title = {Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts},
author = {Gomez, Elaine and Kattel, Shyam and Yan, Binhang and Yao, Siyu and Liu, Ping and Chen, Jingguang G.},
abstractNote = {In this paper, the inherent variability and insufficiencies in the co-production of propylene from steam crackers has raised concerns regarding the global propylene production gap and has directed industry to develop more on-purpose propylene technologies. The oxidative dehydrogenation of propane by CO2 (CO2-ODHP) can potentially fill this gap while consuming a greenhouse gas. Non-precious FeNi and precious NiPt catalysts supported on CeO2 have been identified as promising catalysts for CO2-ODHP and dry reforming, respectively, in flow reactor studies conducted at 823 K. In-situ X-ray absorption spectroscopy measurements revealed the oxidation states of metals under reaction conditions and density functional theory calculations were utilized to identify the most favorable reaction pathways over the two types of catalysts.},
doi = {10.1038/s41467-018-03793-w},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 15 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Kinetics of the reverse-Boudouard reaction over supported nickel catalysts
journal, August 2006


Light alkanes CO2 reforming to synthesis gas over Ni based catalysts
journal, June 2006


Carbon dioxide utilization as a soft oxidant and promoter in catalysis
journal, January 2012

  • Ansari, Mohd Bismillah; Park, Sang-Eon
  • Energy & Environmental Science, Vol. 5, Issue 11
  • DOI: 10.1039/c2ee22409g

Projector augmented-wave method
journal, December 1994


Opportunities and prospects in the chemical recycling of carbon dioxide to fuels
journal, November 2009


Dry reforming of propane over supported Re catalyst
journal, July 2005


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


The role of the Boudouard and water–gas shift reactions in the methanation of CO or CO2 over Ni/γ-Al2O3 catalyst
journal, October 2016


Special points for Brillouin-zone integrations
journal, June 1976

  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Methane activation: the past and future
journal, January 2014

  • Tang, Pei; Zhu, Qingjun; Wu, Zhaoxuan
  • Energy Environ. Sci., Vol. 7, Issue 8
  • DOI: 10.1039/C4EE00604F

Dry Reforming of Ethane and Butane with CO 2 over PtNi/CeO 2 Bimetallic Catalysts
journal, September 2016


Ab initio molecular dynamics for open-shell transition metals
journal, November 1993


Cooperativity and Dynamics Increase the Performance of NiFe Dry Reforming Catalysts
journal, January 2017

  • Kim, Sung Min; Abdala, Paula Macarena; Margossian, Tigran
  • Journal of the American Chemical Society, Vol. 139, Issue 5
  • DOI: 10.1021/jacs.6b11487

Selective oxidehydrogenation of ethane with CO2 over CeO2-based catalysts
journal, August 2000


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Inhomogeneous Electron Gas
journal, November 1964


CO 2 reforming of propane over supported Rh
journal, May 2003


Promoting effects of CO2 on dehydrogenation of propane over a SiO2-supported Cr2O3 catalyst
journal, October 1998


Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992


A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

  • Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
  • DOI: 10.1063/1.1329672

Catalytic Conversion of Alkanes to Olefins by Carbon Dioxide Oxidative DehydrogenationA Review
journal, July 2004


Kinetic Study of Propane CO 2 Reforming over Bimetallic Mo–Ni/Al 2 O 3 Catalyst
journal, June 2013

  • Siahvashi, Arman; Adesina, Adesoji A.
  • Industrial & Engineering Chemistry Research, Vol. 52, Issue 44
  • DOI: 10.1021/ie400637w

An extreme event of sea-level rise along the Northeast coast of North America in 2009–2010
journal, February 2015

  • Goddard, Paul B.; Yin, Jianjun; Griffies, Stephen M.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7346

A review of dry (CO 2 ) reforming of methane over noble metal catalysts
journal, January 2014

  • Pakhare, Devendra; Spivey, James
  • Chem. Soc. Rev., Vol. 43, Issue 22
  • DOI: 10.1039/C3CS60395D

Enhanced Carbon-Resistant Dry Reforming Fe-Ni Catalyst: Role of Fe
journal, March 2015

  • Theofanidis, Stavros Alexandros; Galvita, Vladimir V.; Poelman, Hilde
  • ACS Catalysis, Vol. 5, Issue 5
  • DOI: 10.1021/acscatal.5b00357

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965