Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts
Abstract
An efficient mitigation of abundantly available CO2 is critical for sustainable environmental impact as well as for novel industrial applications. Using ethane, CO2 can be catalytically converted into a useful feedstock (synthesis gas) and a value-added monomer (ethylene) via the dry reforming pathway through the C–C bond scission and the oxidative dehydrogenation pathway through the C–H bond scission, respectively. Results from the current flow-reactor study show that the precious metal bimetallic CoPt/CeO2 catalyst undergoes the reforming reaction to produce syngas with enhanced activity and stability compared to the parent monometallic catalysts. In this paper, in order to replace Pt, the activities of non-precious CoMo/CeO2 and NiMo/CeO2 are investigated and the results indicate that NiMo/CeO2 is nearly as active as CoPt/CeO2 for the reforming pathway. Furthermore, FeNi/CeO2 is identified as a promising catalyst for the oxidative dehydrogenation to produce ethylene. Finally, density functional theory (DFT) calculations are performed to further understand the different pathways of the CoPt/CeO2 and FeNi/CeO2 catalysts.
- Authors:
-
[4];
- Univ. of Delaware, Newark, DE (United States). Dept. of Chemical and Biomolecular Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
- Tsinghua Univ., Beijing (China). College of Materials Science and Engineering
- Univ. of Illinois, Urbana, IL (United States). Dept. of Chemistry
- Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Contributing Org.:
- Univ. of Delaware, Newark, DE (United States); Tsinghua Univ., Beijing (China); Univ. of Illinois, Urbana, IL (United States); Columbia Univ., New York, NY (United States)
- OSTI Identifier:
- 1341673
- Alternate Identifier(s):
- OSTI ID: 1398839
- Report Number(s):
- BNL-113401-2017-JA
Journal ID: ISSN 0021-9517; R&D Project: CO035; KC0302010
- Grant/Contract Number:
- AC02-98CH10886
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Catalysis
- Additional Journal Information:
- Journal Volume: 343; Journal ID: ISSN 0021-9517
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Reforming; Oxidative dehydrogenation; Synthesis gas; Ethylene; CeO2 supports
Citation Formats
Myint, MyatNoeZin, Yan, Binhang, Wan, Jie, Zhao, Shen, and Chen, Jingguang G. Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts. United States: N. p., 2016.
Web. doi:10.1016/j.jcat.2016.02.004.
Myint, MyatNoeZin, Yan, Binhang, Wan, Jie, Zhao, Shen, & Chen, Jingguang G. Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts. United States. https://doi.org/10.1016/j.jcat.2016.02.004
Myint, MyatNoeZin, Yan, Binhang, Wan, Jie, Zhao, Shen, and Chen, Jingguang G. Fri .
"Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts". United States. https://doi.org/10.1016/j.jcat.2016.02.004. https://www.osti.gov/servlets/purl/1341673.
@article{osti_1341673,
title = {Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts},
author = {Myint, MyatNoeZin and Yan, Binhang and Wan, Jie and Zhao, Shen and Chen, Jingguang G.},
abstractNote = {An efficient mitigation of abundantly available CO2 is critical for sustainable environmental impact as well as for novel industrial applications. Using ethane, CO2 can be catalytically converted into a useful feedstock (synthesis gas) and a value-added monomer (ethylene) via the dry reforming pathway through the C–C bond scission and the oxidative dehydrogenation pathway through the C–H bond scission, respectively. Results from the current flow-reactor study show that the precious metal bimetallic CoPt/CeO2 catalyst undergoes the reforming reaction to produce syngas with enhanced activity and stability compared to the parent monometallic catalysts. In this paper, in order to replace Pt, the activities of non-precious CoMo/CeO2 and NiMo/CeO2 are investigated and the results indicate that NiMo/CeO2 is nearly as active as CoPt/CeO2 for the reforming pathway. Furthermore, FeNi/CeO2 is identified as a promising catalyst for the oxidative dehydrogenation to produce ethylene. Finally, density functional theory (DFT) calculations are performed to further understand the different pathways of the CoPt/CeO2 and FeNi/CeO2 catalysts.},
doi = {10.1016/j.jcat.2016.02.004},
journal = {Journal of Catalysis},
number = ,
volume = 343,
place = {United States},
year = {Fri Feb 26 00:00:00 EST 2016},
month = {Fri Feb 26 00:00:00 EST 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 89 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
A Process Integration Approach to the Assessment of CO 2 Fixation through Dry Reforming
journal, March 2015
- Noureldin, Mohamed M. B.; Elbashir, Nimir O.; Gabriel, Kerron J.
- ACS Sustainable Chemistry & Engineering, Vol. 3, Issue 4
Mitigation of CO2 by Chemical Conversion: Plausible Chemical Reactions and Promising Products
journal, March 1996
- Xiaoding, Xu; Moulijn, J. A.
- Energy & Fuels, Vol. 10, Issue 2, p. 305-325
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
Trends in the catalytic reduction of CO2 by hydrogen over supported monometallic and bimetallic catalysts
journal, May 2013
- Porosoff, Marc D.; Chen, Jingguang G.
- Journal of Catalysis, Vol. 301
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
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
The chemistry of methane reforming with carbon dioxide and its current and potential applications
journal, April 1995
- Edwards, J. H.; Maitra, A. M.
- Fuel Processing Technology, Vol. 42, Issue 2-3
High-performance Cr/H-ZSM-5 catalysts for oxidative dehydrogenation of ethane to ethylene with CO2 as an oxidant
journal, June 2002
- Mimura, Naoki; Takahara, Isao; Inaba, Megumu
- Catalysis Communications, Vol. 3, Issue 6
On ethane ODH mechanism and nature of active sites over NiO-based catalysts via isotopic labeling and methanol sorption studies
journal, February 2015
- Skoufa, Z.; Heracleous, E.; Lemonidou, A. A.
- Journal of Catalysis, Vol. 322
Dehydrogenation of ethane to ethylene over a highly efficient Ga2O3/HZSM-5 catalyst in the presence of CO2
journal, March 2009
- Shen, Zhenhao; Liu, Jian; Xu, Hualong
- Applied Catalysis A: General, Vol. 356, Issue 2
Oxidative Dehydrogenation of Ethane to Ethylene with Carbon dioxide over Cr–Ce/SBA-15 Catalysts
journal, July 2008
- Shi, Xuejun; Ji, Shengfu; Wang, Kai
- Catalysis Letters, Vol. 125, Issue 3-4
Dry Reforming and Reverse Water Gas Shift: Alternatives for Syngas Production?
journal, February 2015
- Schwab, Ekkehard; Milanov, Andrian; Schunk, Stephan Andreas
- Chemie Ingenieur Technik, Vol. 87, Issue 4
Oxidative Dehydrogenation of Ethane: Common Principles and Mechanistic Aspects
journal, March 2013
- Gärtner, Christian A.; van Veen, André C.; Lercher, Johannes A.
- ChemCatChem, Vol. 5, Issue 11
Catalytic Conversion of Alkanes to Olefins by Carbon Dioxide Oxidative DehydrogenationA Review
journal, July 2004
- Wang, Shaobin; Zhu, Z. H.
- Energy & Fuels, Vol. 18, Issue 4
Oxidative Dehydrogenation of Ethane to Ethylene with CO 2 over Fe−Cr/ZrO 2 Catalysts
journal, August 2009
- Deng, Shuang; Li, Songgeng; Li, Huiquan
- Industrial & Engineering Chemistry Research, Vol. 48, Issue 16
Activity and characterization of modified Cr2O3/ZrO2 nano-composite catalysts for oxidative dehydrogenation of ethane to ethylene with CO2
journal, May 2007
- Deng, Shuang; Li, Huiquan; Li, Songgeng
- Journal of Molecular Catalysis A: Chemical, Vol. 268, Issue 1-2
Studies on Dehydrogenation of Ethane in the Presence of CO 2 over Octahedral Molecular Sieve (OMS-2) Catalysts
journal, December 2009
- Jin, Lei; Reutenauer, Justin; Opembe, Naftali
- ChemCatChem, Vol. 1, Issue 4
Correlating extent of Pt–Ni bond formation with low-temperature hydrogenation of benzene and 1,3-butadiene over supported Pt/Ni bimetallic catalysts
journal, May 2010
- Lonergan, William W.; Vlachos, Dionisios G.; Chen, Jingguang G.
- Journal of Catalysis, Vol. 271, Issue 2
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Ab initio molecular dynamics for open-shell transition metals
journal, November 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 48, Issue 17
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
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992
- Perdew, John P.; Wang, Yue
- Physical Review B, Vol. 45, Issue 23, p. 13244-13249
Understanding the Role of Metal-Modified Mo(110) Bimetallic Surfaces for C–O/C═O and C–C Bond Scission in C3 Oxygenates
journal, November 2014
- Myint, MyatNoeZin; Chen, Jingguang G.
- ACS Catalysis, Vol. 5, Issue 1
Theoretical and experimental studies of the adsorption geometry and reaction pathways of furfural over FeNi bimetallic model surfaces and supported catalysts
journal, August 2014
- Yu, Weiting; Xiong, Ke; Ji, Na
- Journal of Catalysis, Vol. 317
Optimization and Selection of Reforming Approaches for Syngas Generation from Natural/Shale Gas
journal, November 2013
- Noureldin, Mohamed M. B.; Elbashir, Nimir O.; El-Halwagi, Mahmoud M.
- Industrial & Engineering Chemistry Research, Vol. 53, Issue 5
Effect of reaction temperature on activity of Pt- and Ru-substituted lanthanum zirconate pyrochlores (La2Zr2O7) for dry (CO2) reforming of methane (DRM)
journal, June 2013
- Pakhare, Devendra; Shaw, Christopher; Haynes, Daniel
- Journal of CO2 Utilization, Vol. 1
Identifying Different Types of Catalysts for CO 2 Reduction by Ethane through Dry Reforming and Oxidative Dehydrogenation
journal, November 2015
- Porosoff, Marc D.; Myint, Myat Noe Zin; Kattel, Shyam
- Angewandte Chemie International Edition, Vol. 54, Issue 51
Works referencing / citing this record:
Synergetic Impact of Secondary Metal Oxides of Cr-M/MCM41 Catalyst Nanoparticles for Ethane Oxidative Dehydrogenation Using Carbon Dioxide
journal, December 2019
- Al-Awadi, Abdulrhman S.; El-Toni, Ahmed Mohamed; Alhoshan, Mansour
- Crystals, Vol. 10, Issue 1
Effect of Oxide Support on Catalytic Performance of FeNi‐based Catalysts for CO 2 ‐assisted Oxidative Dehydrogenation of Ethane
journal, November 2019
- Yan, Binhang; Yao, Siyu; Chen, Jingguang G.
- ChemCatChem, Vol. 12, Issue 2
The Distinctive Effects of Glucose-Derived Carbon on the Performance of Ni-Based Catalysts in Methane Dry Reforming
journal, December 2019
- Ashik, Upm; Asano, Shusaku; Kudo, Shinji
- Catalysts, Vol. 10, Issue 1
The effects of bimetallic interactions for CO 2 ‐assisted oxidative dehydrogenation and dry reforming of propane
journal, June 2019
- Gomez, Elaine; Xie, Zhenhua; Chen, Jingguang G.
- AIChE Journal, Vol. 65, Issue 8
Activation Pathway of C‐H and C–C Bonds of Ethane by Pd Atom with CO 2 as a Soft Oxidant
journal, August 2019
- Yang, Zhongqing; Lan, Yan; Yan, Yunfei
- ChemistrySelect, Vol. 4, Issue 33
Supported Porous Nanomaterials as Efficient Heterogeneous Catalysts for CO 2 Fixation Reactions
journal, April 2018
- Bhanja, Piyali; Modak, Arindam; Bhaumik, Asim
- Chemistry – A European Journal, Vol. 24, Issue 29
Active sites for tandem reactions of CO 2 reduction and ethane dehydrogenation
journal, July 2018
- Yan, Binhang; Yao, Siyu; Kattel, Shyam
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 33
Carbon dioxide reduction in tandem with light-alkane dehydrogenation
journal, September 2019
- Gomez, Elaine; Yan, Binhang; Kattel, Shyam
- Nature Reviews Chemistry, Vol. 3, Issue 11
Dry Reforming of Shale Gas and Carbon Dioxide with Ni-Ce-Al 2 O 3 Catalyst: Syngas Production Enhanced over Ni-CeO x Formation
journal, September 2018
- Liu, Yan; Wu, Ye; Akhtamberdinova, Zarina
- ChemCatChem, Vol. 10, Issue 20