Oxygenate Production from Plasma-Activated Reaction of CO2 and Ethane

Biswas, Akash N.; Winter, Lea R.; Loenders, Björn; Xie, Zhenhua; Bogaerts, Annemie; Chen, Jingguang G.

doi:10.1021/acsenergylett.1c02355

Title: Oxygenate Production from Plasma-Activated Reaction of CO₂ and Ethane

Journal Article · 13 December 2021 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.1c02355 · OSTI ID:1839213

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Columbia Univ., New York, NY (United States)
Univ. of Antwerp (Belgium)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Upgrading ethane with CO₂ as a soft oxidant represents a desirable means of obtaining oxygenated hydrocarbons. This reaction is not thermodynamically feasible under mild conditions and has not been previously achieved as a one-step process. Non-thermal plasma was implemented as an alternative means of supplying energy to overcome activation barriers, leading to the production of alcohols, aldehydes, and acids as well as C₁-C₅₊ hydrocarbons under ambient pressure, with a maximum total oxygenate selectivity of 12%. A plasma chemical kinetic computational model was developed and found to be in good agreement with the experimental trends. Results from this study illustrate the potential to use plasma for the direct synthesis of value-added alcohols, acids, and aldehydes from ethane and CO₂ under mild conditions.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: European Research Council (ERC); FWO-SBO; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1839213

Report Number(s):: BNL--222589-2022-JAAM

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 1 Vol. 7; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (26)

One-Step Reforming of CO ₂ and CH ₄ into High-Value Liquid Chemicals and Fuels at Room Temperature by Plasma-Driven Catalysis Wang, Li; Yi, Yanhui; Wu, Chunfei Angewandte Chemie International Edition, Vol. 56, Issue 44 https://doi.org/10.1002/anie.201707131	journal	September 2017
Catalytic Performance and Mechanism for Oxygenated Compound Formation for Ethylene Hydroformylation over Supported Ru-M Bimetallic Carbonyl Cluster-Derived Catalysts Xiao, F. S.; Ichikawa, M. Journal of Catalysis, Vol. 147, Issue 2 https://doi.org/10.1006/jcat.1994.1174	journal	June 1994
Dynamic and LHHW Kinetic Analysis of Heterogeneous Catalytic Hydroformylation Balakos, M. W.; Chuang, S. S. C. Journal of Catalysis, Vol. 151, Issue 2 https://doi.org/10.1006/jcat.1995.1027	journal	February 1995
Hydroformylation and hydrogenation of olefins over rhodium zeolite catalyst Arai, H. Journal of Catalysis, Vol. 75, Issue 1 https://doi.org/10.1016/0021-9517(82)90134-8	journal	May 1982
Ironmaking Yang, Yongxiang; Raipala, Kalevi; Holappa, Lauri Treatise on Process Metallurgy https://doi.org/10.1016/B978-0-08-096988-6.00017-1	book	January 2014
Formation of long-lived CO−2, N2O−, and their dimer anions, by electron attachment to van der waals clusters Knapp, M.; Echt, O.; Kreisle, D. Chemical Physics Letters, Vol. 126, Issue 3-4 https://doi.org/10.1016/S0009-2614(86)80074-4	journal	May 1986
High-performance Cr/H-ZSM-5 catalysts for oxidative dehydrogenation of ethane to ethylene with CO2 as an oxidant Mimura, Naoki; Takahara, Isao; Inaba, Megumu Catalysis Communications, Vol. 3, Issue 6 https://doi.org/10.1016/S1566-7367(02)00117-6	journal	June 2002
Direct conversion of CO2 and CH4 into liquid chemicals by plasma-catalysis Li, Di; Rohani, Vandad; Fabry, Frédéric Applied Catalysis B: Environmental, Vol. 261 https://doi.org/10.1016/j.apcatb.2019.118228	journal	February 2020
Oxidative dehydrogenation of ethane with CO2 over catalyst under pulse corona plasma Zhang, Xiuling; Zhu, Aimin; Li, Xuehui Catalysis Today, Vol. 89, Issue 1-2 https://doi.org/10.1016/j.cattod.2003.11.015	journal	February 2004
N2 Fixation by Plasma-Activated Processes Winter, Lea R.; Chen, Jingguang G. Joule, Vol. 5, Issue 2 https://doi.org/10.1016/j.joule.2020.11.009	journal	February 2021
The Dominant Pathways for the Conversion of Methane into Oxygenates and Syngas in an Atmospheric Pressure Dielectric Barrier Discharge De Bie, Christophe; van Dijk, Jan; Bogaerts, Annemie The Journal of Physical Chemistry C, Vol. 119, Issue 39 https://doi.org/10.1021/acs.jpcc.5b06515	journal	September 2015
Identifying Surface Reaction Intermediates in Plasma Catalytic Ammonia Synthesis Winter, Lea R.; Ashford, Bryony; Hong, Jungmi ACS Catalysis, Vol. 10, Issue 24 https://doi.org/10.1021/acscatal.0c03166	journal	December 2020
Atmospheric Pressure and Room Temperature Synthesis of Methanol through Plasma-Catalytic Hydrogenation of CO ₂ Wang, Li; Yi, Yanhui; Guo, Hongchen ACS Catalysis, Vol. 8, Issue 1 https://doi.org/10.1021/acscatal.7b02733	journal	November 2017
Review of Plasma-Assisted Catalysis for Selective Generation of Oxygenates from CO ₂ and CH ₄ Liu, Shuang; Winter, Lea R.; Chen, Jingguang G. ACS Catalysis, Vol. 10, Issue 4 https://doi.org/10.1021/acscatal.9b04811	journal	January 2020
Plasma Technology: An Emerging Technology for Energy Storage Bogaerts, Annemie; Neyts, Erik C. ACS Energy Letters, Vol. 3, Issue 4 https://doi.org/10.1021/acsenergylett.8b00184	journal	March 2018
Low Temperature Production of Formaldehyde from Carbon Dioxide and Ethane by Plasma-Assisted Catalysis in a Ferroelectrically Moderated Dielectric Barrier Discharge Reactor Gómez-Ramírez, Ana; Rico, Victor J.; Cotrino, José ACS Catalysis, Vol. 4, Issue 2 https://doi.org/10.1021/cs4008528	journal	December 2013
Density Functional Theory Study of Synthesis of Oxygenates and Higher Hydrocarbons from Methane and Carbon Dioxide Using Cold Plasmas Wang, Jian-guo; Liu, Chang-jun; Eliassion, Baldur Energy & Fuels, Vol. 18, Issue 1 https://doi.org/10.1021/ef0300949	journal	January 2004
Activity of Rhodium-Catalyzed Hydroformylation: Added Insight and Predictions from Theory Sparta, Manuel; Børve, Knut J.; Jensen, Vidar R. Journal of the American Chemical Society, Vol. 129, Issue 27 https://doi.org/10.1021/ja070395n	journal	June 2007
Direct Observation of Kinetically Competent Surface Intermediates upon Ethylene Hydroformylation over Rh/Al ₂ O ₃ under Reaction Conditions by Time-Resolved Fourier Transform Infrared Spectroscopy Sivasankar, N.; Frei, H. The Journal of Physical Chemistry C, Vol. 115, Issue 15 https://doi.org/10.1021/jp112391n	journal	March 2011
Plasma-Based Dry Reforming: A Computational Study Ranging from the Nanoseconds to Seconds Time Scale Snoeckx, Ramses; Aerts, Robby; Tu, Xin The Journal of Physical Chemistry C, Vol. 117, Issue 10 https://doi.org/10.1021/jp311912b	journal	March 2013
Reactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates Xie, Zhenhua; Xu, Yuanguo; Xie, Meng Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15849-x	journal	April 2020
Synergistic effects of plasma–catalyst interactions for CH ₄ activation Kim, Jongsik; Go, David B.; Hicks, Jason C. Physical Chemistry Chemical Physics, Vol. 19, Issue 20 https://doi.org/10.1039/C7CP01322A	journal	January 2017
Active sites for tandem reactions of CO ₂ reduction and ethane dehydrogenation Yan, Binhang; Yao, Siyu; Kattel, Shyam Proceedings of the National Academy of Sciences, Vol. 115, Issue 33 https://doi.org/10.1073/pnas.1806950115	journal	July 2018
The influence of power and frequency on the filamentary behavior of a flowing DBD—application to the splitting of CO ₂ Ozkan, A.; Dufour, T.; Silva, T. Plasma Sources Science and Technology, Vol. 25, Issue 2 https://doi.org/10.1088/0963-0252/25/2/025013	journal	February 2016
Active sites for CO ₂ hydrogenation to methanol on Cu/ZnO catalysts Kattel, Shyam; Ramírez, Pedro J.; Chen, Jingguang G. Science, Vol. 355, Issue 6331 https://doi.org/10.1126/science.aal3573	journal	March 2017
Effect of Rh Dispersion on Vapor Phase and Pressurized Hydroformylation of Ethylene over Rh/SiO ₂ Catalyst Arakawa, Hironori; Takahashi, Nobuo; Hanaoka, Takaaki Chemistry Letters, Vol. 17, Issue 11 https://doi.org/10.1246/cl.1988.1917	journal	November 1988

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54 ENVIRONMENTAL SCIENCES
Chemical reactions
Hydrocarbons
Plasma
Power
Selectivity

Title: Oxygenate Production from Plasma-Activated Reaction of CO2 and Ethane

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Title: Oxygenate Production from Plasma-Activated Reaction of CO₂ and Ethane