CO2 conversion; CO2 dissociation; Nozzle; Plasma-based conversion; Power-2-X; Thermal plasma; Microwave plasma; Plasma quenching; Post-plasma; Power; Value-added chemicals; Chemical Engineering (all); Fuel Technology; Energy Engineering and Power Technology; Organic Chemistry; General Chemical Engineering
Abstract :
[en] Transforming CO2 into value-added chemicals is crucial to realizing a carbon–neutral economy, and plasma-based conversion, a Power-2-X technology, offers a promising route to realizing an efficient and scalable process. This paper investigates the effects of post-plasma placement of a converging–diverging nozzle in a vortex-stabilized 2.45 GHz CO2 microwave plasma reactor to increase energy efficiency and conversion. The CDN leads to a 21 % relative increase in energy efficiency (31 %) and CO2 conversion (13 %) at high flow rates and near-atmospheric conditions. The most significant performance improvement was seen at low flow rates and sub-atmospheric pressure (300 mbar), where energy efficiency was 23 % and conversion was 28 %, a 71 % relative increase over conditions without the CDN. Using CFD simulations, we found that the CDN produces a change in the flow geometry, leading to a confined temperature profile at the height of the plasma, and forced extraction of CO to the post-CDN region.
Disciplines :
Chemistry
Author, co-author :
Mercer, E.R.; Research group PLASMANT, Department of Chemistry, University of Antwerp, Antwerpen, Belgium ; Research Group PSFD, Dutch Institute of Fundamental Energy Research, AJ Eindhoven, Netherlands
Van Alphen, S.; Research group PLASMANT, Department of Chemistry, University of Antwerp, Antwerpen, Belgium ; Research group ChIPS, Department of Chemistry, University of Mons, Mons, Belgium
van Deursen, C.F.A.M.; Research Group PSFD, Dutch Institute of Fundamental Energy Research, AJ Eindhoven, Netherlands
Righart, T.W.H.; Plasma Chemistry, Department of Circular Chemical Engineering, Faculty of Science and Engineering, Maastricht University, MD Maastricht, Netherlands
Bongers, W.A.; Research Group PSFD, Dutch Institute of Fundamental Energy Research, AJ Eindhoven, Netherlands
Snyders, Rony ; Université de Mons - UMONS > Faculté des Sciences > Service de Chimie des Interactions Plasma-Surface ; Materia Nova Research Center, Mons, Belgium
Bogaerts, A.; Research group PLASMANT, Department of Chemistry, University of Antwerp, Antwerpen, Belgium
van de Sanden, M.C.M.; Research Group PSFD, Dutch Institute of Fundamental Energy Research, AJ Eindhoven, Netherlands ; Eindhoven Institute for Renewable Energy Systems, Eindhoven University of Technology, MB Eindhoven, Netherlands
Peeters, F.J.J.; Research Group PSFD, Dutch Institute of Fundamental Energy Research, AJ Eindhoven, Netherlands
Language :
English
Title :
Post-plasma quenching to improve conversion and energy efficiency in a CO2 microwave plasma
This research was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement No 810182 – SCOPE ERC Synergy project) and the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023). The computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation - Flanders (FWO) and the Flemish Government. In addition, this work has been carried out as part of the Plasma Power to Gas research program with reference 15325, which is by the Netherlands Organization for Scientific Research (NWO) and Alliander N.V.This research was supported by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement No 810182 – SCOPE ERC Synergy project) and the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023). The computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation - Flanders (FWO) and the Flemish Government. In addition, this work has been carried out as part of the Plasma Power to Gas research program with reference 15325, which is by the Netherlands Organization for Scientific Research (NWO) and Alliander N.V.
Hoffert, M.I., Caldeira, K., Jain, A.K., Haites, E.F., Harvey, L.D.D., Potter, S.D., et al. Energy implications of future stabilization of atmospheric CO2 content. Nature 395:6705 (1998), 881–884.
IEA, “CO2 emissions by energy source, World 1990-2019,” IEA, 2019. https://www.iea.org/data-and-statistics/data-browser/?country=WORLD&fuel=CO2 emissions&indicator=CO2BySource (accessed Dec. 01, 2021).
Wolf, A.J., Peeters, F.J.J., Groen, P.W.C., Bongers, W.A., Van De Sanden, M.C.M., CO2Conversion in nonuniform discharges: disentangling dissociation and recombination mechanisms. J Phys Chem C 124:31 (2020), 16806–16819, 10.1021/ACS.JPCC.0C03637/SUPPL_FILE/JP0C03637_SI_001.PDF.
A. Van De Steeg, P. Viegas, A. Silva, T. Butterworth, A. Van Bavel, and J. Smits, “Redefining the Microwave Plasma Mediated CO 2 Reduction Efficiency Limit: The role of O-CO2 Association,” pp. 1–15.
Legasov, V.A., et al. A nonequilibrium plasma-chemical process of CO2 dissociation in high-frequency and ultrahigh-frequency discharges. Sov Phys Dokl, 23, 1978, 44.
Snoeckx, R., Bogaerts, A., Plasma technology – a novel solution for CO2 conversion?. Chem Soc Rev 46:19 (2017), 5805–5863, 10.1039/C6CS00066E.
Bongers, W., et al. Plasma-driven dissociation of CO2 for fuel synthesis. Plasma Process Polym, 2016, 10.1002/ppap.201600126.
P. Viegas et al., “Insight into contraction dynamics of microwave plasmas for CO2 conversion,” 2020.
Yang, T., Shen, J., Ran, T., Li, J., Chen, P., Yin, Y., Understanding CO2 decomposition by thermal plasma with supersonic expansion quench. Plasma Sci Technol, 20(6), 2018, 65502, 10.1088/2058-6272/aaa969.
Li, J., Zhang, X., Shen, J., Ran, T., Chen, P., Yin, Y., Dissociation of CO2 by thermal plasma with contracting nozzle quenching. J CO2 Util 21 (2017), 72–76, 10.1016/j.jcou.2017.04.003.
Vermeiren, V., Bogaerts, A., Plasma-based CO2 conversion: to quench or not to quench?. J Phys Chem C 124:34 (2020), 18401–18415, 10.1021/acs.jpcc.0c04257.
van Rooij, G.J., Akse, H.N., Bongers, W.A., van de Sanden, M.C.M., Plasma for electrification of chemical industry: a case study on CO2 reduction. Plasma Phys Control Fusion, 60(1), 2017, 14019, 10.1088/1361-6587/aa8f7d.
den Harder, N., et al. Homogeneous CO2 conversion by microwave plasma: Wave propagation and diagnostics. Plasma Process Polym, 14(6), 2016, 1600120, 10.1002/ppap.201600120.
Wolf, A.J., Righart, T.W.H., Peeters, F.J.J., Bongers, W.A., Van De Sanden, M.C.M., Implications of thermo-chemical instability on the contracted modes in CO2 microwave plasmas. Plasma Sources Sci Technol, 29(2), 2020, 25005, 10.1088/1361-6595/ab5eca.
Wolf, A.J., Righart, T.W.H., Peeters, F.J.J., Groen, P.W.C., Van De Sanden, M.C.M., Bongers, W.A., Characterization of CO2 microwave plasma based on the phenomenon of skin-depth-limited contraction. Plasma Sources Sci Technol, 28(11), 2019, pp, 10.1088/1361-6595/ab4e61.
Wolf, A.J., Righart, T.W.H., Peeters, F.J.J., Bongers, W.A., van de Sanden, M.C.M., Implications of thermo-chemical instability on the contracted modes in CO2 microwave plasmas. Plasma Sources Sci Technol, 29(2), 2020, 25005, 10.1088/1361-6595/ab5eca.
T. W. H. Righart, “Gas Temperatures adn Residence Times in a Vortex Stabilized CO2 Microwave Plasma,” TU/e, 2018.
Raposo, G., van de Steeg, A.W., Mercer, E.R., van Deursen, C.F.A.M., Hendrickx, H.J.L., Bongers, W.A., et al. Flame Bands: CO + O chemiluminescence as a measure of gas temperature. J Phys D Appl Phys, 54(37), 2021, 374005.
Slack, M., Grillo, A., High temperature rate coefficient measurements of CO + O chemiluminescence. Combust Flame 59:2 (1985), 189–196, 10.1016/0010-2180(85)90024-0.
Liu, B., Huang, Q., Wang, P., Influence of surrounding gas temperature on thermocouple measurement. Case Stud Therm Eng, 19, 2020, 100627, 10.1016/j.csite.2020.100627.
T. Magin, G. Degrez, and I. Sokolova, “Thermodynamic and transport properties of martian atmosphere for space entry application,” 33rd Plasmadynamics Lasers Conf., no. May, 2002, doi: 10.2514/6.2002-2226.
A. J. Wolf, “Thermal aspects of CO2 conversion in the vortex-stabilized microwave plasma.,” Technische Universiteit Eindhoven, 2020.
Kelly, S., Bogaerts, A., Nitrogen fixation in an electrode-free microwave plasma. Joule 5:11 (2021), 3006–3030, 10.1016/j.joule.2021.09.009.