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Novel Process Concept for Cryogenic CO2 Capture Novel process concept for cryogenic CO2 capture Citation for published version (APA): Tuinier, M. J. (2011). Novel process concept for cryogenic CO2 capture. Technische Universiteit Eindhoven. https://doi.org/10.6100/IR719418 DOI: 10.6100/IR719418 Document status and date: Published: 01/01/2011 Document Version: Publisher’s PDF, also known as Version of Record (includes final page, issue and volume numbers) Please check the document version of this publication: • A submitted manuscript is the version of the article upon submission and before peer-review. There can be important differences between the submitted version and the official published version of record. People interested in the research are advised to contact the author for the final version of the publication, or visit the DOI to the publisher's website. • The final author version and the galley proof are versions of the publication after peer review. • The final published version features the final layout of the paper including the volume, issue and page numbers. Link to publication General rights Copyright and moral rights for the publications made accessible in the public portal are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights. • Users may download and print one copy of any publication from the public portal for the purpose of private study or research. • You may not further distribute the material or use it for any profit-making activity or commercial gain • You may freely distribute the URL identifying the publication in the public portal. If the publication is distributed under the terms of Article 25fa of the Dutch Copyright Act, indicated by the “Taverne” license above, please follow below link for the End User Agreement: www.tue.nl/taverne Take down policy If you believe that this document breaches copyright please contact us at: [email protected] providing details and we will investigate your claim. Download date: 28. Sep. 2021 Novel Process Concept for Cryogenic CO2 Capture Samenstelling promotiecommissie: prof.dr. J. Meuldijk, voorzitter Technische Universiteit Eindhoven prof.dr.ir. M. van Sint Annaland, promotor Technische Universiteit Eindhoven Prof.Dr.-Ing. A. Seidel-Morgenstern Otto-von-Guericke-Universitat¨ Magdeburg prof.dr. G.J. Kramer Shell / Universiteit Leiden prof.dr.ir. J.A.M. Kuipers Technische Universiteit Eindhoven prof.dr.ir. T.H. van der Meer Universiteit Twente dr.ir. D.W.F. Brilman Universiteit Twente The research reported in this thesis was sponsored by Shell Global Solu- tions International. c M.J. Tuinier, Eindhoven, The Netherlands, 2011 No part of this work may be reproduced in any form by print, photocopy or any other means without written permission from the author. Publisher: Ipskamp Drukkers B.V., P.O. Box 333, 7500 AH, Enschede, The Netherlands. A catalogue record is available from the Eindhoven University of Techno- logy Library. ISBN: 978-90-386-2900-1 Novel Process Concept for Cryogenic CO2 Capture PROEFSCHRIFT ter verkrijging van de graad van doctor aan de Technische Universiteit Eindhoven, op gezag van de rector magnificus, prof.dr.ir. C.J. van Duijn, voor een commissie aangewezen door het College voor Promoties in het openbaar te verdedigen op donderdag 24 november 2011 om 16.00 uur door Martin Jan Tuinier geboren te Wijhe Dit proefschrift is goedgekeurd door de promotor: prof.dr.ir. M. van Sint Annaland vi Contents Summary 1 1 Introduction 5 1.1 Climatechange........................... 5 1.2 Carboncaptureandstorage . 8 1.3 Thisthesis ............................. 15 2 Cryogenic packed bed process concept 19 2.1 Introduction ............................ 20 2.2 Theprocessconcept. 20 2.3 Detailednumericalmodel. 24 2.4 Simplifiedmodel: Sharpfrontapproach . 31 2.5 Processanalysis .......................... 37 2.6 Discussionandconclusions . 42 3 Experimental demonstration of the concept 45 3.1 Introduction ............................ 46 3.2 Experimentalsetupandprocedure . 46 3.3 Results ............................... 48 3.4 Simulations............................. 52 3.5 Discussionandconclusions . 56 4 Mass deposition rates of carbon dioxide 59 4.1 Introduction ............................ 60 4.2 Experimental ............................ 61 4.3 Results ............................... 67 4.4 Developmentofafrostgrowthmodel . 73 4.5 Discussionandconclusions . 87 vii viii Contents 5 Experimental demonstration in a pilot scale setup 93 5.1 Introduction ............................ 94 5.2 Experimental ............................ 94 5.3 Experimentalresults . 98 5.4 Simulations............................. 101 5.5 Discussionandconclusions . 107 6 Techno-economic evaluation 111 6.1 Introduction ............................ 112 6.2 Processevaluation. 113 6.3 Comparison with absorption and membrane technology . 124 6.4 Conclusions............................. 131 7 Biogas purification 133 7.1 Introduction ............................ 134 7.2 Adsorption ............................. 135 7.3 Cryogenicpackedbedconcept . 136 7.4 Adsorption versus cryogenic packed bed concept . 142 7.5 Hydrogensulfideremoval. 146 7.6 Discussionandconclusions . 146 8 Epilogue and outlook 149 8.1 Importantaspectsforfuturedevelopment . 150 8.2 Futureoftheproposedconcept . 152 Bibliography 154 List of publications 163 Curriculum Vitae 165 Dankwoord 167 Summary Carbon capture and storage (CCS) is generally considered as one of the necessary methods to mitigate anthropogenic CO2 emissions to combat climate change. The costs of CCS can for a large extent be attributed to the capture process. Several post-combustion CO2 capture processes have been developed, such as scrubbing, membrane processes and pres- sure swing adsorption. Amine scrubbing is currently the state of the art technology, in which CO2 is being removed by contacting the flue gas with a solvent in an absorber. Regeneration is carried out by heat- ing the loaded solvent in a stripping column. The main disadvantages of this process are the energy costs related to the regeneration step and solvent losses due to degradation. A promising novel option is to freeze out (desublimate) CO2 from flue gases using cryogenically cooled sur- faces. High cooling costs could be minimized by exploiting the cold duty available at Liquefied Natural Gas (LNG) regasification sites. No stan- dard process equipment is available to deal with separations based on desublimation. Therefore, a novel process concept has been developed and investigated in this dissertation, based on the periodic operation of cryogenically cooled packed beds. When feeding a flue gas to a previously cryogenically refrigerated packed bed, CO2 will freeze onto the packing surface, while permanent gases such as N2 pass through the bed unaltered. The amount of CO2 depositing onto the packing reaches an equilibrium value, because the amount of cold energy stored in the packing is limited. Therefore, plug- ging of the bed is intrinsically circumvented. A front of desublimating CO2 will move through the bed, until breakthrough is observed. At that point, the bed is switched to a recovery step, in which all previously de- posited CO2 will be removed by recycling gaseous CO2 through the bed. The energy required for the sublimation of CO2 can be provided to the 1 2 Summary bed by feeding the flue gas at elevated temperatures during the capture step. A process cycle is finally finished with a cooling step, in which the bed is again refrigerated to its initial temperature. The proposed process concept has several advantages: simple and low cost equipment can be used, large pressure drops can be avoided, deep CO2 removal is possible and CO2, H2O and other impurities can be separated simultaneously. The development in time of axial temperature, gas concentration and mass deposition profiles in the packed beds during the different process steps can be well described using a one-dimensional, pseudo- homogeneous, axially dispersed plug flow model, in which the mass and energy balances are solved simultaneously using an advanced numerical scheme. When assuming that no axial dispersion and mass deposition rate limitations occur during the process, the fronts which are developed are very well defined (sharp). Based on this assumption, the process can be well described with a simplified model (the ‘sharp front’ approach). With basic mass and energy conversation laws, the axial temperature, gas composition, and mass deposition profiles and front velocities can be calculated very fast using this model, making it a perfect tool for design and evaluation of the process. In the limit of negligible dispersion in the detailed numerical model, the solution converges to the profiles predicted by the sharp front approach. Outcomes of the sharp front approach show that the specific cooling duty required to capture a certain amount of CO2 increases for lower CO2 concentrations in the feed gas and for higher ini- tial bed temperatures. A small scale experimental setup has been designed and constructed to measure axial temperature profiles and CO2 concentrations at the outlet during the capture step. Experiments have been carried out for N2/CO2 and N2/CO2/H2O mixtures. The results showed that a good separation between the single components is possible. The experimental findings have been compared to results calculated using the numerical model. The front velocities and therefore CO2 breakthrough times and the temperature profiles for different CO2 and
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