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Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature

Louise Hamdy, ABEL GOUGSA, Wing Ying Chow Orcid Logo, James Russell, Enrique García-Díez, Viktoriia Kulakova, Susana Garcia, Andrew Barron Orcid Logo, Marco Taddei Orcid Logo, Enrico Andreoli Orcid Logo

Materials Advances, Volume: 3, Issue: 7, Pages: 3174 - 3191

Swansea University Authors: Louise Hamdy, ABEL GOUGSA, James Russell, Andrew Barron Orcid Logo, Marco Taddei Orcid Logo, Enrico Andreoli Orcid Logo

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DOI (Published version): 10.1039/d1ma01072g

Abstract

New self-supported polyamine CO2 adsorbents are prepared by cross-linking branched polyethyleneimine (PEI) with 2,4,6-tris-(4-bromomethyl-3-fluoro-phenyl)-1,3,5-triazine (4BMFPT). Controlling the degree of cross-linking to ensure abundant free amine functionalities while maintaining a structure cond...

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Published in: Materials Advances
ISSN: 2633-5409
Published: Royal Society of Chemistry (RSC) 2022
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URI: https://cronfa.swan.ac.uk/Record/cronfa60514
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Abstract: New self-supported polyamine CO2 adsorbents are prepared by cross-linking branched polyethyleneimine (PEI) with 2,4,6-tris-(4-bromomethyl-3-fluoro-phenyl)-1,3,5-triazine (4BMFPT). Controlling the degree of cross-linking to ensure abundant free amine functionalities while maintaining a structure conducive to efficient mass transfer is key to accessing high CO2 adsorption and fast kinetics at ambient temperature. The polyamine-based adsorbent, PEI-4BMFPT, 10 : 1 (R), is composed of spherical particles up to 3 μm in diameter and demonstrates fast CO2 uptake of 2.31 mmol g−1 under 1 atm, 90% CO2/Ar at 30 °C. Its CO2/N2 selectivity, predicted by the ideal adsorbed solution theory is 575, equalling that of highly selective metal–organic frameworks. Based on humidified thermogravimetric analysis, it was observed that the presence of water promotes CO2 uptake capacity of 10 : 1 (R) to 3.27 mmol g−1 and results in strong chemisorption; likely by formation of ammonium carbonate and bicarbonate species. It is observed that CO2 uptake enhancement is highly subject to relative humidity and CO2 partial pressure conditions. When adsorption conditions combined low temperatures with low partial pressure CO2, 10 : 1 (R) showed reduced uptake. Tested under breakthrough conditions representative of post-combustion conditions, at 75% RH and 40 °C, CO2 uptake was reduced by 83% of the dry adsorption capacity. This body of work further advances the development of support-free CO2 adsorbents for ambient temperature applications and highlights the drastic effect that relative humidity and CO2 partial pressure have on uptake behaviour.
College: Faculty of Science and Engineering
Funders: This work is part of the Flexible Integrated Energy Systems (FLEXIS) and Reducing Industrial Carbon Emissions (RICE) research operations funded by the Welsh European Funding Office (WEFO) through the Welsh Government. Support was provided by the Engineering and Physical Sciences Research Council through the SUSTAIN Manufacturing Hub EP/S018107/1. Financial support was also provided by the Sêr Cymru Chair Programme and the Robert A. Welch Foundation (C-0002). We also acknowledge funding from European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement no 663830. The authors would like to acknowledge Stephen Shearan for assistance with material synthesis and Dr Matthew J. McPherson for assistance in performing BET measurements. We would like to acknowledge the assistance provided by Swansea University College of Engineering AIM Facility, which was funded in part by the EPSRC (EP/M028267/1), the European Regional Development Fund through the Welsh Government (80708) and the Ser Solar project via the Welsh Government. We acknowledge postdoctoral fellowship funding from the German Academic Exchange Service (DAAD) and Leibniz Association for WYC. This work benefited from access to the FMP Berlin NMR facility. This work was also supported in part by the PrISMa Project (299659), funded through the ACT Programme (Accelerating CCS Technologies, Horizon 2020 Project 294766).
Issue: 7
Start Page: 3174
End Page: 3191