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Switchable Aqueous Pentaethylenehexamine System for CO2 Capture: an Alternative Technology with Industrial Potential
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.ORCID iD: 0000-0002-7102-5198
Umeå University, Faculty of Science and Technology, Department of Chemistry. Industrial Chemistry & Reaction Engineering, Department of Chemical Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Biskopsgatan 8, FI-20500 Åbo-Turku, Finland.
2018 (English)In: ACS Sustainable Chemistry & Engineering, ISSN 2168-0485, Vol. 6, no 8, p. 10395-10407Article in journal (Refereed) Published
Abstract [en]

Herein we report the application of polyamine pentaethylenehexamine (PEHA, 3,6,9,12-tetraazatetradecane-1,14-diamine) in CO2 absorption with both neat PEHA and aqueous solutions thereof. The absorption of molecular CO2 in pure PEHA and in PEHA-water systems resulted in the formation of two chemical species, namely, PEHA carbamate and bicarbonate. It was observed that, upon formation of these species, both the CO2 absorption capacity and CO2 absorption rate were controlled by the amount of water in the system. During the CO2 absorption, the neat PEHA and 92 wt % PEHA were capable of forming carbamate species only while other aqueous analogues with higher dilution allowed for the formation of both carbamate and bicarbonate species upon exceeding 8 wt % water in the mixture. The CO2 uptake steadily increased with an increase in the water concentration in the solvent mixture and reached the maximum value of 0.25 g of CO2/(g of solvent) in the case of 56 wt % PEHA in water. However, in the case of more dilute systems (i.e., <56 wt % PEHA in water), the trend reversed and the CO2 loading decreased linearly to 0.05 g of CO2/(g of solvent) for 11 wt % PEHA in water. Meanwhile, it usually took shorter time to achieve the full CO2 absorption capacity (equilibrium) with increasing water content in all cases. The C-13 NMR analysis was used to quantify the relative amount of PEHA carbamate and bicarbonate, respectively, in reaction mixtures. The Kamle-Taft parameters (alpha, beta, and pi*) of aqueous solutions for different concentrations of PEHA were also studied taking advantage of various solvatochromic dyes and correlated with the CO2 absorption capacity. The thermally induced switchable nature of CO2-saturated neat and aqueous PEHA solutions for transformation of ionic PEHA carbamate and bicarbonate moieties to molecular PEHA is also represented. A comparison between aqueous PEHA and aqueous monoethanolamine (industrial solvent) for CO2 capture is reported. Hence, most importantly, a switchable PEHA system is demonstrated for reversible CO2 absorption processes.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018. Vol. 6, no 8, p. 10395-10407
Keywords [en]
aqueous pentaethylenehexamine, PEHA, reversible CO2 capture, carbamate, bicarbonate, kamlet- ft parameters, regeneration
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-151562DOI: 10.1021/acssuschemeng.8b01758ISI: 000441475500094OAI: oai:DiVA.org:umu-151562DiVA, id: diva2:1246868
Projects
Bio4Energy
Funder
Swedish Research Council, 2016-04090Knut and Alice Wallenberg FoundationBio4EnergyThe Kempe FoundationsAvailable from: 2018-09-10 Created: 2018-09-10 Last updated: 2019-08-29Bibliographically approved

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Bui, Thai Q.Khokarale, Santosh G.Shukla, Shashi KantMikkola, Jyri-Pekka

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