Insights into the Oxidative Degradation Mechanism of Solid Amine Sorbents for CO 2 Capture from Air: Roles of Atmospheric Water

Direct air capture (DAC) processes for extraction of CO from ambient air are unique among chemical processes in that they operate outdoors with minimal feed pretreatments. Here, the impact of humidity on the oxidative degradation of a prototypical solid supported amine sorbent, poly(ethylenimine) (P...

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Published inAngewandte Chemie (International ed.) Vol. 62; no. 24; p. e202302887
Main Authors Carneiro, Juliana S A, Innocenti, Giada, Moon, Hyun June, Guta, Yoseph, Proaño, Laura, Sievers, Carsten, Sakwa-Novak, Miles A, Ping, Eric W, Jones, Christopher W
Format Journal Article
LanguageEnglish
Published Germany Wiley Blackwell (John Wiley & Sons) 12.06.2023
Subjects
Amines
CO2 Adsorption
Direct Air Capture
Oxidative Degradation
Solid Sorbents
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Summary:Direct air capture (DAC) processes for extraction of CO from ambient air are unique among chemical processes in that they operate outdoors with minimal feed pretreatments. Here, the impact of humidity on the oxidative degradation of a prototypical solid supported amine sorbent, poly(ethylenimine) (PEI) supported on Al O , is explored in detail. By combining CO adsorption measurements, oxidative degradation rates, elemental analyses, solid-state NMR and in situ IR spectroscopic analysis in conjunction with O labeling of water, a comprehensive picture of sorbent oxidation is achieved under accelerated conditions. We demonstrated that the presence of water vapor can play an important role in accelerating the degradation reactions. From the study we inferred the identity and kinetics of formation of the major oxidative products, and the role(s) of humidity. Our data are consistent with a radical mediated autooxidative degradation mechanism.
Bibliography:USDOE
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202302887