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Competitive and Cooperative CO2-H2O Adsorption through Humidity Control in a Polyimide Covalent Organic Framework

Journal Article (2023)
Authors

H.V. Veldhuizen (Novel Aerospace Materials)

Saira Alam Butt (Student TU Delft)

Annemiek Van Leuken (Student TU Delft)

B Van Der Linden (TU Delft - ChemE/O&O groep)

W. Rook (TU Delft - ChemE/O&O groep)

S Van Der Zwaag (Novel Aerospace Materials)

M.A. Van der Veen (ChemE/Catalysis Engineering)

Research Group
Novel Aerospace Materials
Copyright
© 2023 H.V. Veldhuizen, Saira Alam Butt, Annemiek Van Leuken, B. van der Linden, W. Rook, S. van der Zwaag, M.A. van der Veen
To reference this document use:
https://doi.org/10.1021/acsami.3c04561
More Info
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Publication Year
2023
Language
English
Copyright
© 2023 H.V. Veldhuizen, Saira Alam Butt, Annemiek Van Leuken, B. van der Linden, W. Rook, S. van der Zwaag, M.A. van der Veen
Research Group
Novel Aerospace Materials
Issue number
24
Volume number
15
Pages (from-to)
29186-29194
DOI:
https://doi.org/10.1021/acsami.3c04561
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Abstract

In order to capture and separate CO2 from the air or flue gas streams through nanoporous adsorbents, the influence of the humidity in these streams has to be taken into account as it hampers the capture process in two main ways: (1) water preferentially binds to CO2 adsorption sites and lowers the overall capacity, and (2) water causes hydrolytic degradation and pore collapse of the porous framework. Here, we have used a water-stable polyimide covalent organic framework (COF) in N2/CO2/H2O breakthrough studies and assessed its performance under varying levels of relative humidity (RH). We discovered that at limited relative humidity, the competitive binding of H2O over CO2 is replaced by cooperative adsorption. For some conditions, the CO2 capacity was significantly higher under humid versus dry conditions (e.g., a 25% capacity increase at 343 K and 10% RH). These results in combination with FT-IR studies on equilibrated COFs at controlled RH values allowed us to assign the effect of cooperative adsorption to CO2 being adsorbed on single-site adsorbed water. Additionally, once water cluster formation sets in, loss of CO2 capacity is inevitable. Finally, the polyimide COF used in this research retained performance after a total exposure time of >75 h and temperatures up to 403 K. This research provides insight in how cooperative CO2-H2O can be achieved and as such provides directions for the development of CO2 physisorbents that can function in humid streams.