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Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
Journal of Materials Chemistry A, Volume: 9, Issue: 17, Pages: 10827 - 10837
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Polyamine-based carbon dioxide sorbents suffer from a seesaw relationship between amine content and amine efficiency. High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, espec...
|Published in:||Journal of Materials Chemistry A|
Royal Society of Chemistry (RSC)
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Polyamine-based carbon dioxide sorbents suffer from a seesaw relationship between amine content and amine efficiency. High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, especially at ambient temperature. High polymer contents curtail diffusion pathways, hindering CO2 from reaching and reacting with the numerous amine functions. Here, we overcome this issue using poly(allylamine) (PAA) grafted with short fluoroalkyl chains and then cross-linked with C60. As experimentally evidenced by positron annihilation lifetime spectroscopy, the incorporation of fluoroalkyl chains generates free volume elements that act as additional diffusion pathways within the material. The inclusion of void volume in fluoroalkyl-functionalized PAA sorbents results in radically increased CO2 uptakes and amine efficiencies in diluted gas streams at room temperature, including simulated air. We speculate that the hydrophobic fluorinated functions interfere with the strong amine hydrogen bonding network disrupting and consequently altering the packing and conformation of the polymer chains. The evidence presented here is a blueprint for the development of more efficient amine-based CO2 sorbents.
College of Engineering
Financial support was provided by the Reduce Industrial Carbon Emissions (RICE) and Flexible Integrated Energy Systems (FLEXIS) research operations part funded by the EU's European Regional Development Fund through the Welsh Government. We also acknowledge support from the SUSTAIN Manufacturing Hub funded by the Engineering and Physical Sciences Research Council (EP/S018107/1). Funding for the work of CJY, JJL and CWJ was provided in part by UNCAGE-ME, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award no. DE-SC0012577. MT wish to acknowledge funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 663830. JMU-K wish to acknowledge the project 18A12-210FP of the INL Laboratory Directed Research & Development (LDRD) program.