Direct air capture (DAC) technology is being explored
as a pathway
for reducing greenhouse gas emissions through the efficient removal
of CO2 from the atmosphere. However, there remains a knowledge
gap regarding structure–property–performance factors
that impact the behavior of these systems in diverse, real-world environments.
In aminopolymer-based DAC systems, gas diffusion is tightly coupled
with polymer mobility, which is in turn affected by a large matrix
of variables, including interactions with the pore wall of the support,
nanoconfinement, the presence of co-adsorbates (moisture), and electrostatic
cross-links that develop as a function of CO2 chemisorption.
Higher-throughput, benchtop techniques for studying and understanding
mobility in these systems would lead to more rapid advances in the
field. Here, we demonstrate the value of a fluorescence technique
for monitoring polymer mobility within nanocomposite capture materials
as a function of CO2 and water adsorption in a series of
humidified polyethylenimine-Al2O3 composite
materials. The approach allows us to correlate changes in mobility
with CO2 adsorption kinetics as a function of relative
humidity. We further couple this information with NMR relaxometry
data attained using a portable single-sided magnetic resonance device,
and we employ diffuse reflectance infrared Fourier transform spectroscopy
to correlate the formation of different relative amounts of carbamates
and carbonates with the environmental conditions. These results provide
a blueprint for using benchtop techniques to promote fundamental understanding
in DAC systems that can in turn enable more efficient operation in
real-world conditions.