As a ubiquitous family of enzymes with high performance
in converting
carbon dioxide (CO2) into bicarbonate, carbonic anhydrases
(CAs) sparked enormous attention for carbon capture. Nevertheless,
the high cost and operational instability of CAs hamper their practical
relevance, and the utility of CAs is mainly limited to aqueous applications
where CO2-to-bicarbonate conversion is possible. Taking
advantage of the chemical motif that endows CA-like active sites (metal-coordinated
histidine), here we introduce a new line of high-performance gas separation
membranes with CO2-philic behavior. We first self-assembled
a histidine-based bolaamphiphile (His-Bola) molecule in the aqueous
phase and coordinated the resulting entities with divalent zinc. Optimizing
the supramolecular synthesis conditions ensured that the resultant
nanoparticles (His-NPs) exhibit high CO2 affinity and catalytic
activity. We then exploited the His-NPs as nanofillers to enhance
the separation performance of Pebax MH 1657. The hydrogen-bonding
interactions allowed the dispersion of His-NPs within the polymer
matrix uniformly, as confirmed by microscopic, spectroscopic, and
thermal analyses. The imidazole and amine functionalities of His-NPs
enhanced the solubility of CO2 molecules in the polymer
matrix. The CA-mimic active sites of His-NPs nanozymes, on the other
hand, catalyzed the reversible hydration of CO2 molecules
in humid conditions, facilitating their transport across the membranes.
The resulting nanocomposite membranes displayed excellent CO2 separation performance, with a high level of stability. At a filling
ratio as low as 3 wt %, we achieved a CO2 permeability
of >145 Barrer and a CO2/N2 selectivity of
>95
with retained performance under humid continuous gas feeds. The bio-inspired
approach presented in this work offers a promising platform for designing
durable and highly selective CO2 capture membranes.