Amine-Functionalized Meso-Macroporous Polymers for Efficient CO₂ Capture from Ambient Air

Over the past decade, direct air capture (DAC) of carbon dioxide (CO₂) using solid nanoadsorbents has garnered attention as a negative emission technology with high energy efficiency. Although operational, the large-scale deployment of DAC technologies has been significantly delayed due to the low performance and high cost of solid DAC nanoadsorbents. Herein, we present a novel family of meso-macroporous melamine formaldehyde (MF) materials with a facile preparation methodology, low capital cost, and unique physicochemical characteristics for DAC. The fabricated MF materials exhibit an extra-large pore volume of 5.19 cm³/g with a 24.6 nm average pore diameter. We show that the synthesized MF materials can be used as substrates and impregnated with different amounts of tetraethylenepentamine (TEPA) to act as chemical nanoadsorbents for DAC. Owing to the ultrahigh pore volume of MF, a substantial amount of 71 wt % TEPA (i.e., MF-TEPA71%) can be loaded, resulting in 2.65 mmol/g of CO₂ uptake under DAC conditions. In addition, the superior physicochemical properties of MF lead to a high CO₂ loading of 2.07 mmol/g with low TEPA loading in MF-TEPA33%. The prepared MF-TEPA nanoadsorbents can be successfully employed in different shapes (i.e., droplets, pellets, and coatings) and maintain their superiority across different temperatures and CO₂ concentrations. This study provides a promising approach for developing meso-macroporous substrates through a straightforward and scalable synthesis method, representing a new avenue for the next generation of DAC nanoadsorbents with superior performance for practical applications.