Scalable and Highly Porous Membrane Adsorbents for Direct Air Capture of CO 2 .

Direct air capture (DAC) of CO 2 is a carbon-negative technology to mitigate carbon emissions, and it requires low-cost sorbents with high CO 2 sorption capacity that can be easily manufactured on a large scale. In this work, we develop highly porous membrane adsorbents comprising branched polyethylenimine (PEI) impregnated in low-cost, porous Solupor supports. The effect of the PEI molecular mass and loading on the physical properties of the adsorbents is evaluated, including porosity, degradation temperature, glass transition temperature, and CO 2 permeance. CO 2 capture from simulated air containing 400 ppm of CO 2 in these sorbents is thoroughly investigated as a function of temperature and relative humidity (RH). Polymer dynamics was examined using differential scanning calorimetry (DSC) and broadband dielectric spectroscopy (BDS), showing that CO 2 sorption is limited by its diffusion in these PEI-based sorbents. A membrane adsorbent containing 48 mass% PEI (800 Da) with a porosity of 72% exhibits a CO 2 sorption capacity of 1.2 mmol/g at 25 °C and RH of 30%, comparable to the state-of-the-art adsorbents. Multicycles of sorption and desorption were performed to determine their regenerability, stability, and potential for practical applications.