LAUSR

Low‐cost direct air capture (DAC) systems require efficient gas–solid contactors. These contactors provide rapid rates of heat and mass transport with minimal pressure drops. Triply periodic minimal surfaces (TPMS) are a class of geometries that are shown to have heat transfer properties that exceed those of other geometries, and these benefits are expected to manifest in mass transfer as well due to the analogies between heat and mass transfer. However, creating TPMS contactors is difficult using conventional manufacturing techniques such as injection molding. Non‐solvent‐induced phase separation (NIPS) of a polymeric ink containing the adsorbent is one way to construct adsorption contactors with excellent mass transport rates, but contactors have to date only been fabricated in simple geometries (e.g., films, fibers). This study demonstrates that NIPS of polymeric inks occurs within a simultaneously‐dissolving, water‐soluble, 3D‐printed template. This templated phase inversion (TPI) technique can create seemingly unlimited macroscopic architectures, including TPMS contactors, using a variety of potential DAC adsorbents, including zeolite, silica, activated carbon, and metal–organic frameworks. SEM, micro‐computed tomography, and nitrogen adsorption experiments reveal the microscopic pore structures and macroscopic geometries of the resulting sorbent contactors. TPMS DAC contactors with poly(ethyleneimine)/silica adsorbents are shown to have CO2 capture performances that rival or exceed other contactor geometries.