Dynamic anchoring of phosphotungstate framework with sulfate protons for ultralow‐energy <scp> CO ₂ </scp> capture

Abstract Developing efficient catalysts with low‐temperature CO 2 capture‐desorption cycles is crucial for high energy penalty. Herein, we report a novel dynamic‐anchoring strategy that constructs a “flexible‐rigid” dual‐network system by co‐anchoring sulfate ions and phosphotungstate (H 3 PW 12 O 40 ) onto TiO(OH) 2 . This design enables the sulfate proton‐shuttle to dynamically mediate proton transfer, while the H 3 PW 12 O 40 framework provides a rigid electron‐transport network via its well‐defined d‐p hybridized orbitals. Benefiting from this strategy, the CO 2 absorption/desorption rate was severally increased to 118% and 193%, while the heat load and desorption temperature decreased to 52.8% and 68–76°C, respectively. The enhanced performance originates from the complementary soft‐hard dual network, in which the sulfate proton‐shuttle promotes proton transfer via moderate binding, whereas H 3 PW 12 O 40 maintains structural integrity through strong chemical adsorption, thus a triple synergy of Brønsted‐Lewis acid coupling, d‐p orbital hybridization‐mediated electron transfer and lattice oxygen‐mediated Mars‐van Krevelen radical cycles formed.