A scalable and low‐cost metal–organic framework synthesized under ambient conditions for benchmark CO ₂ capture

The practical application of metal–organic frameworks (MOFs) for CO 2 capture requires balancing high efficiency, cyclability, and scalable production. Herein, we report a novel MOF adsorbent, Cu 3 (ntrz) 2 (ox) 2 , which allows for low‐cost and scalable synthesis in aqueous solutions under ambient conditions. Its tailored large pocket‐like cavities interconnected by narrow pore apertures provide exceptional CO 2 adsorption capacities of 6.80 and 3.48 mmol g −1 at 1.0 bar and 0.15 bar (298 K), achieving a record‐high VPSA working capacity of 5.03 mmol g −1 within 0.05–1.0 bar. Shaped pellets retain 95% CO 2 adsorption capacity and good mechanical strength, fulfilling industrial requirements. Experimental VPSA analysis demonstrates that a 15% CO 2 gas‐stream can be enriched to 91.37% and 95.06% with productivities of 0.402 and 1.86 m 3 t −1 h −1 within 0.08–1.0 bar and 0.08–6.0 bar, outperforming zeolite 13X. The adsorption behaviors and mechanisms are elucidated via Grand Canonical Monte Carlo and dispersion‐corrected density functional theory simulations.