Synthesis and the energetic insights into CO2 adsorption in CAU-10-PDC

The high energy consumption of CO2 capture technologies stems largely from the limited efficiency of the adsorbents and the energy-intensive regeneration process, posing a major barrier to large-scale deployment. This study provides a robust material solution through the first synthesis and energetic evaluation of a stable CAU-10-PDC metal-organic framework, marking a significant step beyond its previously conceptualized membrane forms. By substituting the original benzene-dicarboxylate linkers in CAU-10 with pyridine-3,5-dicarboxylate ligands, we engineered a framework with tailored 4.15 Å pore channels that exhibits exceptional thermal stability up to 397 °C and a high BET surface area of 896.9 m2/g. The material achieves high CO2 uptake of 5.05 mmol/g at 273 K and 4.01 mmol/g at 298 K, along with outstanding cyclic stability (>99.9% capacity retention over 10 TVSA cycles). Multiscale simulations further reveal a low isosteric enthalpy of 26.25 kJ/mol, confirming an energy-efficient physisorption mechanism. This low regeneration energy requirement, coupled with the identification of preferential CO2 binding at pyridinic nitrogen sites (binding energy: −8.44 kJ/mol), positions CAU-10-PDC as a promising candidate for next-generation CO2 capture systems like direct air capture (DAC). Our work provides the first comprehensive dataset for CAU-10-PDC and offers an atomistic blueprint for designing high-performance, low-energy adsorbents.