• • G-5,5'-BPyDC exhibits a N2O adsorption capacity of 2.32 mmol/g at 25°C and 4.0 MPa, which is 14.9% higher than that of G-4,4'-BPyDC (2.02 mmol/g), indicating enhanced uptake for industrial N2O capture processes.
• • IAST selectivity of G-5,5'-BPyDC for N2O/N2 (50:50) is 29.26, and for (10:90) is 111.32, outperforming G-4,4'-BPyDC (6.61 and 17.03) by factors of 4.4 and 6.5, respectively, crucial for efficient separation in dilute N2O streams.
• • Both HOFs exhibit thermal stability with decomposition temperatures ≥290°C, ensuring operational robustness in temperature-swing adsorption processes.
• • Hirshfeld surface analysis shows that G-5,5'-BPyDC has a higher total hydrogen bond contribution (32.0%) compared to G-4,4'-BPyDC (29.7%), correlating with improved adsorption performance and providing a design metric for future HOF synthesis.