Room‐Temperature CO 2 Sorption of NH 2 ‐Appended UiO‐67(Zr) Metal‐Organic Framework

Fossil fuel combustion elevates atmospheric carbon dioxide (CO 2 ) to critical levels, driving climate change and intensifying natural disasters. This reality underscores the urgent need for efficient CO 2 capture technologies. In this regard, UiO‐67(Zr) being a highly porous and thermally stable metal‐organic framework (MOF) could be used as a promising candidate for CO 2 sorption. Herein, we report the in situ synthesis of amine (–NH 2 ) functionalized UiO‐67(Zr)‐NH 2 using a prefunctionalized 3,3′‐diamino‐[1,1′‐biphenyl]‐4,4′‐dicarboxylic acid (dbda) linker. The –NH 2 groups remain as dangling and uncoordinated moieties, preserving the pristine UiO‐67(Zr) topology, and maintain high porosity and thermal stability while exhibiting enhanced CO 2 adsorption. The CO 2 isotherms show a linear and reversible profile with negligible hysteresis, highlighting facile kinetics and good stability. Under ambient conditions (25 °C), maximum CO 2 uptake reaches ~40 mL (STP) g −1 (≈1.8 mmol g −1 ) at 100 kPa pressure. The powder X‐ray diffraction (PXRD) and scanning electron microscopy (SEM) validate crystal integrity and morphology, confirming a robust framework. Furthermore, post‐test PXRD and IR analyses validate its chemical stability and reusability across multiple uses. The theoretical results indicate that incorporating dbda in place of traditional [1,1′‐biphenyl]‐4,4′‐dicarboxylic acid (bpdc) in UiO‐67(Zr) is energetically favorable towards CO 2 and N 2 sorption.