Breakthrough Reassembly of Ultrastable Amino-Framework MIL-101-Glu for Greenhouse-Gas Dynamic Capture

In this work, we redesign Materials of Institute Lavoisier-101 (MIL-101), a typical material among metal–organic frameworks (MOFs), by partially incorporating l -glutamic acid ( l -Glu) via a one-pot synthesis. By embedding flexible active groups within a robust framework, MIL-101-Glu is synthesized in a strongly acidic aqueous solution (pH 1–2) and subsequently washed in hot DMF (pH 9–12), thereby overcoming the stability and surface area limitations of conventional amino-functionalized MIL-101. This innovative strategy preserves the inherent stability of MIL-101 while optimizing its microporous structure via l -Glu active sites, yielding a significantly higher BET surface area compared to conventional MIL-101 and achieving a synthesis yield of 68%. Systematic adsorption tests over a pressure range of 0–5 MPa demonstrated excellent performance for CO 2, CH 4, CF 4, NF 3, SF 6, and C 2 F 6, while reduced N 2 uptake enables precise separation of complex gas mixtures. Dynamic separation experiments conducted at 298 K and 100 kPa confirmed outstanding selectivity for CO 2 /N 2, CH 4 /N 2, CF 4 /N 2, SF 6 /N 2, and NF 3 /N 2 systems. This study not only elucidates the synergistic interplay between flexible active groups and the rigid framework but also provides a pathway for the rational design of multiligand metal–organic frameworks. MIL-101–7%Glu exhibits significant potential for next-generation greenhouse-gas capture, storage, and emission reduction technologies, thereby offering an innovative materials solution to address global climate change.