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 CO2, CH4, CF4, NF3, SF6, and C2F6, while reduced N2 uptake enables precise separation of complex gas mixtures. Dynamic separation experiments conducted at 298 K and 100 kPa confirmed outstanding selectivity for CO2/N2, CH4/N2, CF4/N2, SF6/N2, and NF3/N2 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.