Metal−organic frameworks MIL-53(Al)-TDC and MIL-53(Al)-BDC were explored in the SO 2 adsorption process. MIL-53(Al)-TDC was shown to behave as a rigid-like material upon SO 2 adsorption. On the other hand, MIL-53(Al)-BDC exhibits guest-induced flexibility of the framework with the presence of multiple steps in the SO 2 adsorption isotherm that was related through molecular simulations to the existence of three different pore opening phases narrow pore, intermediate pore, and large pore. Both materials proved to be exceptional candidates for SO 2 capture, even under wet conditions, with excellent SO 2 adsorption, good cycling, chemical stability, and easy regeneration. Further, we propose MIL-53(Al)-TDC and MIL-53(A)-BDC of potential interest for SO 2 sensing and SO 2 storage/transportation, respectively.
MFM-300(Sc) was demonstrated to be an optimal adsorbent for SO2 capture combining high uptake, good stability and excellent cyclability (facile regeneration at only room temperature). A drastic enhancement on its SO2 uptake (40%) was achieved when a small amount of EtOH was preliminary adsorbed.
MIL-53(Al)-TDC was demonstrated to be an optimal adsorbent for acidic H2S capture combining an unprecedented uptake at room temperature, excellent cyclability and low-temperature regeneration.
CO2 capture of InOF-1 was enhanced 3.6-fold, at 1 bar and 30 °C, by confining EtOH within its pores. Direct visualisation by single crystal X-ray diffraction revealed that EtOH divides InOF-1 channels in wide sections separated by "bottlenecks" caused by EtOH molecules bonded to the μ2-OH functional groups of InOF-1.
An unprecedented reversible guest-induced metallinker bond rearrangement in metal−organic framework (MOFs) was revealed by quantum-calculations and DRIFT experiments. As a showcase, the prototypical MOF-type MFM-300(Sc) was demonstrated to undergo a substantial Sc-carboxylate bond dynamics upon ammonia adsorption to enable a strong metal− guest binding mode, a key feature to ensure a highly efficient capture of this toxic molecule. Decisively, we evidenced this adsorption mechanism to be fully reversible, preserving the ammonia capture performance and structure integrity over multiple cycles. Such an unconventional mechanism in MOFs can open up new avenues to design novel materials for an efficient capture of highly corrosive molecules.
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