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- W4387372416 abstract "High or enriched-purity O2 is used widely in numerous industries, and the vast majority of this gas is produced from cryogenic distillation of air, an extremely capital- and energy-intensive process. There is significant interest in the development of new approaches for O2- selective air separations, including the use of porous, crystalline metal–organic frameworks featuring coordinatively unsaturated metal sites that can selectively bind O2 over N2 via electron transfer. However, most of these materials exhibit appreciable and/or reversible O2 uptake only at low temperatures, and their open metal sites are also potential strong binding sites for the water present in air. Here, we study the framework CuI-MFU-4l (CuxZn5−xCl4−x(btdd)3; H2btdd= bis(1H-1,2,3-triazolo[4,5-b ],[4′,5′-i ])dibenzo[1,4]dioxin), which has been shown to bind O2 reversibly at ambient temperature. We develop an optimized synthesis for the material to access a high density of trigonal pyramidal CuI sites, and we show that this material reversibly captures O2 from air at 25 °C, even in the presence of water. When exposed to air of varying humidity levels, CuI-MFU-4l retains a good O2 capacity over the course of repeated cycling under dynamic breakthrough conditions. While the material also simultaneously adsorbs N2, differences in O2 and N2 desorption kinetics allow for the isolation of high-purity O2 (>99%) under relatively mild regeneration conditions. Interestingly, spectroscopic, magnetic, and computational analyses reveal that O2 binds to the copper(I) sites to form copper(II)–superoxide moieties that exhibit temperature-dependent side-on and end-on binding modes. Overall, these results suggest that CuI-MFU-4l is a promising material for the separation of O2 from ambient air even without dehumidification." @default.
- W4387372416 created "2023-10-06" @default.
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- W4387372416 date "2023-10-05" @default.
- W4387372416 modified "2023-10-16" @default.
- W4387372416 title "Selective Adsorption of Oxygen from Humid Air in a Metal–Organic Framework with Trigonal Pyramidal Copper(I) Sites" @default.
- W4387372416 doi "https://doi.org/10.26434/chemrxiv-2023-21gn7" @default.
- W4387372416 hasPublicationYear "2023" @default.
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