The zeolite Cu(I)Y is promising for adsorptive removal of thiophenic sulfur compounds from transportation fuels. However, its application is seriously hindered by the instability of Cu(I), which is easily oxidized to Cu(II) even under atmospheric environment due to the coexistence of moisture and oxygen. Here, we report the adjustment of zeolite microenvironment from hydrophilic to superhydrophobic status by coating polydimethylsiloxane (yielding Cu(I)Y@P), which isolates moisture entering the pores and subsequently stabilizes Cu(I) despite the presence of oxygen. Cu(I) in Cu(I)Y@P is stable upon exposure to humid atmosphere for 6 months, while almost all Cu(I) is oxidized to Cu(II) in Cu(I)Y for only 2 weeks. The optimized Cu(I)Y@P material after moisture exposure can remove 532 μmol g−1 of thiophene and is much superior to Cu(I)Y (116 μmol g−1), regardless of similar uptakes for unexposed adsorbents. Remarkably, Cu(I)Y@P shows excellent adsorption capacity of desulfurization for water-containing model fuel.
Metal-organic polyhedra (MOPs) have emerged as versatile platforms for artificial models of biological systems due to their discrete structure and modular nature. However, the design and fabrication of MOPs with special functionality for mimicking biological processes are challenging. Inspired by the breathing mechanism of lungs, we developed a new type of MOP (a breathing MOP, denoted as NUT-101) by directly using azobenzene units as the pillars of the polyhedra to coordinate with Zr-based metal clusters. In addition to considerable thermal and chemical stability, the obtained MOP exhibits photocontrollable breathing behavior. Upon irradiation with visible or UV light, the configuration of azobenzene units transforms, leading to reversible expansion or contraction of the cages and, correspondingly, capture or liberation of CO 2 molecules. Such a breathing behavior of NUT-101 is further confirmed by density functional theory (DFT) calculation. This system might establish an avenue for the construction of new materials with particular functionality that mimic biological processes.
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