Stepwise synthesis of nanosized Pd-Ru heteronuclear metal-organic cages from predesigned redox- and photo-active Ru(II)-metalloligand and naked Pd(II) ion is described. The resulting cage shows rhombododecahedral shape and contains a 5350 Å(3) cavity and 12 open windows, facilitating effective trapping of both polar and nonpolar guest molecules. Protection of photosensitive guests against UV radiation is studied.
A convenient, fast and selective water analysis method is highly desirable in industrial and detection processes. Here a robust microporous Zn-MOF (metal–organic framework, Zn(hpi2cf)(DMF)(H2O)) is assembled from a dual-emissive H2hpi2cf (5-(2-(5-fluoro-2-hydroxyphenyl)-4,5-bis(4-fluorophenyl)-1H-imidazol-1-yl)isophthalic acid) ligand that exhibits characteristic excited state intramolecular proton transfer (ESIPT). This Zn-MOF contains amphipathic micropores (<3 Å) and undergoes extremely facile single-crystal-to-single-crystal transformation driven by reversible removal/uptake of coordinating water molecules simply stimulated by dry gas blowing or gentle heating at 70 °C, manifesting an excellent example of dynamic reversible coordination behaviour. The interconversion between the hydrated and dehydrated phases can turn the ligand ESIPT process on or off, resulting in sensitive two-colour photoluminescence switching over cycles. Therefore, this Zn-MOF represents an excellent PL water-sensing material, showing a fast (on the order of seconds) and highly selective response to water on a molecular level. Furthermore, paper or in situ grown ZnO-based sensing films have been fabricated and applied in humidity sensing (RH<1%), detection of traces of water (<0.05% v/v) in various organic solvents, thermal imaging and as a thermometer.
Absolute chiral environments are rare in regular polyhedral and prismatic architectures, but are achievable from self-assembly of metal–organic cages/containers (MOCs), which endow us with a promising ability to imitate natural organization systems to accomplish stereochemical recognition, catalysis and separation. Here we report a general assembly approach to homochiral MOCs with robust chemical viability suitable for various practical applications. A stepwise process for assembly of enantiopure ΔΔΔΔΔΔΔΔ- and ΛΛΛΛΛΛΛΛ-Pd6(RuL3)8 MOCs is accomplished by pre-resolution of the Δ/Λ-Ru-metalloligand precursors. The obtained Pd–Ru bimetallic MOCs feature in large D4-symmetric chiral space imposed by the predetermined Ru(II)-octahedral stereoconfigurations, which are substitutionally inert, stable, water-soluble and are capable of encapsulating a dozen guests per cage. Chiral resolution tests reveal diverse host–guest stereoselectivity towards different chiral molecules, which demonstrate enantioseparation ability for atropisomeric compounds with C2 symmetry. NMR studies indicate a distinctive resolution process depending on guest exchange dynamics, which is differentiable between host–guest diastereomers.
The COVID-19 pandemic triggered an unprecedented rise in mortality that translated into life expectancy losses around the world, with only a few exceptions. We estimate life expectancy changes in 29 countries since 2020 (including most of Europe, the United States and Chile), attribute them to mortality changes by age group and compare them with historic life expectancy shocks. Our results show divergence in mortality impacts of the pandemic in 2021. While countries in western Europe experienced bounce backs from life expectancy losses of 2020, eastern Europe and the United States witnessed sustained and substantial life expectancy deficits. Life expectancy deficits during fall/winter 2021 among people ages 60+ and <60 were negatively correlated with measures of vaccination uptake across countries (r60+ = −0.86; two-tailed P < 0.001; 95% confidence interval, −0.94 to −0.69; r<60 = −0.74; two-tailed P < 0.001; 95% confidence interval, −0.88 to −0.46). In contrast to 2020, the age profile of excess mortality in 2021 was younger, with those in under-80 age groups contributing more to life expectancy losses. However, even in 2021, registered COVID-19 deaths continued to account for most life expectancy losses.
Direct white-light emission and further a dual-channel readable barcode module in both visible and NIR region was established by single-component homo-metallic Pr(iii)-MOF crystals for the first time.
Hexagonal CuSe nanoflakes with a lateral size of 200-800 nm and a thickness of 15-40 nm have been successfully synthesized by a concentrated alkaline hydrothermal method in which CuCl and Se powder were used as raw materials. Experimental results show that the amount of polyvinylpyrrolidone and the NaOH concentration play important roles in the formation of hexagonal CuSe nanoflakes. The photocatalytic activity of the as-synthesized hexagonal CuSe nanoflakes was investigated by the photocatalytic degradation of organic methylene blue (MB) under natural sunlight irradiation. It is found that hexagonal CuSe nanoflakes exhibit excellent photocatalytic activity and repeatability and above 99% MB in wastewater can be degraded after sunlight irradiation for 25 min in the presence of hydrogen peroxide.
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