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The design of novel materials for sulfur dioxide (SO2) capture and conversion with considerable efficiency under mild conditions is of great significance for human health and environmental protection yet highly challenging. Herein, we report a series of triazine‐based multicomponent metallacages via coordination‐driven self‐assembly of 2,4,6‐tri(4‐pyridyl)‐1,3,5‐triazine, cis‐Pt(PEt3)2(OTf)2 and different tetracarboxylic ligands. As the increase of the length of the tetracarboxylates, the structures of the metallacages change from pyramids to extended octahedrons. Owing to their N‐rich structure, these metallacages are further used for selective SO2 capture, showing good adsorption capacity and remarkable SO2/CO2 selectivity in ambient conditions, suggesting their potential applications toward real flue gas desulfurization. The metallacages are further employed for the conversion of SO2 into value‐added compounds, showing exceptional efficiency even dilute SO2 is used as the reactant. This study represents a type of structure‐tunable triazine‐based metallacages for SO2 capture and conversion, which will pave the way on the applications of metal‐organic complexes for gas adsorption. [ABSTRACT FROM AUTHOR]

With the continuous research and development of amidoxime (AO)‐based adsorbents, industrialization production of uranium from seawater gradually becomes a reality. However, the currently available AO‐based adsorbents still suffer from low adsorption rate and poor selectivity. Herein, vertically aligned polyamioxime–graphene oxide (VA‐PG) sheet membrane is fabricated by directional freeze casting. The run‐through microchannels contribute to the free diffusion of uranyl ions (UO22+), leading to the fast adsorption kinetics. Furthermore, partially reduced graphene oxide allows high photothermal conversion efficiency and rapid in‐plane heat transfer, resulting in the fast temperature rise under simulated sunlight irradiation. Because of the endothermic behavior of UO22+, light‐irradiated VA‐PG can simultaneously satisfy the requirements of high adsorption capacity (13.63 mg‐U g‐Ads−1), high adsorption rate (0.43 mg g−1 day−1), and excellent selectivity toward U(VI) over V(V) (U/V = 1.24) in natural seawater, indicating the right direction for a breakthrough in the field of uranium extraction from seawater. [ABSTRACT FROM AUTHOR]

Extraordinary electronic and photonic features (e.g., tunable direct bandgap, high ambipolar carrier mobility) render few‐layer black phosphorus (BP) nanosheets/quantum dots an important optoelectronic material. However, most of the BP applied in metal halide perovskite solar cells (PSCs) are produced by sonication‐assisted liquid exfoliation, which inevitably brings inferior electronic properties, thus leading to limited beneficial effects. Furthermore, this study uncovers that the intrinsic instability of BP nanosheets sandwiched between (CsFAMA)Pb(BrI)3 perovskite and spiro‐OMeTAD has a deleterious effect on the performance stabilization of PSCs. To address the above constraints, a feasible strategy herein is developed by introducing high‐quality fluorinated BP (F‐BP) nanosheets synthesized by one‐step electrochemical delamination. In addition to P‐Pb coordination, there is a strong hydrogen bond between F− and MA+/FA+ as well as an ionic bond between F− and Pb2+ for the perovskite/F‐BP interface, thus leading to fewer interfacial traps than perovskite/BP, which is responsible for the highest power conversion efficiency (22.06%) of F‐BP devices. More importantly, F‐BP devices exhibit significantly improved humidity and shelf‐life stabilities due to the excellent ambient stability of F‐BP, resulting from the antioxidation and antihydration behavior of fluorine adatoms. Overall, the findings provide a promising strategy to simultaneously enhance the photovoltaic performance and long‐term stability of BP‐based PSCs. [ABSTRACT FROM AUTHOR]

Monomolecular VB2 (vitamin B2) was doped into UiO-66 [Zr6O4(OH)4(BDC)12, BDC = 1,4-benzenedicarboxylic acid] via chemical bonds and the obtained VB2@UiO-66 could be used as a heterogeneous photocatalyst. The coordination with UiO-66 was found to be able to positively shift the conduction band of VB2, which thermodynamically precluded the formation of other reactive oxygen species (like O2˙−) except 1O2 under visible light irradiation and led to 1O2 as the only reactive oxygen species for VB2@UiO-66. This result was totally different from that for VB2, which produced various reactive oxygen species, such as O2˙− and 1O2. Due to the fact that 1O2 was the only reactive oxygen species, VB2@UiO-66 displayed excellent photocatalytic selectivity (∼100%) towards benzyl alcohol oxidation. At the same time, chemical bonding with UiO-66 greatly improved the stability of VB2 under visible light. After 5 cycles, the conversion was still 91% and the selectivity was close to 100%. This work offers not only a solution to the poor recyclability, stability and selectivity of VB2 as a photocatalyst but also a new efficient strategy to extend the photocatalytic applications of MOFs by immobilizing common biological antioxidants on their particular sites. [ABSTRACT FROM AUTHOR]

Two transition metal (Co and Ni) ion phosphonates as isostructural organic inorganic hybrids are prepared and investigated in terms of photocatalytic hydrogen evolution from water and CO2 reduction under UV light irradiation. A photocatalytic mechanism of ligand-to-metal charge transfer (LMCT) is proposed. [ABSTRACT FROM AUTHOR]

The structures of the crosslinks in supramolecular polymer networks play an important role on their properties and functions. Herein, emissive metallacages are used as crosslinks to prepare metallacage-cored polyurethanes. The mechanical properties including storage modulus, toughness, Young's modulus and breaking strength of polymers are greatly enhanced with the increase of crosslinking densities. Moreover, such polymers not only exhibit good fluorescence in the solid state, but also show self-healing and shape memory properties owing to the dynamic reversible non-covalent bonds in their structures. This study not only offers a convenient strategy to prepare metallacage-crosslinked networks, but also explores their applications as self-healing and shape memory materials, which will promote the study of metallacage-cored supramolecular networks as smart materials., (© 2022 Wiley-VCH GmbH.)

Two transition metal (Co and Ni) ion phosphonates as isostructural organic inorganic hybrids are prepared and investigated in terms of photocatalytic hydrogen evolution from water and CO2 reduction under UV light irradiation. A photocatalytic mechanism of ligand-to-metal charge transfer (LMCT) is proposed.