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Lead halide hybrids have shown great potentials in CO2 photoreduction, but challenging to afford C2+ reduced products, especially using H2O as the reductant. This is largely due to the trade‐off problem between instability of the benchmark 3D structures and low carrier mobility of quasi‐2D analogues. Herein, the lead halide dimensionality of robust coordination polymers (CP) was modulated by organic ligands differing in a single‐atom change (NH vs. CH2), in which the NH groups coordinate with interlamellar [PbI2] clusters to achieve the important 2D→3D transition. This first CP based on 3D cationic lead iodide sublattice possesses both high aqueous stability and a low exciton binding energy of 25 meV that is on the level of ambient thermal energy, achieving artificial photosynthesis of C2H5OH. Photophysical studies combined with theoretical calculations suggest the bridging [PbI2] clusters in the 3D structure not only results in enhanced carrier transport, but also promotes the intrinsic charge polarization to facilitate the C−C coupling. With trace loading of Rh cocatalyst, the apparent quantum efficiency of the 3D CP reaches 1.4 % at 400 nm with a high C2H5OH selectivity of 89.4 % (product basis), which presents one of the best photocatalysts for C2 products to date. [ABSTRACT FROM AUTHOR]

Keywords: coordination polymers; CP glass; healing; membrane separation; molecular sieving EN coordination polymers CP glass healing membrane separation molecular sieving 21764 21764 1 09/16/21 20210920 NES 210920 B Selbstheilende Gastrennmembranen b auf Basis von Koordinationspolymeren (CPs) werden im Forschungsartikel auf S. 21474 von Xiao Feng, Bo Wang et al. vorgestellt. Rücktitelbild: Coordination Polymer Glasses with Lava and Healing Ability for High-Performance Gas Sieving (Angew. Coordination polymers, CP glass, healing, membrane separation, molecular sieving. [Extracted from the article]

Coordination polymer (CP) glasses offer a way to tackle the fabrication challenges encountered by inorganic porous membranes and show great potentials for size‐exclusive gas separation. However, their processability and performance still cannot simultaneously meet the requirements for high‐performance membrane separation. Herein, we have developed a series of CP glasses (M‐P‐dmbIm, M=Zn, Cd, Cu, and Mn), which possess low vitrification temperature as well as low viscosity (η) and lave capability above the transition temperatures. The derived glass (agM‐P‐dmbIm) membranes show outstanding performances for H2/CO2, H2/N2, and H2/CH4 separation, which all far surpass the Robeson upper bound and even rival against the best of the state‐of‐the‐art gas separation membranes. The low viscosities not only allow us to hot‐cast or hot‐press the CP glasses into thin membranes within 5 min without sacrificing their selectivity and permeability, but also endow the resulted glass membranes with healing ability. [ABSTRACT FROM AUTHOR]

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