Cu-based catalysts have attracted much interest in CO 2 hydrogenation to methanol because of their high activity. However, the effect of interface, coordination structure, particle size and other underlying factors existed in heterogeneous catalysts render to complex active sites on its surface, therefore it is di cult to study the real active sites for methanol synthesis. Here, we report a novel Cu-based catalyst with isolated Cu active sites (Cu 1 -O 3 units) for highly selective hydrogenating CO 2 to methanol at low temperature (100% selectivity for methanol at 180 o C). Experimental and theoretical results reveal that the single-atom Cu-Zr catalyst with Cu 1 -O 3 units is only contributed to synthesize methanol at 180 o C, but the Cu clusters or nanoparticles with Cu-Cu or Cu-O-Cu active sites will promote the process of reverse water gas shift (RWGS) side reaction to form undesirable byproducts CO. Furthermore, the Cu 1 -O 3 units with tetrahedral structure could gradually migrate to the catalyst surface for accelerating CO 2 hydrogenation reaction during catalytic process. The high activity isolated Cu-based catalyst with legible structure will be helpful to understand the real active sites of Cu-based catalysts for methanol synthesis from CO 2 hydrogenation, thereby guiding further design the Cu catalyst with high performance to meet the industrial demand, at the same time as extending the horizontal of single atom catalyst for application in the thermal catalytic process of CO 2 hydrogenation.

The physical properties of scintillators determine X‐ray detection performance directly, which plays a vital role in computed tomography (CT) imaging for medical radiography and security checks. Recently, lead halide perovskite materials have shown higher photoluminescence quantum yield (PLQY) than conventional X‐ray scintillators, but there are still some limitations, including instability and the use of heavy metal lead. In this study, a low‐temperature solution method is used to prepare 0D lead‐free Cs3Cu2I5 perovskite nanocrystals (NCs), and a corresponding optical fiber panel with Cs3Cu2I5 NCs is fabricated for high‐resolution X‐ray CT imaging. The Cs3Cu2I5 NCs exhibit a high PLQY of 59% and outstanding stability for more than three months. Importantly, the Cs3Cu2I5 NCs show a high radioluminescence (RL) light yield, that is four times higher than that of CsPbBr3 NCs (80 kV, 70 µA). In addition, an X‐ray detector based on a Cs3Cu2I5 NC scintillator is designed. Using this system, a clear projection image of a chip is obtained, and a 3D CT image of a snail is reconstructed. Therefore, the use of lead‐free perovskite nanocrystal scintillators is a promising technique for commercial X‐ray detection.

Water radical cations, the crucial intermediates in many aqueous reactions and biochemical processes, are difficult to be experimentally investigated due to its short lifetime and low abundance. Herein, a homemade device based on energy-tunable discharge was employed to deposit suitable amounts of energy to atmospheric pressure pure water vapor for abundant production of water radical cations, which were stabilized as (H 2 O) n +• (n=2-5) with the maximal abundance (≥ 8.3×10 6 cps) for (H 2 O) 2 +• as characterized by mass spectrometry (MS).The abundance of water radical cations was optimized by adjusting the experimental parameters such as discharge voltage (2.5 kV), temperature of the MS inlet (140 o C), carrier gas flow (20 mL/min) and the distance between the discharge tip and the MS inlet (12 mm). The ambient formation of water radical cations was further confirmed by the high reactivity of the as-prepared water radical cations, which instantly reacted with benzene, ethyl acetate and dimethyl disulfide, showing rich chemistry with the ionic and radical characters. Moreover, the computations confirm that the O-O single-electron bound dimer (B) as well as the hydronium hydroxyl radical complex (A) accounts for the unusual chemistry of the water radical cations, providing a facile approach to access the high reactivity of water radical cations under the ambient condition.

An computational study using density functional theory and grand-canonical Monte Carlo simulation that explore the adsorption mechanism of C 2 H 2 , CO 2 , and CH 4 to metal−organic frameworks (MOFs) with coordinatively unsaturated metal sites (M-MOF-74, M = Mg and Zn) has been carried out. The theoretical studies reveal that open metal sites have important roles in adsorption. The high CO 2 adsorption ability of M-MOF-74 is due to the strong Lewis acid and base interactions between metal ions and oxygen atom of CO 2 , as well as carbon atom of CO 2 with oxygen atoms in organic linkers. Meanwhile, the high C 2 H 2 adsorption for M-MOF-74 is contributed by the strong complexation between the metal ions and the π orbital of C 2 H 2 . The different adsorption mechanisms of CO 2 , C 2 H 2 , and CH 4 in M-MOF-74 can qualitatively explain the high CO 2 selectivity in CO 2 /CH 4 mixture and high C 2 H 2 selectivity in C 2 H 2 /CH 4 mixture. Energy decomposition analysis reveals that electrostatic energy, exchange energy, and repulsive energy are key factors in the binding strength of gas molecules on M-MOF-74. The preferential adsorption sites are confirmed to be located near the five-coordinate metal ions decorating the edges of the hexagonal channels. The elucidation of the adsorption mechanism at the molecular level provides key information for designing novel MOFs with high capacity and selectivity for CO 2 from light hydrocarbon mixtures.

Although tremendous effort has been devoted to the development of methods for iron catalysis, few of the catalysts reported to date exhibit clear superiority to other metal catalysts, and the mechanisms of most iron catalysis remain unclear. Herein, we report that iron complexes bearing 2,9-diaryl-1,10-phenanthroline ligands exhibit not only unprecedented catalytic activity but also unusual ligand-controlled divergent regioselectivity in hydrosilylation reactions of various alkynes. The hydrosilylation protocol described herein provides a highly efficient method for preparing useful di- and trisubstituted olefins on a relatively large scale under mild conditions, and its use markedly improved the synthetic efficiency of a number of bioactive compounds. Mechanistic studies based on control experiments and density functional theory calculations were performed to understand the catalytic pathway and the observed regioselectivity.

Cu/SBA-15 was successfully prepared by ammonia evaporation method and exhibited a high activity for the hydrogenation of ethylene carbonate to co-produce ethylene glycol and methanol.

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