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首页> 外文期刊>Chemistry: A European journal >Heterogenized Water Oxidation Catalysts Prepared by Immobilizing Klaui-Type Organometallic Precursors
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Heterogenized Water Oxidation Catalysts Prepared by Immobilizing Klaui-Type Organometallic Precursors

机译：固定化克劳伊型有机金属前体制备的多相水氧化催化剂

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摘要

An efficient heterogenized water oxidation catalyst (2_TiO2) has been synthesized by immobilizing the Klaui-type organometallic precursor [Cp*Ir{P(O)(OH)(2)}(3)]Na (2, Cp*=1,2,3,4,5-pentamethylcyclopentadienyl ligand) onto rutile TiO2. Iridium is homogeneously distributed at the molecular and atomic/small cluster level in 2_TiO2 and 2'_TiO2 (solid catalyst recovered after the first catalytic run), respectively, as indicated by STEM-HAADF (scanning transmission electron microscopy - high angle annular dark field) studies. 2'_TiO2 exhibits TOF values up to 23.7 min(-1) in the oxidation of water to O-2 driven by NaIO4 at nearly neutral pH, and a TON only limited by the amount of NaIO4 used, as indicated by multiple run experiments. Furthermore, while roughly 40% leaching is observed during the first catalytic run, 2'_TiO2 does not undergo any further leaching even when in contact with strongly basic solutions and completely maintains its activity for thousands of cycles. NMR studies, in combination with ICP-OES (inductively coupled plasma optical emission spectrometry), indicate that the activation of 2_TiO2 occurs through the initial oxidative dissociation of PO43-, ultimately leading to active centers in which a 1:1 P/Ir ratio is present (derived from the removal of two PO43- units) likely missing the Cp* ligand.
机译：通过固定Klaui型有机金属前体[Cp * Ir {P（O（OH）（2）}（3）] Na（2，Cp * = 1,2）合成了一种高效的异质水氧化催化剂（2_TiO2） （3,4,5-五甲基环戊二烯基配体）到金红石型TiO2上。如STEM-HAADF（扫描透射电子显微镜-高角度环形暗场）所示，铱分别在2_TiO2和2'_TiO2（在第一次催化运行后回收的固体催化剂）中以分子和原子/小簇水平均匀分布。学习。如多次实验所示，在接近中性pH的条件下，由NaIO4驱动的水氧化成O-2时，2'_TiO2的TOF值高达23.7 min（-1），而TON仅受所用NaIO4量的限制，如多次实验所示。此外，尽管在第一次催化运行中观察到大约40％的浸出，但是即使与强碱性溶液接触，2'_TiO2也不会经历任何进一步的浸出，并且在数千个循环中完全保持其活性。 NMR研究与ICP-OES（电感耦合等离子体发射光谱法）相结合，表明2_TiO2的活化通过PO43-的初始氧化解离而发生，最终导致活性中心的P / Ir比为1：1。 （从两个PO43-单元的去除中得出）可能缺少Cp *配体。

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