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首页> 外文期刊>Chemistry: A European journal >Probing the Redox Chemistry of Titanium Silicalite-1: Formation of Tetrahedral Ti~(3+) Centers by Reaction with Triethylaluminum
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Probing the Redox Chemistry of Titanium Silicalite-1: Formation of Tetrahedral Ti~(3+) Centers by Reaction with Triethylaluminum

机译：钛硅沸石-1的氧化还原化学研究：通过与三乙基铝反应形成四面体Ti〜（3+）中心

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摘要

Transition-metal ions with open-shell configurations hold promise in the development of novel coordination chemistry and potentially unprecedented redox catalysis. Framework-substituted Ti~(3+) ions with tetrahedral coordination are generated by reductive activation of titanium silicalite- 1 with triethylaluminum, an indispensable co-catalyst for heterogeneous Ziegler–Natta polymerization catalysts. Continuous-wave and pulse electron paramagnetic resonance methods are applied to unravel details on the local environment of the reduced transition metal-ions, which are shown to be part of the silica framework by detection of ~(29)Si hyperfine interactions. The chemical accessibility of the reduced sites is probed using ammonia as probe molecule. Evidence is found for the coordination of a single ammonia molecule. Comparison to similar systems, such as TiAlPO-5, reveals clear differences in the coordination chemistry of the reduced Ti sites in the two solids, which may be understood considering the different electronic properties of the solid frameworks.
机译：具有开壳结构的过渡金属离子在新型配位化学和潜在的空前的氧化还原催化的发展中具有广阔的前景。具有四面体配位的骨架取代的Ti〜（3+）离子是通过三乙基铝（一种非均相的齐格勒-纳塔聚合催化剂必不可少的助催化剂）对钛硅沸石-1进行还原活化而生成的。应用连续波和脉冲电子顺磁共振方法来揭示还原的过渡金属离子的局部环境的细节，通过检测〜（29）Si超精细相互作用，它们被证明是二氧化硅骨架的一部分。使用氨作为探针分子来探测还原位点的化学可及性。发现单个氨分子配位的证据。与类似系统（例如TiAlPO-5）的比较表明，两种固体中还原的Ti位点的配位化学存在明显差异，考虑到固体骨架的不同电子性质，可以理解这一点。

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