Iridium and Palladium CO2 Hydrogenation in Water by Catalyst Precursors with Electron-Rich Tetrazole Ligands,Organometallics

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Iridium and Palladium CO2 Hydrogenation in Water by Catalyst Precursors with Electron-Rich Tetrazole Ligands
Organometallics ( IF 2.5 ) Pub Date : 2020-09-02 , DOI: 10.1021/acs.organomet.0c00276
Edward Ocansey ₁ , James Darkwa ₁ , Banothile C. E. Makhubela ₁

Affiliation

Hydrogenation of CO₂ to formate serves as a means of H₂ storage. By utilizing robust, electron-rich and bulky N^∧N bidentate tetrazolylpyridyl ligands, we have prepared CO₂ hydrogenation iridium(III) and palladium(II) catalyst precursors (3–7) that operate in water as a solvent. In situ¹H NMR spectroscopic data obtained when the hydrogenation catalyst is 5 detect that a hydrido-bridged binuclear iridium intermediate compound is formed prior to the formation of the catalytically active iridium hydride species. This hydrido-bridged iridium intermediate is observable by in situ¹H NMR spectroscopy even after extended periods of storage. In addition, we demonstrate that product formation in the CO₂ hydrogenation, catalyzed by these tetrazolylpyridyl iridium catalysts, proceeds via either CO₂ hydrogenation or NaHCO₃ reduction.

中文翻译：

富电子型四唑配体的催化剂前体在水中氢化铱和钯CO ₂的反应

CO ₂加氢成甲酸酯是H ₂储存的一种手段。通过利用健壮的，笨重的富电子-N ^∧ Ñ二齿配位体tetrazolylpyridyl，我们准备了CO ₂加氢铱（III）和钯（II）催化剂前体（3 - 7），在作为溶剂的水进行操作。当氢化催化剂为5时获得的原位¹ H NMR光谱数据检测到在形成催化活性的氢化铱物质之前形成了氢化桥联的双核铱中间化合物。这种氢化桥铱中间体可以通过原位¹观察到即使长时间保存，1 H NMR光谱也是如此。另外，我们证明了通过这些四唑基吡啶基铱催化剂催化的在CO ₂氢化中的产物形成是通过CO ₂氢化或NaHCO ₃还原而进行的。

更新日期：2020-09-14

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