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Cobalt salophen complexes for light-driven water oxidation

机译：钴salophen light-driven水复合物氧化

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摘要

Earth-abundant molecular complexes have been found to be excellent catalysts for the light-driven water oxidation reaction. Here, we demonstrate the photochemical water oxidation catalysed by three cobalt salophen complexes with different axial ligands in the presence of [Ru(bpy)(3)](2+) as a photosensitizer and Na2S2O8 as an electron acceptor in phosphate buffer of pH 9 and 7. The electrochemical investigation of the complexes in pH 9 including cyclic voltammetry (CV) and linear sweep voltammetry (LSV) verify the deposition of catalytic films on the surface of the working electrode. The deposited film characterization using scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS) confirms that the complexes decomposed to form nanoparticles. Electrospray ionization mass spectrometry (ESI-MS) studies along with dynamic light-scattering (DLS) measurements of the catalyst solution during the course of photochemical water oxidation suggest the catalyst decomposition and the formation of nanoparticles. The XPS measurements of the produced nanoparticles suggest that the surface of the particles is composed of Co(II) and OH species. In contrast, multiple experiments argue that light- driven water oxidation using the same complexes in pH 7 is homogeneous. We thus conclude that cobalt salophen complexes act as precatalysts that decompose under basic conditions to form cobalt hydroxide nanoparticles which act as a real catalyst for the light- driven water oxidation reaction, whereas the same complexes act as a homogeneous catalyst in the photochemical water oxidation reaction under neutral conditions.
机译：发现了地球上充足的分子复合物light-driven是良好的催化剂水氧化反应。水的光化学氧化催化了三个salophen钴配合物不同轴向配体的存在[俄文(bpy) (3)] (2 +)作为光敏剂和Na2S2O8一个电子受体在磷酸缓冲的pH值9和7。配合物的电化学研究pH值9包括循环伏安法(CV)和线性的扫描伏安法(LSV)验证的沉积催化膜表面的工作电极。利用扫描电子显微镜(SEM)和能量色散x射线能谱(EDS)确认了复合物分解形成纳米粒子。质谱)的研究动态光散射(DLS)的测量解决方案的过程中催化剂光化学氧化水建议分解和形成的催化剂纳米粒子。产生纳米颗粒显示表面粒子的由公司(II)和哦物种。使用相同的光——驱动水氧化复合物在pH值7是均匀的。得出结论:salophen钴配合物作为precatalysts下分解的基础条件形成氢氧化钴纳米颗粒作为一个真正的催化剂的光-驱动水氧化反应,而相同配合物作为均相催化剂光化学氧化反应在水中性的条件。

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