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首页> 外文期刊>ChemPlusChem >Homogeneous Photocatalytic H-2 Production Using a Ru-II Bathophenanthroline Metal-to-Ligand Charge-Transfer Photosensitizer
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Homogeneous Photocatalytic H-2 Production Using a Ru-II Bathophenanthroline Metal-to-Ligand Charge-Transfer Photosensitizer

机译：均相光催化H-2使用Ru-II洗银蝶啉蒽金属与配体电荷转移光敏剂

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摘要

The prototypical [Ru(bpy)(3)](2+) (bpy=2,2-bipyridine) photosensitizer has been previously demonstrated to be labile in aqueous photocatalytic solutions, especially in the presence of coordinating electron donors. Here, an alternative Ru-II molecular sensitizer, [Ru(dpp)(3)](2+) (dpp=4,7-diphenyl-1,10-phenanthroline or bathophenanthroline), is described, which is considerably more stable than its bpy congener, allowing enhanced photocatalysis metrics in conjunction with a cobalt glyoxime ([Co(dmgH)(2)pyCl], dmgH=dimethylglyoxime, py=pyridine) water reduction catalyst and N,N-dimethyl-p-toluidine (DMT) as the sacrificial donor in a 1:1 mixture of CH3CN/H2O. Photoluminescence studies revealed that DMT reductively quenches the excited state of [Ru(dpp)(3)](2+) with a bimolecular rate constant of k(q)=4.9x10(9)m(-1)s(-1). The rate constant measured for electron transfer from the reduced sensitizer to the [Co(dmgH)(2)pyCl] was found to be near the diffusion limit, k(Co)=2.4x10(9)m(-1)s(-1). H-2 production by photocatalysis was independently monitored by using a high-throughput photochemical reactor equipped with pressure transducers, gas chromatogram, and a mass spectrometer for detection; this illustrated that the composition yields high turnover numbers (TONs), approaching 10000 (H-2/Ru) with respect to the sensitizer and deuteration studies using D2O confirmed that H-2 is primarily produced from protons derived from water in these systems.
机译：原型[Ru（BPY）（3）]（3）（2+）（BPY = 2,2-硼胺）光敏剂已被证明是在含水光催化溶液中的不稳定，特别是在配位电子供体存在下。这里描述了一种替代的Ru-II分子敏化剂[Ru（DPP）（3）]（2+）（DPP = 4,7-二苯基-1,10-菲咯啉或洗银蒽），这比稳定性相当稳定其Bpy Congener，允许增强的光催化度量与钴乙醛（[CO（DMGH）（2）PYCl]，DMGH =二甲基乙基肟，PY =吡啶）水还原催化剂和N，N-二甲基-P-甲苯胺（DMT）作为CH 3 CN / H 2 O的1：1混合物中的牺牲供体。光致发光研究表明，DMT还原性地将[Ru（dpp）（3）]（2+）的激发状态与K（q）= 4.9x10（9）m（-1）s（-1）的共分率常数（-1） 。从降低的敏化剂到[CO（DMGH）（2）PYCL]的电子转移测量的速率常数在扩散极限附近，K（CO）= 2.4x10（9）m（-1）s（ - 1）。通过使用配备有压力传感器，气相色谱和质谱仪的高通量光化学反应器独立地监测光催化的H-2生产;这表明该组合物产生高端数（吨），相对于使用D2O的敏化剂和氘化研究接近10000（H-2 / Ru）证实，H-2主要由来自这些系统中的水的质子产生。

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