Single-Site Photocatalytic H2 Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts,Journal of the American Chemical Society

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Single-Site Photocatalytic H2 Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-11-03 00:00:00 , DOI: 10.1021/jacs.7b07489
Tanmay Banerjee ₁ , Frederik Haase _{1,

2} , Gökcen Savasci _{1,

2} , Kerstin Gottschling _{1,

2} , Christian Ochsenfeld _{2,

3} , Bettina V. Lotsch _{1,

2,

3,

4}

Affiliation

We demonstrate photocatalytic hydrogen evolution using COF photosensitizers with molecular proton reduction catalysts for the first time. With azine-linked N2-COF photosensitizer, chloro(pyridine)cobaloxime co-catalyst, and TEOA donor, H₂ evolution rate of 782 μmol h^–1 g^–1 and TON of 54.4 has been obtained in a water/acetonitrile mixture. PXRD, solid-state spectroscopy, EM analysis, and quantum-chemical calculations suggest an outer sphere electron transfer from the COF to the co-catalyst which subsequently follows a monometallic pathway of H₂ generation from the Co^III-hydride and/or Co^II-hydride species.

中文翻译：

单价光催化H ₂从分子共钴肟助催化剂的共价有机框架演变而来。

我们首次展示了使用COF光敏剂与分子质子还原催化剂的光催化氢释放。使用嗪键连接的N2-COF光敏剂，氯（吡啶）钴肟助催化剂和TEOA供体，在水/乙腈混合物中H _2的析出速率为782μmolh ^–1 g ^–1，TON为54.4。PXRD，固态光谱法，EM分析和量子化学计算表明，外层电子从COF转移到助催化剂，随后遵循从Co ^III-氢化物和/或Co ^II生成H ₂的单金属途径-氢化物种类。

更新日期：2017-11-05

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