Photo‐recycling the Sacrificial Electron Donor: Towards Sustainable Hydrogen Evolution in a Biphasic System,ChemPhysChem

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Photo‐recycling the Sacrificial Electron Donor: Towards Sustainable Hydrogen Evolution in a Biphasic System
ChemPhysChem ( IF 2.3 ) Pub Date : 2020-11-09 , DOI: 10.1002/cphc.202000844
Peiyu Ge ₁ , Mohamad Hojeij ₁ , Micheál D. Scanlon _{2,

3} , Hubert H. Girault ₁

Affiliation

H₂ may be evolved biphasically using a polarised liquid|liquid interface, acting as a “proton pump”, in combination with organic soluble metallocenes as electron donors. Sustainable H₂ production requires methodologies to recycle the oxidised donor. Herein, the photo‐recycling of decamethylferrocenium cations (DcMFc⁺) using aqueous core‐shell semiconductor CdSe@CdS nanoparticles is presented. Negative polarisation of the liquid|liquid interface is required to extract DcMFc⁺ to the aqueous phase. This facilitates the efficient capture of electrons by DcMFc⁺ on the surface of the photo‐excited CdSe@CdS nanoparticles, with hydrophobic DcMFc subsequently partitioning back to the organic phase and resetting the system. TiO₂ (P25) and CdSe semiconductor nanoparticles failed to recycle DcMFc⁺ due to their lower conduction band energy levels. During photo‐recycling, CdS (on CdSe) may be self‐oxidised and photo‐corrode, instead of water acting as the hole scavenger.

中文翻译：

牺牲电子给体的光回收：在双相系统中实现可持续的氢释放

H ₂可以与作为电子给体的有机可溶性茂金属组合，使用起“质子泵”作用的极化液界面双相析出。可持续的H ₂生产需要循环利用氧化供体的方法。本文介绍了使用含水核壳半导体CdSe @ CdS纳米粒子对十甲基二茂铁鎓阳离子（DcMFc ⁺）的光循环。为了将DcMFc ⁺提取到水相中，需要液界面的负极性。这有助于DcMFc ⁺高效捕获电子在光激发的CdSe @ CdS纳米颗粒的表面上，疏水性DcMFc随后分配回有机相并重置系统。TiO ₂（P25）和CdSe半导体纳米颗粒由于其较低的导带能级而无法回收DcMFc ⁺。在光循环过程中，CdS（在CdSe上）可能会被自氧化并被光腐蚀，而不是充当空穴清除剂的水。

更新日期：2020-12-17

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