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Issue 6, 2016
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Comparison of H2 photogeneration by [FeFe]-hydrogenase mimics with CdSe QDs and Ru(bpy)3Cl2 in aqueous solution

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Abstract

Two water soluble [FeFe]-hydrogenase ([FeFe]-H2ase) mimics, Fe2S2-2SO3Na (1) and Fe2S2-SO3Na (2), were designed to compare the performance of photocatalytic H2 evolution systems using quantum dots (QDs) and the molecular photosensitizer [Ru(bpy)3]2+ in water. Under the same conditions, the resulting systems showed that CdSe QDs display much higher activity than [Ru(bpy)3]2+, meanwhile, the turnover numbers (TONs) of 2.65 × 104 (1) and 1.88 × 104 (2) for CdSe QD systems and 178 (1) and 114 (2) for [Ru(bpy)3]2+ systems were comparable with the highest reported H2 evolution systems using the same photosensitizers. Spectroscopic and electrochemical analyses revealed that the excited [Ru(bpy)3]2+ undergoes reductive-quenching while the excited CdSe QDs proceed via oxidative-quenching during the catalytic process. The greater free energy change and faster electron transfer rate in the CdSe QD system made the electron transfer between the photosensitizer and [FeFe]-H2ase mimics more efficient, which was subsequently corroborated by emission quenching and transient absorption experiments. The reduced [FeFe]-H2ase mimics generated from the CdSe QDs were demonstrated to react with protons at a rate of 1.17 × 107 M−1 s−1 for 1 and 8.62 × 106 M−1 s−1 for 2.

Graphical abstract: Comparison of H2 photogeneration by [FeFe]-hydrogenase mimics with CdSe QDs and Ru(bpy)3Cl2 in aqueous solution

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Publication details

The article was received on 29 Feb 2016, accepted on 15 Apr 2016 and first published on 15 Apr 2016


Article type: Paper
DOI: 10.1039/C6EE00629A
Citation: Energy Environ. Sci., 2016,9, 2083-2089
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    Comparison of H2 photogeneration by [FeFe]-hydrogenase mimics with CdSe QDs and Ru(bpy)3Cl2 in aqueous solution

    J. Jian, C. Ye, X. Wang, M. Wen, Z. Li, X. Li, B. Chen, C. Tung and L. Wu, Energy Environ. Sci., 2016, 9, 2083
    DOI: 10.1039/C6EE00629A

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