POLYMERS AND POLYMER MATRIX COMPOSITES |
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Performance and Possible Mechanism of Photocatalytic Water Splitting for Hydrogen Production Based on Two [2Fe2S] Compounds |
ZHENG Huiqin1,*, FAN Yaoting2
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1 College of Environment, Henan Finance University, Zhengzhou 450046, China 2 College of Chemistry, Zhengzhou University, Zhengzhou 450001, China |
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Abstract Two new [2Fe2S] compounds 1 and 2 containing the bridging ligand 6, 8-lipoic acid methyl ester (pdte) were synthesized, and their structures were characterized by IR, 1HNMR, 31PNMR(compound 2), elemental analysis and X-ray single crystal diffraction (compound 1), etc. A three-component photo-catalytic hydrogen production system was constructed, in which compounds 1 or 2 was used as the photo-catalyst, EY2-as the photo-sensitizer, TEA as the electron donor and proton source, respectively. The results showed that the maximum hydrogen production was 106.5 μmol (TON 13.3 vs.1 ) and 136.2 μmol (TON 17 vs.2), with corresponding hydrogen production rates 7 607 μmol·g-1·h-1and 6 595.6 μmol·g-1·h-1, respectively, under the optimal hydrogen production conditions of V(CH3CN)/V(H2O)=1/1, pH=11, and visible light (λ>420 nm) irradiation for 3.5 h. Probing into the mechanism of hydrogen production, it was shown that the deactivation of the system was mainly due to the photo-degradation of the photo-sensitizer EY2-and the catalyst in the photo-catalytic process. Photogenerated electrons can be transferred from 1*EY2- or EY3-· to the FeⅠFeⅠ center via two pathways to form the important intermediate FeⅠFe0 species in the present system. Furthermore, the important hydrogen-producing active intermediates HFeⅡFeⅠ species and (η2-H2) FeⅡ-FeⅠ species were formed by further protonation, finally releasing H2 and regenerating FeⅠFeⅠspecies. The result implicated that the title catalyst (especially 2) was a potential molecular catalyst for photo-catalytic hydrogen production.
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Published: 10 May 2023
Online: 2023-05-04
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Fund:National Natural Science Foundation of China (21171147), Young Backbone Teachers Project of Henan Province (2020GGJS266), and Key Scientific Research Projects of Colleges and Universities in Henan Province (21B150001). |
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