Visible Light-Driven Dye-Sensitized Photocatalytic Hydrogen Production by Porphyrin and its Cyclic Dimer and Trimer: Effect of Multi-Pyridyl-Anchoring Groups on Photocatalytic Activity and Stability

Visible Light-Driven Dye-Sensitized Photocatalytic Hydrogen Production by Porphyrin and its Cyclic Dimer and Trimer: Effect of Multi-Pyridyl-Anchoring Groups on Photocatalytic Activity and Stability
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DOI:
10.1021/acsaem.8b01113
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发表时间:
2018-10
影响因子:
6.4
通讯作者:
Motonori Watanabe;Songmei Sun;T. Ishihara;Takuya Kamimura;Masato Nishimura;F. Tani
Motonori Watanabe;Songmei Sun;T. Ishihara;Takuya Kamimura;Masato Nishimura;F. Tani
中科院分区:
材料科学3区
文献类型:
--
作者:
Motonori Watanabe;Songmei Sun;T. Ishihara;Takuya Kamimura;Masato Nishimura;F. Tani

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以5,15-二苯基-10,20-二(吡啶-4-基)卟啉的单体、二聚体和三聚体为研究对象,研究了其在水介质中可见光催化制氢中对TiO 2的多重锚定效应.此外,制备卟啉三聚体,并通过核磁共振(NMR)光谱、吸收光谱、电化学伏安法、快原子轰击(FAB)质谱和密度泛函理论(DFT)计算进行分析。研究结果表明,随着卟啉单元数目的增加,吸收光谱的峰强度增加,而最高占据分子轨道(HOMO)-最低未占据分子轨道(LUMO)带隙几乎没有变化.在1 wt % Pt负载的TiO 2粉末光催化剂体系中,卟啉二聚体在80 h内表现出最佳的稳定产氢性能,其产氢上级速率为1023 μmol. g-1. h-1.并对光催化体系的稳定性进行了系统的研究。
The monomer, dimer, and trimer of 5,15-diphenyl-10,20-di(pyridin-4-yl)porphyrin are used to investigate the multianchoring effect on TiO2 for visible light-driven photocatalytic hydrogen production in a water medium. Further, the porphyrin trimer is prepared and analyzed by nuclear magnetic resonance (NMR) spectroscopy, absorption spectroscopy, electrochemical voltammetry, fast atom bombardment (FAB) mass spectroscopy, and density functional theory (DFT) computation. The results of this study indicate that the peak intensities of the absorption spectra increase as the number of porphyrin units increases, while changes could be barely observed in the highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gaps. The porphyrin dimer in a 1 wt % Pt-loaded TiO2 powder photocatalyst system exhibited optimal hydrogen production performance in a stable state over a period of 80 h and at a superior rate of 1023 μmol·g–1·h–1. Further, the stability of the photocatalytic system was syste...