Department of Chemistry, and Yale Energy Sciences Institute , Yale University , New Haven , Connecticut 06520-8107 , United States.
ACS Appl Mater Interfaces. 2019 Feb 27;11(8):8000-8008. doi: 10.1021/acsami.8b20996. Epub 2019 Feb 12.
The development of light-harvesting architectures with broad absorption coverage in the visible region continues to be an important research area in the field of artificial photosynthesis. Here, we introduce a new class of ethynyl-linked panchromatic dyads composed of dibenzophenazines coupled ortho and meta to tetrapyrroles with an anchoring group that can be grafted onto metal oxide surfaces. Quantum chemical calculations and photophysical measurements of the synthesized materials reveal that both of the dibenzophenazine dyads absorb broadly from 300 to 636 nm and exhibit absorption bands different from those of the constituent chromophore units. Moreover, the different points of attachment of dibenzophenazines to tetrapyrroles give different absorption profiles which computations suggest result from differences in the planarity of the two dyads. Applicability of the dyads in artificial photosynthesis systems was assessed by their incorporation and characterization of their performance in dye-sensitized solar cells.
在人工光合作用领域,开发具有宽可见光吸收覆盖范围的光收集结构仍然是一个重要的研究领域。在这里,我们介绍了一类新的乙炔基连接的全色二聚体,由联苯并嗪组成,联苯并嗪与四吡咯通过邻位和间位偶联,并带有一个可以接枝到金属氧化物表面的锚定基团。合成材料的量子化学计算和光物理测量表明,这两个联苯并嗪二聚体从 300nm 到 636nm 都有广泛的吸收,并表现出与组成发色团单元不同的吸收带。此外,联苯并嗪连接到四吡咯的不同连接点给出了不同的吸收曲线,计算表明这是由于两个二聚体的平面性差异所致。通过将二聚体掺入染料敏化太阳能电池并对其性能进行表征,评估了它们在人工光合作用系统中的适用性。