Yeap W S, Liu X, Bevk D, Pasquarelli A, Lutsen L, Fahlman M, Maes W, Haenen K
Institute for Materials Research (IMO), Hasselt University , B-3590 Diepenbeek, Belgium.
ACS Appl Mater Interfaces. 2014 Jul 9;6(13):10322-9. doi: 10.1021/am501783b. Epub 2014 Jun 23.
N3 dye molecules [cis-bis(isothiocyanato)bis(2,2'-bipyridyl-4,4'-dicarboxylato)ruthenium(II)] are covalently attached to boron-doped nanocrystalline diamond (B:NCD) thin films through a combination of coupling chemistries, i.e., diazonium, Suzuki, and EDC-NHS. X-ray and ultraviolet photoelectron spectroscopy and near-edge X-ray absorption fine structure spectroscopy are used to verify the covalent bonding of the dye on the B:NCD surface (compared to a hydrogen-terminated reference). The spectroscopic results confirm the presence of a dense N3 chromophore layer, and the positions of the frontier orbitals of the dye relative to the band edge of the B:NCD thin film are inferred as well. Proof-of-concept photoelectrochemical measurements show a strong increase in the photocurrent compared to non-dye-functionalized B:NCD films. This study opens up the possibility of applying N3-sensitized B:NCD thin films as hole conductors in dye-sensitized solar cells.
N3染料分子[顺式双（异硫氰酸根合）双（2,2'-联吡啶-4,4'-二羧酸根）钌（II）]通过重氮、铃木和EDC-NHS等偶联化学方法的组合，共价连接到硼掺杂的纳米晶金刚石（B:NCD）薄膜上。利用X射线和紫外光电子能谱以及近边X射线吸收精细结构光谱来验证染料在B:NCD表面的共价键合（与氢终止的参考物相比）。光谱结果证实了致密的N3发色团层的存在，并且还推断了染料的前沿轨道相对于B:NCD薄膜带边的位置。概念验证光电化学测量表明，与未进行染料功能化的B:NCD薄膜相比，光电流有显著增加。这项研究开辟了将N3敏化的B:NCD薄膜用作染料敏化太阳能电池中空穴导体的可能性。
