Laboratory of Photonics and Interfaces, Department de Chimie, Ecole Polytechnique Federale de Lausanne, CH-1015 Lausanne, Switzerland.
Phys Chem Chem Phys. 2012 Aug 14;14(30):10631-9. doi: 10.1039/c2cp41611e. Epub 2012 Jun 29.
We report a series of cobalt complexes with various polypyridyl ligands, where the oxidation potential is tuned from 0.17 to 0.34 V vs. ferrocene. The highest occupied molecular orbitals (HOMO) of the cobalt complexes were stabilized by adding electron acceptor groups on pyridyl or replacing pyridyl by pyrazole. These complexes are then used as one-electron redox mediators in dye sensitized solar cells (DSSCs) together with polymer based cathode resulting in an excellent performance. The performance of DSSCs using the molecularly engineered cobalt redox shuttle and poly(3,4-alkylthiophenes) based cathode is better than the triiodide/iodide redox shuttle with platinized cathode. The use of high surface area poly(3,4-propylenedioxythiophene) based nanoporous layers allows higher catalytic activity thus minimizing the electrode-electrolyte interface issues.
我们报道了一系列具有不同多吡啶配体的钴配合物，其中氧化电位可调节至相对于 Ferrocene 为 0.17 至 0.34 V。通过在吡啶上添加电子受体基团或将吡啶替换为吡唑，钴配合物的最高占据分子轨道（HOMO）得到稳定。这些配合物随后与基于聚合物的阴极一起用作染料敏化太阳能电池（DSSC）中的单电子氧化还原介体，从而获得优异的性能。使用分子工程钴氧化还原穿梭体和基于聚（3,4-烷基噻吩）的阴极的 DSSC 的性能优于使用铂化阴极的三碘化物/碘化物氧化还原穿梭体。使用高表面积的基于聚（3,4-亚丙基二氧噻吩）的纳米多孔层可以提高催化活性，从而最小化电极-电解质界面问题。
