期刊
INORGANIC CHEMISTRY
卷 54, 期 2, 页码 560-569出版社
AMER CHEMICAL SOC
DOI: 10.1021/ic502438g
关键词
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资金
- Army Research Office [59842-CH-II]
- North Carolina State University
- U.S. Department of Energy Office of Science [DE-AC52-06NA25396, DE-AC04-94AL85000]
- U.S. Department of Education Graduate Assistantship in Areas of National Need (GAANN) fellowship program at North Carolina State University
Dye-sensitized solar cells (DSSCs) often utilize transition metal-based chromophores for light absorption and semiconductor sensitization. Ru(II)-based dyes are among the most commonly used sensitizers in DSSCs. As ruthenium is both expensive and rare, complexes based on cheaper and more abundant iron could serve as a good alternative. In this study, we investigate Fe(II)-bis(terpyridine) and its cyclometalated analogues, in which pyridine ligands are systematically replaced by aryl groups, as potential photosensitizers in DSSCs. We employ density functional theory at the B3LYP/6-31G*,SDD level to obtain the ground state electronic structure of these complexes. Quantum dynamics simulations are utilized to study interfacial electron transfer between the Fe(II) photosensitizers and a titanium dioxide semiconductor. We find that cyclometalation stabilizes the singlet ground state of these complexes by 819 kcal/mol but reduces the electron density on the carboxylic acid attached to the aryl ring. The results suggest that cyclometalation provides a feasible route to increasing the efficiency of Fe(II) photosensitizers but that care should be taken in choosing the substitution position for the semiconductor anchoring group.
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