期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 120, 期 15, 页码 7923-7940出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.5b12489
关键词
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资金
- program POSITIF [ANR-12-PRGE-0016-01]
- European Research Council (ERC) [Marches -278845]
- Region des Pays de la Loire
- Knut and Alice Wallenberg Foundation
- Swedish Energy Agency
- Swedish Research Council
- Chinese Scolarship Council
- Europe for COST CM1202 program
In this study, four new diketopyrrolopyrrole (DPP) sensitizers, with a dicarboxylated triphenylamine anchoring group for attachment to NiO, were prepared and their electronic absorption, emission and electrochemical properties were recorded. The nature of the electronic excited-states was also modeled with Time-Dependent Density Functional Theory (TD-DFT) quantum chemistry calculations. The photovoltaic performances of these new dyes were characterized in NiO-based dye-sensitized solar cells (DSCs) with the classical iodide/triiodide and cobalt(II/III)-polypyridine electrolytes, in which they proved to be quite active. Laser spectroscopy on dye/NiO/electrolyte films gave evidence for ultrafast hole injection into NiO (0.2-10 ps time scales). For the dyes with an appended naphtalenediimide (NDI) acceptor unit, ultrafast electron transfer to the NDI dramatically prolonged the lifetime of the charge separated NiO+/dye(-), from the ps time scale to an average lifetime approximate to 0.25 ms, which is among the slowest charge recombinations ever reported for dye/NiO systems. This allowed for efficient regeneration by Co-III-polypyridine electrolytes, which translated into much improved PV-performance compared to the DPP dyes without appended NDI. Overall, these results underscore the suitability of DPP as sensitizers for NiO-based photoelectrochemical devices for photovoltaic and photocatalysis.
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