• Energy Research

Searching suitable panchromatic QD sensitizers for expanding the light-harvesting range, accelerating charge separation, and retarding charge recombination is an effective way to improve power conversion efficiency (PCE) of quantum-dot-sensitized solar cells (QDSCs). One possible way to obtain a wide absorption range is to use the exciplex state of a type-II core/shell-structured QDs. In addition, this system could also provide a fast charge separation and low charge-recombination rate. Herein, we report on using a CdTe/CdSe type-II core/shell QD sensitizer with an absorption range extending into the infrared region because of its exciplex state, which is covalently linked to TiO2 mesoporous electrodes by dropping a bifunctional linker molecule mercaptopropionic acid (MPA)-capped QD aqueous solution onto the film electrode. High loading and a uniform distribution of QD sensitizer throughout the film electrode thickness have been confirmed by energy dispersive X-ray (EDX) elemental mapping. The accelerated electron injection and retarded charge-recombination pathway in the built CdTe/CdSe QD cells in comparison with reference CdSe QD-based cells have been confirmed by impedance spectroscopy, fluorescence decay, and intensity-modulated photocurrent/photovoltage spectroscopy (IMPS/IMVS) analysis. With the combination of the high QD loading and intrinsically superior optoelectronic properties of type-II core/shell QD (wide absorption range, fast charge separation, and slow charge recombination), the resulting CdTe/CdSe QD-based regenerative sandwich solar cells exhibit a record PCE of 6.76% (J(sc) = 19.59 mA cm(-2), V(oc) = 0.606 V, and FF = 0.569) with a mask around the active film under a full 1 sun illumination (simulated AM 1.5), which is the highest reported to date for liquid-junction QDSCs.

CdSe0.45Te0.55 alloyed quantum dots (QDs) with excitonic absorption onset at 800 nm and particle size of 5.2 nm were prepared via a noninjection high-temperature pyrolysis route and used as a sensitizer in solar cells. A postsynthesis assembly approach with use of bifunctional linker molecule mercaptopropionic acid (MPA) capped water-soluble QDs, obtained via ex situ ligand exchange from the initial oil-dispersible QDs, was adopted for tethering QDs onto mesoporous TiO2 film. With the combination of high loading of the QD sensitizer and intrinsic superior optoelectronic properties (wide absorption range, high conduction band edge, high chemical stability, etc., relative to their constituents CdSe and CdTe) of the adopted CdSe0.45Te0.55 QD sensitizer, the resulting CdSexTe1-x alloyed QD-based solar cells exhibit a record conversion efficiency of 6.36% (Jsc = 19.35 mA/cm(2), Voc = 0.571 V, FF = 0.575) under full 1 sun illumination, which is remarkably better than that of the reference CdSe and CdTe QD based ones. Furthermore, the solar cells with Cu2S counter electrodes based on eletrodeposition of Cu on conductive glass show long-term (more than 500 h) stability.