To boost the photoconversion efficiency (PCE) of ever promising quantum dot sensitized solar cells (QDSSCs), and to improve the design of photoanodes, the ability of the counter electrode (CE) to effectively reduce the oxidized electrolyte needs special attention. A composite of a 15 wt% graphene oxide nanoribbon (GOR), obtained by unzipping multi-walled carbon nanotubes (MWCNTs), and CuxS intersecting hexagonal nanoplates, synthesized by a low cost, facile and scalable microwave synthesis route, is reported as a fascinating CE for QDSSCs. The best performing Cu1.18S-GOR CE could notably achieve a record PCE of ∼3.55% for CdS sensitized QDSSCs, ∼5.42% for in situ deposited CdS/CdSe co-sensitized QDSSCs and ∼6.81% for CdTe/CdS/CdS dual sensitized QDSSCs, apart from increasing the PCE of previously reported QDSSCs. A systematic investigation of the CE design revealed the high electrocatalytic activity of GOR due to the presence of organic functional groups, graphitic edge sites and a quasi-one-dimensional (quasi-1D) structure, which increases the interfacial charge transfer kinetics from the CE to the polysulfide electrolyte. The highly stable Cu1.18S-GOR CE has the added advantage of a favourable energy band alignment with the redox potential of the polysulfide electrolyte, which reduces the loss of charge carriers and thus can increase the PCE of QDSSCs.
One of the strategies to boost the efficiency of highly promising yet struggling quantum dot solar cells (QDSCs) is to dope the QDs with optically active Mn 2+ ions to create long-lived charge carriers and reduce the electron-hole recombination. The in situ deposition of QDs although offers good surface coverage and better charge separation, in "doped" QDSCs the type of doping responsible for higher efficiencies cannot be ascertained. In the electrophoretically deposited Mn:CdS QDSCs, highest lattice doping of Mn 2+ ions in pre-synthesized colloidal CdS QDs results in the highest efficiency, whereas exchange coupled Mn 2+ -Mn 2+ pairs increase nonradiative electron-hole recombination and decrease the efficiency of QDSCs. With Mn:Cd at% of 1.44, the efficiency could be increased to 2.1% as compared to 1.3% for CdS QDSC. The increase in efficiency by 61.5% is due to slower charge recombination in the photoanode and the electrolyte interface and higher electron lifetime in the doped QDSCs.
The unique properties of II-VI semiconductor nanocrystals such as superior light absorption, size-dependent optoelectronic properties, solution processability, and interesting photophysics prompted quantum-dot-sensitized solar cells (QDSSCs) as promising candidates for next-generation photovoltaic (PV) technology. QDSSCs have advantages such as low-cost device fabrication, multiple exciton generation, and the possibility to push over the theoretical power conversion efficiency (PCE) limit of 32%. In spite of dedicated research efforts to enhance the PCE, optimize individual solar cell components, and better understand the underlying science, QDSSCs have unfortunately not lived up to their potential due to shortcomings in the fabrication process and with the QDs themselves. In this feature article, we briefly discuss the QDSSC concepts and mechanisms of the charge carrier recombination pathways that occur at multiple interfaces, viz., (i) metal oxide (MO)/QDs, (ii) MO/QDs/electrolyte, and (iii) counter electrode (CE)/electrolyte. The rational strategies that have been developed to minimize/block these charge recombination pathways are elaborated. The article concludes with a discussion of the present challenges in fabricating efficient devices and future prospects for QDSSCs.
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