The iodide/triiodide redox shuttle has limited the efficiencies accessible in dye-sensitized solar cells. Here, we report mesoscopic solar cells that incorporate a Co((II/III))tris(bipyridyl)-based redox electrolyte in conjunction with a custom synthesized donor-π-bridge-acceptor zinc porphyrin dye as sensitizer (designated YD2-o-C8). The specific molecular design of YD2-o-C8 greatly retards the rate of interfacial back electron transfer from the conduction band of the nanocrystalline titanium dioxide film to the oxidized cobalt mediator, which enables attainment of strikingly high photovoltages approaching 1 volt. Because the YD2-o-C8 porphyrin harvests sunlight across the visible spectrum, large photocurrents are generated. Cosensitization of YD2-o-C8 with another organic dye further enhances the performance of the device, leading to a measured power conversion efficiency of 12.3% under simulated air mass 1.5 global sunlight.
We report on solid-state mesoscopic heterojunction solar cells employing nanoparticles (NPs) of methyl ammonium lead iodide (CH3NH3)PbI3 as light harvesters. The perovskite NPs were produced by reaction of methylammonium iodide with PbI2 and deposited onto a submicron-thick mesoscopic TiO2 film, whose pores were infiltrated with the hole-conductor spiro-MeOTAD. Illumination with standard AM-1.5 sunlight generated large photocurrents (JSC) exceeding 17 mA/cm2, an open circuit photovoltage (VOC) of 0.888 V and a fill factor (FF) of 0.62 yielding a power conversion efficiency (PCE) of 9.7%, the highest reported to date for such cells. Femto second laser studies combined with photo-induced absorption measurements showed charge separation to proceed via hole injection from the excited (CH3NH3)PbI3 NPs into the spiro-MeOTAD followed by electron transfer to the mesoscopic TiO2 film. The use of a solid hole conductor dramatically improved the device stability compared to (CH3NH3)PbI3 -sensitized liquid junction cells.
Photoelectrochemical (PEC) cells offer the ability to convert electromagnetic energy from our largest renewable source, the Sun, to stored chemical energy through the splitting of water into molecular oxygen and hydrogen. Hematite (α-Fe(2)O(3)) has emerged as a promising photo-electrode material due to its significant light absorption, chemical stability in aqueous environments, and ample abundance. However, its performance as a water-oxidizing photoanode has been crucially limited by poor optoelectronic properties that lead to both low light harvesting efficiencies and a large requisite overpotential for photoassisted water oxidation. Recently, the application of nanostructuring techniques and advanced interfacial engineering has afforded landmark improvements in the performance of hematite photoanodes. In this review, new insights into the basic material properties, the attractive aspects, and the challenges in using hematite for photoelectrochemical (PEC) water splitting are first examined. Next, recent progress enhancing the photocurrent by precise morphology control and reducing the overpotential with surface treatments are critically detailed and compared. The latest efforts using advanced characterization techniques, particularly electrochemical impedance spectroscopy, are finally presented. These methods help to define the obstacles that remain to be surmounted in order to fully exploit the potential of this promising material for solar energy conversion.
Metal halide perovskites of the general formula ABX 3 -where A is a monovalent cation such as caesium, methylammonium or formamidinium; B is divalent lead, tin or germanium; and X is a halide anion-have shown great potential as light harvesters for thin-film photovoltaics [1][2][3][4][5] . Among a large number of compositions investigated, the cubic α-phase of formamidinium lead triiodide (FAPbI 3 ) has emerged as the most promising semiconductor for highly efficient and stable perovskite solar cells [6][7][8][9] , and maximizing the performance of this material in such devices is of vital importance for the perovskite research community. Here we introduce an anion engineering concept that uses the pseudo-halide anion formate (HCOO − ) to suppress anion-vacancy defects that are present at grain boundaries and at the surface of the perovskite films and to augment the crystallinity of the films. The resulting solar cell devices attain a power conversion efficiency of 25.6 per cent (certified 25.2 per cent), have long-term operational stability (450 hours) and show intense electroluminescence with external quantum efficiencies of more than 10 per cent. Our findings provide a direct route to eliminate the most abundant and deleterious lattice defects present in metal halide perovskites, providing a facile access to solution-processable films with improved optoelectronic performance.Perovskite solar cells (PSCs) have attracted much attention since their first demonstration in 2009 [1][2][3][4][5] . The rapid expansion of research into PSCs has been driven by their low-cost solution processing and attractive optoelectronic properties, including a tunable bandgap 6 , high absorption coefficient 10 , low recombination rate 11 and high mobility of charge carriers 12 . Within a decade, the power conversion efficiency (PCE) of single-junction PSCs progressed from 3% to a certified value of 25.5% 13 , the highest value obtained for thin-film photovoltaics. Moreover, through the use of additive and interface engineering strategies, the long-term operational stability of PSCs now exceeds 1,000 hours in full sunlight 14,15 . PSCs therefore show great promise for deployment as the next generation of photovoltaics.Compositional engineering plays a key part in achieving highly efficient and stable PSCs. In particular, mixtures of methylammonium lead triiodide (MAPbI 3 ) with formamidinium lead triiodide (FAPbI 3 ) have been extensively studied 5,7 . Compared to MAPbI 3 , FAPbI 3 is thermally more stable and has a bandgap closer to the Shockley-Queisser limit 6 , rendering FAPbI 3 the most attractive perovskite layer for single-junction PSCs.Unfortunately, thin FAPbI 3 films undergo a phase transition from the black α-phase to a photoinactive yellow δ-phase below a temperature of 150 °C. Previous approaches to overcome this problem have included mixing FAPbI 3 with a combination of methylammonium (MA + ), caesium (Cs + ) and bromide (Br − ) ions; however, this comes at the cost of blue-shifted absorbance and phase segregation under...
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