High‐Performance,Transparent, Dye‐Sensitized Solar Cells for See‐Through Photovoltaic Windows

Dye‐sensitized solar cells (DSCs) have attracted great interest as one of the most promising photovoltaic technologies, and transparent DSCs show potential applications as photovoltaic windows. However, the competition between light absorption for photocurrent generation and light transmittance for obtaining high transparency limits the performance of transparent DSCs. Here, transparent DSCs exhibiting a high light transmittance of 60.3% and high energy conversion efficiency (3.66%) are reported. The strategy is to create a cocktail system composed of ultraviolet and near‐infrared dye sensitizers that selectively and efficiently harvest light in the invisible or low‐eye‐sensitivity region while transmitting light in high‐eye‐sensitivity regions. This new design provides a reasonable approach for realizing high efficiency and transparency DSCs that have potential applications as photovoltaic windows.     

Development of Next‐Generation Organic‐Based Solar Cells: Studies on Dye‐Sensitized and Perovskite Solar Cells

Next‐generation organic solar cells such as dye‐sensitized solar cells (DSSCs) and perovskite solar cells (PSCs) are studied at the National Institute of Advanced Industrial Science and Technology (AIST), and their materials, electronic properties, and fabrication processes are investigated. To enhance the performance of DSSCs, the basic structure of an electron donor, π‐electron linker, and electron acceptor, i.e., D–π–A, is suggested. In addition, special organic dyes containing coumarin, carbazole, and triphenylamine electron donor groups are synthesized to find an effective dye structure that avoids charge recombination at electrode surfaces. Meanwhile, PSCs are manufactured using both a coating method and a laser deposition technique. The results of interfacial studies demonstrate that the level of the conduction band edge (CBE) of a compact TiO₂ layer is shifted after TiCl₄ treatment, which strongly affects the solar cell performance. Furthermore, a special laser deposition system is developed for the fabrication of the perovskite layers of PSCs, which facilitates the control over the deposition rate of methyl ammonium iodide used as their precursor.     

Surface‐Plasmon Assisted Energy Conversion in Dye‐Sensitized Solar Cells

In this study, the effect of plasmonic core‐shell structures, consisting of dielectric cores and metallic nanoshells, on energy conversion in dye‐sensitized solar cells (DSSCs) is investigated. The structure of the core‐shell particles is controlled to couple with visible light so that the visible component of the solar spectrum is amplified near the core‐shell particles. In core‐shell particle – TiO₂ nanoparticle films, the local field intensity and light pathways are increased due to the surface plasmons and light scattering. This, in turn, enlarges the optical cross‐section of dye sensitizers coated onto the mixed films. When 22 vol% of core‐shell particles are added to a 5 μm thick TiO₂ film, the energy conversion efficiency of DSSCs increases from 2.7% to 4.0%, in spite of a more than 20% decrease in the amount of dyes adsorbed on the composite films. The correlation between core‐shell particle content and energy conversion efficiency in DSSCs is explained by the balance among near‐field effects, light scattering efficiency, and surface area in the composite films.     

Hybrid Dye‐Titania Nanoparticles for Superior Low‐Temperature Dye‐Sensitized Solar Cells

In this work, a new strategy to design low‐temperature (≤200 °C) sintered dye‐sensitized solar cells (lt‐DSSC) is reported to enhance charge collection efficiencies (η_coll), photoconversion efficiencies (η), and stabilities under continuous operation conditions. Realization of lt‐DSSC is enabled by the integration of hybrid nanoparticles based on TiO₂‐Ru(II) complex (TiO₂_Ru_IS)—obtained by in situ bottom‐up construction of Ru(II) N3 dye‐sensitized titania—into the photoelectrode. Incentives for the use of TiO₂_Ru_IS are i) dye stability due to its integration into the TiO₂ anatase network and ii) enhanced charge collection yield due to its significant resistance toward electron recombination with electrolytes. It is demonstrated that devices with single‐layer photoelectrodes featuring blends of P25 and TiO₂_Ru_IS give rise to a 60% η_coll relative to a 46% η_coll for devices with P25‐based photoelectrodes. Responsible for this trend is a better charge transport and a reduced electron recombination. When using a multilayered photoelectrode architecture with a top layer based only on TiO₂_Ru_IS, devices with an even higher η_coll (74%) featuring a η of around 8.75% and stabilities of 600 h are achieved. This represents the highest values reported for lt‐DSSC to date.     

Dominating Energy Losses in NiO p‐Type Dye‐Sensitized Solar Cells

Nickel oxide based p‐type dye‐sensitized solar cells (DSCs) are limited in their efficiencies by poor fill factors (FFs). This work explores the origins of this limitation. Transient absorption spectroscopy identifies fast recombination between the injected hole and the dye anion under applied load as one of the predominant reasons for the poor FF of NiO‐based DSCs. A reduced hole injection efficiency, η_INJ, under applied load is found to play an equally important role. Both, the dye regeneration yield, Φ_REG, and η_INJ decrease by approximately 40%–50% when moving from short‐ to open‐circuit conditions. Spectroelectrochemical measurements reveal that the electrochromic properties of NiO are a further limiting factor for the device performance leading to variable light‐harvesting efficiencies, η_LH, under applied load. The peak light‐harvesting efficiency decreases from 63% at short circuit to 57% at 600 mV reducing the FF of NiO DSCs by 5%. This effect is expected to be more pronounced for future devices with higher operating voltages. Incident, photon‐to‐electron conversion efficiency front–back analysis at applied bias is utilized to characterize the interfacial charge recombination. It is found that the recombination between the injected hole and the redox mediator has a surprisingly small effect on the FF.     

Rational Design of Metal Oxide–Based Cathodes for Efficient Dye‐Sensitized Solar Cells

Recently, there is an urgent need for alternative energy resources due to the nonrenewable nature of fossil fuels and increasing CO₂ greenhouse gas emissions. The photovoltaic technologies which directly utilize the abundant and sustainable solar energy are critical. Among various photovoltaic devices (solar cells), dye‐sensitized solar cells (DSSCs) have gained increasing attention due to their high efficiency and easy fabrication process in the past decade. The cathode is a critical part in DSSCs while the benchmark Pt cathode suffers from high cost and scarcity. Thus, the development of alternative Pt‐free cathodes has attracted significant attention with the aim to heighten the cost competitiveness of DSSCs. Among various cathodes, metal oxides are of growing interest due to their superior activity, robust stability, and low cost. Simple oxides such as WO₃ and SnO₂ are used as cathodes for DSSCs. Considering the fixed atomic environment in simple oxides, complex oxides are more attractive as cathodes because of their more flexible physical and chemical properties. This review attempts to present the rational design of simple/complex metal oxide–based cathodes in DSSCs and then to provide useful guidance for the future design of Pt‐free cathodes. The demonstrated design strategies can be extended to other electrocatalysis‐based applications.     

Indolizine‐Based Donors as Organic Sensitizer Components for Dye‐Sensitized Solar Cells

Strong electron‐donating functionality is desirable for many organic donor‐π‐bridge‐acceptor (D‐π‐A) dyes. Strategies for increasing the electron‐donating strength of common nitrogen‐based donors include planarization of nitrogen substituents and the use of low resonance‐stabilized energy aromatic ring‐substituted nitrogen atoms. Organic donor motifs based on the planar nitrogen containing heterocycle indolizine are synthesized and incorporated into dye‐sensitized solar cell (DSC) sensitizers. Resonance active substitutions at several positions on indolizine in conjugation with the D‐π‐A π‐system are examined computationally and experimentally. The indolizine‐based donors are observed to contribute electron density with strengths greater than triarylamines and diarylamines, as evidenced by UV/Vis, IR absorptions, and oxidation potential measurements. Fluorescence lifetime studies in solution and on TiO₂ yield insights in understanding the performance of indolizine‐based dyes in DSC devices.     

Quantum Dot–Sensitized Solar Cells Featuring CuS/CoS Electrodes Provide 4.1% Efficiency

CuS, CoS, and CuS/CoS onto fluorine‐doped tin oxide glass substrates were deposited to function as counter electrodes for polysulfide redox reactions in CdS/CdSe quantum dot–sensitized solar cells (QDSSCs). Relative to a Pt electrode, the CuS, CoS, and CuS/CoS electrodes provide greater electrocatalytic activity, higher reflectivity, and lower charge‐transfer resistance. Measurements of fill factor and short‐current density reveal that the electrocatalytic activities, reflectivity, and internal resistance of counter electrodes play strong roles in determining the energy‐conversion efficiency (η) of the QDSSCs. Because the CuS/CoS electrode has a smaller internal resistance and higher reflectivity relative to those of the CuS and CoS electrodes, it exhibits a higher fill factor and short‐circuit current density. As a result, the QDSSC featuring a CuS/CoS electrode provides a higher value of η. Under illumination of one sun (100 mW cm^?2), the QDSSCs incorporating Pt, CuS, CoS, and CuS/CoS counter electrodes provide values of η of 3.0 ± 0.1, 3.3 ± 0.3, 3.8 ± 0.2, and 4.1 ± 0.2%, respectively.     

Nitrogen‐Doped CNx/CNTs Heteroelectrocatalysts for Highly Efficient Dye‐Sensitized Solar Cells

The use of polydopamine as a nitrogen containing precursor to generate catalytically active nitrogen‐doped carbon (CN_x) materials on carbon nanotubes (CNTs) is reported. These N‐doped CN_x/CNT materials display excellent electrocatalytic activity toward the reduction of triiodide electrolyte in dye‐sensitized solar cells (DSSCs). Further, the influence of various synthesis parameters on the catalytic performance of CN_x/CNTs is investigated in detail. The best performing device fabricated with the CN_x/CNTs material delivers power conversion efficiency of 7.3%, which is comparable or slightly higher than that of Pt (7.1%) counter electrode‐based DSSC. These CN_x/CNTs materials show great potential to address the issues associated with the Pt electrocatalyst including the high cost and scarcity.     

Convergent/Divergent Synthesis of a Linker‐Varied Series of Dyes for Dye‐Sensitized Solar Cells Based on the D35 Donor

A series of four new dyes, based on the D35 type donor moiety with varied linker units, is synthesized using a facile convergent/divergent method, enabled by an improved synthesis of the D35 donor. The dyes are evaluated in dye sensitized solar cells with Co(II/III)(bpy)₃‐based electrolytes. By extending the linker fragment, higher photocurrents and solar energy conversion efficiencies are achieved. It is also found that the linker unit plays a crucial role in maintaining a high open‐circuit photovoltage. Based on the photovoltaic performance it is concluded that the hexylthiophene unit is the most suitable for this purpose, as it allows further enhancement of the already high open‐circuit voltage of D35 to 0.92 V. The best dye in this series reaches an efficiency of 6.8%.     

Solid‐State Dye‐Sensitized Solar Cells Using a Novel Class of Ullazine Dyes as Sensitizers

Here we present the photovoltaic performance of solid‐state dye‐sensitized solar cells (DSCs) using a series of ullazine‐based metal‐free organic sensitizers and spiro‐MeOTAD as a hole‐transport material. A maximum of 4.95% power conversion efficiency measured under standard AM 1.5G illumination (100 mW cm^?2) was achieved with the best performing ullazine dye, and was further improved to 5.40% through co‐sensitization with the triphenylamine‐based organic sensitizer, D35. This study investigates the effect of the molecular structure of the ullazine sensitizer on the performance in solid‐state DSCs.     

Click‐Functionalized Ru(II) Complexes for Dye‐Sensitized Solar Cells

Three heteroleptic ruthenium complexes incorporating new ancillary ligands synthesized by sequential connection of different alkyl functionalities with triazole as a linker are prepared using click chemistry. These sensitizers exhibit low‐energy metal‐to‐ligand charge transfer bands centered at 540 nm with molar extinction coefficients of up to 1.54 × 10⁴ L mol^?1 cm^?1. The devices using these sensitizers in conjunction with a volatile electrolyte show high photovoltaic conversion efficiencies of 8.7 to 9.9% under standard AM 1.5G sunlight (100 mW cm^?2) conditions. Using an ionic liquid electrolyte, the cells show not only a good power‐conversion efficiency of up to 7.1%, but also promising long‐term stability under full sunlight intensity at 60 °C. The difference in the photovoltaic parameters during the ageing process is investigated by employing transient photoelectrical measurements.     

Recent Progress in Dye‐Sensitized Solar Cells Using Nanocrystallite Aggregates

Nanocrystallite aggregates are spherical assemblies of nanometer‐sized crystallites and feature a size on the order of sub‐micrometers. This paper reports and summarizes recent progress in nanocrystallite aggregates for applications in dye‐sensitized solar cells. It emphasizes that nanocrystallite aggregates are a promising class of materials with the capability to generate light scattering, enhance electron transport, retain high specific surface area for dye adsorption, and facilitate electrolyte diffusion while serving as the photoelectrode film of a dye‐sensitized solar cell. In the Perspectives section, it is suggested that optimization of the porosity of the aggregates, the facets of nanocrystallites forming the aggregates, and the structure of photoelectrode film could possibly lead to breakthroughs in improving the power conversion efficiency of the current state‐of‐the‐art dye‐sensitized solar cells.     

Mesh‐Shaped Nanopatterning of Pt Counter Electrodes for Dye‐Sensitized Solar Cells with Enhanced Light Harvesting

A facile process to produce large‐area platinum (Pt) counter electrode platforms with well‐arrayed, mesh‐shaped nanopatterns using commercially available TiO₂ paste and poly(dimethyl siloxane) (PDMS) nanostamps is presented. The process involves mesh‐shaped (200 nm × 200 nm) nanopatterning of a TiO₂ scaffold onto a fluorine‐doped tin oxide (FTO) substrate, followed by Pt sputtering. The structure and morphology of the counter electrodes are characterized by a field emission scanning electron microscope (FE‐SEM) and an atomic force microscope (AFM). Solid‐state dye‐sensitized solar cells (ssDSSCs) fabricated with these mesh‐shaped Pt counter electrodes showed an efficiency of 7.0%. This is one of the highest efficiencies observed for N719 dye and is much higher than that of devices with non‐patterned, thermally deposited electrodes (5.4%) or non‐patterned, sputtering deposited electrodes (5.7%). This improvement is attributed to enhanced light harvesting and a greater surface area and has been confirmed by incident photon‐to current efficiency (IPCE), electrochemical impedance spectroscopy (EIS), and cyclic voltammetry (CV) measurements.