UV‐Light‐Driven Immobilization of Surface‐Functionalized Oxide Nanocrystals onto Silicon

TiO₂ nanorods (NRs) and γ‐Fe₂O₃ nanocrystals (NCs) passivated with unsaturated long‐chain carboxylic acids, namely 10‐undecylenic acid (10UDA) and oleic acid (OLEA), are covalently anchored to Si(100) at room temperature by UV‐light‐driven reaction of hydrogenated silicon with the carbon–carbon double bond (–C?C–) moieties of the capping surfactants. The high reactivity of vinyl groups towards Si provides a general tool for attaching particles of both materials via Si–C bonds. Interestingly, TiO₂ NRs were efficiently attached to silicon even when capped by OLEA. This latter finding has been explained by a photocatalytic mechanism involving the primary role of hydroxyl radicals that can be generated upon bandgap TiO₂ photoexcitation with UV light. The increased oxide coverage achievable on Si opens access to further surface manipulation, as demonstrated by the possibility of depositing an additional film of Au nanoparticles onto TiO₂ via TiO₂‐catalyzed visible‐light‐driven reduction of aqueous AuCl₄^– ions. Extensive morphological and chemical characterization of the obtained NC‐functionalized Si substrates is provided to support the effectiveness of proposed photochemical approaches.     

Self‐Assembling TiO2 Nanorods on Large Graphene Oxide Sheets at a Two‐Phase Interface and Their Anti‐Recombination in Photocatalytic Applications

TiO₂ nanorods are self‐assembled on the graphene oxide (GO) sheets at the water/toluene interface. The self‐assembled GO–TiO₂ nanorod composites (GO–TiO₂ NRCs) can be dispersed in water. The effective anchoring of TiO₂ nanorods on the whole GO sheets is confirmed by transmission electron microscopy (TEM), X‐ray diffraction (XRD), Fourier transform IR spectroscopy (FTIR), and thermogravimetric analysis (TGA). The significant increase of photocatalytic activity is confirmed by the degradation of methylene blue (MB) under UV light irridiation. The large enhancement of photocatalytic activity is caused by the effective charge anti‐recombination and the effective absorption of MB on GO. The effective charge transfer from TiO₂ to GO sheets is confirmed by the significant photoluminescence quenching of TiO₂ nanorods, which can effectively prevent the charge recombination during photocatalytic process. The effective absorption of MB on GO is confirmed by the UV‐vis spectra. The degradation rate of MB in the second cycle is faster than that in the first cycle because of the reduction of GO under UV light irradiation.     

Structure‐Dependent Optical Modulation of Propulsion and Collective Behavior of Acoustic/Light‐Driven Hybrid Microbowls

Hybrid light/acoustic‐powered microbowl motors, composed of gold (Au) and titanium dioxide (TiO₂) with a structure‐dependent optical modulation of both their movement and collective behavior are reported by reversing the inner and outer positions of Au and TiO₂. The microbowl propels in an acoustic field toward its exterior side. UV light activates the photochemical reaction on the TiO₂ surface in the presence of hydrogen peroxide and the Au/TiO₂ system moves toward its TiO₂ side by self‐electrophoresis. Controlling the light intensity allows switching of the dominant propulsion mode and provides braking or reversal of motion direction when TiO₂ is on the interior, or accelerated motion when the TiO₂ is on its exterior. Theoretical simulations offer an understanding of the acoustic streaming flow and self‐electrophoretic fluid flow induced by the asymmetric distribution of ions around the microbowl. The light‐modulation behavior along with the tunable structure also leads to the control of the swarm behaviors under the acoustic field, including expansion or compaction of ensembles of microbowls with interior and exterior TiO₂, respectively. Such structure‐dependent motion control thus paves the way for a variety of complex microscale operations, ranging from cargo transport to drug delivery in biomedical and environmental applications.     

Infiltration of Regioregular Poly[2,2′‐(3‐hexylthiopene)] into Random Nanocrystalline TiO2 Networks

Polymer infiltration into random nanocrystalline TiO₂ networks is examined using a combination of imaging, surface analysis, and depth‐profiling techniques. Nanocrystalline TiO₂ network substrates were fabricated by established methods; the resulting networks were examined using scanning electron microscopy and found to be typical of those reported in the literature. Regioregular poly[2,2′‐(3‐hexylthiopene)] (rrP3HT) was drop‐cast from solution onto the TiO₂‐network substrates. Infiltration of the polymer into the nanoporous TiO₂ network was determined by monitoring the ratio of carbon‐ion signal—by means of secondary‐ion mass spectrometry from a top overlayer of rrP3HT—to the carbon signal from the same polymer within the TiO₂ network. A very low incorporation of polymer was found (0.5 %), even for highly porous (≈ 65 %) networks. Several strategies were used to increase the degree of polymer infiltration, including heat treatment, surface derivatization, and the use of low‐molecular‐weight fractions. A high of 22 % rrP3HT as a percentage of the total volume of a random nanocrystalline film is reported. Previous results for hybrid rrP3HT/random nanocrystalline TiO₂ network devices are examined and analyzed in the context of these findings.     

Phase‐Separation‐Induced Micropatterned Polymer Surfaces and Their Applications

We report a route to fabricate micropatterned polymer films with micro‐ or nanometer‐scale surface concavities by spreading polymer solutions on a non‐solvent surface. The route is simple, versatile, highly efficient, low‐cost, and easily accessible. The concavity density of the patterned films is tuned from 10⁶ to 10⁹ features cm^–2, and the concavity size is controlled in the range from several micrometers to less than 100 nm, by changing the film‐forming parameters including the polymer concentration, the temperature of the non‐solvent and the interactions between polymer, solvent, and non‐solvent. We further demonstrate that these concavity‐patterned films have significantly enhanced hydrophobicity, owing to the existence of the surface concavities, and their hydrophobicity could be controlled by the concavity density. These films have been used as templates to successfully fabricate convex‐patterned polymer films, inorganic TiO₂ microparticles, and NaCl nanocrystals. Their other potential applications are also discussed.     

Multifunctional Au‐Coated TiO2 Nanotube Arrays as Recyclable SERS Substrates for Multifold Organic Pollutants Detection

A multifunctional Au‐coated TiO₂ nanotube array is made via synthesis of a TiO₂ nanotube array through a ZnO template, followed by deposition of Au particles onto the TiO₂ surface using photocatalytic deposition and a hydrothermal method, respectively. Such arrays exhibit superior detection sensitivity with high reproducibility and stability. In addition, due to possessing stable catalytic properties, the arrays can clean themselves by photocatalytic degradation of target molecules adsorbed to the substrate under irradiation with UV light into inorganic small molecules using surface‐enhanced Raman spectroscopy (SERS) detection, so that recycling can be achieved. Finally, by detection of Rhodamine 6G (R6G) dye, herbicide 4‐chlorophenol (4‐CP), persistent organic pollutant (POP) dichlorophenoxyacetic acid (2,4‐D), and organophosphate pesticide methyl‐parathion (MP), the unique recyclable properties indicate a new route in eliminating the single‐use problem of traditional SERS substrates and show promising applications for detecting other organic pollutants.     

Trilevel‐Structured Superhydrophobic Pillar Arrays with Tunable Optical Functions

Water‐repelling surfaces inspired by lotus leaves have been developed for their commercial needs in superhydrophobic and self‐cleaning coatings on glasses and windows. The extraordinary properties originate from their multiscale structures with waxy materials. To obtain high transparency as well as superhydrophobicity, microhair arrays are designed with large spacing to reduce optical scattering effects caused by microstructures, but with a trilevel hierarchical structure to compensate for the loss of superhydrophobicity. In this study, a soft molding technique on wet pastes consisting of nanoparticles (NPs) is proposed to create a multilevel hierarchical structure of sub‐100 nm nanoparticles, which demonstrates excellent water repellency. Additionally, full advantage is taken of the TiO₂ NP mesoporous structure for UV protection and for its ability to attach to various kinds of functional (for example, photoresponsive) dyes. Furthermore, the stability of fluorinated surfaces against UV light is enhanced by the passivation of the TiO₂ surface with a thin silica coating.     

Hybrid Solar Cells from a Blend of Poly(3‐hexylthiophene) and Ligand‐Capped TiO2 Nanorods

Hybrid bulk heterojunction solar cells based on nanocrystalline TiO₂ (nc‐TiO₂) nanorods capped with trioctylphosphine oxide (TOPO) and regioregular poly(3‐hexylthiophene) (P3HT) are processed from solution and characterized in order to relate the device function (optical absorption, charge separation, and transport and photovoltaic properties) to active‐layer properties and device parameters. Annealing the blend films is found to greatly improve the polymer–metal oxide interaction at the nc‐TiO₂/P3HT interface, resulting in a six‐fold increase of the charge separation yield and improved photovoltaic device performance under simulated solar illumination. In addition, the influence of the organic ligand at the nc‐TiO₂ particle surface is found to be crucial for charge separation. Ligand‐exchange procedures applied on the TOPO‐capped nc‐TiO₂ nanorods with an amphiphilic ruthenium‐based dye are found to further improve the charge‐separation yield at the polymer–nanocrystal interface. However, the poor photocurrents generated in the hybrid blend devices, before and after ligand exchange, suggest that transport within or between nanoparticles limits performance. By comparison with other donor–acceptor bulk heterojunction systems, we conclude that charge transport in the nc‐TiO₂:P3HT blend films is limited by the presence of an intrinsic trap distribution mainly associated with the nc‐TiO₂ particles.     

Bioinspired,Stimuli‐Responsive,Multifunctional Superhydrophobic Surface with Directional Wetting,Adhesion, and Transport of Water

A novel smart stimuli responsive surface can be fabricated by the subsequent self‐assembly of the graphene monolayer and the TiO₂ nanofilm on various substrates, that is, fabrics, Si wafers, and polymer thin films. Multiscale application property can be achieved from the interfacial interaction between the hierarchical graphene/TiO₂ surface structure and the underlying substrate. The smart surface possesses superhydrophobic property as a result of its hierarchical micro‐ to nanoscale structural roughness. Upon manipulating the UV induced hydrophilic conversion of TiO₂ on graphene/TiO₂ surface, smart surface features, such as tunable adhesiveness, wettability, and directional water transport, can be easily obtained. The existence of graphene indeed enhances the electron–hole pair separation efficiency of the photo‐active TiO₂, as the time required for the TiO₂ superhydrophilic conversion is largely reduced. Multifunctional characteristics, such as gas sensing, droplet manipulation, and self‐cleaning, are achieved on the smart surface as a result of its robust superhydrophobicity, tunable wettability, and high photo‐catalytic activity. It is also revealed that the superhydrophilic conversion of TiO₂ is possibly caused by the atomic rearrangement of TiO₂ under UV radiation, as a structural transformation from {101} to {001} is observed after the UV treatment.     

Atomic Layer Deposition of UV‐Absorbing ZnO Films on SiO2 and TiO2 Nanoparticles Using a Fluidized Bed Reactor

Atomic layer deposition (ALD) was used to apply conformal, nanothick ZnO coatings on particle substrates using a fluidized bed reactor. Diethylzinc (DEZ) and water were used as precursors at 177 °C. Observed growth rates were ca. 2.0 Å/cycle on primary particles as verified by HRTEM. ICP‐AES and XPS were used to quantify Zn:substrate ratios. Layers of 6, 18, and 30 nm were deposited on 550 nm SiO₂ spheres for UV blocking cosmetics particles. TiO₂ nanoparticles were coated in the second part of this work by ZnO shells of 2, 5, and 10 nm thickness as novel inorganic sunscreen particles. The specific surface area of powders changed appropriately after nanothick film deposition using optimized conditions, signifying that high SA particles can be functionalized without agglomeration. The ZnO layers were polycrystalline as deposited and narrowing of the FWHM occurred upon annealing. Annealing the ZnO‐TiO₂ nanocomposite powder to 600 °C caused the formation of zinc titanate (Zn₂TiO₄) in both oxygen‐rich and oxygen‐deficient environments. The non‐ideal surface behavior of the DEZ precursor became problematic for the much longer times required for high surface area nanoparticle processing and results in Zn‐rich films at this growth temperature. In situ mass spectrometry provides process control capability to functionalize bulk quantities of nano‐ and ultrafine particles without significant precursor waste or process overruns. ZnO overlayers can be efficiently deposited on the surfaces of primary particles using ALD processing in a scalable fluidized bed reactor.     

Conformal Nano‐Sized Inorganic Coatings on Mesoporous TiO2 Films for Low‐Temperature Dye‐Sensitized Solar Cell Fabrication

Here, a new method based on sol–gel electrophoretic deposition to produce uniform high‐quality inorganic conformal coatings on mesoporous nano‐particulate films is presented. This novel sol preparation method allows for very fine control of the coating properties, thus inducing new adjustable functionalities to these electrodes. It is shown that the deposition of an amorphous TiO₂ and/or MgO shell onto photoanodes used in dye‐sensitized solar cells (DSSCs) improves their light‐to‐electric‐power conversion efficiency without the need for sintering. It is proposed that the amorphous TiO₂ coating improves the electronic inter‐particle connection and passivates the surface states. The insulating MgO coating further reduces the electron transfer from the conduction band into the electrolyte while the electron injection from the excited dye state remains unperturbed for thin coatings. Using a low‐temperature method for DSSC production on plastic substrates, a maximum efficiency of 6.2% applying pressure together with an optimized TiO₂ coating is achieved. For systems that cannot be pressed a conversion efficiency of 5.1% is achieved using a double shell TiO₂/MgO coating.     

Self‐Sterilized EVOH‐TiO2 Nanocomposites: Interface Effects on Biocidal Properties

Nanocomposite materials obtained by TiO₂ incorporation into ethylene–vinyl alcohol copolymers, extensively used in food packaging, are prepared via a straightforward melting process. The structural characteristics of the nanocomposites are examined using wide and small angle X‐ray scattering (WAXS/SAXS), and vibrational infrared and Raman spectroscopies. A microscopy (SEM/TEM) study shows that the materials obtained are highly homogeneous at the nanometric scale, exhibiting an intimate contact between both the organic and inorganic components. TiO₂ incorporation into this polymer matrix renders self‐sterilized nanocomposite materials upon light excitation, which are tested against nine micro‐organisms (gram‐positive and gram‐negative bacteria, cocci, and yeasts) typically involved in food contamination and/or degradation. Overall, the nanocomposites display an impressive performance in the killing of all micro‐organisms with a maximum for an oxide content between 2–5 wt %. The measurement of the physico‐chemical properties together with the structural characterization of the materials provide conclusive evidence that the nanocomposites biocidal capability born of the nanometric organo‐inorganic interface and rationalize the existence of a maximum as a function of the TiO₂ content.     

Pulsed Laser Ablation Based Synthesis of PbS‐Quantum Dots‐Decorated One‐Dimensional Nanostructures and Their Direct Integration into Highly Efficient Nanohybrid Heterojunction‐Based Solar Cells

The pulsed laser deposition (PLD) technique is used for the direct fabrication of nanohybrid heterojunctions (NH‐HJs) solar cells exhibiting high PCE and excellent stability in air without any encapsulation and/or resorting to any surface treatment, ligand engineering and/or post‐synthesis processing. The NH‐HJs are achieved through the PLD‐based decoration of hydrothermally‐grown one‐dimensional TiO₂ nanorods (TiO₂‐NRs) by PbS quantum dots (PbS‐QDs). By optimizing both the amount of PbS‐QDs (via the number of laser ablation pulses) and the length of the TiO₂‐NRs, it is possible to achieve optimal NH‐HJs based PV devices with high power conversion efficiency (PCE) of 4.85%. This high PCE is found to occur for an optimal length of the NRs (≈290 nm) which coincides with the average penetration depth of PbS‐QDs into the porous TiO₂‐NRs matrix, leading thereby to the formation of the largest extent of NH‐HJs. Most importantly, the PCE of these novel devices is found to be fairly stable for several months under ambient air. The addition of single‐wall carbon nanotubes (SWCNTs) onto the TiO₂‐NRs prior to their decoration by PbS‐QDs is shown to further enhance their PCE to a value as high as 5.3%, because of additional light absorption and improved charge collection ensured by SWCNTs.     

Enhanced Light‐Harvesting and Photocatalytic Properties in Morph‐TiO2 from Green‐Leaf Biotemplates

The unique structure of green leaves endows them with an extremely high light‐harvesting efficiency. In this work, green leaves are applied as biotemplates to synthesize morph‐TiO₂. The structural features favorable for light harvesting from the macro‐ to the nanoscale are replicated in morph‐TiO₂ through a two‐step infiltration process and the N contained in the original leaves is self‐doped into the resulting samples. The absorbance intensities within the visible‐light range of morph‐TiO₂ derived from different leaves increase by 103–258% and the band‐gap‐absorption onsets at the edge of the UV and visible‐light range show a red‐shift of 25–100 nm compared to those in TiO₂ without the template. The photocatalytic activity of morph‐TiO₂ is also improved, as proven by an electron paramagnetic resonance (EPR) study and degradation of rhodamine dye under irradiation with UV and visible light. The present work, as a new strategy, is of far‐reaching significance in learning from nature, driving us to make full use of the most‐abundant resources and structure‐introduced functions endowed by nature, opening up possibilities for extensive study of the physical and chemical properties of morph‐structured oxides and extending their potential for use in applications such as solar cells, photocatalysts, photoelectrical devices, and photoinduced sensors.     

Versatile Nanocomposite Coatings with Tunable Cell Adhesion and Bactericidity

TiO₂‐Ag nanocomposites are known for their bactericidal effect during exposure to appropriate UV radiation. While involving hazardous radiation, and limited to accessible areas, the bactericidity of these coatings is not persistent in the absence of UV light, which impedes their commercial application. Herein it is shown that TiO₂‐Ag nanocomposites can be made highly bactericidal without the need of irradiation. Beyond this, bactericidity can even be mitigated in the presence of pre‐irradiated coatings. Biocompatibility and cell adhesion are also negligibly small for the as‐processed, non‐irradiated coatings, and become fairly high when the coatings are irradiated prior to testing. This opens the possibility to pattern the coatings into areas with high and low cell adhesion properties. Indeed by irradiating the coating through a mechanical mask it is shown that fibroblast cell adherence is sharply confined to the irradiated area. These properties are achieved using TiO₂‐Ag thin films with high silver loadings of 50 wt%. The films are processed on stainless steel substrates using solution deposition. Microstructural characterization by means of X‐ray diffraction, Raman, and X‐ray photoelectron spectroscopy, high‐resolution scanning electron microscopy, and atomic force microscopy show a highly amorphous TiO₂‐Ag_xO nanocomposite matrix with scattered silver nanoparticles. UV irradiation of the films results in the precipitation of a high density of silver nanoparticles at the film surface. Bactericidal properties of the films are tested on α‐haemolyzing streptococci and in‐vitro biocompatibility is assessed on primary human fibroblast cultures. The results mentioned above as to the tunable bactericidity and biocompatibility of the TiO₂‐Ag coatings developed herein, are amenable to silver ion release, to catalytic effects of silver nanoparticles, and to specific wettabilities of the surfaces.     

Tailoring Metal/TiO2 Interface to Influence Motion of Light‐Activated Janus Micromotors

Catalytic light‐powered micromotors have become a major focus in current autonomous self‐propelled micromotors research. The attractiveness of such machines stems from the fact that these motors are “fuel‐free,” with their motion modulated by light irradiation. In order to study how different metals affect the velocities of metal/TiO₂ micromachines in the presence of UV irradiation in pure water, Pt/TiO₂, Cu/TiO₂, Fe/TiO₂, Ag/TiO₂, and Au/TiO₂ Janus micromotors are prepared. The metals have different chemical potentials and catalytic effects toward water splitting reaction, with both the effects expected to alter the photoelectrochemically‐induced reaction and propulsion rates. Analysis of structures, elemental compositions, motion patterns, velocities, and overall performances of different metals (Pt, Au, Ag, Fe, Cu) on TiO₂ are observed by scanning electron microscopy, energy dispersive X‐ray spectroscopy, and optical microscopy. Electrochemical Tafel analysis is performed for the different metal/TiO₂ structures and it is concluded that the effective velocity is a result of the synergistic effect of chemical potential and catalysis. It is found that the Pt/TiO₂ Janus micromotors exhibit the fastest motion compared to the rest of the prepared materials. Furthermore, after exposure to UV light, every fabricated micromotor shows high possibility of forming assembled chains which influence their velocity.     

Fabrication of All‐Water‐Based Self‐Repairing Superhydrophobic Coatings Based on UV‐Responsive Microcapsules

Superhydrophobic coatings that are also self‐healing have drawn much attention in recent years for improved durability in practical applications. Typically, the release of the self‐healing agents is triggered by temperature and moisture change. In this study, UV‐responsive microcapsules are successfully synthesized by Pickering emulsion polymerization using titania (TiO₂) and silica (SiO₂) nanoparticles as the Pickering agents to fabricate all‐water‐based self‐repairing, superhydrophobic coatings. These coatings are environmentally friendly and can be readily coated on various substrates. Compared to conventional superhydrophobic coatings, these coatings can regenerate superhydrophobicity and self‐cleaning ability under UV light, mimicking the outdoor environment, after they are mechanically damaged or contaminated with organics. They can maintain the superhydrophobicity after multiple cycles of accelerated weathering tests.     

Bioprocess‐Inspired Microscale Additive Manufacturing of Multilayered TiO2/Polymer Composites with Enamel‐Like Structures and High Mechanical Properties

Natural structure‐forming processes found in biological systems are fantastic and perform at ambient temperatures, in contrast with anthropogenic technologies that commonly require harsh conditions. A new research direction “bioprocess‐inspired fabrication” is proposed to develop novel fabrication techniques for advanced materials. Enamel, an organic–inorganic composite biomaterial with outstanding mechanical performance and durability, is formed by repeating the basic blocks consisting of columnar hydroxyapatite or fluorapatite and an organic matrix. Inspired by the enamel formation process, a microscale additive manufacturing method is proposed for achieving a multilayered organic–inorganic columnar structure. In this approach, rutile titanium dioxide (TiO₂) nanorods, polymers, and graphene oxide (GO) are sequentially assembled in a layer‐by‐layer fashion to form an organic–inorganic structure. In particular, GO serves as a substrate for TiO₂ nanorods and interacts with polymers, jointly leading to the strength of the composites. Impressively, this enamel‐like structure material has hardness (1.56 ± 0.05 GPa) and ultrahigh Young's modulus (81.0 ± 2.7 GPa) comparable to natural enamel, and viscoelastic property (0.76 ± 0.12 GPa) superior to most solid materials. Consequently, this biomimetic synthetic approach provides an in‐depth understanding for the formation process of biomaterials and also enables the exploration of a new avenue for the preparation of organic–inorganic composite materials.     

Enhanced Performance of I2‐Free Solid‐State Dye‐Sensitized Solar Cells with Conductive Polymer up to 6.8%

An iodine‐free solid‐state dye‐sensitized solar cell (ssDSSC) is reported here, with 6.8% energy conversion efficiency—one of the highest yet reported for N719 dye—as a result of enhanced light harvesting from the increased transmittance of an organized mesoporous TiO₂ interfacial layer and the good hole conductivity of the solid‐state‐polymerized material. The organized mesoporous TiO₂ (OM‐TiO₂) interfacial layer is prepared on large‐area substrates by a sol‐gel process, and is confirmed by scanning electron microscopy (SEM) and grazing incidence small‐angle X‐ray scattering (GISAXS). A 550‐nm‐thick OM‐TiO₂ film coated on fluorine‐doped tin oxide (FTO) glass is highly transparent, resulting in transmittance increases of 8 and 4% compared to those of the bare FTO and conventional compact TiO₂ film on FTO, respectively. The high cell performance is achieved through careful control of the electrode/hole transport material (HTM) and nanocrystalline TiO₂/conductive glass interfaces, which affect the interfacial resistance of the cell. Furthermore, the transparent OM‐TiO₂ film, with its high porosity and good connectivity, exhibits improved cell performance due to increased transmittance in the visible light region, decreased interfacial resistance ( Ω ), and enhanced electron lifetime ( τ ). The cell performance also depends on the conductivity of HTMs, which indicates that both highly conductive HTM and the transparent OM‐TiO₂ film interface are crucial for obtaining high‐energy conversion efficiencies in I₂‐free ssDSSCs.     

Cold isostatic pressing technique for producing highly efficient flexible dye‐sensitised solar cells on plastic substrates

One of the biggest challenges for making dye‐sensitised solar cells (DSCs) on plastic substrates is the difficulty in making good quality nanoporous TiO₂ films with both good mechanical stability and high electrical conductivity. Cold isostatic pressing (CIP) is a powder compaction technique that applies an isostatic pressure to a powder sample in all directions. It is particularly suitable for making thin films on plastic substrates, including non‐flat surfaces. Cold isostatically pressed nanocrystalline TiO₂ electrodes with excellent mechanical robustness were prepared on indium tin oxide (ITO)‐coated polyethylene naphthalate (PEN) substrates in the absence of organic binders and without heat treatment. The morphology and the physical properties of the TiO₂ films prepared by the CIP method were found to be very compatible with requirements for flexible DSCs on plastics. This room‐temperature processing technique has led to an important technical breakthrough in producing high efficiency flexible DSCs. Devices fabricated on ITO/PEN films by this method using standard P‐25 TiO₂ films with a Ru‐complex sensitiser yielded a maximum incident photon‐to‐current conversion efficiency of 72% at the wavelength of 530 nm and showed high conversion efficiencies of 6.3% and 7.4% for incident light intensities of 100 and 15 mW cm⁻², respectively, which are the highest power conversion efficiencies achieved so far for any DSC on a polymer substrate using the widely used, commercially available P‐25 TiO₂ powder. Copyright © 2011 John Wiley & Sons, Ltd.