Fabrication of Mesoporous Titania Nanoparticles with Controlled Porosity and Connectivity for Studying the Photovoltaic Properties in Perovskite Solar Cells
Abstract:Mesoporous titania (TiO2) nanoparticles (NPs) were synthesized by treating prehydrolyzed titanium precursors with polyethylene glycol (PEG). By varying the amount of PEG, their different physical properties were tuned appropriately in terms of surface area, pore size/volume, and electrical conductivity. By increasing the amount of PEG in TiO2, the surface area and pore volume of mesoporous TiO2 increased, and no direct correlation with the photovoltaic performance of perovskite solar cells was observed. In com… Show more
“…It was indeed demonstrated that the porosity of the titania scaffold, which mainly depends on the dimensions of spherical nanoparticles, determines both the perovskite coverage and crystallinity [ 98 , 99 , 100 , 101 , 102 , 103 ]. Improved coverage of the titania scaffold, obtained by increasing the porosity, gives rise to better light harvesting capabilities and hence results in higher short circuit current density generation [ 101 , 102 , 104 ]. Another consequence of the improvement of the TiO 2 scaffold coverage is the reduction of undesired electron–hole recombination, which occurs at the interface between electron and hole-transport layers; accordingly, a more effective capability of charge extraction from the perovskite was demonstrated by measuring the photoluminescence intensity, which decreases for increased titania film porosity while maintaining the same thickness.…”
Section: Photovoltaic Energy Conversionmentioning
confidence: 99%
“…Another consequence of the improvement of the TiO 2 scaffold coverage is the reduction of undesired electron–hole recombination, which occurs at the interface between electron and hole-transport layers; accordingly, a more effective capability of charge extraction from the perovskite was demonstrated by measuring the photoluminescence intensity, which decreases for increased titania film porosity while maintaining the same thickness. It was also reported that when maintaining the same morphology, when the titania film thickness exceeds an optimal value, the transport characteristics of the electrode [ 104 ] degrade because the perovskite coverage decreases, allowing recombination processes, and also, as widely discussed above, the number of interparticles connections decreases, lengthening the electron path. Moreover, many papers report on the impact of the perovskite grain size on the charge recombination processes not explicitly addressing the role of the titania scaffold morphology [ 100 , 105 , 106 ] but showing the improved performance of cells with larger grains, which are less affected by trap-assisted recombination at the grain boundaries.…”
Nanostructured titania is one of the most commonly encountered constituents of nanotechnology devices for use in energy-related applications, due to its intrinsic functional properties as a semiconductor and to other favorable characteristics such as ease of production, low toxicity and chemical stability, among others. Notwithstanding this diffusion, the quest for improved understanding of the physical and chemical mechanisms governing the material properties and thus its performance in devices is still active, as testified by the large number of dedicated papers that continue to be published. In this framework, we consider and analyze here the effects of the material morphology and structure in determining the energy transport phenomena as cross-cutting properties in some of the most important nanophase titania applications in the energy field, namely photovoltaic conversion, hydrogen generation by photoelectrochemical water splitting and thermal management by nanofluids. For these applications, charge transport, light transport (or propagation) and thermal transport are limiting factors for the attainable performances, whose dependence on the material structural properties is reviewed here on its own. This work aims to fill the gap existing among the many studies dealing with the separate applications in the hope of stimulating novel cross-fertilization approaches in this research field.
“…It was indeed demonstrated that the porosity of the titania scaffold, which mainly depends on the dimensions of spherical nanoparticles, determines both the perovskite coverage and crystallinity [ 98 , 99 , 100 , 101 , 102 , 103 ]. Improved coverage of the titania scaffold, obtained by increasing the porosity, gives rise to better light harvesting capabilities and hence results in higher short circuit current density generation [ 101 , 102 , 104 ]. Another consequence of the improvement of the TiO 2 scaffold coverage is the reduction of undesired electron–hole recombination, which occurs at the interface between electron and hole-transport layers; accordingly, a more effective capability of charge extraction from the perovskite was demonstrated by measuring the photoluminescence intensity, which decreases for increased titania film porosity while maintaining the same thickness.…”
Section: Photovoltaic Energy Conversionmentioning
confidence: 99%
“…Another consequence of the improvement of the TiO 2 scaffold coverage is the reduction of undesired electron–hole recombination, which occurs at the interface between electron and hole-transport layers; accordingly, a more effective capability of charge extraction from the perovskite was demonstrated by measuring the photoluminescence intensity, which decreases for increased titania film porosity while maintaining the same thickness. It was also reported that when maintaining the same morphology, when the titania film thickness exceeds an optimal value, the transport characteristics of the electrode [ 104 ] degrade because the perovskite coverage decreases, allowing recombination processes, and also, as widely discussed above, the number of interparticles connections decreases, lengthening the electron path. Moreover, many papers report on the impact of the perovskite grain size on the charge recombination processes not explicitly addressing the role of the titania scaffold morphology [ 100 , 105 , 106 ] but showing the improved performance of cells with larger grains, which are less affected by trap-assisted recombination at the grain boundaries.…”
Nanostructured titania is one of the most commonly encountered constituents of nanotechnology devices for use in energy-related applications, due to its intrinsic functional properties as a semiconductor and to other favorable characteristics such as ease of production, low toxicity and chemical stability, among others. Notwithstanding this diffusion, the quest for improved understanding of the physical and chemical mechanisms governing the material properties and thus its performance in devices is still active, as testified by the large number of dedicated papers that continue to be published. In this framework, we consider and analyze here the effects of the material morphology and structure in determining the energy transport phenomena as cross-cutting properties in some of the most important nanophase titania applications in the energy field, namely photovoltaic conversion, hydrogen generation by photoelectrochemical water splitting and thermal management by nanofluids. For these applications, charge transport, light transport (or propagation) and thermal transport are limiting factors for the attainable performances, whose dependence on the material structural properties is reviewed here on its own. This work aims to fill the gap existing among the many studies dealing with the separate applications in the hope of stimulating novel cross-fertilization approaches in this research field.
“…Renewable resources are produced in abundance on Earth, and include hydropower [ 71 , 72 ], wind power [ 73 ], and solar power [ 74 , 75 ]. However, harvesting these energies often requires large and complex infrastructures, which make it challenging to harness renewable energy sources in miniaturized and portable electronics.…”
Section: Cellulose-based Composites For Energy Conversionmentioning
The various forms of cellulose-based materials possess high mechanical and thermal stabilities, as well as three-dimensional open network structures with high aspect ratios capable of incorporating other materials to produce composites for a wide range of applications. Being the most prevalent natural biopolymer on the Earth, cellulose has been used as a renewable replacement for many plastic and metal substrates, in order to diminish pollutant residues in the environment. As a result, the design and development of green technological applications of cellulose and its derivatives has become a key principle of ecological sustainability. Recently, cellulose-based mesoporous structures, flexible thin films, fibers, and three-dimensional networks have been developed for use as substrates in which conductive materials can be loaded for a wide range of energy conversion and energy conservation applications. The present article provides an overview of the recent advancements in the preparation of cellulose-based composites synthesized by combining metal/semiconductor nanoparticles, organic polymers, and metal-organic frameworks with cellulose. To begin, a brief review of cellulosic materials is given, with emphasis on their properties and processing methods. Further sections focus on the integration of cellulose-based flexible substrates or three-dimensional structures into energy conversion devices, such as photovoltaic solar cells, triboelectric generators, piezoelectric generators, thermoelectric generators, as well as sensors. The review also highlights the uses of cellulose-based composites in the separators, electrolytes, binders, and electrodes of energy conservation devices such as lithium-ion batteries. Moreover, the use of cellulose-based electrodes in water splitting for hydrogen generation is discussed. In the final section, we propose the underlying challenges and outlook for the field of cellulose-based composite materials.
“…Up to now, only few reports have focused on optimizing the pore size of mesoscopic layers to improve the photovoltaic performance of the PSCs [73,74] and this strategy needs to be further explored. Naturally, methods to passivate the GBs and reduce trap densities there also represent a promising approach to reduce the V OC gap with the radiative limit.…”
Section: Outlining Promising Strategies To Improve the Pce Of Cpscsmentioning
Carbon‐based electrodes represent a promising approach to improve stability and up‐scalability of perovskite photovoltaics. The temperature at which these contacts are processed defines the absorber grain size of the perovskite solar cell: in cells with low‐temperature carbon‐based electrodes (L‐CPSCs), layer‐by‐layer deposition is possible, allowing perovskite crystals to be large (>100 nm), while in cells with high‐temperature carbon‐based contacts (H‐CPSCs), crystals are constrained to 10–20 nm in size. To enhance the power conversion efficiency of these devices, the main loss mechanisms are identified for both systems. Measurements of charge carrier lifetime, quasi‐Fermi level splitting (QFLS) and light‐intensity‐dependent behavior, supported by numerical simulations, clearly demonstrate that H‐CPSCs strongly suffer from non‐radiative losses in the perovskite absorber, primarily due to numerous grain boundaries. In contrast, large crystals of L‐CPSCs provide a long carrier lifetime (1.8 µs) and exceptionally high QFLS of 1.21 eV for an absorber bandgap of 1.6 eV. These favorable characteristics explain the remarkable open‐circuit voltage of over 1.1 V in hole‐selective layer‐free L‐CPSCs. However, the low photon absorption and poor charge transport in these cells limit their potential. Finally, effective strategies are provided to reduce non‐radiative losses in H‐CPSCs, transport losses in L‐CPSCs, and to improve photon management in both cell types.
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