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The vacuum flash solution method has gained widespread recognition in the preparation of perovskite thin films, laying the foundation for the industrialization of perovskite solar cells. However, the low volatility of dimethyl sulfoxide and its weak interaction with formamidine-based perovskites significantly hinder the preparation of cell modules and the further improvement of photovoltaic performance. In this study, we describe an efficient and reproducible method for preparing large-scale, highly uniform formamidinium lead triiodide (FAPbI3) perovskite films. This is achieved by accelerating the vacuum flash rate and leveraging the complex synergism. Specifically, we designed a dual pump system to accelerate the depressurization rate of the vacuum system and compared the quality of perovskite film formed at different depressurization rates. Further, to overcome the limitations posed by DMSO, we substituted N-methylpyrrolidone as the ligand solvent, creating a stable intermediate complex phase. After annealing, it can be transformed into a uniform and pinhole-free FAPbI3 film. Due to the superior quality of these films, the large area perovskite solar module achieved a power conversion efficiency of 22.7% with an active area of 21.4 cm2. Additionally, it obtained an official certified efficiency of 22.1% with an aperture area of 22 cm2, and it demonstrated long-term stability.
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Antimony selenide (Sb2Se3) has sparked significant interest in high-efficiency photovoltaic applications due to its advantageous material and optoelectronic properties. In recent years, there has been considerable development in this area. Nonetheless, defects and suboptimal [hk0] crystal orientation expressively limit further device efficiency enhancement. This study used Zinc (Zn) to adjust the interfacial energy band and strengthen carrier transport. For the first time, it is discovered that the diffusion of Zn in the cadmium sulfide (CdS) buffer layer can affect the crystalline orientation of the Sb2Se3 thin films in the superstrate structure. The effect of Zn diffusion on the morphology of Sb2Se3 thin films with CdxZn1-xS buffer layer has been investigated in detail. Additionally, Zn doping promotes forming Sb2Se3 thin films with the desired [hk1] orientation, resulting in denser and larger grain sizes which will eventually regulate the defect density. Finally, based on the energy band structure and high-quality Sb2Se3 thin films, this study achieves a champion power conversion efficiency (PCE) of 8.76%, with a VOC of 458 mV, a JSC of 28.13 mA cm-2, and an FF of 67.85%. Overall, this study explores the growth mechanism of Sb2Se3 thin films, which can lead to further improvements in the efficiency of Sb2Se3 solar cells.
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Perovskite solar cells (PSCs) have shown great potential for reducing costs and improving power conversion efficiency (PCE). One effective method to achieve the latter is to use an all-inorganic charge transport layer (ICTL). However, traditional methods for crystallizing inorganic layers often result in the formation of a powder instead of a continuous film. To address this issue, we designed a dual-layer inorganic electron transport layer (IETL). This dual-layer structure consists of a layer of SnO2 nanocrystals (SnO2 NCs) deposited via a solution process and a dense SnO2 layer deposited through atomic layer deposition (ALD SnO2) to fill the cracks and gaps between the SnO2 NCs. PSCs having these dual-layer SnO2 ETLs achieved a high efficiency of 23.0%. This efficiency surpasses the recorded performance of ICTLs deposited on the perovskite. Furthermore, the PCE is comparable to that achieved with a C60 ETL. Moreover, the high-density structure of the ALD SnO2 layer inhibits the vertical migration of ions, resulting in improved thermal stability. After continuous heating at 85 °C in 10% humidity for 1000 h, the PCE of the dual-layer SnO2 structure decreased by 18%, whereas that of the C60/BCP structure decreased by 36%. The integration of dual-layer SnO2 into PSCs represents a significant advancement in achieving high-performance, commercially viable inverted monolithic PSCs or tandem solar cells.
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Efficiency reduction in perovskite solar cells (PSCs) during the magnification procedure significantly hampers commercialization. Vacuum-flash (VF) has emerged as a promising method to fabricate PSCs with consistent efficiency across scales. However, the slower solvent removal rate of VF compared to the anti-solvent method leads to perovskite films with buried defects. Thus, this work employs low-toxic Lewis base ligand solvent N-ethyl-2-pyrrolidone (NEP) to improve the nucleation process of perovskite films. NEP, with a mechanism similar to that of N-methyl-2-pyrrolidone in FA-based perovskite formation, enhances the solvent removal speed owing to its lower coordination ability. Based on this strategy, p-i-n PSCs with an optimized interface attain a power conversion efficiency (PCE) of 24.19% on an area of 0.08 cm2. The same nucleation process enables perovskite solar modules (PSMs) to achieve a certified PCE of 23.28% on an aperture area of 22.96 cm2, with a high geometric fill factor of 97%, ensuring nearly identical active area PCE (24%) in PSMs as in PSCs. This strategy highlights the potential of NEP as a ligand solvent choice for the commercialization of PSCs.
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Developing an additive to effectively regulate the perovskite crystallization kinetics for the optimized optoelectronic properties of perovskite film plays a vital role in obtaining high efficiency and stable perovskite solar cells (PSCs). Herein, a new additive is designed and directly synthesized in perovskite precursor solution by utilizing an addition reaction between but-3-yn-1-amine hydrochloride (BAH) and formamidinium iodide. It is found that its product may control the intermediate precursor phase for regulating perovskite nucleation, leading to advantageous 2D perovskite to induce growth of perovskite along the preferred [001] orientation with not only released lattice strain but also strong interaction with perovskite to passivate its surface defects. By taking advantage of the above synergistic effects, the optimized PSC delivers an efficiency of 25.19% and a high open-circuit voltage (VOC) of 1.22 V. Additionally, the devices demonstrate good stability, remaining over 90% of their initial efficiencies under ambient atmosphere conditions for 60 days, high temperature of 85 °C for 200 h, or maximum power point tracking for 500 h.
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0D Bi-based 329-type halide perovskite is demonstrated as a promising semiconductor for X-ray detection due to its strong X-ray absorption, superior stability, availability of large single crystals (SCs) and solution processibility at low temperature. However, its low mobility-lifetime product (µτ) limits its further improvement in detection sensitivity. Based on the first-principles calculations, this work designs a new 2D Bi-based 329-type halide perovskite using a mixed-halide-induced structural dimension regulation strategy. By using a continuous supply of a precursor solution, this work successfully grows inch-sized high-quality SCs. These SCs exhibit large µτ product, high resistivity, and low ion migration. The detectors fabricated using the SCs show X-ray detection sensitivity as high as 24,509 µC Gyair -1 cm-2, short response time of 315 µs, low detection limit of 4.3 nGy s-1, and superior stability. These properties are the best among all lead-free perovskite detectors and are comparable to those of the best lead-based perovskite detectors. The linear array detector assembled on the SCs for the first time also shows a high spatial resolution of 10.6 lp mm-1 during X-ray imaging. The high performance combined with superior stability of these new 329-type lead-free halide perovskite SCs is expected to promote a new generation of X-ray detection technologies.
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The creation of hierarchical nanostructures can effectively strengthen phonon scattering to reduce lattice thermal conductivity for improving thermoelectric properties in inorganic solids. Here, we use Zn doping to induce a remarkable reduction in the lattice thermal conductivity in SnTe, approaching the theoretical minimum limit. Microstructure analysis reveals that ZnTe nanoprecipitates can embed within SnTe grains beyond the solubility limit of Zn in the Zn alloyed SnTe. These nanoprecipitates result in a substantial decrease of the lattice thermal conductivity in SnTe, leading to an ultralow lattice thermal conductivity of 0.50â W m-1 K-1 at 773â K and a peak ZT of ~0.48 at 773â K, marking an approximately 45 % enhancement compared to pristine SnTe. This study underscores the effectiveness of incorporating ZnTe nanoprecipitates in boosting the thermoelectric performance of SnTe-based materials.
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Perovskite photovoltaics have emerged as the most promising candidates for next-generation light-to-electricity technology. However, their practical application still suffers from energy loss induced by intrinsic defects within the perovskite lattice. Here, a refined defect passivation in perovskite films is designed, which shows a multi-interaction mechanism between the perovskite and passivator. Interestingly, a shift of molecular bonding is observed upon cooling down the film, leading to a stronger passivation of iodine/formamidine vacancies. Such mechanism on device under low-light and low-temperature conditions is further leveraged and a record efficiency over 45% with durable ambient stability (T90 > 4000 h) is obtained. The pioneer application of perovskite solar cells in above dual extreme conditions in this work reveals the key principles of designing functional groups for the passivators, and also demonstrates the capability of perovskites for diverse terrestrial energy conversion applications in demanding environments such as polar regions and outer space.
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The heterogeneity of perovskite film crystallization along the vertical direction leads to voids and traps at the buried interfaces, hampering both efficiency and stability of perovskite solar cells. Here, bovine serum albumin-functionalized Au nanoclusters (ABSA), combined with heavy gravity, high surface charge density, and strong interactions with the electron transport layer, are designed to reconstruct the buried interfaces for not only high-quality crystallization, but also improved carrier transfer. The ABSA macromolecules with amine function groups and larger surface charge density interact with the perovskite to improve the crystallinity, and gradually migrate towards the buried interface, healing the defective voids, hence suppressing surface recombination velocity from 3075 to 452 cm s-1 . The healed buried interface and the higher surface potential of ABSA-modified TiO2 lead to improved carrier extraction at the interface. The resulting solar cell attains a power conversion efficiency of 25.0% with negligible hysteresis and remarkable stability, maintaining 92.9% of their initial efficiency after 3200 h of exposure to the ambient atmosphere, they also exhibit better continuous irradiation stability compared to control devices. These findings provide a new metal-protein complex to eliminate the deleterious voids and defects at the buried interface for improved photovoltaic performance and stability.
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Low-thermal-conductivity materials are ideal candidates for high-performance thermoelectric materials. CsAg5Te3 is a new metal-rich chalcogenide with an inherent low-thermal conductivity. However, due to its complex crystal structure, obtaining high-purity CsAg5Te3 poses a serious challenge. In addition, the high price of pure metals Cs, Ag, and Te leads to the high cost of traditional solid-state methods for preparing CsAg5Te3. To address these issues, the preparation of CsAg5Te3 with a nanostructured fiber morphology was carried out using a low-energy-intensity scalable microwave method. The CsAg5Te3 nanofibers were then assembled using spark plasma sintering technology to prepare CsAg5Te3 bulk with a layered structure. The lattice thermal conductivity of the CsAg5Te3 nanostructured material is 0.19 W m-1 K-1, which is almost the lowest among the state-of-the-art thermoelectric materials. Finally, at 673 K, the maximum zT value of CsAg5Te3 can reach â¼0.67. This study provides a feasible pathway for low-cost preparation of nanostructured thermoelectric materials.
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Reducing the interfacial defects between the perovskite/electron transport layer (ETL) is the key point to improving the efficient and stable performance of perovskite solar cells (PSCs). In this study, two self-assembled molecules ((aminomethyl)phosphonic acid and glycine) with different functional groups (phosphonic acid (-H2PO3) and carboxylic acid (-COOH)) were mixed to form the buried bottom interface of PSCs. The synergistic effect of -H2PO3 with its higher anchoring ability and -COOH with its fast carrier transport improved the performance of PSCs. Additionally, the SnO2 modified by mixed self-assembly molecules (M-SAM) showed a more appropriate energy level alignment, favoring charge transport and minimizing energy loss. In addition, the amine group (-NH2) on the two small molecules effectively interacted with uncoordinated Pb2+ in perovskite and improved the quality of the perovskite films. Consequently, the (FAPbI3)0.992(MAPbBr3)0.008 PSCs with M-SAM reached a PCE of 24.69% (0.08 cm2) and the perovskite modules achieved a champion efficiency of 18.57% (12.25 cm2 aperture area). Meanwhile, it still maintained more than 91% of its initial PCE after being placed in nitrogen atmosphere at 25 °C for 1500 h, which is better than that of the single-SAM and control devices. Further reference is provided for the future commercialization of perovskite with efficient and stable characteristics.
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The efficiency of antimony selenide (Sb2 Se3 ) solar cells is still limited by significant interface and deep-level defects, in addition to carrier recombination at the back contact surface. This paper investigates the use of lithium (Li) ions as dopant for Sb2 Se3 films, using lithium hydroxide (LiOH) as a dopant medium. Surprisingly, the LiOH solution not only reacts at the back surface of the Sb2 Se3 film but also penetrate inside the film along the (Sb4 Se6 )n molecular chain. First, the Li ions modify the grain boundary's carrier type and create an electric field between p-type grain interiors and n-type grain boundary. Second, a gradient band structure is formed along the vertical direction with the diffusion of Li ions. Third, carrier collection and transport are improved at the surface between Sb2 Se3 and the Au layer due to the reaction between the film and alkaline solution. Additionally, the diffusion of Li ions increases the crystallinity, orientation, surface evenness, and optical electricity. Ultimately, the efficiency of Sb2 Se3 solar cells is improved to 7.57% due to the enhanced carrier extraction, transport, and collection, as well as the reduction of carrier recombination and deep defect density. This efficiency is also a record for CdS/Sb2 Se3 solar cells fabricated by rapid thermal evaporation.
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The disordered transformation of the ordered aligned polar liquid crystal molecules in liquid crystal elastomers (LCEs) under the influence of an external field imbues them with the unique property of thermally reversible shape memory, making them highly valuable for various applications, particularly in actuators. In this study, we examined the high dielectric constant exhibited by the orientation polarization of polar liquid crystal molecules in RM257-LCE films, which holds significant potential for developing flexible capacitive sensors. By manipulating the flexibility of the molecular chain network and introducing hydrogen bonds and metal ions into the main chain, we were able to enhance the relative dielectric constant of LCEs to an impressive value of 62 (at 100 Hz), which is approximately 23 times higher than for polydimethylsiloxane (PDMS). This elevated dielectric constant displays a noteworthy positive temperature coefficient within a specific temperature range, starting from room temperature and extending to the clearing point. Using this property, we fabricated highly sensitive capacitive, flexible temperature sensors. Moreover, we successfully engineered a flexible pressure sensor with an excellent pressure-sensing range of 0-2 MPa by combining the porous structure of the prepared LCEs with mushroom electrodes. Additionally, the sensor showcases a remarkable capacitance recovery time of 0.8 s at 90 °C. These outstanding features collectively contribute to the excellent pressure-sensing characteristics of our sensor. The findings of this study offer valuable insights and serve as a reference for the design of innovative flexible sensors, enabling advancements in sensor technology.
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Monodomain liquid crystal elastomers (m-LCEs) exhibit large reversible deformations when subjected to light and heat stimuli. Herein, we developed a new method for the large-scale continuous preparation of m-LCE fibers. These m-LCE fibers exhibit a reversible contraction ratio of 55.6%, breaking strength of 162 MPa (withstanding a load of 1 million times its weight), and maximum output power density of 1250 J/kg, surpassing those of previously reported m-LCEs. These excellent mechanical properties are mainly attributed to the formation of a homogeneous molecular network. Furthermore, the fabrication of m-LCEs with permanent plasticity using m-LCEs with impermanent instability without external intervention was realized by the synergistic effects of the self-restraint of mesogens and the prolonged relaxation process of LCEs. The designed LCE fibers, which are similar to biological muscle fibers and can be easily integrated, exhibit broad application prospects in artificial muscles, soft robots, and micromechanical systems.
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Hole-transport materials (HTMs) play an important role in perovskite solar cells (PSCs) to enhance the power conversion efficiency (PCE). The innovation of HTMs can increase the hole extraction ability and reduce interfacial recombination. Three organic small molecule HTMs with 4H-cyclopenta[2,1-b:3,4-b']dithiophene (CPDT) as the central unit was designed and synthesized, namely, CPDTE-MTP (with the 2-ethylhexyl substituent and diphenylamine derivative end-group), CPDT-MTP (with the hexyl substituent and diphenylamine derivative end-group), and CPDT-PMTP (with the hexyl substituent and triphenylamine derivative end-group), which can form bifunctional and robust hole transport layer (HTL) on ITO and is tolerable to subsequent solvent and thermal processing. The X-ray photoelectron spectroscopy (XPS) results proved that CPDT-based HTMs can both interact with ITO through the nitrogen element in them and the tin element in ITO and passivate the upper perovskite layer. It is worth noting that the champion efficiency of MAPbI3 PSCs based on CPDT-PMTP achieved 20.77%, with an open circuit voltage (VOC) of 1.10 V, a short-circuit current (JSC) of 23.39 mA cm-2, and a fill factor (FF) of 80.83%, as three new materials were introduced into p-i-n PSCs as dopant-free HTMs.
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Monodomain liquid crystal elastomers (mLCEs) are flexible and biocompatible smart materials that show unique behaviors of soft elasticity, anisotropy, and reversible shape changes above the nematic-isotropic transition temperature. Therefore, it has great potential for application in wearable devices and biologically. However, most of the reported mLCEs have nematic-isotropic transition temperature (TNI) higher than 60 °C; and above this TNI, the tensile strength of the mLCEs decreases by orders of magnitude. These issues have received little attention, limiting their application in humans. Herein, the TNI of mLCEs was reduced from 78.4 °C to 23.5 °C by substituting part of the rigid LC mesogens with a flexible backbone. The physical entanglement of hydrogen bonds between molecular chains alleviated the molecular chain slip caused by the long flexible backbone. The tensile strength remained constant during the phase transformation. Furthermore, dynamic disulfide bonds were used to modify the LC polymer network, imparting it with excellent antimicrobial, programmable, and self-healing properties. To realize its application in the closure of skin wounds, a porous PHG-mLCE/hydrogel patch that was breathable and waterproof was designed to increase skin adhesion (262 N/m).
Asunto(s)
Elastómeros , Cristales Líquidos , Humanos , Elastómeros/química , Cristales Líquidos/química , Polímeros/química , Elasticidad , Antibacterianos/farmacología , Materiales Biocompatibles/farmacologíaRESUMEN
MXene film electrodes for supercapacitors, assembled with MXene nanosheets as structure units, inevitably suffer from self-restacking, which severely restrains ion transport kinetics and results in insufficient active site utilization and poor rate capability. Herein, an in situ foaming strategy employing the accumulated gas generated during the etching of sacrificial templates, combined with the confinement between the MXene film, has been proposed to fabricate pores between stacked MXene sheets and along the vertical direction of the film. The surface chemistry of the foamed film was further modified by alkali washing treatment to replace hydrophobic -F groups with hydrophilic -OH groups to improve electrolyte penetration and introduce more active sites. The resultant porous MXene film electrode exhibits a greatly improved specific capacitance (354.1 F g-1 at 5 mV s-1) and unparalleled rate capability (with a capacitance retention of 96.1% at 2000 mV s-1). This work demonstrates a facile but efficient method for the construction of porous MXene films, simultaneously providing insights into the promising applications of MXenes.
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Correction for 'Enhanced energy harvester performance by a tension annealed carbon nanotube yarn at extreme temperatures' by Xinghao Hu et al., Nanoscale, 2022, 14, 16185-16192, https://doi.org/10.1039/D2NR05303A.
RESUMEN
The main feature of perovskite solar cells (PSCs) is that the perovskite layer can be fabricated by the solution method, while the long-time stability of the precursor solution is critical. During the fabrication of formamidinium (FA)-based PSCs, the introduction of methylammonium cations (MA+) in the precursor solution can accelerate the crystallization process of the perovskite layer, stabilize the perovskite structure, and passivate defects. However, MA+ is easy to deprotonate to generate MA molecules, and it then condensates with formamidinium iodide (FAI) to form adverse byproducts. Herein, perovskite microcrystals (MCs) for preparing perovskite precursor solution were investigated in details, which can improve the long-term stability of the precursor solution and the perovskite film. We found that FA+ in MC solution was confined in the three-dimensional scaffold, preventing it from reacting with MA+. Meanwhile, MCs can effectively promote nucleation to form large grains in perovskite films. The photoelectric conversion efficiency (PCE) of the device with 3 week-aged MC solution remains at 90% and is only reduced by 10% after 160 h of continuous operation, which far exceeds the performance of the PCE of those based on mixed monomer powder (MP) solution. Therefore, perovskite MCs, an effective reactive inhibitor to improve the stability of perovskite precursor solutions, are of great significance for large-scale commercial fabrication.
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Carbon nanotube (CNT) yarns generate electrical energy when they were stretched in an electrolyte, and they have been exploited for diverse applications such as self-powered sensors and human health monitoring systems. Here we improved the capacitance change and harvester performance of a coiled CNT yarn by using an incandescent tension annealing process (ITAP). When undergoing stretching cycles at 1 Hz, a coiled ITAP yarn can produce 2.5 times peak electrical power and 1.6 times output voltage than that of a neat CNT yarn. Electrochemical analysis shows that the capacitance of the ITAP yarn decreased by 20.4% when it was stretched to 30% strain. Microstructure results demonstrate that the large capacitance change may result from the densified electrochemical surface by the ITAP. Moreover, the potential of the zero charge (PZC) of ITAP yarns was shifted to a more negative value than that of the neat CNT yarn, which means that more charges were injected into the ITAP yarn once it was immersed in an electrolyte. Thus, the large capacitance change and initial injected charge are two main reasons for enhancing the harvester performance of the ITAP yarn. In addition, by annealing a twisted CNT yarn before it was coiled, we further increased the output peak power density to 170 W kg-1 at a strain of 55%.