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991.
Organic–inorganic formamidinium lead triiodide (FAPbI3) hybrid perovskite quantum dot (QD) is of great interest to photovoltaic (PV) community due to its narrow band gap, higher ambient stability, and long carrier lifetime. However, the surface ligand management of FAPbI3 QD is still a key hurdle that impedes the design of high-efficiency solar cells. Herein, this study first develops a solution-mediated ligand exchange (SMLE) for preparing FAPbI3 QD film with enhanced electronic coupling. By dissolving optimal methylammonium iodide (MAI) into antisolvent to treat the FAPbI3 QD solution, the SMLE can not only effectively replace the long-chain ligands, but also passivate the A- and X-site vacancies. By combining experimental and theoretical results, this study demonstrates that the SMLE engineered FAPbI3 QD exhibits lower defect density, which is beneficial for fabricating high-quality QD arrays with desired morphology and carrier transport. Consequently, the SMLE FAPbI3 QD based solar cell outputs a champion efficiency of 15.10% together with improved long-term ambient storage stability, which is currently the highest reported value for hybrid perovskite QD solar cells. These results would provide new design principle of hybrid perovskite QDs toward high-performance optoelectronic application.  相似文献   
992.
Photodynamic therapy (PDT) as a non-invasive strategy shows high promise in cancer treatment. However, owing to the hypoxic tumor microenvironment and light irradiation-mediated rapid electron–hole pair recombination, the therapeutic efficacy of PDT is dramatically discounted by limited reactive oxygen species (ROS) generation. Herein, a multifunctional theranostic nanoheterojunction is rationally developed, in which 2D niobium carbide (Nb2C) MXene is in situ grown with barium titanate (BTO) to generate a robust photo-pyroelectric catalyst, termed as BTO@Nb2C nanosheets, for enhanced ROS production, originating from the effective electron–hole pair separation induced by the pyroelectric effect. Under the second near-infrared (NIR-II) laser irradiation, Nb2C MXene core-mediated photonic hyperthermia regulates temperature variation around BTO shells facilitating the electron–hole spatial separation, which reacts with the surrounding O2 and H2O molecules to yield toxic ROS, achieving a synergetic effect by means of combinaterial photothermal therapy with pyrocatalytic therapy. Correspondingly, the engineered BTO@Nb2C composite nanosheets feature benign biocompatibility and high antitumor efficiency with the tumor-inhibition rate of 94.9% in vivo, which can be applied as an imaging-guided real-time non-invasive synergetic dual-mode therapeutic nanomedicine for efficient tumor nanotherapy.  相似文献   
993.
Polydimethylsiloxanes (PDMS) foam as one of next-generation polymer foam materials shows poor surface adhesion and limited functionality, which greatly restricts its potential applications. Fabrication of advanced PDMS foam materials with multiple functionalities remains a critical challenge. In this study, unprecedented self-adhesive PDMS foam materials are reported with worm-like rough structure and reactive groups for fabricating multifunctional PDMS foam nanocomposites decorated with MXene/cellulose nanofiber (MXene/CNF) interconnected network by a facile silicone foaming and dip-coating strategy followed by silane surface modification. Interestingly, such self-adhesive PDMS foam produces strong interfacial adhesion with the hybrid MXene/CNF nano-coatings. Consequently, the optimized PDMS foam nanocomposites have excellent surface super-hydrophobicity (water contact angle of ≈159o), tunable electrical conductivity (from 10−8 to 10 S m−1), stable compressive cyclic reliability in both wide-temperature range (from −20 to 200 oC) and complex environments (acid, sodium, and alkali conditions), outstanding flame resistance (LOI value of >27% and low smoke production rate), good thermal insulating performance and reliable strain sensing in various stress modes and complex environmental conditions. It provides a new route for the rational design and development of advanced PDMS foam nanocomposites with versatile multifunctionalities for various promising applications such as intelligent healthcare monitoring and fire-safe thermal insulation.  相似文献   
994.
Photocatalytic selective oxidation of 5-hydroxymethylfurfural (HMF) coupled H2 production offers a promising approach to producing valuable chemicals. Herein, an efficient in situ topological transformation tactic is developed for producing porous O-doped ZnIn2S4 nanosheets for HMF oxidation cooperative with H2 evolution. Aberration-corrected high-angle annular dark-field scanning TEM images show that the hierarchical porous O-ZIS-120 possesses abundant atomic scale edge steps and lattice defects, which is beneficial for electron accumulation and molecule adsorption. The optimal catalyst (O-ZIS-120) exhibits remarkable performance with 2,5-diformylfuran (DFF) yields of 1624 µmol h−1 g−1 and the selectivity of >97%, simultaneously with the H2 evolution rate of 1522 µmol h−1 g−1. Mechanistic investigations through theoretical calculations show that O in the O-ZIS-120 lattice can reduce the oxidation energy barrier of hydroxyl groups of HMF. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) results reveal that DFF* (C4H2(CHO)2O*) intermediate has a weak interaction with O-ZIS-120 and desorb as the final product. This study elucidates the topotactic structural transitions of 2D materials simultaneously with electronic structure modulation for efficient photocatalytic DFF production.  相似文献   
995.
The development of high-performance (K,Na)NbO3 (KNN)-based lead-free piezoceramics for next-generation electronic devices is crucial for achieving environmentally sustainable society. However, despite recent improvements in piezoelectric coefficients, correlating their properties to underlying multiscale structures remains a key issue for high-performance KNN-based ceramics with complex phase boundaries. Here, this study proposes a medium-entropy strategy to design “local polymorphic distortion” in conjunction with the construction of uniformly oversize grains in the newly developed KNN solid-solution, resulting in a novel large-size hierarchical domain architecture (≈0.7 µm wide). Such a structure not only facilitates polarization rotation but also ensures a large residual polarization, which significantly improves the piezoelectricity (≈3.2 times) and obtains a giant energy harvesting performance (Wout = 2.44 mW, PD = 35.32 µW mm−3, outperforming most lead-free piezoceramics). This study confirms the coexistence of multiphase through the atomic-resolution polarization features and analyzes the domain/phase transition mechanisms using in situ electric field structural characterizations, revealing that the electric field induces highly effective multiscale polarization configuration transitions based on T–O–R sequential phase transitions. This study demonstrates a new strategy for designing high-performance piezoceramics and facilitates the development of lead-free piezoceramic materials in energy harvesting applications.  相似文献   
996.
MXene aerogels have shown great potential for many important functional applications, in particular electromagnetic interference (EMI) shielding. However, it has been a grand challenge to create mechanically hyperelastic, air-stable, and durable MXene aerogels for enabling effective EMI protection at low concentrations due to the difficulties in achieving tailorable porous structures, excellent mechanical elasticity, and desired antioxidation capabilities of MXene in air. Here, a facile strategy for fabricating MXene composite aerogels by co-assembling MXene and cellulose nanofibers during freeze-drying followed by surface encapsulation with fire-retardant thermoplastic polyurethane (TPU) is reported. Because of the maximum utilization of pore structures of MXene, and conductive loss enhanced by multiple internal reflections, as-prepared aerogel with 3.14 wt% of MXene exhibits an exceptionally high EMI shielding effectiveness of 93.5 dB, and an ultra-high MXene utilization efficiency of 2977.71 dB g g−1, tripling the values in previous works. Owing to the presence of multiple hydrogen bonding and the TPU elastomer, the aerogel exhibits a hyperelastic feature with additional strength, excellent stability, superior durability, and high fire safety. This study provides a facile strategy for creating multifunctional aerogels with great potential for applications in EMI protection, wearable devices, thermal management, pressure sensing, and intelligent fire monitoring.  相似文献   
997.
Underwater optical communication (UOC) has attracted considerable interest in the continuous expansion of human activities in marine/ocean environments. The water-durable and self-powered photoelectrodes that act as a battery-free light receiver in UOC are particularly crucial, as they may directly face complex underwater conditions. Emerging photoelectrochemical (PEC)-type photodetectors are appealing owing to their intrinsic aqueous operation characteristics with versatile tunability of photoresponses. Herein, a self-powered PEC photodetector employing n-type gallium nitride (GaN) nanowires as a photoelectrode, which is decorated with an iridium oxide (IrOx) layer to optimize charge transfer dynamics at the GaN/electrolyte interface, is reported. Strikingly, the constructed n-GaN/IrOx photoelectrode breaks the responsivity-bandwidth trade-off limit by simultaneously improving the response speed and responsivity, delivering an ultrafast response speed with response/recovery times of only 2 µs/4 µs while achieving a high responsivity of 110.1 mA W−1. Importantly, the device exhibits a large bandwidth with 3 dB cutoff frequency exceeding 100 kHz in UOC tests, which is one of the highest values among self-powered photodetectors employed in optical communication system.  相似文献   
998.
Solar steam generation (SSG) through hydrogel-based evaporators has shown great promise for freshwater production. However, developing hydrogel-based evaporators with stable SSG performance in high-salinity brines remains challenging. Herein, phase-separated polyzwitterionic hydrogel-based evaporators are presented with sponge-like structures comprising interconnected pores for stable SSG performance, which are fabricated by photopolymerization of sulfobetaine methacrylate (SBMA) in water-dimethyl sulfoxide (DMSO) mixed solvents. It is shown that driven by competitive adsorption, the structures of the resulting poly(sulfobetaine methacrylate) (PSBMA) hydrogels can be readily tuned by the volume ratio of DMSO to achieve phase separation. The optimized phase-separated PSBMA hydrogels, combining the unique anti-polyelectrolyte effects of polyzwitterionic hydrogels, demonstrate a rapid water transport capability in brines. After introducing photothermal polypyrrole particles on the surface of the phase-separated PSBMA hydrogel evaporators, a stable water evaporation rate of ≈2.024 kg m−2 h−1 and high solar-to-vapor efficiency of ≈97.5% in a 3.5 wt.% brine are obtained under simulated solar light irradiation (1.0 kW m−2). Surprisingly, the evaporation rates remain stable even under high-intensity solar irradiation (2.0 kW m−2). It is anticipated that the polyzwitterionic hydrogel evaporators with sponge-like porous structures will contribute to developing SSG technology for high-salinity seawater applications.  相似文献   
999.
Li-rich layered oxides (LLOs) have been considered as the most promising cathode materials for achieving high energy density Li-ion batteries. However, they suffer from continuous voltage decay during cycling, which seriously shortens the lifespan of the battery in practical applications. This review comprehensively elaborates and summarizes the state-of-the-art of the research in this field. It is started from the proposed mechanism of voltage decay that refers to the phase transition, microscopic defects, and oxygen redox or release. Furthermore, several strategies to mitigate the voltage decay of LLOs from different scales, such as surface modification, elemental doping, regulation of components, control of defect, and morphology design are summarized. Finally, a systematic outlook on the real root of voltage decay is provided, and more importantly, a potential solution to voltage recovery from electrochemistry. Based on this progress, some effective strategies with multiple scales will be feasible to create the conditions for their commercialization in the future.  相似文献   
1000.
Methanol steam reforming (MSR) is viewed as an important technology in the growth of a future hydrogen economy, with methanol serving as an easily transportable and storable liquid hydrogen carrier. However, the thermocatalytic MSR reaction is energy intensive as it requires high temperatures. Herein, a novel L-Cu catalyst is successfully fabricated for photo-driven MSR through reduction of CuAl layered double hydroxide (CuAl-LDH) nanosheets. L-Cu offers outstanding activity for the photothermal conversion of methanol and water to hydrogen (160.5 µmol gcat−1 s−1) under ultraviolet-visible irradiation, with this rate being much higher than that achieved for L-Cu at the same temperature in the dark. Characterization studies using X-ray diffraction, X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and high-resolution transmission electron microscopy determine that L-Cu catalyst comprise Cu nanoparticles on an amorphous alumina support. Computational calculations reveale that Cu localized surface plasmon resonance effects promote the activation of H2O, thereby underpinning the remarkable hydrogen production rates achieved during photo-driven MSR. This study introduces a novel photothermal strategy for hydrogen generation from methanol, demonstrating the enormous potential of photothermal catalysis in the chemical and energy sectors.  相似文献   
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