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221.
We consider an ensemble of three-level configuration atoms in an optical cavity, interacting through two-photon transitions with a cavity mode, driven by a broad-band squeezed input of finite amplitude. The atom-cavity system is coupled to reservoirs to describe the losses of the atoms and the cavity. Optical spectra in the transmitted and the reflected field are calculated and analysed in the good cavity limit, for the purely absorptive resonant case and the general case, respectively.  相似文献   
222.
Organic redox-active materials are promising electrode candidates for lithium-ion batteries by virtue of their designable structure and cost-effectiveness. However, their poor electrical conductivity and high solubility in organic electrolytes limit the device's performance and practical applications. Herein, the π-conjugated nitrogen-containing heteroaromatic molecule hexaazatriphenylene (HATN) is strategically embedded with redox-active centers in the skeleton of a Cu-based 2D conductive metal–organic framework (2D c-MOF) to optimize the lithium (Li) storage performance of organic electrodes, which delivers improved specific capacity (763 mAh g−1 at 300 mA g−1), long-term cycling stability (≈90% capacity retention after 600 cycles at 300 mA g−1), and excellent rate performance. The correlation of experimental and computational results confirms that this high Li storage performance derives from the maximum number of active sites (CN sites in the HATN unit and CO sites in the CuO4 unit), favorable electrical conductivity, and efficient mass transfer channels. This strategy of integrating multiple redox-active moieties into the 2D c-MOF opens up a new avenue for the design of high-performance electrode materials.  相似文献   
223.
Perovskite light-emitting diodes (PeLEDs) show promising prospects in the wide color gamut display owing to their ultra-narrow full width at half maximum (FWHM). However, up to now, all perovskite white LEDs integrated by standard red, green, and blue perovskite emitters, namely, monolithic white PeLEDs (WPeLEDs), have been rarely reported, owing to facing some issues, e.g., solvent incompatibility in solution technique, ion exchange, and energy transfer between different emission centers. Herein, centered on these issues, an optimal intermediate connection layer (ICL) of Po-T2T/LiF/Ag/HAT-CN/MoO3 is adopted to successfully develop monolithic tandem multicolor PeLEDs and WPeLEDs for the first time. The multicolor PeLEDs can achieve the best external quantum efficiency of 1.8% and the highest luminance of 4844 cd m−2. Besides, the red/green/blue (R/G/B) monolithic tandem WPeLED shows a standard white International Commission on Illumination coordinate of (0.33, 0.33) and achieves an extremely wide color gamut reaching  National Television Standards Committee of 130%. This study is the first to realize the standard R/G/B co-electroluminescence in a monolithic perovskite device and offers a feasible strategy for developing wide-color gamut perovskite displays.  相似文献   
224.
MXene materials emerge as promising candidates for energy harvesting and storage application. In this study, the effect of the surface chemistry on the work function of MXenes, which determines the performance of MXene-based triboelectric nanogenerator (TENG), is elucidated. First-principles calculations reveal that the surface functional group greatly influences MXene work function:  OH termination reduces the work function with respect to that of bare surface, while  F and  Cl increase it. Then, work functions are experimentally determined by Kelvin probe force microscopy. The MXene prepared by gentle etching at 40 °C for 48 h (GE40/48) has the largest work function. Furthermore, an electron-cloud potential-well model is established to explain the mechanism of electron emission-dominated charge transfer and assemble a triboelectric device to verify experimentally its conclusions. It is found that GE40/48 has the best performance with a 281 V open-circuit voltage, 9.7 µA short-current current, and storing 1.019 µC of charge, which is consistent with the model. Last, a patterned TENG is demonstrated for self-powered human–machine interaction application. This finding enhances the understanding of the inherent mechanism between the surface structure and the output performance of MXene-based TENG, which can be applied to other TENG based on 2D materials.  相似文献   
225.
Electrocatalytic hydrogenation (ECH) is a burgeoning strategy for the sustainable utilization of hydrogen. However, how to effectively suppress the competitive hydrogen evolution reaction (HER) is a big challenge to ECH catalysis. In this study, amine (NH2 R)-coordinated Pd nanoparticles loaded on carbon felt (Pd@CF) as a catalyst is successfully synthesized by a one-step solvothermal reduction method using oleylamine as the reducing agent. An exceptional ECH reactivity on benzaldehyde is achieved on the optimal Pd@CF catalyst in terms of a high conversion (89.7%) and selectivity toward benzyl alcohol (89.8%) at −0.4 V in 60 min. Notably, the Faradaic efficiency for producing benzyl alcohol is up to 90.2%, much higher than that catalyzed by Pd@CF-without N-group (41.1%) and thecommercial Pd/C (20.9%). The excellent ECH performance of Pd@CF can be attributed to the enriched electrons on Pd surface resulted from the introduction of NH2 R groups, which strengthens both the adsorption of benzaldehyde and the adsorbed hydrogen (Hads) on Pd, preventing the combination of Hads to form H2, that is, inhibiting the HER. This study gives a new insight into design principles of highly efficient electrocatalysts for the hydrogenation of unsaturated aldehydes molecules.  相似文献   
226.
Despite the outstanding power conversion efficiency (PCE) of perovskite solar cells (PSCs) achieved over the years, unsatisfactory stability and lead toxicity remain obstacles that limit their competitiveness and large-scale practical deployment. In this study, in situ polymerizing internal encapsulation (IPIE) is developed as a holistic approach to overcome these challenges. The uniform polymer internal package layer constructed by thermally triggered cross-linkable monomers not only solidifies the ionic perovskite crystalline by strong electron-withdrawing/donating chemical sites, but also acts as a water penetration and ion migration barrier to prolong shelf life under harsh environments. The optimized MAPbI3 and FAPbI3 devices with IPIE treatment yield impressive efficiencies of 22.29% and 24.12%, respectively, accompanied by remarkably enhanced environmental and mechanical stabilities. In addition, toxic water-soluble lead leakage is minimized by the synergetic effect of the physical encapsulation wall and chemical chelation conferred by the IPIE. Hence, this strategy provides a feasible route for preparing efficient, stable, and eco-friendly PSCs.  相似文献   
227.
Metal nanoclusters (MNCs) are compositionally well-defined and also structurally precise materials with unique molecule-like properties and discrete electronic energy levels. Atomically precise ligand-protected Cu nanoclusters (LP-CuNCs) are one category of typical MNCs that usually demonstrate unique geometric and electronic structures to serve as electrocatalysts. However, the synthesis, application, as well as structure-performance relationship of LP-CuNCs are not adequately studied. Significantly, the ligands are essential to the geometric structure, crystal structure, size, and electronic structure of LP-CuNCs, which determine their physiochemical properties and applications. In this review, significant progress in the ligand design of LP-CuNCs, and their application in electrocatalytic reactions is introduced. The general basics of ligand-protected MNCs (LP-MNCs) are first introduced and the functions of ligands are emphasized. Subsequently, a series of different ligands for LP-CuNCs including thiolates, phosphines, alkynyl, polymers, and biomolecules are highlighted. Thereafter, their applications in different electrocatalytic reactions are discussed. It is believed that this review will not only inspire the design and synthesis of novel LP-CuNCs, but also contribute to the extension of their applications in electrocatalytic reactions and the establishment of accurate structure-performance relationships.  相似文献   
228.
Precise adjustment of the pore size, damage repair, and efficient cleaning is all challenges for the wider application of inorganic membranes. This study reports a simple strategy of combining dry-wet spinning and electrosynthesis to fabricate stainless-steel metal–organic framework composite membranes characterized by customizable pore sizes, targeted reparability, and high catalytic activity for membrane cleaning. The membrane pore size can be precisely customized in the range of 14–212 nm at nanoscale, and damaged membranes can be repaired by targeted treatment in 120 s. In addition, advanced oxidation processes can be used to quickly clean the membrane and achieve 98% flux recovery. The synergistic actions of the membrane matrix and the selective layer increase the adsorption energy of active sites to oxidant, shorten the electron transfer cycle, and enhance the overall catalytic performance. This study can provide a new direction for the development of advanced membranes for water purification and high-efficiency membrane cleaning methods.  相似文献   
229.
Smart textiles with good mechanical adaptability play an important role in personal protection, health monitoring, and aerospace applications. However, most of the reported thermally responsive polymers has long response time and poor processability, comfort, and wearability. Skin-core structures of thermally responsive fibers with multiple commercial fiber cores and temperature-responsive hydrogel skins are designed and fabricated, which exhibit rapid mechanical adaptability, good thermohardening, and thermal insulation. This universal method enables tight bonding between various commercial fiber cores and hydrogel skins via specific covalently anchored networks. At room temperature, prepared fibers show softness, flexibility, and skin compatibility similar to those of ordinary fibers. As temperature rises, smart fibers become hard, rigid, and self-supporting. The modulus of hydrogel skin increases from 304% to 30883%, showing good mechanoadaptability and impact resistance owing to the synergy between hydrophobic interactions and ionic bonding. Moreover, this synergistic effect leads to an increase in heat absorption, and fibers exhibit good thermal insulation, which reduces the contact temperature of the body surface by ≈25 °C under the external temperature of 95 °C, effectively preventing thermal burns. Notably, the active mechanoadaptability of these smart fibers using conductive fibers as cores is demonstrated. This study provides feasibility for fabricating environmentally adaptive intelligent textiles.  相似文献   
230.
Following logic in the silicon semiconductor industry, the existence of native oxide and suitable fabrication technology is essential for 2D semiconductors in planar integronics, which are surface-sensitive to typical coating technologies. To date, very few types of integronics are found to possess this feature. Herein, the 2D Bi2O2Te developed recently is reported to possess large-area synthesis and controllable thermal oxidation behavior toward single-crystal native oxides. This shows that surface-adsorbed oxygen atoms are inclined to penetrate across [Bi2O2]n2n+ layers and bond with the underlying [Te]n2n− at elevated temperatures, transforming directly into [TeO4]n2n− with the basic architecture remaining stable. The oxide can be adjusted to form in an accurate layer-by-layer manner with a low-stress sharp interface. The native oxide Bi2TeO6 layer (bandgap of ≈2.9 eV) exhibits visible-light transparency and is compatible with wet-chemical selective etching technology. These advances demonstrate the potential of Bi2O2Te in planar-integrated functional nanoelectronics such as tunnel junction devices, field-effect transistors, and memristors.  相似文献   
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