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Mantis shrimp–inspired organic photodetector for simultaneous hyperspectral and polarimetric imagingnull (Ed.)Combining hyperspectral and polarimetric imaging provides a powerful sensing modality with broad applications from astronomy to biology. Existing methods rely on temporal data acquisition or snapshot imaging of spatially separated detectors. These approaches incur fundamental artifacts that degrade imaging performance. To overcome these limitations, we present a stomatopod-inspired sensor capable of snapshot hyperspectral and polarization sensing in a single pixel. The design consists of stacking polarization-sensitive organic photovoltaics (P-OPVs) and polymer retarders. Multiple spectral and polarization channels are obtained by exploiting the P-OPVs’ anisotropic response and the retarders’ dispersion. We show that the design can sense 15 spectral channels over a 350-nanometer bandwidth. A detector is also experimentally demonstrated, which simultaneously registers four spectral channels and three polarization channels. The sensor showcases the myriad degrees of freedom offered by organic semiconductors that are not available in inorganics and heralds a fundamentally unexplored route for simultaneous spectral and polarimetric imaging.more » « less
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Abstract Solid‐state lithium (Li) metal batteries (LMBs) have been developed as a promising replacement for conventional Li‐ion batteries due to their potential for higher energy. However, the current solid‐state electrolytes used in LMBs have limitations regarding mechanical and electrochemical properties and interfacial stability. Here, a fluorine (F)‐containing solid polymer electrolyte (SPE) having a bi‐continuous structure of F‐containing elastomers and plastic crystals is reported. The trifluoroethyl acrylate‐based SPE (T‐SPE) exhibits high ionic conductivity over 10−3 S cm−1, superior mechanical elasticity, and robust LiF‐rich interphases at both the Li metal anode and the LiNi0.83Mn0.06Co0.11O2cathode. Full cells with thin T‐SPEs and low negative/positive capacity ratios below 0.5 at the high‐operating voltage of 4.5 V demonstrate a high specific energy of 538 Wh kganode+cathode+electrolyte−1and maintain 393 Wh kg−1at a high specific power of 804 W kganode+cathode+electrolyte−1. The F‐containing phase‐separated SPE system provides a powerful strategy for achieving high‐energy and ‐power solid‐state LMBs.
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Abstract Traditional challenges of poor cycling stability and low Coulombic efficiency in Zinc (Zn) metal anodes have limited their practical application. To overcome these issues, this work introduces a single metal‐atom design featuring atomically dispersed single copper (Cu) atoms on 3D nitrogen (N) and oxygen (O) co‐doped porous carbon (CuNOC) as a highly reversible Zn host. The CuNOC structure provides highly active sites for initial Zn nucleation and further promotes uniform Zn deposition. The 3D porous architecture further mitigates the volume changes during the cycle with homogeneous Zn2+flux. Consequently, CuNOC demonstrates exceptional reversibility in Zn plating/stripping processes over 1000 cycles at 2 and 5 mA cm−2with a fixed capacity of 1 mAh cm−2, while achieving stable operation and low voltage hysteresis over 700 h at 5 mA cm−2and 5 mAh cm−2. Furthermore, density functional theory calculations show that co‐doping N and O on porous carbon with atomically dispersed single Cu atoms creates an efficient zincophilic site for stable Zn nucleation. A full cell with the CuNOC host anode and high loading V2O5cathode exhibits outstanding rate‐capability up to 5 A g−1and a stable cycle life over 400 cycles at 0.5 A g−1.
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Abstract The surging demand for environmental‐friendly and safe electrochemical energy storage systems has driven the development of aqueous zinc (Zn)‐ion batteries (ZIBs). However, metallic Zn anodes suffer from severe dendrite growth and large volume change, resulting in a limited lifetime for aqueous ZIB applications. Here, it is shown that 3D mesoporous carbon (MC) with controlled carbon and defect configurations can function as a highly reversible and dendrite‐free Zn host, enabling the stable operation of aqueous ZIBs. The MC host has a structure‐controlled architecture that contains optimal sp2‐carbon and defect sites, which results in an improved initial nucleation energy barrier and promotes uniform Zn deposition. As a consequence, the MC host shows outstanding Zn plating/stripping performance over 1000 cycles at 2 mA cm−2and over 250 cycles at 6 mA cm−2in asymmetric cells. Density functional theory calculations further reveal the role of the defective sp2‐carbon surface in Zn adsorption energy. Moreover, a full cell based on Zn@MC900 anode and V2O5cathode exhibits remarkable rate performance and cycling stability over 3500 cycles. These results establish a structure‐mechanism‐performance relationship of the carbon host as a highly reversible Zn anode for the reliable operation of ZIBs.
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Abstract Solid‐state lithium (Li)‐metal batteries (LMBs) are garnering attention as a next‐generation battery technology that can surpass conventional Li‐ion batteries in terms of energy density and operational safety under the condition that the issue of uncontrolled Li dendrite is resolved. In this study, various plastic crystal‐embedded elastomer electrolytes (PCEEs) are investigated with different phase‐separated structures, prepared by systematically adjusting the volume ratio of the phases, to elucidate the structure‐property‐electrochemical performance relationship of the PCEE in the LMBs. At an optimal volume ratio of elastomer phase to plastic‐crystal phase (i.e., 1:1), bicontinuous‐structured PCEE, consisting of efficient ion‐conducting, plastic‐crystal pathways with long‐range connectivity within a crosslinked elastomer matrix, exhibits exceptionally high ionic conductivity (≈10−3S cm−1) at 20 °C and excellent mechanical resilience (elongation at break ≈ 300%). A full cell featuring this optimized PCEE, a 35 µm thick Li anode, and a high loading LiNi0.83Mn0.06Co0.11O2(NMC‐83) cathode delivers a high energy density of 437 Wh kganode+cathode+electrolyte−1. The established structure–property–electrochemical performance relationship of the PCEE for solid‐state LMBs is expected to inform the development of the elastomeric electrolytes for various electrochemical energy systems.
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Abstract Sodium‐metal batteries (SMBs) are considered as a compliment to lithium‐metal batteries for next‐generation high‐energy batteries because of their low cost and the abundance of sodium (Na). Herein, a 3D nanostructured porous carbon particle containing carbon‐shell‐coated Fe nanoparticles (PC‐CFe) is employed as a highly reversible Na‐metal host. PC‐CFe has a unique 3D hierarchy based on sub‐micrometer‐sized carbon particles, ordered open channels, and evenly distributed carbon‐coated Fe nanoparticles (CFe) on the surface. PC‐CFe achieves high reversibility of Na plating/stripping processes over 500 cycles with a Coulombic efficiency of 99.6% at 10 mA cm–2with 10 mAh cm–2in Na//Cu asymmetric cells, as well as over 14 400 cycles at 60 mA cm–2in Na//Na symmetric cells. Density functional theory calculations reveal that the superior cycling performance of PC‐CFe stems from the stronger adsorption of Na on the surface of the CFe, providing initial nucleation sites more favorable to Na deposition. Moreover, the full cell with a PC‐CFe host without Na metal and a high‐loading Na3V2(PO4)3cathode (10 mg cm–2) maintains a high capacity of 103 mAh g–1at 1 mA cm–2even after 100 cycles, demonstrating the operation of anode‐free SMBs.
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Abstract The photophysical tuning is reported for a series of tetraphenylphosphonium (TPP) metal halide hybrids containing distinct metal halides, TPP2MX
n (MXn =SbCl5, MnCl4, ZnCl4, ZnCl2Br2, ZnBr4), from efficient phosphorescence to ultralong afterglow. The afterglow properties of TPP+cations could be suspended for the hybrids containing low band gap emissive metal halide species, such as SbCl52−and MnCl42−, but significantly enhanced for the hybrids containing wide band gap non‐emissive ZnCl42−. Structural and photophysical studies reveal that the enhanced afterglow is attributed to stronger π–π stacking and intermolecular electronic coupling between TPP+cations in TPP2ZnCl4than in the pristine organic ionic compound TPPCl. Moreover, the afterglow in TPP2ZnX4can be tuned by controlling the halide composition, with the change from Cl to Br resulting in a shorter afterglow due to the heavy atom effect. -
Abstract The photophysical tuning is reported for a series of tetraphenylphosphonium (TPP) metal halide hybrids containing distinct metal halides, TPP2MX
n (MXn =SbCl5, MnCl4, ZnCl4, ZnCl2Br2, ZnBr4), from efficient phosphorescence to ultralong afterglow. The afterglow properties of TPP+cations could be suspended for the hybrids containing low band gap emissive metal halide species, such as SbCl52−and MnCl42−, but significantly enhanced for the hybrids containing wide band gap non‐emissive ZnCl42−. Structural and photophysical studies reveal that the enhanced afterglow is attributed to stronger π–π stacking and intermolecular electronic coupling between TPP+cations in TPP2ZnCl4than in the pristine organic ionic compound TPPCl. Moreover, the afterglow in TPP2ZnX4can be tuned by controlling the halide composition, with the change from Cl to Br resulting in a shorter afterglow due to the heavy atom effect.