LiFePO4 Particles Embedded in Fast Bifunctional Conductor rGO&C@Li3V2(PO4)3 Nanosheets as Cathodes for High‐Performance Li‐Ion Hybrid Capacitors

The sluggish kinetics of Faradaic reactions in bulk electrodes is a significant obstacle to achieve high energy and power density in energy storage devices. Herein, a composite of LiFePO₄ particles trapped in fast bifunctional conductor rGO&C@Li₃V₂(PO₄)₃ nanosheets is prepared through an in situ competitive redox reaction. The composite exhibits extraordinary rate capability (71 mAh g^?1 at 15 A g^?1) and remarkable cycling stability (0.03% decay per cycle over 1000 cycles at 10 A g^?1). Improved extrinsic pseudocapacitive contribution is the origin of fast kinetics, which endows this composite with high energy and power density, since the unique 2D nanosheets and embedded ultrafine LiFePO₄ nanoparticles can shorten the ion and electron diffusion length. Even applied to Li‐ion hybrid capacitors, the obtained devices still achieve high power density of 3.36 kW kg^?1 along with high energy density up to 77.8 Wh kg^?1. Density functional theory computations also validate that the remarkable rate performance is facilitated by the desirable ionic and electronic conductivity of the composite.     

Combustion Synthesized Zinc Oxide Electron‐Transport Layers for Efficient and Stable Perovskite Solar Cells

Perovskite solar cells (PSCs) have advanced rapidly with power conversion efficiencies (PCEs) now exceeding 22%. Due to the long diffusion lengths of charge carriers in the photoactive layer, a PSC device architecture comprising an electron‐ transporting layer (ETL) is essential to optimize charge flow and collection for maximum performance. Here, a novel approach is reported to low temperature, solution‐processed ZnO ETLs for PSCs using combustion synthesis. Due to the intrinsic passivation effects, high crystallinity, matched energy levels, ideal surface topography, and good chemical compatibility with the perovskite layer, this combustion‐derived ZnO enables PCEs approaching 17–20% for three types of perovskite materials systems with no need for ETL doping or surface functionalization.     

Creating an Air‐Stable Sulfur‐Doped Black Phosphorus‐TiO2 Composite as High‐Performance Anode Material for Sodium‐Ion Storage

With the increasing demand for low cost, long lifetime, high energy density storage systems, an extensive amount of effort has recently been focused on the development of sodium‐ion batteries (SIBs), and a variety of cathode materials have been discovered. However, looking for the most suitable anode material for practical application is a major challenge for SIBs. Herein, a high capacity sulfur‐doped black phosphorus‐TiO₂ (TiO₂‐BP‐S) anode material for SIBs is first synthesized by a feasible and large‐scale high‐energy ball‐milling approach, and its stability in air exposure is investigated through X‐ray photoelectron spectroscopy. The morphology of TiO₂‐BP‐S is characterized using transmission electron microscopy, indicating that the TiO₂ nanoparticles produce P? Ti bonds with BP. The TiO₂‐BP‐S composite with P? S and P? Ti bonds exhibits excellent stability in air and the superior electrochemical performance. For example, the discharge specific capacity is up to 490 mA h g^?1 after 100 cycles at 50 mA g^?1, and it remains at 290 mA h g^?1 after 600 cycles at 500 mA g^?1. Meanwhile, the scientific insight that the formation of stable P? S and P? Ti bonds can provide a guide for the practical large‐scale application of SIBs in other titanium base and black phosphorus materials is looked forward.     

Compositional and Dimensional Control of 2D and Quasi‐2D Lead Halide Perovskites in Water

Blue light emitting two dimensional (2D) and quasi‐2D layered halide perovskites (LHPs) are gaining attention in solid‐state lighting applications but their fragile stability in humid condition is one of the most pressing issues for their practical applications. Though water is much greener and cost effective, organic solvents must be used during synthesis as well as the device fabrication process for these LHPs due to their water‐sensitivity/instability and consequently, water‐stable blue‐light emitting 2D and quasi‐2D LHPs have not been documented yet. Here, water‐mediated facile and cost‐effective syntheses, characterizations, and optical properties of 16 organic–inorganic hybrid compounds are reported including 2D (A′)₂PbX₄ (A′ = butylammonium, X = Cl/Br/I) (8 compounds), 3D perovskites (4), and quasi‐2D (A′)_pA_x?1B_xX_3x+1 LHPs (A = methylammonium) (4) in water. Here, both composition and dimension of LHPs are tuned in water, which has never been explored yet. Furthermore, the dual emissive nature is observed in quasi‐2D perovskites, where the intensity of two photoluminescence (PL) peaks are governed by 2D and 3D inorganic layers. The Pb(OH)₂‐coated 2D and quasi‐2D perovskites are highly stable in water even after several months. In addition, single particle imaging is performed to correlate structural–optical property of these LHPs.     

Reversible Conversion Reactions and Small First Cycle Irreversible Capacity Loss in Metal Sulfide‐Based Electrodes Enabled by Solid Electrolytes

Solid‐state batteries can potentially enable new classes of electrode materials which are unstable against liquid electrolytes. Here, SnS nanocrystals, synthesized by a wet chemical method, are used to fabricate a Li‐ion electrode, and the electrochemical properties of this electrode are examined in both solid and liquid electrolyte designs. The SnS‐based solid‐state cell delivers a capacity of 629 mAh g^?1 after 100 cycles and exhibits an unprecedentedly small irreversible capacity in the first cycle (8.2%), while the SnS‐based liquid cell shows a rapid capacity decay and large first cycle irreversible capacity (44.6%). Cyclic voltammetry (CV) experiments show significant solid electrolyte interphase (SEI) formation in the liquid cell during the first discharge while SEI formation by electrolyte reduction in the solid‐state cell appears negligible. Along with CV, X‐ray photoelectron spectroscopy and energy dispersive spectroscopy are used to investigate the differences between the solid‐state and liquid cells. The reaction chemistry of SnS in solid‐state cells is also studied in detail by ex situ X‐ray diffraction and X‐ray absorption spectroscopy. The overarching findings are that use of a solid electrolyte suppresses materials degradation and electrolyte reduction which leads to a small first cycle irreversible capacity and stable cycling.     

Transparent,Highly Stretchable,Rehealable, Sensing,and Fully Recyclable Ionic Conductors Fabricated by One‐Step Polymerization Based on a Small Biological Molecule

To date, various stretchable conductors have been fabricated, but simultaneous realization of the transparency, high stretchability, electrical conductivity, self‐healing capability, and sensing property through a simple, fast, cost‐efficient approach is still challenging. Here, α‐lipoic acid (LA), a naturally small biological molecule found in humans and animals, is used to fabricate transparent (>85%), electrical conductivity, highly stretchable (strain up to 1100%), and rehealable (mechanical healing efficiency of 86%, electrical healing efficiency of 96%) ionic conductor by solvent‐free one‐step polymerization. Furthermore, the ionic conductors with appealing sensitivity can be served as strain sensors to detect and distinguish various human activities. Notably, this ionic conductor can be fully recycled and reprocessed into new ionic conductors or adhesives by a direct heating process, which offers a promising prospect in great reduction of electronic wastes that have brought acute environmental pollution. In consideration of the extremely facile preparation process, biological available materials, satisfactory functionalities, and full recyclability, the emergence of LA‐based ionic conductors is believed to open up a new avenue for developing sustainable and wearable electronic devices in the future.     

Tunable Emission in Heteroepitaxial Ln‐SURMOFs

By using a layer‐by‐layer (LbL) approach, lanthanide‐based, monolithic metal–organic framework (MOF) thin films are fabricated for optical applications. In particular, the LbL approach allows manufacturing of heteroepitaxial Tb(III)‐Eu(III)(BTC) coatings with precise thickness control. Adjusting the Tb(III)‐to‐Eu(III) ratio allows tuning of the emission color. The hetero‐multilayer architecture makes it possible to suppress the direct Tb(III)‐to‐Eu(III) energy transfer, an unwanted phenomenon present in the corresponding mixed‐metal bulk MOF structures. The resulting Ln‐MOF thin films, or Ln‐surface‐anchored MOFs (SURMOFs), are characterized by X‐ray diffraction, infra‐red reflection absorption spectroscopy, UV–vis, and photoluminescence measurements. The results demonstrate that the heteroepitaxial SURMOF architectures carry huge potential for fabricating optical coatings for a wide range of applications.     

Strain‐Visualization with Ultrasensitive Nanoscale Crack‐Based Sensor Assembled with Hierarchical Thermochromic Membrane

As eidetic signal recognition has become important, displaying mechanical signals visually has imposed huge demands for simple readability and without complex signal processing. Such visualization of mechanical signals is used in delicate urgent medical or safety‐related industries. Accordingly, chromic materials are considered to facilitate visualization with multiple colors and simple process. However, the response and recovery time is very long, such that rapid regular signals are unable to be detected, i.e., physiological signals, such as respiration. Here, the simple visualization of low strain ≈2%, with ultrasensitive crack‐based strain sensors with a hierarchical thermochromic layer is suggested. The sensor shows a gradient color change from red to white color in each strain, which is attributed to the hierarchical property, and the thermal response (recovery) time is dramatically minimized within 0.6 s from 45 to 37 °C, as the hierarchical membrane is inspired by termite mounds for efficient thermal management. The fast recovery property can be taken advantage of in medical fields, such as monitoring regular respiration, and the color changes can be delicately monitored with high accuracy by software on a mobile phone.     

Side‐Chain Engineering on Dopant‐Free Hole‐Transporting Polymers toward Highly Efficient Perovskite Solar Cells (20.19%)

A variety of dopant‐free hole‐transporting materials (HTMs) is developed to serve as alternatives to the typical dopant‐treated ones; however, their photovoltaic performance still falls far behind. In this work, the side chain of a polymeric HTM is engineered by partially introducing diethylene glycol (DEG) groups in order to simultaneously optimize the properties of both the bulk of the HTM layer and the HTM/perovskite interface. The intermolecular π–π stacking interaction in the HTM layer is unexpectedly weakened after the incorporation of DEG groups, whereas the lamellar packing interaction is strengthened. A doubled hole mobility is obtained when 3% of the DEG groups replace the original alkyl side chains, and a champion power conversion efficiency (PCE) of 20.19% (certified: 20.10%) is then achieved, which is the first report of values over 20% for dopant‐free organic HTMs. The device maintains 92.25% of its initial PCE after storing at ambient atmosphere for 30 d, which should be due to the enhanced hydrophobicity of the HTM film.     

Distinctive Performance of Terahertz Photodetection Driven by Charge‐Density‐Wave Order in CVD‐Grown Tantalum Diselenide

The quantum behavior of carriers in solid is the foundation of modern electronic and optoelectronic technology, but it is still facing huge challenges within inherited single‐particle quantum processes working at the millimeter wave/terahertz (THz) band. Here, a straightforward strategy for the direct detection of millimeter wave/THz photons in a sub‐wavelength metal‐TaSe₂‐metal structure under strong interaction with a localized field of surface plasmon is proposed. By breaking the inversion symmetry under the perturbations of electric field and atomic reconstruction from van der Waals integration, the nonequilibrium electronic states under a radiant field can be manipulated in a collective fashion, leading to a large photocurrent responsivity over 40 A W^?1 and noise equivalent power less than 1 pW Hz^?1/2 even at room temperature. A more than 40‐fold enhancement in responsivity is achieved when transitioning from the normal phase to the CDW phase. The findings shed fresh light on the understanding of the delicate balance in the charge‐ordered phase, and facilitate the exploitation of a correlated electron system for optoelectronic applications in fields of security, remote sensing, and imaging.