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71.
MXene, a new class of 2D materials, has gained significant attention owing to its attractive electrical conductivity, tunable work function, and metallic nature for wide range of applications. Herein, delaminated few layered Ti3C2Tx MXene contacted Si solar cells with a maximum power conversion efficiency (PCE) of ≈11.5% under AM1.5G illumination are demonstrated. The formation of an Ohmic junction of the metallic MXene to n+‐Si surface efficiently extracts the photogenerated electrons from n+np+‐Si, decreases the contact resistance, and suppresses the charge carrier recombination, giving rise to excellent open‐circuit voltage and short‐circuit current density. The rapid thermal annealing process further improves the electrical contact between Ti3C2Tx MXene and n+‐Si surface by reducing sheet resistance, increasing electrical conductivity, and decreasing cell series resistance, thus leading to a remarkable improvement in fill factor and overall PCE. The work demonstrated here can be extended to other MXene compositions as potential electrodes for developing highly performing solar cells.  相似文献   
72.
Alkali metal–O2 batteries, by coupling high‐capacity alkali metal anodes with gaseous oxygen, possess extremely high gravimetric energy density that is comparable to gasoline and are potential energy storage technologies beyond lithium–ion batteries. The development of alkali metal–O2 batteries has achieved great progress in recent years, from materials to prototype devices and on fundamental mechanisms. The stability of alkali metal–O2 batteries is still poor, however, leading to a huge gap between laboratory research and commercial applications. A series of parasitic reactions result in the instability, which occur during electrochemical discharging and charging. The ubiquitous active oxygen species attack both the organic electrolyte and the carbon cathode, triggering various parasitic reactions. Meanwhile, dendrite growth and volume expansion upon repeated plating/stripping and O2 crossover severely limit the reversibility of alkali metal anodes. Here, an overview of the strategies against these issues is given to improve the stability of nonaqueous alkali metal–O2 batteries, which is discussed from three aspects: air cathodes, alkali metal anodes, and aprotic electrolytes. Furthermore, perspectives for future research of stable alkali metal–O2 batteries are outlined.  相似文献   
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Thanks to low costs and the abundance of the resources, sodium‐ion (SIBs) and potassium‐ion batteries (PIBs) have emerged as leading candidates for next‐generation energy storage devices. So far, only few materials can serve as the host for both Na+ and K+ ions. Herein, a cubic phase CuSe with crystal‐pillar‐like morphology (CPL‐CuSe) assembled by the nanosheets are synthesized and its dual functionality in SIBs and PIBs is comprehensively studied. The electrochemical measurements demonstrate that CPL‐CuSe enables fast Na+ and K+ storage as well as the sufficiently long duration. Specifically, the anode delivers a specific capacity of 295 mA h g?1 at current density of 10 A g?1 in SIBs, while 280 mA h g?1 at 5 A g?1 in PIBs, as well as the high capacity retention of nearly 100% over 1200 cycles and 340 cycles, respectively. Remarkably, CPL‐CuSe exhibits a high initial coulombic efficiency of 91.0% (SIBs) and 92.4% (PIBs), superior to most existing selenide anodes. A combination of in situ X‐ray diffraction and ex situ transmission electron microscopy tests fundamentally reveal the structural transition and phase evolution of CuSe, which shows a reversible conversion reaction for both cells, while the intermediate products are different due to the sluggish K+ insertion reaction.  相似文献   
75.
The electron–hole recombination kinetics of organic photovoltaics (OPVs) are known to be sensitive to the relative energies of triplet and charge‐transfer (CT) states. Yet, the role of exciton spin in systems having CT states above 1.7 eV—like those in near‐ultraviolet‐harvesting OPVs—has largely not been investigated. Here, aggregation‐induced room‐temperature intersystem crossing (ISC) to facilitate exciton harvesting in OPVs having CT states as high as 2.3 eV and open‐circuit voltages exceeding 1.6 V is reported. Triplet excimers from energy‐band splitting result in ultrafast CT and charge separation with nonradiative energy losses of <250 meV, suggesting that a 0.1 eV driving force is sufficient for charge separation, with entropic gain via CT state delocalization being the main driver for exciton dissociation and generation of free charges. This finding can inform engineering of next‐generation active materials and films for near‐ultraviolet OPVs with open‐circuit voltages exceeding 2 V. Contrary to general belief, this work reveals that exclusive and efficient ISC need not require heavy‐atom‐containing active materials. Molecular aggregation through thin‐film processing provides an alternative route to accessing 100% triplet states on photoexcitation.  相似文献   
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Freestanding layered membrane–based devices have broad applications in highly efficient energy‐storage/conversion systems. The liquid–solid interface is considered as a unique yet versatile interface for constructing such layered membrane–based devices. In this review, the authors outline recent developments in the fabrication of soft materials to functionalize layered devices from the aspect of liquid–solid interfacial assembly and engineering arts. Seven liquid–solid interfacial assembly strategies, including flow‐directed, superlattice, solvent‐casting, evaporation‐induced, dip‐coating, spinning, and electrospinning assemblies, are comprehensively highlighted with a focus on their synthetic pathways, formation mechanisms, and interface engineering strategies. Meanwhile, recent representative works on layered membrane–based devices for electrochemical energy applications are presented. Finally, challenges and opportunities of this research area are highlighted in order to stimulate future developments. This review not only offers comprehensive and practical approaches to assemble liquid–solid interfaces with soft materials for various important layered electrochemical energy devices but also sheds lights on fundamental insights by thoughtful discussions on performance enhancement mechanisms of these electrochemical energy systems.  相似文献   
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79.
As technologically important materials for solid‐state batteries, Li super‐ionic conductors are a class of materials exhibiting exceptionally high ionic conductivity at room temperature. These materials have unique crystal structural frameworks hosting a highly conductive Li sublattice. However, it is not understood why certain crystal structures of the super‐ionic conductors lead to high conductivity in the Li sublattice. In this study, using topological analysis and ab initio molecular dynamics simulations, the crystal structures of all Li‐conducting oxides and sulfides are studied systematically and the key features pertaining to fast‐ion conduction are quantified. In particular, a unique feature of enlarged Li sites caused by large local spaces in the crystal structural framework is identified, promoting fast conduction in the Li‐ion sublattice. Based on these quantified features, the high‐throughput screening identifies many new structures as fast Li‐ion conductors, which are further confirmed by ab initio molecular dynamics simulations. This study provides new insights and a systematic quantitative understanding of the crystal structural frameworks of fast ion‐conductor materials and motivates future experimental and computational studies on new fast‐ion conductors.  相似文献   
80.
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