Considering the ever‐growing climatic degeneration, sustainable and renewable energy sources are needed to be effectively integrated into the grid through large‐scale electrochemical energy storage ...and conversion (EESC) technologies. With regard to their competent benefit in cost and sustainable supply of resource, room‐temperature sodium‐ion batteries (SIBs) have shown great promise in EESC, triumphing over other battery systems on the market. As one of the most fascinating cathode materials due to the simple synthesis process, large specific capacity, and high ionic conductivity, Na‐based layered transition metal oxide cathodes commonly suffer from the sluggish kinetics, multiphase evolution, poor air stability, and insufficient comprehensive performance, restricting their commercialization application. Here, this review summarizes the recent advances in layered oxide cathode materials for SIBs through different optimal structure modulation technologies, with an emphasis placed on strategies to boost Na+ kinetics and reduce the irreversible phase transition as well as enhance the store stability. Meanwhile, a thorough and in‐depth systematical investigation of the structure–function–property relationship is also discussed, and the challenges as well as opportunities for practical application electrode materials are sketched. The insights brought forward in this review can be considered as a guide for SIBs in next‐generation EESC.
The recent research progress of structure modulation technology on layered transition metal oxide cathodes for sodium‐ion batteries is summarized, concentrating especially on morphology design, coating technology, phase transition, ordering‐disordering, air stability, and composite structure to boost Na+ kinetics, suppress the irreversible phase transition, enhance the storage stability, improve the overall performance, and further realize sodium‐ion battery commercialization for market applications.
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Rechargeable Li‐metal batteries (RLBs) can boost energy yet possess poor cycle stability and safety concerns when utilizing carbonate electrolytes. Countless effort has been invested in researching ...and developing electrolytes for RLBs to obtain stable and safe batteries. However, only few existing electrolytes meet the requirements for practical RLBs. In this perspective, the challenges of organic liquid electrolytes in the application in RLBs are summarized, and requirements for electrolytes for practical RLBs are proposed. This perspective briefly reviews the recent achievements of electrolytes (liquid‐ and solid‐state) for RLBs and analyzes the corresponding drawbacks of each electrolyte. Further, possible solutions to the existing shortcomings of various electrolytes are proposed. In particular, this perspective outlines the development strategy of in situ gelation electrolytes, accompanied by a call for people using pouch cells to evaluate performance and paying more attention to battery safety research. This perspective aims to expound on the challenges and the possible research directions of RLBs electrolytes to promote practical RLBs better.
Constructing safe and stable rechargeable Li‐metal batteries (RLBs) require electrolytes with proper properties in Li+ conductivity, processability, stability, non‐flammability, and strength. This perspective summarizes the achievements of different electrolytes for RLBs and outlined the remaining challenges. The possible strategies for the further development of electrolytes are proposed, accompanied by recalling for improving evaluation standards and safety research of RLBs.
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Garnet‐type electrolytes suffer from unstable chemistry against air exposure, which generates contaminants on electrolyte surface and accounts for poor interfacial contact with the Li metal. Thermal ...treatment of the garnet at >700 °C could remove the surface contaminants, yet it regenerates the contaminants in the air, and aggravates the Li dendrite issue as more electron‐conducting defective sites are exposed. In a departure from the removal approach, here we report a new surface chemistry that converts the contaminants into a fluorinated interface at moderate temperature <180 °C. The modified interface shows a high electron tunneling barrier and a low energy barrier for Li+ surface diffusion, so that it enables dendrite‐proof Li plating/stripping at a high critical current density of 1.4 mA cm−2. Moreover, the modified interface exhibits high chemical and electrochemical stability against air exposure, which prevents regeneration of contaminants and keeps high critical current density of 1.1 mA cm−2. The new chemistry presents a practical solution for realization of high‐energy solid‐state Li metal batteries.
The detrimental contaminants on a garnet surface are converted into an air‐stable fluorinated interface by a facile chemical approach at moderate temperature (<180 °C). The modified interface shows a high electron tunneling barrier and a low energy barrier for Li+ surface diffusion, enabling a high critical current density of 1.4 mA cm−2.
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Safety concerns are impeding the applications of lithium metal batteries. Flame‐retardant electrolytes, such as organic phosphates electrolytes (OPEs), could intrinsically eliminate fire hazards and ...improve battery safety. However, OPEs show poor compatibility with Li metal though the exact reason has yet to be identified. Here, the lithium plating process in OPEs and Li/OPEs interface chemistry were investigated through ex situ and in situ techniques, and the cause for this incompatibility was revealed to be the highly resistive and inhomogeneous interfaces. Further, a nitriding interface strategy was proposed to ameliorate this issue and a Li metal anode with an improved Li cycling stability (300 h) and dendrite‐free morphology is achieved. Meanwhile, the full batteries coupled with nickel‐rich cathodes, such as LiNi0.8Co0.1Mn0.1O2, show excellent cycling stability and outstanding safety (passed the nail penetration test). This successful nitriding‐interface strategy paves a new way to handle the incompatibility between electrode and electrolyte.
A nitriding interface has been developed for the successful application of flame‐retardant electrolytes in high‐energy‐density cells using a Li metal anode and a high‐voltage, high‐capacity cathode. The homogeneity of the solid electrolyte interface (SEI) layer is crucially important for the uniform Li deposition required for high‐voltage batteries.
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The key issue holding back the application of solid polymeric electrolytes in high‐energy density lithium metal batteries is the contradictory requirements of high ion conductivity and mechanical ...stability. In this work, self‐healable solid polymeric electrolytes (SHSPEs) with rigid‐flexible backbones and high ion conductivity are synthesized by a facile condensation polymerization approach. The all‐solid Li metal full batteries based on the SHSPEs possess freely bending flexibility and stable cycling performance as a result of the more disciplined metal Li plating/stripping, which have great implications as long‐lifespan energy sources compatible with other wearable devices.
Solid but flexible: A self‐healing solid polymer electrolyte (featuring fast self‐healing within 60 s after a deep cut with a blade) endows solid Li metal full batteries with freely bending flexibility and superior cycling stability as demonstrated by the small capacity decay of 0.1 % per cycle over 100 cycles.
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Fast and ultrasensitive detection of pathogens is very important for efficient monitoring and prevention of viral infections. Here, we demonstrate a label‐free optical detection approach that uses a ...printed nanochain assay for colorimetric quantitative testing of viruses. The antibody‐modified nanochains have high activity and specificity which can rapidly identify target viruses directly from biofluids in 15 min, as well as differentiate their subtypes. Arising from the resonance induced near‐field enhancement, the color of nanochains changes with the binding of viruses that are easily observed by a smartphone. We achieve the detection limit of 1 PFU μL−1 through optimizing the optical response of nanochains in visible region. Besides, it allows for real‐time response to virus concentrations ranging from 0 to 1.0×105 PFU mL−1. This low‐cost and portable platform is also applicable to rapid detection of other biomarkers, making it attractive for many clinical applications.
A printed nanochain‐based colorimetric assay is utilized for point‐of‐care quantitative testing and real‐time monitoring of viral infection with high sensitivity, specificity, and reliability. It enables rapid detection of various pathogens from tiny amounts of clinical sample with a smartphone.
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Rechargeable lithium–metal batteries with a cell‐level specific energy of >400 Wh kg−1 are highly desired for next‐generation storage applications, yet the research has been retarded by poor ...electrolyte–electrode compatibility and rigorous safety concerns. We demonstrate that by simply formulating the composition of conventional electrolytes, a hybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li‐metal anode and the nickel‐rich layered oxide cathodes. By employing the new electrolyte, Li∥LiNi0.6Co0.2Mn0.2O2 cells show favorable cycling and rate performance, and a 10 Ah Li∥LiNi0.8Co0.1Mn0.1O2 pouch cell demonstrates a practical specific energy of >450 Wh kg−1. Our findings shed light on reasonable design principles for electrolyte and electrode/electrolyte interfaces toward practical realization of high‐energy rechargeable batteries.
Formulation of conventional electrolyte composition yields a hybrid solid/liquid electrolyte that is electrochemically compatible with the Li‐metal anode and the nickel‐rich layered oxide cathodes, which promises stable operation of a practical 10‐Ah‐grade pouch cell with a specific energy of >450 Wh kg−1.
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Solid polymer electrolytes (SPEs) are promising candidates for developing high‐energy‐density Li metal batteries due to their flexible processability. However, the low mechanical strength as well as ...the inferior interfacial regulation of ions between SPEs and Li metal anode limit the suppress ion of Li dendrites and destabilize the Li anode. To meet these challenges, interfacial engineering aiming to homogenize the distribution of Li+/electron accompanied with enhanced mechanical strength by Mg3N2 layer decorating polyethylene oxide is demonstrated. The intermediary Mg3N2 in situ transforms to a mixed ion/electron conducting interlayer consisting of a fast ionic conductor Li3N and a benign electronic conductor Mg metal, which can buffer the Li+ concentration gradient and level the nonuniform electric current distribution during cycling, as demonstrated by a COMSOL Multiphysics simulation. These characteristics endow the solid full cell with a dendrite‐free Li anode and enhanced cycling stability and kinetics. The innovative interface design will accelerate the commercial application of high‐energy‐density solid batteries.
An in situ formed mixed ion/electron conducting interlayer formed from an intermediary Mg3N2 layer decorated on polyethylene oxide is designed. The as‐synthesized electrolyte manipulates ion and electron distributions on the surface of the Li anode, endowing the solid full cell with a dendrite‐free Li anode and enhanced cycling stability and kinetics.
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The uncontrollable dendrite growth and unstable solid electrolyte interphase have long plagued the practical application of Li metal batteries. Herein, a dual‐layered artificial interphase ...LiF/LiBO–Ag is demonstrated that is simultaneously reconfigured via an electrochemical process to stabilize the lithium anode. This dual‐layered interphase consists of a heterogeneous LiF/LiBO glassy top layer with ultrafast Li‐ion conductivity and lithiophilic Li–Ag alloy bottom layer, which synergistically regulates the dendrite‐free Li deposition, even at high current densities. As a result, Li||Li symmetric cells with LiF/LiBO–Ag interphase achieve an ultralong lifespan (4500 h) at an ultrahigh current density and area capacity (20 mA cm−2, 20 mAh cm−2). LiF/LiBO–Ag@Li anodes are successfully applied in quasi‐solid‐state batteries, showing excellent cycling performances in symmetric cells (8 mA cm−2, 8 mAh cm−2, 5000 h) and full cells. Furthermore, a practical quasi‐solid‐state pouch cell coupling with a high‐nickel cathode exhibits stable cycling with a capacity retention of over 91% after 60 cycles at 0.5 C, which is comparable or even better than that in liquid‐state pouch cells. Additionally, a high‐energy‐density quasi‐solid‐state pouch cell (10.75 Ah, 448.7 Wh kg−1) is successfully accomplished. This well‐orchestrated interphase design provides new guidance in engineering highly stable interphase toward practical high‐energy‐density lithium metal batteries.
A spontaneously reconfigured, dual‐layered artificial interphase of LiF/LiBO–Ag is proposed to stabilize Li anode at high current densities. The LiF/LiBO top layer guarantees fast Li‐ion transition, and the lithiophilic Li–Ag bottom layer enables uniform Li deposition. Benefiting from the well‐orchestrated interphase design, the quasi‐solid‐state lithium metal batteries demonstrate a high practical specific energy (448.7 Wh kg−1), superior high‐rate performances, and high safety.
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In overcoming the Li+ desolvation barrier for low‐temperature battery operation, a weakly‐solvated electrolyte based on carboxylate solvent has shown promises. In case of an organic‐anion‐enriched ...primary solvation sheath (PSS), we found that the electrolyte tends to form a highly swollen, unstable solid electrolyte interphase (SEI) that shows a high permeability to the electrolyte components, accounting for quickly declined electrochemical performance of graphite‐based anode. Here we proposed a facile strategy to tune the swelling property of SEI by introducing an inorganic anion switch into the PSS, via LiDFP co‐solute method. By forming a low‐swelling, Li3PO4‐rich SEI, the electrolyte‐consuming parasitic reactions and solvent co‐intercalation at graphite‐electrolyte interface are suppressed, which contributes to efficient Li+ transport, reversible Li+ (de)intercalation and stable structural evolution of graphite anode in high‐energy Li‐ion batteries at a low temperature of −20 °C.
Inclusion of difluorophosphate anion in the primary solvation sheath of a weakly‐solvated electrolyte helps to switch the swelling properties of solid electrolyte interphase (SEI) on a graphite (Gr) composite anode. By forming a low‐swelling, Li3PO4‐enriched SEI, reversible Li+ (de)intercalation was enabled at a stable Gr‐electrolyte interface, contributing to improved low‐temperature electrochemical performance of a Li‐ion battery.
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