A panoramic view of Li_(7)P_(3)S_(11) solid electrolytes synthesis, structural aspects and practical challenges for all-solid-state lithium batteries

The development of an inorganic electrochemical stable solid-state electrolyte is essentially responsible for future state-of-the-art all-solid-state lithium batteries(ASSLBs).Because of their advantages in safety,working temperature,high energy density,and packaging,ASSLBs can develop an ideal energy storage system for modern electric vehicles(EVs).A solid electrolyte(SE)model must have an economical synthesis approach,exhibit electrochemical and chemical stability,high ionic conductivity,and low interfacial resistance.Owing to its highest conductivity of 17 mS·cm^(-1),and deformability,the sulfide-based Li_(7)P_(3)S_(11) solid electrolyte is a promising contender for the high-performance bulk type of ASSLBs.Herein,we present a current glimpse of the progress of synthetic procedures,structural aspects,and ionic conductivity improvement strategies.Structural elucidation and mechanistic approaches have been extensively discussed by using various characterization techniques.The chemical stability of Li_(7)P_(3)S_(11) could be enhanced via oxide doping,and hard and soft acid/base(HSAB)concepts are also discussed.The issues to be undertaken for designing the ideal solid electrolytes,interfacial challenges,and high energy density have been discoursed.This review aims to provide a bird’s eye view of the recent development of Li_(7)P_(3)S_(11)-based solid-state electrolyte applications and explore the strategies for designing new solid electrolytes with a target-oriented approach to enhance the efficiency of high energy density allsolid-state lithium batteries.

Space Charge Layer Eff ect in Sulfide Solid Electrolytes in All-Solid-State Batteries: In-situ Characterization and Resolution

All-solid-state lithium batteries(ASSLBs)have advantages of safety and high energy density,and they are expected to become the next generation of energy storage devices.Sulfide-based solid-state electrolytes(SSEs)with high ionic conduc-tivity and low grain boundary resistance exhibit remarkable practical application.However,the space charge layer(SCL)eff ect and high interfacial resistance caused by a mismatch with the current commercial oxide cathodes restrict the develop-ment of sulfide SSEs and ASSLBs.This review summarizes the research progress on the SCL eff ect of sulfide SSEs and oxide cathodes,including the mechanism and direct evidence from high performance in-situ characterizations,as well as recent progress on the interfacial modification strategies to alleviate the SCL eff ect.This study provides future direction to stabilize the high performance sulfide-based solid electrolyte/oxide cathode interface for state-of-the-art ASSLBs and future all-SSE storage devices.

Evaluation of solid electrolytes: Development of conventional and interdisciplinary approaches

Solid-state lithium batteries(SSLBs)have received considerable attention due to their advantages in thermal stability,energy density,and safety.Solid electrolyte(SE)is a key component in developing high-performance SSLBs.An in-depth understanding of the intrinsic bulk and interfacial properties is imperative to achieve SEs with competitive performance.This review first introduces the traditional electrochemical approaches to evaluating the fundamental parameters of SEs,including the ionic and electronic conductivities,activation barrier,electrochemical stability,and diffusion coefficient.After that,the characterization techniques to evaluate the structural and chemical stability of SEs are reviewed.Further,emerging interdisciplinary visualization techniques for SEs and interfaces are highlighted,including synchrotron X-ray tomography,ultrasonic scanning imaging,time-of-flight secondary-ion mass spectrometry,and three-dimensional stress mapping,which improve the understanding of electrochemical performance and failure mechanisms.In addition,the application of machine learning to accelerate the screening and development of novel SEs is introduced.This review article aims to provide an overview of advanced characterization from a broad physical chemistry view,inspiring innovative and interdisciplinary studies in solid-state batteries.

高离子电导率硫化物固态电解质的空气稳定性研究进展

全固态锂电池兼具安全性和高能量密度,作为下一代储能器件备受关注.硫化物固态电解质具有锂离子电导率高、晶界电阻低、机械延展性好等优点,作为最具商业化潜力的固态电解质,引起了产业界和科研单位的广泛兴趣.但是硫化物固态电解质较差的空气稳定性导致其制备以及后续组装的硫化物固态全电池需要在氩气保护的环境下进行操作,使得生产成本居高不下,严重制约其产业化的步伐.本文对硫化物固态电解质空气稳定性的相关研究包括空气稳定性的研究方法和衰减反应机制进行详细的梳理和客观分析,并提炼出提高硫化物固态电解质空气稳定性相应的策略与方法.

Electrode materials derived from plastic wastes and other industrial wastes for supercapacitors

The present review not only devotes on the environmental consequences of plastic bag wastes and other industrial wastes observable in the landfills,in the oceans or elsewhere but also gives a new insight idea on conversion of them into worth material,carbon,for the best electrochemical supercapacitor.Transformation of plastic wastes into high-value materials is the incentive for plastic recycling,end-oflife handling case for plastic bag wastes in practice quite limited.The plastic recycling waste for reuse saves energy compared with manufacturing virgin materials.Herein,we identified several synthetic methods to convert plastic waste and other industrial wastes into carbon material for supercapacitor.Different kinds of carbon materials,including nanofiber,nanotube,graphene,mesoporous carbon,etc.,have been derived from plastic waste,and thus give a superior potential for transforming trash into a"gold capacitor".Finally,conclusions and future trends of high-voltage supercapacitors were made as well as the easy and mass production of high-performance electrode materials for supercapacitors.Our work offers a promising sustainable approach to handle plastic bags,waste,and other industrial wastes and provides a new avenue in supercapacitor applications and other areas.

Orderly defective superstructure for enhanced pseudocapacitive storage in titanium niobium oxide

Artificial defect engineering in transition metal oxides is of important terms for numerous applications.In the present work,we proposed an in-situ gas reduction strategy to introduce ordered defects into titanium niobium oxide embedding on vapor grew carbon fibers(Ti_(2)Nb_(10)O_(29-x)@VGCFs).High-resolution transmission electron microscopy(HRTEM)and fast Fourier transform(FFT)simulation indicate that the ordered oxygen defects locate at interval layers,which leads to a new superstructure in Ti_(2)Nb_(10)O_(29).The ordered defects could provide extra active sites for lithium-ion storage and modulate ionic migration,resulting an enhanced pseudocapacitive performance.In addition,the excellent structural stability of the superstructure was proved by in-situ HRTEM under a harsh electrochemical process.Our work provides a directly observation of orderly defective superstructure in transition metal oxide,and its functionality on electrochemistry was revealed.

Tailored Carrier Transport Path by Interpenetrating Networks in Cathode Composite for High Performance All‑Solid‑State Li‑SeS_(2) Batteries

All-solid-state Li-SeS_(2) batteries(ASSLSs)are more attractive than traditional liquid Li-ion batteries due to superior thermal stability and higher energy density.However,various factors limit the practical application of all-solid-state Li-SeS_(2) batteries,such as the low ionic conductivity of the solid-state electrolyte and the poor kinetic property of the cathode composite,resulting in unsatisfactory rate capability.Here,we employed a traditional ball milling method to design a Li_(7)P_(2.9)W_(0.05)S_(10.85) glass–ceramic electrolyte with high conductivity of 2.0 mS cm^(−1) at room temperature.In order to improve the kinetic property,an interpenetrating network strategy is proposed for rational cathode composite design.Signifcantly,the disordered cathode composite with an interpenetrating network could promote electronic and ionic conduction and intimate contacts between the electrolyte–electrode particles.Moreover,the tortuosity factor of the carrier transport channel is considerably reduced in electrode architectures,leading to superior kinetic performance.Thus,assembled ASSLS exhibited higher capacity and better rate capability than its counterpart.This work demonstrates that an interpenetrating network is essential for improving carrier transport in cathode composite for high rate all-solid-state Li-SeS_(2) batteries.

Design of Solid Electrolytes with Fast Ion Transport:Computation-Driven and Practical Approaches

For next-generation all-solid-state metal batteries,the computation can lead to the discovery of new solid electrolytes with increased ionic conductivity and excellent safety.Based on computational predictions,a new proposed solid electrolyte with a flat energy landscape and fast ion migration is synthesized using traditional synthesis methods.Despite the promise of the predicted solid electrolyte candidates,conventional synthetic methods are frequently hampered by extensive optimization procedures and overpriced raw materials.It is impossible to rationally develop novel superionic conductors without a comprehensive understanding of ion migration mechanisms.In this review,we cover ion migration mechanisms and all emerging computational approaches that can be applied to explore ion conduction in inorganic materials.The general illustrations of sulfide and oxide electrolyte structures as well as their fundamental features,including ion migration paths,dimensionalities,defects,and ion occupancies,are systematically discussed.The major challenges to designing the solid electrolyte and their solving strategies are highlighted,such as lattice softness,polarizability,and structural disorder.In addition to an overview of recent findings,we propose a computational and experimental approach for designing high-performance solid electrolytes.This review article will contribute to a practical understanding of ion conduction,designing,rapid optimization,and screening of advanced solid electrolytes in order to eliminate liquid electrolytes.