Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.I...Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.In this study,we propose an entropy-assisted multi-element doping strategy to mitigate these issues.Specifically,two routes are designed and compared:bulk-like localized high-entropy doping(BHE-NCM)and surface-distributed high-entropy-zone doping(SHE-NCM).The surface entropy-doped NCM cathode delivers enhanced electrochemical performance,including higher capacity retention under 4.5 V cycling and superior rate capability,compared to both bulk-like and pristine counterparts.Comprehensive material characterization reveals that surface-localized doping stabilizes the layered structure with reduced microcrack formation and creates a uniform dopant-rich surface region with improved thermal and electrochemical stability.Overall,entropy-assisted doping at the near surface zone effectively alleviates structural degradation and interface reactions in Ni-rich NCM,enabling improved cycling performance at high voltage.This work highlights the significance of surface entropy engineering as a promising strategy for designing high-voltage cathodes with improved safety and longevity.展开更多
Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been d...Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn^(2+)diffusion kinetics.By employing electrodeposition to coat MoS_(2)on the surface of BaV_(6)O_(16)·3H_(2)O nanowires,the directional builtin electric field generated at the heterointerface acts as a cation accelerator,continuously accelerating Zn^(2+)diffusion into the active material.The optimized Zn^(2+)diffusion coefficient in CC@BaV-V_(6)O_(16)·3H_(2)@MoS_(2)(7.5×10^(8)cm^(2)s^(-1)) surpasses that of most reported V-based cathodes.Simultaneously,MoS_(2)serving as a cathodic armor extends the cycling life of the Zn-CC@BaV_(6)O_(16)·3H_(2)@MoS_(2)full batteries to over 10000 cycles.This work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.展开更多
Aqueous zinc-ion batteries(AZIBs)are an appealing battery system due to their low cost,intrinsic safety,and environmental-friendliness,while their application is plagued by the obstacles from the cathode,electrolyte,a...Aqueous zinc-ion batteries(AZIBs)are an appealing battery system due to their low cost,intrinsic safety,and environmental-friendliness,while their application is plagued by the obstacles from the cathode,electrolyte,and zinc anode.Summarizing the design principles and strategies toward the optimization of cathode,electrolyte,and zinc anode is crucial for the development of AZIBs.Herein,we present a comprehensive analysis of the design principles and promising strategies toward the improvement of AZIBs.Firstly,the various reaction mechanisms are summarized and the existing issues associated with the cathode,electrolyte,and zinc anode are discussed to guide the rational design of AZIBs.Subsequently,we provide an in-depth and comprehensive discussion on the design principles and strategies for the electrodes/electrolyte/separator optimization,and analyze the advantages and disadvantages of various strategies.Importantly,the design principles and strategies of the newly appeared conversion-type AZIBs,such as Zn-S battery and Zn-Se battery,are also discussed and analyzed.The effect of design strategies on the electrochemical performance and the relationship between the current issues and strategies are also unveiled in detail.Finally,some research trends and perspectives are provided for designing better AZIBs.展开更多
Inorganic solid electrolyte-based all-solid-state lithium-sulfur batteries(ASSLSBs)have garnered significant attention due to their inherent safety and higher energy density,making them a promising candidate for the u...Inorganic solid electrolyte-based all-solid-state lithium-sulfur batteries(ASSLSBs)have garnered significant attention due to their inherent safety and higher energy density,making them a promising candidate for the upcoming lithium batteries.However,employing sulfur as the active material in all-solid-state composite cathodes introduces two critical challenges:sluggish electrochemical reaction kinetics and insufficient solid-solid contact between the sulfur,conductive additive,and solid electrolyte phases.These issues directly impact battery performance and hinder the commercialization of ASSLSBs.In this comprehensive review,the underlying causes of these issues are first discussed to gain a fundamental understanding of potential improvement directions.Subsequently,we summarize the recent progress in enhancing sulfur reaction kinetics and optimizing solid-solid contact.The fundamental principles,fabrication techniques,and resultant performance enhancement of diverse strategies are systematically categorized,summarized,and evaluated.Finally,the challenges and future outlook of advanced ASSLSB cathode research are discussed at the end of this review.展开更多
基金supported by the Australian Research Council via Discovery Projects(Nos.DP200103315,DP200103332 and DP230100685)Linkage Projects(No.LP220200920)+1 种基金support from the IONTOF M6 ToF-SIMS(funded by ARC LIEF,LE190100053)the Kratos Axis Ultra XPS(ARC LIEF,LE120100026)。
文摘Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.In this study,we propose an entropy-assisted multi-element doping strategy to mitigate these issues.Specifically,two routes are designed and compared:bulk-like localized high-entropy doping(BHE-NCM)and surface-distributed high-entropy-zone doping(SHE-NCM).The surface entropy-doped NCM cathode delivers enhanced electrochemical performance,including higher capacity retention under 4.5 V cycling and superior rate capability,compared to both bulk-like and pristine counterparts.Comprehensive material characterization reveals that surface-localized doping stabilizes the layered structure with reduced microcrack formation and creates a uniform dopant-rich surface region with improved thermal and electrochemical stability.Overall,entropy-assisted doping at the near surface zone effectively alleviates structural degradation and interface reactions in Ni-rich NCM,enabling improved cycling performance at high voltage.This work highlights the significance of surface entropy engineering as a promising strategy for designing high-voltage cathodes with improved safety and longevity.
基金National Natural Science Foundation of China (61761047 and 41876055)Program for Innovative Research Team (in Science and Technology) in University of Yunnan Province。
文摘Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn^(2+)diffusion kinetics.By employing electrodeposition to coat MoS_(2)on the surface of BaV_(6)O_(16)·3H_(2)O nanowires,the directional builtin electric field generated at the heterointerface acts as a cation accelerator,continuously accelerating Zn^(2+)diffusion into the active material.The optimized Zn^(2+)diffusion coefficient in CC@BaV-V_(6)O_(16)·3H_(2)@MoS_(2)(7.5×10^(8)cm^(2)s^(-1)) surpasses that of most reported V-based cathodes.Simultaneously,MoS_(2)serving as a cathodic armor extends the cycling life of the Zn-CC@BaV_(6)O_(16)·3H_(2)@MoS_(2)full batteries to over 10000 cycles.This work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.
基金supported by the research funds from South-Central University for Nationalities(Grant No.YZZ19001)financial support from the National Natural Science Foundation of China(51873233)the Hubei Provincial Natural Science Foundation(2018CFA023)。
文摘Aqueous zinc-ion batteries(AZIBs)are an appealing battery system due to their low cost,intrinsic safety,and environmental-friendliness,while their application is plagued by the obstacles from the cathode,electrolyte,and zinc anode.Summarizing the design principles and strategies toward the optimization of cathode,electrolyte,and zinc anode is crucial for the development of AZIBs.Herein,we present a comprehensive analysis of the design principles and promising strategies toward the improvement of AZIBs.Firstly,the various reaction mechanisms are summarized and the existing issues associated with the cathode,electrolyte,and zinc anode are discussed to guide the rational design of AZIBs.Subsequently,we provide an in-depth and comprehensive discussion on the design principles and strategies for the electrodes/electrolyte/separator optimization,and analyze the advantages and disadvantages of various strategies.Importantly,the design principles and strategies of the newly appeared conversion-type AZIBs,such as Zn-S battery and Zn-Se battery,are also discussed and analyzed.The effect of design strategies on the electrochemical performance and the relationship between the current issues and strategies are also unveiled in detail.Finally,some research trends and perspectives are provided for designing better AZIBs.
基金supported by the National Natural Science Foundation of China(U22A20118)the Natural Science Foundation of Fujian Province(2023J01400)。
文摘Inorganic solid electrolyte-based all-solid-state lithium-sulfur batteries(ASSLSBs)have garnered significant attention due to their inherent safety and higher energy density,making them a promising candidate for the upcoming lithium batteries.However,employing sulfur as the active material in all-solid-state composite cathodes introduces two critical challenges:sluggish electrochemical reaction kinetics and insufficient solid-solid contact between the sulfur,conductive additive,and solid electrolyte phases.These issues directly impact battery performance and hinder the commercialization of ASSLSBs.In this comprehensive review,the underlying causes of these issues are first discussed to gain a fundamental understanding of potential improvement directions.Subsequently,we summarize the recent progress in enhancing sulfur reaction kinetics and optimizing solid-solid contact.The fundamental principles,fabrication techniques,and resultant performance enhancement of diverse strategies are systematically categorized,summarized,and evaluated.Finally,the challenges and future outlook of advanced ASSLSB cathode research are discussed at the end of this review.
