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Monophase-homointerface electrodes intrinsically stabilize high-voltage all-solid-state batteries

Science China Chemistry 2024年第5期67卷 1729-1739页

作者： Xiaolin Xiong Xianguo Ma Tianshi Lv liquan chen Liumin Suo Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of ScienceBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

The electrochemical stability and contact reliability of heterointerfaces between the solid electrolyte(SE) and electrode are critical for all-solid-state batteries(ASSBs), particularly much more challenging for high-voltage ASSBs, owing to the limited thermodynamically electrochemical window and mechanical inflexibility of SE, aggravating interfacial side reactions and contact failure. Considering all those issues originating from intrinsic heterogeneity in physicochemical features between the cathode material and SE, we are thinking about simplifying the heterointerfaces into a homointerface as a permanent cure to solve all electrochemical-mechanical interfacial failure. Herein, we propose monophase cathodes to construct thermodynamically stable all-in-one homointerfaces in ASS electrodes, removing unstable heterointerfaces by excluding SEs and intrinsically eliminating the Li chemical potential gap to avoid the formation of lithium-depleted space-charge layer and highly resistive mixed ion–electron conductor interphase. Our conception is successfully validated in the layered transition-metal oxide cathodes, which display outstanding stability no matter the MH-LiCoO_(2) cathode charging to 4.7 V or MH-Li_(1.2)Mn_(0.54)Ni_(0.13)-Co_(0.13)O_(2) cathode charging to 5.3 V. It is undeniable that our current version of above-illustrated MH-cathodes would bring out some new challenges for the practical application due to abandoning the SE. However, we believe our work also offers a brandnew direction to ultimately address the electrochemical–mechanical interfacial issues that would be promising for high-energy ASSBs with more discoveries of advanced monophase cathodes in the future.

关键词： monophase-homointerface electrode high-voltage all-solid-state batteries electrochemical-mechanical interfacial issue

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Anode Interfacial Issues in Solid-State Li Batteries:Mechanistic Understanding and Mitigating Strategies

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Energy & Environmental Materials 2023年第4期6卷 384-404页

作者： Jiacheng Wang liquan chen Hong Li Fan Wu Tianmu Lake Institute of Advanced Energy Storage Technologies Liyang 213300China Henry Royce Institute and Department of Materials School of Natural SciencesThe University of ManchesterManchester M139PLUK Yangtze River Delta Physics Research Center Liyang 213300China Beijing Advanced Innovation Center for Materials Genome Engineering Key Laboratory for Renewable EnergyBeijing Key Laboratory for New Energy Materials and DevicesInstitute of PhysicsChinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China Nano Science and Technology Institute University of Science and Technology of ChinaSuzhou 215123China

All-solid-state Li metal batteries(ASSLBs)using inorganic solid electrolyte(SE)are considered promising alternatives to conventional Li-ion batteries,offering improved safety and boosted energy density.While significant progress has been made on improving the ionic conductivity of SEs,the degradation and instability of Li metal/inorganic SE interfaces have become the critical challenges that limit the coulombic efficiency,power performance,and cycling stability of ASSLBs.Understanding the mechanisms of complex/dynamic interfacial phenomena is of great importance in addressing these issues.Herein,recent studies on identifying,understanding,and solving interfacial issues on anode side in ASSLBs are comprehensively reviewed.Typical issues at Li metal/SE interface include Li dendrite growth/propagation,SE cracking,physical contact loss,and electrochemical reactions,which lead to high interfacial resistance and cell failure.The causes of these issues relating to the chemical,physical,and mechanical properties of Li metal and SEs are systematically discussed.Furthermore,effective mitigating strategies are summarized and their effects on suppressing interfacial reactions,improving interfacial Li-ion transport,maintaining interfacial contact,and stabilizing Li plating/stripping are highlighted.The in-depth mechanistic understanding of interfacial issues and complete investigations on current solutions provide foundations and guidance for future research and development to realize practical application of high-performance ASSLB.

关键词： all-solid-state Li metal batteries anode interfacial issues interface protection and modification interfacial reaction and evolution li dendrite growth

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Air/Water Stability Problems and Solutions for Lithium Batteries

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Energy Material Advances 2022年第1期2022卷 165-205页

作者： Ming Yang liquan chen Hong Li Fan Wu Tianmu Lake Institute of Advanced Energy Storage Technologies Liyang213300 JiangsuChina Nano Science and Technology Institute University of Science and Technology of ChinaSuzhou 215123China Yangtze River Delta Physics Research Center Liyang213300 JiangsuChina Beijing Advanced Innovation Center for Materials Genome Engineering Key Laboratory for Renewable EnergyBeijing Key Laboratory for New Energy Materials and DevicesInstitute of PhysicsChinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China

Recently,lithium-ion batteries(LIBs)have faced bottlenecks in terms of energy/power density and safety issues caused by flammable electrolytes.In this regard,all-solid-state batteries(ASSBs)may be one of the most promising solutions.However,many key battery materials(such as solid electrolytes(SEs),cathodes,and anodes)are unstable to air/water,which greatly limits their production,storage,transportation,practical applications,and the development of ASSBs.Herein,the research status on air/water stability of SEs,cathodes,and anodes is reviewed.The mechanisms for their air/water instability are revealed in details.The corresponding modification methods are also proposed,with emphasis on the construction strategies of air/water stable protective layers,including ex situ coatings and in situ reactions.Moreover,the application of air/water-stable protective layers in ASSBs is discussed correspondingly.Last but not least,the advantages and disadvantages of various protective layer construction strategies are analyzed,in which their applications in practical production are prospected.

关键词： battery protective details

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A Provably Secure and PUF-Based Authentication Key Agreement Scheme for Cloud-Edge IoT

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China Communications 2023年第5期20卷 198-216页

作者： liquan chen Jinlong Wang Bangwei Yin Kunliang Yu Jinguang Han School of Cyber Science and Engineering Southeast UniversityNanjing 210096China Purple Mountain Laboratories Nanjing 211189China

With the exponential growth of intelligent Internet of Things(IoT)applications,Cloud-Edge(CE)paradigm is emerging as a solution that facilitates resource-efficient and timely services.However,it remains an underlying issue that frequent end-edgecloud communication is over a public or adversarycontrolled channel.Additionally,with the presence of resource-constrained devices,it’s imperative to conduct the secure communication mechanism,while still guaranteeing efficiency.Physical unclonable functions(PUF)emerge as promising lightweight security primitives.Thus,we first construct a PUF-based security mechanism for vulnerable IoT devices.Further,a provably secure and PUF-based authentication key agreement scheme is proposed for establishing the secure channel in end-edge-cloud empowered IoT,without requiring pre-loaded master keys.The security of our scheme is rigorously proven through formal security analysis under the random oracle model,and security verification using AVISPA tool.The comprehensive security features are also elaborated.Moreover,the numerical results demonstrate that the proposed scheme outperforms existing related schemes in terms of computational and communication efficiency.

关键词： Internet of Things end-edge-cloud orchestration secure communication physical unclonable function authentication key agreement

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Electrolyte and current collector designs for stable lithium metal anodes

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International Journal of Minerals,Metallurgy and Materials 2022年第5期29卷 953-964页

作者： Simeng Zhang Gaojing Yang Xiaoyun Li Yejing Li Zhaoxiang Wang liquan chen Key Laboratory for Renewable Energy Chinese Academy of SciencesBeijing Key Laboratory for New Energy Materials and DevicesInstitute of PhysicsChinese Academy of SciencesBeijing 100190China College of Materials Science and Opto-Electronic Technology University of Chinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100190China

With the increasing demand for high energy-density batteries for portable electronics and large-scale energy storage systems,the lithium metal anode(LMA)has received tremendous attention because of its high theoretical capacity and low redox potential.However,the commercial application of LMAs is impeded by the uncontrolled growth of lithium dendrites.Such dendrite growth may result in internal short circuits,detrimental side reactions,and the formation of dead lithium.Therefore,the growth of lithium metal must be controlled.This article summarizes our recent efforts in inhibiting such dendrite growth,decreasing the detrimental side reactions,and elongating the LMA lifespan by optimizing the electrolyte structure and by designing appropriate current collectors.After identifying that the unstable solid electrolyte inter-face(SEI)film is responsible for the potential dropping in carbonate electrolytes,we developed LiPF_(6)-LiNO_(3) dual-salt electrolyte and lithium bis(fluorosulfonyl)imide(LiFSI)-carbonate electrolyte to stabilize the SEI film of LMAs.In addition,we achieved controlled lithium depos-ition by designing the structure and material of the current collectors,including selective lithium deposition in porous current collectors,lithio-philic metal guided lithium deposition,and iron carbide induced underpotential lithium deposition in nano-cavities.The limitations of the cur-rent strategies and prospects for future research are also presented.

关键词： lithium metal anode electrolyte current collector lithium dendrite solid electrolyte interface

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A One-Time Pad Encryption Scheme Based on Efficient Physical-Layer Secret Key Generation for Intelligent IoT System

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China Communications 2022年第7期19卷 185-196页

作者： liquan chen Kailin Cao Tianyu Lu Yi Lu Aiqun Hu School of Cyber Science and Engineering Southeast UniversityNanjing 210096China Purple Mountain Laboratories Nanjing 211189China National Mobile Communications Research Laboratory Southeast UniversityNanjing 210096China

The one-time pad(OTP)is an applicationlayer encryption technique to achieve the informationtheoretic security,and the physical-layer secret key generation(SKG)technique is a promising candidate to provide the random keys for OTP.In this paper,we propose a joint SKG and OTP encryption scheme with the aid of a reconfigurable intelligent surface(RIS)to boost secret key rate.To maximize the efficiency of secure communication,we divide the process of secure transmission into two stages:SKG and then encrypted packet transmission.Meanwhile,we design an optimal algorithm for allocating time slots for SKG to maximize SKG efficiency without security risk.Furthermore,we design a key updating protocol based on our SKG scheme for OTP encryption.Simulation results verify that our scheme can generate keys securely and efficiently,and significantly improve the secure communication performance in an intelligent IoT system.

关键词： physical layer security intelligent internet of things one-time pad reconfigurable intelligent surface

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Air Stability of Solid‑State Sulfide Batteries and Electrolytes

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Electrochemical Energy Reviews 2022年第3期5卷 213-258页

作者： Pushun Lu Dengxu Wu liquan chen Hong Li Fan Wu Tianmu Lake Institute of Advanced Energy Storage Technologies Liyang 213300JiangsuChina Yangtze River Delta Physics Research Center Liyang 213300JiangsuChina Beijing Advanced Innovation Center for Materials Genome Engineering Key Laboratory for Renewable EnergyBeijing Key Laboratory for New Energy Materials and DevicesInstitute of PhysicsChinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China

Sulfides have been widely acknowledged as one of the most promising solid electrolytes(SEs)for all-solid-state batteries(ASSBs)due to their superior ionic conductivity and favourable mechanical properties.However,the extremely poor air stability of sulfide SEs leads to destroyed structure/performance and release of toxic H_(2)S gas,which greatly limits mass-production/practical application of sulfide SEs and ASSBs.This review is designed to serve as an all-inclusive handbook for studying this critical issue.First,the research history and milestone breakthroughs of this field are reviewed,and this is followed by an in-depth elaboration of the theoretical paradigms that have been developed thus far,including the random network theory of glasses,hard and soft acids and bases(HSAB)theory,thermodynamic analysis and kinetics of interfacial reactions.Moreover,the characterization of air stability is reviewed from the perspectives of H2S generation,morphology evolution,mass change,component/structure variations and electrochemical performance.Furthermore,effective strategies for improving the air stabilities of sulfide SEs are highlighted,including H_(2)S absorbents,elemental substitution,design of new materials,surface engineering and sulfide-polymer composite electrolytes.Finally,future research directions are proposed for benign development of air stability for sulfide SEs and ASSBs.

关键词： Sulfide solid electrolytes Air stability Superionic conductors All-solid-state batteries

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Improving thermal stability of sulfide solid electrolytes:An intrinsic theoretical paradigm

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InfoMat 2022年第8期4卷 105-120页

作者： Shuo Wang Yujing Wu Hong Li liquan chen Fan Wu Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijingChina University of Chinese Academy of Sciences BeijingChina Tianmu Lake Institute of Advanced Energy Storage Technologies LiyangJiangsuChina Yangtze River Delta Physics Research Center LiyangJiangsuChina Nano Science and Technology Institute University of Science and Technology of ChinaSuzhouChina

All-solid-state batteries(ASSBs)have been widely acknowledged as the key next-generation energy storage technology/device,due to their high safety and energy density.Among all solid electrolytes(SEs)that have been studied for ASSBs,sulfide SEs represent the most promising technical route due to their ultra-high ionic conductivity and desirable mechanical property.However,few results have been reported to study the thermal stability/safety issue of sulfide SEs and ASSBs.Herein,we develop the first-of-its-kind theoretical paradigm and a new conceptual parameter Th to quantitatively calculate/predict the essential thermal stability of sulfide SEs.This theoretical paradigm takes all types of parameters(e.***.crystal structure,localized polyhedra configuration,bond energy,bond type,bond number,normalization factor,and the energy correction factor)into consideration,and more importantly,can be simplified into one straightforward equation for its convenient application in any crystal-line systems.To prove its functionality,the typical experimental strategies(stoichiometric ratio control and elemental doping)are adopted for typical sul-fide SEs(Li7P3S11,Li3PS4)to improve their thermal stabilities,based on the predictions obtained from the derived theory and equation.Moreover,the potential doping elements to improve thermal stability of sulfide SEs are screened throughout the whole periodic table,and the theoretically predicted trends correspond well with experimental evidence.This work may represent the most critical breakthroughs in the research field of thermal stability for sul-fide SEs,not only because it fills the gap of this field,but also due to its precise and quantitative prediction based on a complete consideration of all parameters that determine their thermal stabilities.The handy model devel-oped herein can also be applied to any crystalline materials.

关键词： all-solid-state batteries safety sulfide solid electrolytes theoretical paradigm thermal stability

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Intrinsic effects of precursor functional groups on the Na storage performance in carbon anodes

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Nano Research 2023年第11期16卷 12579-12586页

作者： Xiaohan Tang Fei Xie Yaxiang Lu Zhao chen Xiangfei Li Hong Li Xuejie Huang liquan chen Yuanjiang Pan Yong-Sheng Hu Department of Chemistry Zhejiang UniversityHangzhou 310027China Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China Huairou Division Institute of PhysicsChinese Academy of SciencesBeijing 101400China Yangtze River Delta Physics Research Center Co. Ltd.Liyang 213300China College of Materials Science and Optoelectronic Technology University of Chinese Academy of SciencesBeijing 100049China

The oxygen-containing functional groups in disordered carbon anodes have been widely reported to influence the Na storage performance.However,the effect of original oxygen-containing groups in the precursors on the final structures and electrochemical performance is rarely studied.Herein,we used the anthraquinone derivatives with different oxygen-containing functional groups as precursors to make the disordered carbon anodes for Na-ion batteries(NIBs).Through comprehensive structural and electrochemical analyses,we found that the different types of functional groups in carbon precursors directly affect the cross-linking process during carbonization.The original precursors containing enough inter-chain oxygen or oxygen-containing functional groups with unsaturated bonds unattached to the ring are beneficial for the oxygen atoms to remain or cross-link in structure to result in more C–O–C group,forming nanovoids and disordered structure,which then determine the high performance of the carbon anodes in NIBs.This work highlights the importance of the type/content of functional groups in precursor and provides guidance for the future design of carbon anodes in NIBs from the perspective of precursor selection.

关键词： disordered carbon precursor oxygen-contained functional group Na-ion batteries

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Application of Liquid Metal Electrodes in Electrochemical Energy Storage

Precision Chemistry

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Precision Chemistry 2023年第8期1卷 452-467页

作者： Jian Peng Hong Li liquan chen Fan Wu Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Tianmu Lake Institute of Advanced Energy Storage Technologies LiyangJiangsu 213300China Yangtze River Delta Physics Research Center LiyangJiangsu 213300China

Lithium metal is considered to be the most ideal anode because of its highest energy density,but conventional lithium metal−liquid electrolyte battery systems suffer from low Coulombic efficiency,repetitive solid electrolyte interphase formation,and lithium dendrite growth.To overcome these limitations,dendrite-free liquid metal anodes exploiting composite solutions of alkali metals,aromatics,and ether solvents have been studied.These composite solutions are much easier to control and stabilize than molten alkali metals or alkali metal alloys.Herein,we provide a detailed overview of complex solutions of alkali metals,aromatics,and ether solvents,including their development history,principles,and characteristics.In addition,the obstacles limiting their practical applications and the future research directions are discussed/proposed for the benign development of this field.

关键词： alkali metal liquid metal dendrite composite solutions Li-BP-DME

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