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Localized high-concentration electrolytes for lithium metal batteries: progress and prospect

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1354-1371 doi: 10.1007/s11705-022-2286-4

摘要： With the increasing development of digital devices and electric vehicles, high energy-density rechargeable batteries are strongly required. As one of the most promising anode materials with an ultrahigh specific capacity and extremely low electrode potential, lithium metal is greatly considered an ideal candidate for next-generation battery systems. Nevertheless, limited Coulombic efficiency and potential safety risks severely hinder the practical applications of lithium metal batteries due to the inevitable growth of lithium dendrites and poor interface stability. Tremendous efforts have been explored to address these challenges, mainly focusing on the design of novel electrolytes. Here, we provide an overview of the recent developments of localized high-concentration electrolytes in lithium metal batteries. Firstly, the solvation structures and physicochemical properties of localized high-concentration electrolytes are analyzed. Then, the developments of localized high-concentration electrolytes to suppress the formation of dendritic lithium, broaden the voltage window of electrolytes, enhance safety, and render low-temperature operation for robust lithium metal batteries are discussed. Lastly, the remaining challenges and further possible research directions for localized high-concentration electrolytes are outlined, which can promisingly render the practical applications of lithium metal batteries.

关键词： high-concentration electrolyte localized high-concentration electrolyte lithium metal battery solid electrolyte interphase dendrite

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A review on the development of electrolytes for lithium-based batteries for low temperature applications

《能源前沿（英文）》 2023年第17卷第1期页码 43-71 doi: 10.1007/s11708-022-0853-5

摘要： The aerospace industry relies heavily on lithium-ion batteries in instrumentation such as satellites and land rovers. This equipment is exposed to extremely low temperatures in space or on the Martian surface. The extremely low temperatures affect the discharge characteristics of the battery and decrease its available working capacity. Various solvents, cosolvents, additives, and salts have been researched to fine tune the conductivity, solvation, and solid-electrolyte interface forming properties of the electrolytes. Several different resistive phenomena have been investigated to precisely determine the most limiting steps during charge and discharge at low temperatures. Longer mission lifespans as well as self-reliance on the chemistry are now highly desirable to allow low temperature performance rather than rely on external heating components. As Martian rovers are equipped with greater instrumentation and demands for greater energy storage rise, new materials also need to be adopted involving next generation lithium-ion chemistry to increase available capacity. With these objectives in mind, tailoring of the electrolyte with higher-capacity materials such as lithium metal and silicon anodes at low temperatures is of high priority. This review paper highlights the progression of electrolyte research for low temperature performance of lithium-ion batteries over the previous several decades.

关键词： electrolyte lithium-ion low temperature aerospace solid-electrolyte interface

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Ion conduction path in composite solid electrolytes for lithium metal batteries: from polymer rich to

Zhouyu ZHANG, Hao CHEN, Zhenglin HU, Shoubin ZHOU, Lan ZHANG, Jiayan LUO

《能源前沿（英文）》 2022年第16卷第5期页码 706-733 doi: 10.1007/s11708-022-0833-9

摘要： Solid-state electrolytes (SSEs) can address the safety issue of organic electrolyte in rechargeable lithium batteries. Unfortunately, neither polymer nor ceramic SSEs used alone can meet the demand although great progress has been made in the past few years. Composite solid electrolytes (CSEs) composed of flexible polymers and brittle but more conducting ceramics can take advantage of the individual system for solid-state lithium metal batteries (SSLMBs). CSEs can be largely divided into two categories by the mass fraction of the components: “polymer rich” (PR) and “ceramic rich” (CR) systems with different internal structures and electrochemical properties. This review provides a comprehensive and in-depth understanding of recent advances and limitations of both PR and CR electrolytes, with a special focus on the ion conduction path based on polymer-ceramic interaction mechanisms and structural designs of ceramic fillers/frameworks. In addition, it highlights the PR and CR which bring the leverage between the electrochemical property and the mechanical property. Moreover, it further prospects the possible route for future development of CSEs according to their rational design, which is expected to accelerate the practical application of SSLMBs.

关键词： composite solid electrolytes active filler/framework ion conduction path interphase compatibility multilayer design

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Recent advances toward high voltage, EC-free electrolytes for graphite-based Li-ion battery

Tong Zhang, Elie Paillard

《化学科学与工程前沿（英文）》 2018年第12卷第3期页码 577-591 doi: 10.1007/s11705-018-1758-z

摘要：

Lithium-ion batteries are a key technology in today’s world and improving their performances requires, in many cases, the use of cathodes operating above the anodic stability of state-of-the-art electrolytes based on ethylene carbonate (EC) mixtures. EC, however, is a crucial component of electrolytes, due to its excellent ability to allow graphite anode operation–also required for high energy density batteries–by stabilizing the electrode/electrolyte interface. In the last years, many alternative electrolytes, aiming at allowing high voltage battery operation, have been proposed. However, often, graphite electrode operation is not well demonstrated in these electrolytes. Thus, we review here the high voltage, EC-free alternative electrolytes, focusing on those allowing the steady operation of graphite anodes. This review covers electrolyte compositions, with the widespread use of additives, the change in main lithium salt, the effect of anion (or Li salt) concentration, but also reports on graphite protection strategies, by coatings or artificial solid electrolyte interphase (SEI) or by use of water-soluble binder for electrode processing as these can also enable the use of graphite in electrolytes with suboptimal intrinsic SEI formation ability.

关键词： lithium-ion electrolyte solid electrolyte interphase additives high voltage graphite

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零相频下离子导体的焦耳加热及其电解反应抑制 Letter

石磊, 韩宗益, 冯逸轩, 张长庚, 张祺, 朱贺, 朱世平

《工程（英文）》 2023年第25卷第6期页码 138-143 doi: 10.1016/j.eng.2022.03.004

摘要：

It is well known that heat is generated when an electric current passes through an electrical conductor. While various applications in our daily lives and industries utilize the heating of electronic conductors, little attention has been paid to the potential of ionic conductors for heating purposes. This is because of the “inevitable” electrochemical reactions, which can result in unwanted electrolysis of conductors, corrosion of electrodes, and surface fouling. This paper reports the Joule heating of ionic conductors without electrochemical reactions. Electricity with a zero-phase frequency is employed to suppress the electrolysis of ionic conductors at high voltages. Demonstrations with various ionic conductors, both liquids and solids, show highly efficient energy conversion free of electrochemical reactions. This heating method is simple, direct, fast, clean, and uniform, and it has great potential in numerous industrial and household applications.

关键词： Joule heating Ionic conductors Electrolytes Zero-phase frequency Electrochemical corrosion

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钠超离子导体型固体电解质的改性及其在钠离子电池中的应用 Article

张强强, 周权, 陆雅翔, 邵元骏, 戚钰若, 戚兴国, 钟贵明, 杨勇, 陈立泉, 胡勇胜

《工程（英文）》 2022年第8卷第1期页码 170-180 doi: 10.1016/j.eng.2021.04.028

摘要：

固体电解质的低离子电导率及固体电解质与固态电极之间较差的界面可靠性是阻碍固态钠电池（SSSB）应用的两大紧迫挑战。本文采用简单的两步固相法合成了名义成分为Na_3+2xZr_2‒xMg_xSi₂PO₁₂ 的钠（Na）超离子导体（NASICON）型固体电解质，其中在25 ℃时Na_3.3Zr_1.85Mg_0.15Si₂PO₁₂（x=0.15, NZSP-Mg_0.15)表现出了3.54 mS∙cm^‒1的最高离子电导率。通过深入研究，本文证实晶界成分在决定NASICON总离子电导率中起着至关重要的作用。此外，由于文献中缺乏关于NASICON是否能够提供足够的阳极电化学稳定性来实现高压固态钠电池的研究，我们首先使用了高压Na₃(VOPO₄)₂F (NVOPF)正极来验证其与优化后的NZSP-Mg_0.15固体电解质之间的兼容性。通过比较不同配置（低压阴极与高压阴极、液态电解质与固体电解质）电池的电化学性能，以及对循环后的NZSP-Mg_0.15进行X射线光电子能谱（XPS）评估，结果表明，NASICON固体电解质在高电压下不够稳定，这证明了研究NASICON固体电解质和高压阴极之间界面的重要性。此外，通过将NZSP-Mg_0.15 NASICON 粉末涂在聚乙烯（PE）隔膜（PE@NASICON）上，形成了2.42 A∙h 的碳|PE@NASICON|NaNi_2/9Cu_1/9Fe_1/3Mn_1/3O₂ 非水系钠离子电池，其具有出色的循环性能，在2000 周循环后容量保持率为88%，从而证明涂有NASICON型固体电解质的隔膜具有高可靠性。