High-performance lithium–sulfur battery based on porous N-rich g-C3N4 nan-otubes via a self-template method

The commercial development of lithium–sulfur batteries (Li–S) is severely limited by the shuttle effect of lithium polysulfides (LPSs) and the non-conductivity of sulfur. Herein, porous g-C3N4 nanotubes (PCNNTs) are synthesized via a self-template method and util-ized as an efficient sulfur host material. The one-dimensional PCNNTs have a high specific surface area (143.47 m2·g?1) and an abundance of macro-/mesopores, which could achieve a high sulfur loading rate of 74.7wt%. A Li–S battery bearing the PCNNTs/S composite as a cathode displays a low capacity decay of 0.021% per cycle over 800 cycles at 0.5 C with an initial capacity of 704.8 mAh·g?1. PCNNTs with a tubular structure could alleviate the volume expansion caused by sulfur and lithium sulfide during charge/discharge cycling. High N contents could greatly enhance the adsorption capacity of the carbon nitride for LPSs. These synergistic effects contribute to the excellent cycling stability and rate performance of the PCNNTs/S composite electrode.     

CoO/SnO2@NC/S复合材料的制备及其应用于高稳定性锂硫电池正极材料

To improve the sulfur loading capacity of lithium-sulfur batteries (Li–S batteries) cathode and avoid the inevitable “shuttle effect”, hollow N doped carbon coated CoO/SnO₂ (CoO/SnO₂@NC) composite has been designed and prepared by a hydrothermal-calcination method. The specific surface area of CoO/SnO₂@NC composite is 85.464 m2·g–1, and the pore volume is 0.1189 cm3·g–1. The hollow core-shell structure as a carrier has a sulfur loading amount of 66.10%. The initial specific capacity of the assembled Li–S batteries is 395.7 mAh·g–1 at 0.2 C, which maintains 302.7 mAh·g–1 after 400 cycles. When the rate increases to 2.5 C, the specific capacity still has 221.2 mAh·g–1. The excellent lithium storage performance is attributed to the core-shell structure with high specific surface area and porosity. This structure effectively increases the sulfur loading, enhances the chemical adsorption of lithium polysulfides, and reduces direct contact between CoO/SnO₂ and the electrolyte.     

先进能源储存和转换材料专刊社论

The ever-increasing environmental problems and energy challenges have called urgent demand for utilizing green, ef-ficient, and sustainable energy, thus promoting the develop-ment of new technologies associated with energy storage and conversion systems. Amongst a wealth of energy storage devices, Li/Na/K/Zn/Mg ion batteries, metal-air batteries, and lithium–sulfur/all-solid-state batteries together with su-percapacitors as advanced power sources have attracted con-siderable interest due to their conspicuous merits of high en-ergy density, long cycle life, and good rate capability. In the energy conversion systems, solar cells and fuel cells can be considered as mainstream renewable energy resources once their manufacturing cost has decreased to an affordable level. However, the developments of advanced power sources de-pend critically on advances in materials innovation. There-fore, to promote the practical applications of these promising systems, developing high-performance electrode materials has been taken into the center stage in current research areas from chemistry, physics, and materials science fields.     

Application prospects of high-voltage cathode materials in all-solid-state lithium-ion batteries

All-solid-state lithium-ion batteries are lithiumion batteries with solid-state electrolytes instead of liquid electrolytes.They are hopeful in solving the safety problems of lithium-ion batteries,once their large capacity and long life are achieved,they will have broad application prospects in the field of electric vehicles and large-scale energy storage.The working potential window of solid electrolytes is wider than that of liquid electrolytes,so high-voltage cathode materials could be used in all-solidstate lithium-ion batteries to get higher energy density and larger capacity by elevating the working voltage of the batteries.The spinel LiNi0.5Mn1.5O4material,layered Li–Ni–Co–Mn–O cathode materials and lithium-rich cathode materials can be expected to be applied to all-solid-state lithium-ion batteries as cathode materials due to their highvoltage platforms.In this review,the electrochemical properties and structures of spinel LiNi0.5Mn1.5O4material,layered Li–Ni–Co–Mn–O cathode materials and lithiumrich cathode materials are introduced.More attentions are paid on recent research progress of conductivity and interface stability of these materials,in order to improve their compatibility with solid electrolytes as cathode materials in all-solid-state lithium-ion batteries and fully improve the properties of all-solid-state batteries.Finally,the existing problems of their application in all-solid-state lithium-ion batteries are summarized,the main research directions are put forward and their application prospects in all-solid-state lithium-ion batteries are discussed.     

In Situ XRD and XAS Investigation of Cathode Materials in Li-ion Battery

1 Results Lithium ion batteries have been widely used in modern portable electronics,such as cellular phones and notebook computers,because of their low cost,long life,and high energy density.In the lithium ion batteries,the cathode provides lithium ion source and plays a critical role to determinate the performance of battery.Lithium transition metal oxides have been investigated as active cathode materials due to their high potential versus Li/Li and large proportion of the lithium ions can be insert...     

MXenes电催化析氢的研究进展

面向“碳达峰”“碳中和”国家重大战略,氢能作为一种能量密度高、无污染的绿色能源,将成为我国乃至世界未来能源战略领域发展的重中之重.电解水制氢由于其制备方法简单、制氢纯度高、制备过程无污染等优势而备受关注,但是该方法存在一个严重的缺陷,就是缺乏低成本、高效率析氢反应(HER)催化剂.MXenes是一种新兴的二维(2D)过渡金属碳化物、氮化物和碳氮化物,由于其具有极好的导电性、良好的亲水性、极大的比表面积、可调节的分子结构及多样的化学组成等优势,在析氢催化剂领域存在着潜在的巨大应用.该文总结了 MXenes制备、MXenes基电催化析氢性能调控策略及利用机器学习设计MXenes基析氢电催化剂面临的挑战和新的机遇.该文为今后开发新型高效的MXenes基析氢电催化剂,推动氢能的绿色制备提供了参考.     

富镍三元层状过渡金属氧化物正极材料的改性方法研究综述

富镍三元层状过渡金属氧化物正极材料因具有比容量高、价格低廉以及对环境友好等特性而备受关注,但受锂镍混排、相变反应、产气、微裂纹、过渡金属溶出、表面结构等影响,材料本身存在循环容量衰减等问题。针对正极材料循环容量衰减过快、高温性能不佳等问题,总结了近年来国内外关于富镍三元层状过渡金属氧化物正极材料的改性方法,包括表面包覆材料合成、元素掺杂材料制备、核壳结构材料开发、浓度梯度材料设计等优化方法,指出高镍层状过渡金属氧化物正极材料的应用需要从不断完善材料制备方法、改变材料性状、降低材料成本等方面入手,开发高能量密度的锂离子电池,使富镍三元层状过渡金属氧化物正极材料在动力电池领域尽早得到广泛应用。     

A deformable spinel-type chloride cathode with high ionic conductivity for all-solid-state Li batteries

All-solid-state Li batteries (ASSLBs) are now considered to be next-generation energy storage devices due to their advantages in safety and energy density. With liquid electrolytes replaced by solid electrolytes, novel cathode active materials (CAMs) with different characteristics are needed. The solid-solid contact in ASSLBs requires CAMs to have good deformability. In addition, higher ionic conductivity is also essential to reduce the mass of the Li-ion conductive agent, thus accessing a higher overall capacity. Herein, we report a spinel-type chloride cathode Li_2?2xMn_1?xZr_xCl₄, which has good deformability and high ionic conductivity (up to 0.16 mS?cm?1 at 25 °C). The ASSLB using the optimal composition of LiMn_0.5Zr_0.5Cl₄ as the cathode exhibits promising cycling stability for 200 cycles at room temperature.     

Practical development and challenges of garnet-structured Li7La3Zr2O12 electrolytes for all-solid-state lithium-ion batteries: A review

All-solid-state Li-ion batteries (ASSLIBs) have been widely studied to achieve Li-ion batteries (LIBs) with high safety and energy density. Recent reviews and experimental papers have focused on methods that improve the ionic conductivity, stabilize the electrochemical performance, and enhance the electrolyte/electrode interfacial compatibility of several solid-state electrolytes (SSEs), including oxides, sulf-ides, composite and gel electrolytes, and so on. Garnet-structured Li7La3Zr2O12 (LLZO) is highly regarded an SSE with excellent application potential. However, this type of electrolyte also possesses a number of disadvantages, such as low ionic conductivity, unstable cubic phase, and poor interfacial compatibility with anodes/cathodes. The benefits of LLZO have urged many researchers to explore effective solutions to over-come its inherent limitations. Herein, we review recent developments on garnet-structured LLZO and provide comprehensive insights to guide the development of garnet-structured LLZO-type electrolytes. We not only systematically and comprehensively discuss the preparation, ele-ment doping, structure, stability, and interfacial improvement of LLZOs but also provide future perspectives for these materials. This review expands the current understanding on advanced solid garnet electrolytes and provides meaningful guidance for the commercialization of ASSLIBs.     

钠离子电池电解质的研究进展

相比锂离子电池来说,钠离子电池因高能量密度和低成本引起广泛关注。作为电池重要组成部分的电解质,对电池性能的发挥至关重要。简要介绍了液、固态电解质体系在钠离子电池中的研究进展,讨论这些电解质体系的电导率、电性能、电化学性能、热稳定性等特点。现今钠离子电池大多使用的是液体电解液,而液体电解液在具有高离子电导率的同时,安全性仍有待改善。而固态电解质还有许多基础科学需要探索,并且需要考虑电导率、成本等因素。基于以上评述,希望对钠离子电池电解质的研究发展提供帮助。     

Development and application of phase diagrams for Li-ion batteries using CALPHAD approach

Phase diagrams provide fundamental knowledge about design map of new electrode materials for Li-ion batteries. The CALPHAD (CALculation of PHAse Diagrams) approach is widely applied to the development of phase diagrams and property diagrams in a thermodynamic language. Within the CALPHAD framework, the theoretical modeling can be performed to predict phase equilibria, thermodynamics, electrochemical and physical properties of electrodes. This review provides the successful application of high quality calculated phase diagrams and thermodynamic property diagrams in CALPHAD investigation to both cathodes and anodes of Li-ion batteries, including Li–Co–O, Li–Ni–O, Li–Co–Ni–O, Li–Mn–O, Li–Cu–O, Li–Si, Li–Sb and Li–Sn systems with. The intensive CALPHAD-type research may also predict electrochemical properties, cell performance of the Li-ion batteries to achieve more efficient development of electrode materials.     

钛基材料用于锂硫电池正极改性研究进展

锂硫电池因其高比容量、高能量密度和低成本等特点已被视为超越锂离子电池的下一代可充电电池。由于反应产物可溶性多硫化物的穿梭效应和循环中硫电极的体积膨胀导致电池的循环寿命较差。为了解决锂硫电池中存在的问题,研究人员开发了多种纳米结构的金属材料。总结了利用钛元素和钛基化合物（包括钛基氧化物、钛基硫化物和钛基氮化物）与硫的反应形成牢固化学键,通过金属基复合材料的结构设计来提升锂硫电池的综合性能。     

超支化聚三唑固态聚电解质及其锂离子和锌离子导电性

带刚性结构的超支化聚合物具有优良的溶解性，度低黏与力学性能优异，可用于制备固态电解质.含叠氮基的单体M1和含炔基的单体M2在亚铜离子Cu⁺的催化下发生叠氮-炔点击化学反应，得到超支化聚三唑hb-GPTA.该聚合物具有良好的溶解性、成膜性和热稳定性（热分解温度为350 ℃）.将该聚合物分别与三氟甲基磺酰亚胺锂 (LiTFSI)及三氟甲基磺酸锌 (Zn(OTf)₂)进行掺杂，制备固态电解质，对其电化学性能进行表征.结果表明，hb-GPTA/LiTFSI体系具有更高的电导率（32.7 μ S·cm^-1），电化学窗口为5.2 V；相比之下，hb-GPTA/Zn（OTf）₂体系电导率较低（0.42 μS·cm^-1），但其在-1~6 V电压范围内一直保持稳定.结合电化学稳定性分析结果，可以推断含三氮唑的聚合物在制作锌离子电池方面具有潜在的应用价值.     

超支化聚三唑固态聚电解质及其锂离子和锌离子导电性

带刚性结构的超支化聚合物具有优良的溶解性，度低黏与力学性能优异，可用于制备固态电解质.含叠氮基的单体M1和含炔基的单体M2在亚铜离子Cu⁺的催化下发生叠氮-炔点击化学反应，得到超支化聚三唑hb-GPTA.该聚合物具有良好的溶解性、成膜性和热稳定性（热分解温度为350 ℃）.将该聚合物分别与三氟甲基磺酰亚胺锂 (LiTFSI)及三氟甲基磺酸锌 (Zn(OTf)₂)进行掺杂，制备固态电解质，对其电化学性能进行表征.结果表明，hb-GPTA/LiTFSI体系具有更高的电导率（32.7 μ S·cm^-1），电化学窗口为5.2 V；相比之下，hb-GPTA/Zn（OTf）₂体系电导率较低（0.42 μS·cm^-1），但其在-1~6 V电压范围内一直保持稳定.结合电化学稳定性分析结果，可以推断含三氮唑的聚合物在制作锌离子电池方面具有潜在的应用价值.     

LiSiPON固态薄膜电解质的结构和性能分析

以Li3PO4和Si3N4为靶材,利用离子束辅助沉积N离子流轰击法制备非晶结构的固态电解质LiSiPON薄膜.实验中,通过控制N2气和Ar气的流量比,调节薄膜的含氮量.利用X线衍射、X线能量色散谱仪和X线光电子能谱仪研究薄膜的结构和组织成分的变化,并通过电化学阻抗测试仪获得薄膜的离子电导率,研究不同氮氩比对LiSiPON薄膜结构、组成和电学性质的影响.结果表明:N2和Ar流量比为1∶1时,薄膜含氮量最高,离子电导率达到最大值,在室温时电解质薄膜的离子电导可达6.8×10-6S/cm,是一种有潜力应用于全固态薄膜锂离子电池的电解质材料.     

Metal–air batteries: A review on current status and future applications

Metal–air batteries(MABs) have been paid much more attention owing to their greater energy density than the most advanced lithium-ion batteries(LIBs). Rechargeable MABs are considered as promising candidates for the next-generation of energy storage techniques for applications ranging from large-scale energy storage systems to electric vehicles and portable devices. However, there are still numerous scientific problems that must be overcome before their commercial application. With the aim of pr...     

Nano-sized transition-metal oxides as negative-electrode materials for lithium-ion batteries

Rechargeable solid-state batteries have long been considered an attractive power source for a wide variety of applications, and in particular, lithium-ion batteries are emerging as the technology of choice for portable electronics. One of the main challenges in the design of these batteries is to ensure that the electrodes maintain their integrity over many discharge-recharge cycles. Although promising electrode systems have recently been proposed, their lifespans are limited by Li-alloying agglomeration or the growth of passivation layers, which prevent the fully reversible insertion of Li ions into the negative electrodes. Here we report that electrodes made of nanoparticles of transition-metal oxides (MO, where M is Co, Ni, Cu or Fe) demonstrate electrochemical capacities of 700 mA h g(-1), with 100% capacity retention for up to 100 cycles and high recharging rates. The mechanism of Li reactivity differs from the classical Li insertion/deinsertion or Li-alloying processes, and involves the formation and decomposition of Li2O, accompanying the reduction and oxidation of metal nanoparticles (in the range 1-5 nanometres) respectively. We expect that the use of transition-metal nanoparticles to enhance surface electrochemical reactivity will lead to further improvements in the performance of lithium-ion batteries.     

A black phosphorus-graphite hybrid as a Li-ion regulator enabling stable lithium deposition

Lithium (Li) metal anodes have been regarded as the most promising candidates for high energy density secondary lithium batteries due to their high specific capacity and low redox potential. However, the issues of Li dendrites caused by nonuniform lithium deposition during battery cycling severely hinder the practical applications of Li metal anodes. Herein, a hybrid of black phosphorus-graphite (BP-G) is introduced to serve as an artificial protective layer for the Li metal anode. The two-dimensional few-layer BP, which is lithophilic, combined with the high electronic conductive graphite can act as a regulator to adjust the migration of Li ions, delivering a uniform and stable lithium deposition. As the growth of lithium dendrites is inhibited, the utilization of Li metal achieves > 98.5% for over 500 cycles in Li||Cu half cells, and the life span is maintained over 2000 h in Li||Li symmetric cells with a low voltage hysteresis of 50 mV. Moreover, the LiFePO₄||Li full cell with a BP-G Li-ion regulator presents significantly better specific capacity and cycling stability than that with the bare Li metal anode. Therefore, the introduction of the BP-G Li-ion regulator is demonstrated to be an effective approach to enable stable lithium deposition for rechargeable Li metal batteries.     

Synthesis and Electrochemical Properties of Nanostructured Cathode Materials for Lithium Batteries

1 Results For electrode materials in lithium batteries,a high surface area can provide higher electrode/electrolyte contact areas,thus eventually causing the shorter diffusion paths with the particles,and provides more facile intercalation for Li ions[1-4].In addition,reduced strain of intercalation and contributions from charge storage at the surface may also contribute to Li capacity,compared with bulk counterparts.In this regard,I am going to talk about the preparation and electrochemical properties o...     

Anion-immobilized solid composite electrolytes based on metal-organic frameworks and superacid ZrO2 fillers for high-performance all solid-state lithium metal batteries

Anion-immobilized solid composite electrolytes (SCEs) are important to restrain the propagation of lithium dendrites for all solid-state lithium metal batteries (ASSLMBs). Herein, a novel SCEs based on metal-organic frameworks (MOFs, UiO-66-NH2) and superacid ZrO2 (S-ZrO2) fillers are proposed, and the samples were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive X-ray spectroscopy (EDS), thermo-gravimetric analyzer (TGA) and some other electrochemical measurements. The –NH2 groups of UiO-66-NH2 combines with F atoms of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) chains by hydrogen bonds, leading to a high electrochemical stability window of 5 V. Owing to the incorporation of UiO-66-NH2 and S-ZrO2 in PVDF-HFP polymer, the open met-al sites of MOFs and acid surfaces of S-ZrO2 can immobilize anions by strong Lewis acid-base interaction, which enhances the effect of im-mobilization anions, achieving a high Li-ion transference number (t+) of 0.72, and acquiring a high ionic conductivity of 1.05×10–4 S·cm–1 at 60°C. The symmetrical Li/Li cells with the anion-immobilized SCEs may steadily operate for over 600 h at 0.05 mA·cm–2 without the short-circuit occurring. Besides, the solid composite Li/LiFePO4 (LFP) cell with the anion-immobilized SCEs shows a superior discharge specific ca-pacity of 158 mAh·g–1 at 0.2 C. The results illustrate that the anion-immobilized SCEs are one of the most promising choices to optimize the performances of ASSLMBs.