Rechargeable Lithium Batteries Research Articles

Study of a Rechargeable Lithium-Ion Battery Based on a Copper Hexacyanoferrate Cathode

Rechargeable lithium-ion batteries are among the most promising battery technologies to meet energy conversion and storage requirements. However, this technology is still limited due to its high cost, which prevents its use on a large scale. Therefore, cheaper energy storage systems with long cycle life, high power/efficiency, and safety are in great demand and interest. Prussian blue analogs are promising candidates for use in large-scale energy storage applications due to their long-life cycles, high power density, and high energy efficiency [1]. Along with the change of the transition metal, some structural parameters and some fundamental properties of these compounds can be changed, affecting some parameters such as the battery's storage capacity.This work studied the electrochemical insertion of lithium ions into Copper Hexacyanoferrate (CuHCF). This compound was synthesized by a hydrothermal process using a factorial design for determining the significance variables, i. e., precursor concentrations, temperature, and reaction time, on the electrochemical performance of the battery. The samples obtained were characterized by FESEM, TEM, XRD, and TGA. The results show cubic structures with a high degree of crystallinity and an evident dependence of the crystallite size (50 - 140 nm) with the variation of the synthesis conditions. Finally, lithium-ion batteries were measured using a CuHCF cathode (theoretical charge 85.1 mAhg-1). The capacity values depended on the crystallite size, obtaining the best results in the synthesis under lower concentrations, reaction time, and temperature. This sample was submitted to deep charge/discharge cycles at a rate of C/20, where the capacity value was close to 60 mAhg-1 (right image). This demonstrates the influence of the crystallite size on the material's performance, managing to find the optimal synthesis conditions to maximize the battery capacity. References. [1] 1. Marzhana Omarova, Aibolat Koishybay, Nulati Yesibolati, Almagul Mentbayeva, Nurzhan Umirov, Kairat Ismailov, Desmond Adair, Moulay-Rachid Babaa, Indira Kurmanbayeva, Zhumabay Bakenov, Electrochim. Acta, 184 (2015) 58-63. Figure 1

(Battery Division Research Award) A New Perspective on Layered Transition Metal Oxides As Cathode Active Materials

High energy rechargeable lithium batteries (RLBs) continue to be the most favorite choice for vehicle electrification [1]. Among all cathode active materials, layered transition metal oxides containing nickel (Ni), manganese (Mn), or cobalt (Co), remain the most desired to improve energy density and performance [2]. As the current electrolyte system restricts high voltage operation, new cathode active materials with higher capacity are being sought today. How to seek a better cathode active material needs some better guidance as well. Here, a new perspective on the layered transition metal oxide cathode active materials is proposed based on our recent analysis of the performance characteristics of these current cathode active materials that were evaluated or reported in the literature. This new perspective is supposed to provide a more coherent framework to explain their commonality of the performance in realizing higher capacity within the same stability range. With this perspective, the principle of seeking a better cathode active material could be improved with this understanding.

Printable Lithium - LIOVIXTM Assisted All Solid-State Lithium-Ion and Lithium-Metal Batteries for Enhanced Electrochemical Properties

All solid-state lithium-ion and lithium-metal batteries, which utilize a solid electrolyte in place of liquid electrolytes, are considered next-generation devices for energy storage due to their advantages in safety and potentially higher energy density. However, currently many solid-state lithium-ion and lithium-metal batteries are limited by their low Coulombic efficiency, poor power performance, and short cycling life due to the high resistance at the solid-state interfaces. Because of the diverse physical, chemical, and mechanical properties of various solid components in all solid-state batteries as well as the nature of solid-solid contact, many types of interfaces are present in a solid-state battery that can result in loose physical contact, formation of grain boundaries, and undesired chemical and electrochemical side reactions. All of these contribute to increasing resistance at the interface, which diminishes the cell performance, making solid state batteries not suitable for practical application.LIOVIXTM is a unique printable formulation of lithium metal and other specialty materials, which can be used in both lithium-ion and lithium metal-based rechargeable batteries. In the case of lithium-ion batteries, it can be printed on a range of anode materials including silicon-containing anodes for the pre-lithiation process to improve the first cycle columbic efficiency and cell performance. In the case of lithium metal-based batteries, LIOVIXTM can be printed directly onto the current collectors or solid electrolyte separators to fabricate all solid-state batteries utilizing printed lithium metal anodes. This approach has the potential to enable improved performance, safety, recyclability, and lower cost compared to the current advanced lithium-ion systems. In both categories, printable lithium formulation can reduce the interface resistance between the anode and solid electrolyte layer, which enhances the cell performance enabling practical application. The printable lithium formulation is easily scalable using industry standard coating and printing equipment and is adaptable to any anode or cathode chemistry where an independent source of lithium is required. In addition, the lithium loading can be accurately controlled based on the applications’ requirements. We have demonstrated improved electrochemical performance of silicon containing anodes with liquid electrolytes in a full cell format. The present work will demonstrate the concept of all solid-state batteries incorporating printable lithium with enhanced electrochemical properties compared to conventional solid-state batteries.

Electrochemically Dealloyed 3D Porous Copper Nanostructure As High-Performance Anode Current Collector of Li-Metal Batteries

Li metal anode is the ultimate choice for Li batteries owning to its highest theoretical capacity (3806 mAh/g) and lowest redox potential (-3.04 V vs. standard hydrogen electrode) among possible candidates.[1] However, despite the advantages of Li metal anodes, a number of remaining challenges must be addressed before its commercialization: undesired dendrite growth of Li, and irreversible parasitic reactions between Li and electrolyte, etc.Stabilization of Li metal is essential for commercial application of Li metal anodes. In the past few years, several strategies have been developed to suppress Li dendrite growth and stabilize SEI formation during Li plating/stripping processes. Among these strategies, 3D current collectors showed its high potential in Li anode stabilization due to its much larger surface area, which can provide much more Li nucleation sites, alleviate volumetric changes of Li anode, and decrease practical current density. Thus, compared to flat Cu foil used in commercial Li-ion batteries, 3D Cu current collectors can facilitate uniform Li deposition, mitigate Li dendrite growth, and enhance Li cycling stability.[2]Our previous work reported a 3D porous Cu current collector fabricated via a facile one-step electrodeposition method directly on commercial Cu foil. [3] The fabricated 3D porous Cu current collector showed stable long-term cycling with a high areal capacity of 6 mAh/cm2 and no Li dendrite growth was observed during cycling process. However, for the one-step electrodeposition method, the thickness of the porous Cu deposition layer is limited. Thus, preparation of 3D porous Cu layers with both high thickness and high porosity is necessary to further improve the areal capacity of this current collector. Recently, we developed a new two-step electrochemical process to fabricate thick and porous Cu layer: a thick Cu-Zn alloy was first electrodeposited on commercial Cu foil, and Zn was then removed electrochemically, leaving a thick and highly porous 3D Cu layer. Compared to our previous method, this 3D Cu layer has a high thickness of ~14 um and porosity of ~72%. This new 3D Cu current collector can achieve stable Li cycling up to 230 h at high areal capacity of ~10 mAh/cm2 at a high current density of 10 mA/cm2, demonstrated its high commercial application potential in Li-metal batteries. Tarascon, J.M. and M. Armand, Issues and challenges facing rechargeable lithium batteries. Nature, 2001. 414(6861): p. 359-367.Yang, C.P., et al., Accommodating lithium into 3D current collectors with a submicron skeleton towards long-life lithium metal anodes. Nature Communications, 2015. 6.Ma, X., Z. Liu, and H. Chen, Facile and scalable electrodeposition of copper current collectors for high-performance Li-metal batteries. Nano Energy, 2019. 59: p. 500-507.

Next Generation Batteries: Status and Challenges of High Energy Rechargeable Lithium Batteries

Batteries play a critical role in modern society. The electrification of transportation and deep decarbonization of the energy infrastructure require the development and deployment of high energy, low-cost battery materials and technologies. Among the many different battery chemistries investigated, rechargeable batteries using lithium metal anode remain as one of the most feasible approaches for next generation high-performance and low-cost batteries. Here we will discuss and summarize the progresses and status of the research supported by the Battery500 Consortium. The consortium addresses both fundamental level materials and mechanistic problems and cell level integration and manufacturing challenges. The scope includes developing new electrolytes to reduce the side reactions and improve lithium metal deposition/stripping efficiency, improving cathode cycling stability and cathode utilization, understanding and controlling solid electrolyte interfacial reactions, cell design, optimization and validation. The consortium has made significant progress towards high energy cells (>350 Wh kg-1) and stable cycling life (>600 cycles). The research from the consortium also sheds new lights on the degradation and failure mechanisms of high energy lithium cells and the associated the interfacial reactions.

Composite Cathode with High Active Mass Loading for Sulfide-Based All-Solid-State Lithium Batteries

Due to the global warming and resulting environmental regulations, the use of rechargeable lithium batteries is rapidly growing. However, the current lithium-ion batteries (LIBs) employing liquid electrolytes have a safety concern, since the liquid electrolytes are highly flammable, which can lead to a fire or an explosion under abnormal conditions. Accordingly, all-solid-state lithium batteries are considered promising alternatives to current LIBs. Among various types of solid electrolytes, sulfide-based electrolytes exhibit high ionic conductivities at room temperature, comparable with those of liquid electrolytes. In order to improve the energy density of the solid-state batteries, it is essential to increase the loading of active mass in the composite cathode. In this study, we tried to increase the active mass loading by investigating the optimum conditions with respect to types of active materials. As a result, we could obtain good cycling performance of the sulfide-based all-solid-state lithium batteries employing the composite cathode with high active mass loading (> 4.5 mAh cm-2).

(Invited) High-Energy Mn-Rich Disordered Rocksalt Cathodes

In recent years, cation-disordered Li-excess rocksalts (DRX) have emerged as a promising new class of high-energy cathode materials for lithium-ion batteries. [1] Aside from the desirable Co-free chemistry, these compounds offer exceptionally large charge storage capacities by utilizing the redox reactions of both cationic transition-metals and anionic oxygen in the lattice. While early research focused on DRX oxides, which met with significant challenges in voltage stability and capacity retention upon cycling [2-3], recent studies shifted towards oxyfluorides with a substantial level of F substitution. It was found that incorporating F into the anionic sublattice can reduce oxygen gas release, impedance rise and capacity fade, consequently improving cathode cycling stability. [4-5] To this end, developing synthesis methods to incorporate large F content in the lattice as well as designing and optimizing oxyfluoride chemistry for both high energy density and cycling stability are imperative.While high F substitution levels (up to 30-40 at.%) in DRX have been achieved through mechanochemical synthesis, the method has limitations in industrial application due to poor scalability. Solid-state synthesis, on the other hand, are readily scalable and often offers drop-in replacement in materials processing. In this presentation, we show our recent effort in developing calcination-based fluorination approach to achieve high-level fluorination of Mn-redox-active DRX materials. [6] The unique behavior of capacity rise upon cycling of a new class of Mn-rich DRX oxyfluoride cathodes will be reported. Our understanding in how chemistry can impact local and long-range structures and their evolution during electrochemical cycling will also be presented, as well as perspectives on future directions in DRX development. References Lee, J.; Urban, A.; Li, X.; Su, D.; Hautier, G.; Ceder, G. Unlocking the Potential of Cation-Disordered Oxides for Rechargeable Lithium Batteries. Science 2014, 343, 519.Yabuuchi, N.; Takeuchi, M.; Nakayama, M.; Shiiba, H.; Ogawa, M.; Nakayama, K.; Ohta, T.; Endo, D.; Ozaki, T.; Inamasu, T.; Sato, K.; Komaba, S., High-Capacity Electrode Materials for Rechargeable Lithium Batteries: Li3NbO4-based System with Cation-Disordered Rocksalt Structure. Natl. Acad. Sci. 2015, 112, 7650.Chen, D.; Kan, W. H.; Chen, G. Understanding Performance Degradation in Cation-Disordered Rock-Salt Oxide Cathodes. Energy Mater. 2019, 9, 1901255.Lee, J.; Papp, J. K.; Clément, R. J.; Sallis, S.; Kwon, D.-H.; Shi, T.; Yang, W.; McCloskey, B. D.; Ceder, G. Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials. Commun. 2017, 8, 981.Lun, Z.; Ouyang, B.; Kitchaev, D. A.; Clément, R. J.; Papp, J. K.; Balasubramanian, M.; Tian, Y.; Lei, T.; Shi, T.; McCloskey, B. D.; Lee, J.; Ceder, G. Improved Cycling Performance of Li-Excess Cation-Disordered Cathode Materials upon Fluorine Substitution. Energy Mater. 2018, 9,1802959.Ahn, J.; Chen, D.; Chen, G.. A Fluorination Method for Improving Cation-Disordered Rocksalt Cathode Performance. Energy Mater. 2020, 10, 2001671.

(Invited) Electrolytes and Additives to Enhance Low-Temperature Performance of the Lithium-Ion Battery

We report the investigation of several electrolyte additives, which has the potential to enhance the low temperature performance of current lithium-ion rechargeable battery. Lithium-ion batteries (LIBs) power virtually all modern portable devices and electric vehicles, and their ubiquity continues to grow. With increasing applications, however, come increasing challenges, especially when operating conditions deviate from room temperature. While high-temperature performance and degradation has been extensively studied in LIBs, sub-zero Celsius performance has received less attention, despite being critical for batteries in transportation roles. Although many individual processes contribute to the capacity loss commonly observed in LIBs at low temperatures, most of them are governed to some extent by the non-aqueous liquid electrolyte present throughout the cell interior. Therefore, electrolyte engineering presents an unparalleled opportunity to study and address the fundamental causes of low-temperature failure. In this talk, we first outline recent literature on electrolyte-based strategies to improve said performance, including various additives, solvents and lithium salts. Then, we will detail the standard techniques and procedures we used to test the electrolytes and additives at sub-ambient temperature; and will discuss the results of the low temperature performance of new electrolytes and additives tested in our laboratory.

Novel Rechargeable Lithium-Ion Battery Based on a Cathode of Potassium-Cobalt(II) Octacyanomolybdate

In this work, the influence of the synthesis parameters (concentration, temperature, and reaction time) on the electrochemical performance of potassium-cobalt(II) octacyanomolybdate (KCoOCM) as a cathode material for its application in lithium-ion batteries was studied. The compound was synthesized hydrothermally using a chemometric approach and characterized by different techniques (FESEM, XRD, TGA). The KCoOCM showed a change in its morphology from prismatic structures to nanorods according to the synthesis conditions. Additionally, there was an influence on the specific capacity as a function of the synthesis parameters, i.e., precursor’s concentrations, temperature, and reaction time. The capacity values reached by the material was 50 mAh g−1, which is close to the theoretical value of the KCoOCM (60 mAh g−1). The statistical method employed would allow finding a condition where it is possible to maximize the capacity value of the material, which has been scarcely studied in this area. Finally, the performance of a lithium-ion battery based on a cathode of KCoOCM is reported for the first time in literature. Figure 1

Lithium Recovery from NCM Lithium Ion Battery by Carbonation Roasting Followed by Water Leaching

Lithium is a representative rare metal and ranks 32nd in abundance among elements in the earth’s crust. Lithium is used in a variety of applications, including the production of organolithium compounds, as an alloying addition to aluminum and magnesium, and as the anode in rechargeable lithium ion batteries especially for electronic devices and electric vehicles. Today, lithium is an indispensable metal in our daily lives. It is important to recycle lithium from used lithium-ion batteries to prepare for lithium shortages and protect lithium resources. The active cathode material of a lithium ion battery contains other valuable metals including Ni, Co, and Mn. In this study, the effect of carbonation temperature on Li recovery from NCM (LiNixCoyMnzO2) powder as Li2CO3 was investigated. First, a carbonation roasting was performed to convert the Li in the NCM powder into Li2CO3 at various temperature using a thermo-gravimetric analyzer. The roasted cinder leached into the water to dissolve the Li2CO3. The results showed that in Ar gas atmosphere the NCM phase was decomposed into Li2O and Li1-xM1+xO2 phases and the weight decreased by 4.7%, but in a CO2 atmosphere Li2CO3 was formed, resulting in a 12.1% increase in weight. In the isothermal experiment, the weight and carbon concentration of cinder increased with temperature, and the Li ratio in the NCM gradually decreased. The NCM powder was able to react with CO2 above 853 K, while some nickel, cobalt and manganese were regenerated into different Li1-xM1+xO2 crystalline phases. The maximum Li recovery rate of 76% wsa achieved for 2 h carbonation roasting at 1073 K followed by water leaching, filtering and an evaporative crystallization process.

Regulating Dynamic Electrochemical Interface of LiNi0.5Mn1.5O4 Spinel Cathode for Realizing Simultaneous Mn and Ni Redox in Rechargeable Lithium Batteries

AbstractThe exploding electric‐vehicle market requires cost‐effective high‐energy materials for rechargeable lithium batteries. The manganese‐rich spinel oxide LiNi0.5Mn1.5O4 (LNMO) can store a capacity greater than 200 mAh g−1 based on the multi‐cation (Ni2+/Ni4+ and Mn3+/Mn4+) redox centers. However, its practical capacity is limited to Ni2+/Ni4+ redox (135 mAh g−1) due to the poor reversibility of Mn3+/Mn4+ redox. This instability is generally attributed to the Jahn–Teller distortion of Mn3+ and its disproportionation, which leads to severe Mn dissolution. Herein, for the first time, the excellent reversibility of Mn3+/Mn4+ redox within 2.3–4.3 V is demonstrated, requiring revisiting the previous theory. LNMO loses capacity only within a wide voltage range of 2.3–4.9 V. It is revealed that a dynamic evolution of the electrochemical interface, for example, potential‐driven rocksalt phase formation and decomposition, repeatedly occurs during cycling. The interfacial evolution induces electrolyte degradation and surface passivation, impeding the charge‐transfer reactions. It is further demonstrated that stabilizing the interface by electrolyte modification extends the cycle life of LNMO while using the multi‐cation redox, enabling 71.5% capacity retention of LNMO after 500 cycles. The unveiled dynamic oxide interface will propose a new guideline for developing Mn‐rich cathodes by realizing the reversible Mn redox.

Implementation of a global trailer tracking system using a microcontroller

This paper underlines the importance of goods transport and mostly, the importance of knowing at all times where the trailers and trucks of a fleet are, in order to manage the fleet properly. The authors have proposed a prototype that connects to the 24 volt power supply of the truck and charges the lithium rechargeable batteries. After disconnecting the trailer, the tracking prototype can be located via SMS on any national or international route, depending on the GSM mounted in the device. The proposed prototype will be tested further and several directions of improvement have been proposed.

Strain effects on Li+ diffusion in solid electrolyte interphases: A molecular dynamics study

Dilithium ethylene dicarbonate (Li2EDC) and dilithium butylene dicarbonate (Li2BDC) are the common organic compositions of the solid electrolyte interphase (SEI) layers in rechargeable lithium-ion batteries. The Li+ diffusion in the amorphous and ordered phases of Li2EDC and Li2BDC under various strains has been investigated by using molecular dynamics simulations. It is found that different strains lead to diverse changes in Li+ diffusivity. The tensile strain makes the Li+ diffusion coefficients increase in amorphous and ordered Li2EDC or Li2BDC, and the compressive strain makes the Li+ diffusion coefficients decrease in them. The average Li+ coordination number calculation, ion conductivity calculation and the calculation of the residence autocorrelation function in amorphous and ordered Li2EDC or Li2BDC are performed to further analyze the strain effects on Li+ transport in them. The factors influencing Li+ diffusion in amorphous and ordered Li2EDC or Li2BDC under the strain are discussed.

Improving high-voltage cycling performance of nickel-rich NMC layered oxide cathodes for rechargeable lithium–ion batteries by Mg and Zr co-doping

Regarding the cost and safety concerns arising together with the increasing demands on lithium–ion batteries, high energy density Ni-rich LiNi0.8Co0.1Mn0.1O2 (NMC811) materials are of substantial interest as cathode materials for the next-generation commercial lithium–ion batteries. However, their low cycling stability hinders their use in large-scale applications (Schipper et al., 2018) [1]. In this work, we report two NMC811 materials, pristine and Mg/Zr co-doped, both synthesized through a facile sol-gel method followed by a stepwise calcination process. The doped cathode presents enhanced structural stability and shows a specific capacity of 232 mAh/g, at 0.1C and high charge cut-off voltage of 4.8 V vs. Li+/Li, and significant good cycling stability after 100 cycles; better than pristine NMC811. To unravel the origin of the enhancement, we have investigated the ionic and electronic transport properties by means of electrochemical impedance spectroscopy measurements, as well as the behavior of the electrode–electrolyte interphase layer.

Synthesis and Electrochemical Performance of KVO/GO Composites as Anodes for Aqueous Rechargeable Lithium-Ion Batteries.

K0.25V2O5 (KVO) and K0.25V2O5/graphene oxide (KVO/GO) have been successfully synthesized by a chemical coprecipitation method and a subsequent calcination process. The structure and morphology of KVO and KVO/GO were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. The as-obtained vanadate and vanadate modified by GO materials were used as anodes with LiMn2O4 as a cathode and saturated LiNO3 as an electrolyte to assemble an aqueous rechargeable lithium-ion battery (ARLB). The cyclic voltammogram curves of both KVO and KVO/GO electrodes exhibited three pairs of redox peaks corresponding to charge/discharge platforms. We found that a small amount of graphene oxide added improved the electrochemical performance more significantly than excess graphene oxide. The as-prepared KVO/GO//LiMn2O4 could not only improve the initial discharge capacity but could also reduce the attenuation at a high current density. Furthermore, the ARLB with a KVO/GO anode exhibited an excellent rate performance and super long cycle life. These good electrochemical properties of this new ARLB system actually provided feasibility for application in large-scale power sources and energy storage devices.

Bi2Se3 Nanostructured Thin Films as Perspective Anodes for Aqueous Rechargeable Lithium-Ion Batteries

In recent years, aqueous rechargeable lithium-ion batteries (ARLIBs) have attracted attention as an alternative technology for electrical storage. One of the perspective battery anode materials for application in ARLIBs is Bi2Se3, which has already shown good perspectives in the application of conventional lithium-ion batteries (LIBs) that use organic electrolytes. In this study, the electrochemical properties of Bi2Se3 thin films with two different layers on the electrode surface—the solid electrolyte interphase (SEI) and the Bi2O3 layer—were investigated. The results of this work show that the formation of the SEI layer on the surface of Bi2Se3 thin films ensures high diffusivity of Li+, high electrochemical stability, and high capacity up to 100 cycles, demonstrating the perspectives of Bi2Se3 as anode material for ARLIBs.

DFT Modelling of Li6SiO4Cl2 Electrolyte Material for Li-Ion Batteries

There is significant interest in finding a promising lithium-containing oxide that can act as a solid electrolyte in a rechargeable lithium-ion battery. Li6SiO4Cl2 is a candidate electrolyte material which was recently characterized using both experimental and computational techniques. In this study, density functional theory simulation was used to examine the intrinsic defects, solution of promising isovalent and aliovalent dopants, possible reaction routes for the formation of Li6SiO4Cl2, and the feasibility of incorporating additional Li in this material. The results revealed that the O–Cl anti-site cluster was the lowest energy defect in this material. The LiCl Schottky was the second lowest energy defect process, and the Li Frenkel was higher—only by 0.06 eV—than the LiCl Schottky. The candidate dopants on the Li, Si and Cl were Na, Ge and F, respectively. Substituting Al on the Si site was an efficient way of increasing the amount of Li in this material. Incorporation of extra Li (up to three) was considered and this process was endothermic. Different chemical reaction routes were constructed and their reaction energies were calculated to predict the feasibility of the formation of Li6SiO4Cl2. The formation of Li6SiO4Cl2 from constituent elements (Li, Si O2 and Cl2) is thermodynamically feasible.

Effect of Static Jahn-Teller Distortion on the Li+ Transport in a Copper Hexacyanoferrate Framework.

Prussian blue (PB) and its analogues (PBAs) are potential cathode-active materials for rechargeable lithium-ion batteries. Although a body of research has assessed the performances of various PB/PBA cathodes with an eye to practical use, the underlying Li+-transport mechanism is still unclear. Focusing on copper hexacyanoferrate (CuHCF), a PBA that exhibits static Jahn-Teller (JT) distortion, we theoretically investigate how the framework's distortion affects the pathways and energetics of the Li+ transport. Density functional theory calculations of a local structure model of CuHCF reveal that the static JT distortion makes the favorable Li+-transport pathways quasi-two-dimensional, contrary to an intuitive picture of isotropic Li+ diffusion within the regular jungle-gym framework. The pathways are mutually interconnected, thereby creating an almost barrierless transport network. To better understand the distortion-induced transport anisotropy, we visually analyze the framework's electronic structure and noncovalent Li+-framework interactions. This study helps deepen the fundamental understanding of intrinsic Li+-transport properties of a distorted porous framework.

Metal‐organic framework derived porous structures towards lithium rechargeable batteries

AbstractBatteries are a promising technology in the field of electrical energy storage and have made tremendous strides in recent few decades. In particular, lithium‐ion batteries are leading the smart device era as an essential component of portable electronic devices. From the materials aspect, new and creative solutions are required to resolve the current technical issues on advanced lithium (Li) batteries and improve their safety. Metal‐organic frameworks (MOFs) are considered as tempting candidates to satisfy the requirements of advanced energy storage technologies. In this review, we discuss the characteristics of MOFs for application in different types of Li batteries. A review of these emerging studies in which MOFs have been applied in lithium storage devices can provide an informative blueprint for future MOF research on next‐generation advanced energy storage devices.image

Rechargeable LiNi0.65Co0.15Mn0.2O2||Graphite Batteries Operating at −60 °C

AbstractThe rechargeability of contemporary lithium‐ion batteries (LIBs) is challenging at low temperatures, mainly due to the hurdles faced by graphite anodes. Herein, by exploiting the Li‐solvent co‐intercalation into graphite, its low‐temperature rechargeability is boosted. Experimental characterizations aided by theoretical calculations demonstrate that the co‐intercalation process is featured by low interfacial resistance with a small charge transfer activation energy (0.23 eV atom−1) and an extremely low diffusion energy barrier (0.09 eV atom−1) which leads to nearly temperature‐independent diffusion coefficients of the solvated Li‐ion in graphite, enabling graphite to be stably charged‐discharged at −60 °C with 73.7 % of its room‐temperature capacity. Consequently, the full‐cell consisting of a LiNi0.65Co0.15Mn0.2O2cathode and a graphite anode shows impressive rechargeability under −60 °C. This work provides an alternative approach to develop low‐temperature rechargeable LIBs.