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Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganeseoxide batteries from reactive force field (ReaxFF) based molecular dynamics

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

《能源前沿（英文）》 2017年 第11卷 第3期   页码 365-373 doi: 10.1007/s11708-017-0500-8

摘要： Lithium manganese oxide (LiMn O ) is a principal cathode material for high power and high energy density electrochemical storage on account of its low cost, non-toxicity, and ease of preparation relative to other cathode materials. However, there are well-documented problems with capacity fade of lithium ion batteries containing LiMn O . Experimental observations indicate that the manganese content of the electrolyte increases as an electrochemical cell containing LiMn O ages, suggesting that active material loss by dissolution of divalent manganese from the LiMn O surface is the primary reason for reduced cell life in LiMn O batteries. To improve the retention of manganese in the active material, it is key to understand the reactions that occur at the cathode surface. Although a thin layer of electrolyte decomposition products is known to form at the cathode surface, the speciation and reaction mechanisms of Mn in this interface layer are not yet well understood. To bridge this knowledge gap, reactive force field (ReaxFF) based molecular dynamics was applied to investigate the reactions occurring at the LiMn O cathode surface and the mechanisms that lead to manganese dissolution. The ReaxFFMD simulations reveal that the cathode-electrolyte interface layer is composed of oxidation products of electrolyte solvent molecules including aldehydes, esters, alcohols, polycarbonates, and organic radicals. The oxidation reaction pathways for the electrolyte solvent molecules involve the formation of surface hydroxyl species that react with exposed manganese atoms on the cathode surface. The presence of hydrogen fluoride (HF) induces formation of inorganic metal fluorides and surface hydroxyl species. Reaction products predicted by ReaxFF-based MD are in agreement with experimentally identified cathode-electrolyte interface compounds. An overall cathode-electrolyte interface reaction scheme is proposed based on the molecular simulation results.

关键词： lithium manganese oxide batteries     reactive force field (ReaxFF)     cathode-electrolyte interface layer     molecular dynamics    

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Preparation of lithium ion-sieve and utilizing in recovery of lithium from seawater

Lu WANG, Changgong MENG, Wei MA

《化学科学与工程前沿（英文）》 2009年 第3卷 第1期   页码 65-67 doi: 10.1007/s11705-009-0105-9

摘要： Lithium is one of the most important light metals, which is widely used as raw materials for large-capacity rechargeable batteries, light aircraft alloys and nuclear fusion fuel. Seawater, which contains 250 billion tons of lithium in total, has thus recently been noticed as a possible resource of lithium. While, since the average concentration of lithium in seawater is quite low (0.17 mg·L ), enriching it to an adequate high density becomes the primary step for industrial applications. The adsorption method is the most prospective technology for increasing the concentration of lithium in liquid. Among the adsorbents for lithium, the ion-sieve is a kind of special absorbent which has high selectivity for Li , especially the spinel manganese oxides (SMO), which among the series of ion-sieves, has become the most promising adsorption material for lithium. In this study, the SMO ion-sieve was prepared by a coprecipitation method. The preparation conditions were discussed and the sample characters were analyzed. Recovery of Li from seawater were studied in batch experiments using prepared ion-sieve, and the effect of solution pH and the uptake rates were also investigated in different Li solutions.

关键词： lithium     ion-sieve     seawater     spinel manganese oxide    

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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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下一代锂电池在能源化学工程方面的研究进展 Review

张学强, 赵辰孜, 黄佳琦, 张强

《工程（英文）》 2018年 第4卷 第6期   页码 831-847 doi: 10.1016/j.eng.2018.10.008

摘要：

锂离子电池（LIB）对当今人们的生活产生了深远的影响。然而由于插层化学本质上的限制，锂离子电池的能量密度已接近理论上限，难以满足人们在多方面日益增长的储能需求，如便携式电子设备、电动汽车和大规模储能。因此，下一代锂（Li）电池正在广泛研究中。其中，采用金属锂作为负极，插层或转化型材料作为正极的下一代锂电池是最受关注的体系，因其具有高能量密度和巨大的商业化潜力。近年来，随着材料和反应机理方面研究的深入以及技术手段的进步，锂电池取得了不断的发展。本文从下一代锂电池的电解液/ 电解质的设计出发，从能源化学工程的角度梳理锂离子电池、锂硫电池和锂空电池中的关键科学问题和研究进展，并阐述下一代锂电池未来的发展方向。下一代锂电池有望促进人类文明的可持续发展。

关键词： 锂离子电池     锂硫电池     锂空电池     锂金属     固态电池     电池化学     电解质    

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Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

《化学科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 415-421 doi: 10.1007/s11705-013-1360-3

摘要： Two catalysts, alumina and manganese oxide supported on alumina, have been prepared by calcination and precipitation-impregnation methods, respectively. The catalysts are characterised by the following techniques: Brunner-Emmett-Teller-N adsorption-desorption for surface area, temperature programmed desorption of NH and -butyl amine back titration methods for surface acidity, powder X-ray diffraction for textural properties, and Fourier transform infrared spectroscopy for the anionic radicals. The catalytic activity has been determined under heterogeneous conditions in the condensation reaction between -phenylenediamine and benzil. The product purity is checked by thin-layer chromatography and melting point. The products are also analysed by LC-MS and H-NMR techniques. The yields of the products have been found to be good and catalysts exhibited excellent recyclability. The effect of changing the reaction parameters such as temperature, reaction time, amount of the catalyst, nature of solvent and molar ratio of reactants on the yield of the product has been studied. The surface acidity of the catalysts plays an important role in activating the reaction.

关键词： alumina     manganese oxide deposited on alumina     quinoxaline synthesis    

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Continuous amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur batteries

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 194-205 doi: 10.1007/s11705-022-2206-7

摘要： The shuttle effect of soluble polysulfides is a serious problem impeding the development of lithium−sulfur batteries. Herein, continuous amino-functionalized University of Oslo 66 membranes supported on carbon nanotube films are proposed as ion-permselective interlayers that overcome these issues and show outstanding suppression of the polysulfide shuttle effect. The proposed membrane material has appropriately sized pores, and can act as ionic sieves and serve as barriers to polysulfides transport while allowing the passage of lithium ions during electrochemical cycles, thereby validly preventing the shuttling of polysulfides. Moreover, a fast catalytic conversion of polysulfides is also achieved with the as-developed interlayer. Therefore, lithium−sulfur batteries with this interlayer show a desirable initial capacity of 999.21 mAh·g–1 at 1 C and a durable cyclic stability with a decay rate of only 0.04% per cycle over 300 cycles. Moreover, a high area capacity of 4.82 mAh·cm–2 is also obtained even under increased sulfur loading (5.12 mg·cm–2) and a lean-electrolyte condition (E/S = 4.8 μL·mg–1).

关键词： lithium−sulfur batteries     amino-functionalized University of Oslo 66 membrane     polysulfide     interlayer    

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Spent rechargeable lithium batteries in e-waste: composition and its implications

Xianlai ZENG,Jinhui LI

《环境科学与工程前沿（英文）》 2014年 第8卷 第5期   页码 792-796 doi: 10.1007/s11783-014-0705-6

摘要： The amount of spent rechargeable lithium batteries (RLBs) is growing rapidly owing to wide application of these batteries in portable electronic devices and electric vehicles, which obliges that spent RLBs should be handled properly. Identification of spent RLBs can supply fundamental information for spent RLBs recycling. This study aimed to determine the differences of physical components and chemical compositions among various spent RLBs. All the samplings of RLBs were rigorously dismantled and measured by an inductive coupled plasma atomic emission spectrometer. The results indicate that the average of total weight of the separator, the anode and the cathode accounted for over 60% of all the RLBs. The weight ratio of valuable metals ranged from 26% to 76%, and approximately 20% of total weight was Cu and Al. Moreover, no significant differences were found among different manufacturers, applications, and electrolyte types. And regarding portable electronic devices, there is also no significant difference in the Co-Li concentration ratios in the leaching liquid of RLBs.

关键词： rechargeable lithium batteries     e-waste     physical components     difference analysis     recycling    

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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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Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for

《化学科学与工程前沿（英文）》 2022年 第16卷 第5期   页码 731-744 doi: 10.1007/s11705-021-2110-6

摘要： Catalytic ozonation technology has attracted copious attention in water purification owing to its favorable oxidative degradation of pollutants and mitigation of membrane fouling capacity. However, its extensive industrial application has been restricted by the low ozone utilization and limited mass transfer of the short-lived radical species. Interlayer space-confined catalysis has been theoretically proven to be a viable strategy for achieving high catalytic efficiency. Here, a two-dimensional MnO2-incorporated ceramic membrane with tunable interspacing, which was obtained via the intercalation of a carbon nanotube, was designed as a catalytic ozonation membrane reactor for degrading methylene blue. Benefiting from the abundant catalytic active sites on the surface of two-dimensional MnO2 as well as the ultralow mass transfer resistance of fluids due to the nanolayer confinement, an excellent mineralization effect, i.e., 1.2 mg O3(aq) mg–1 TOC removal (a total organic carbon removal rate of 71.5%), was achieved within a hydraulic retention time of 0.045 s of pollutant degradation. Further, the effects of hydraulic retention time and interlayer spacing on methylene blue removal were investigated. Moreover, the mechanism of the catalytic ozonation employing catalytic ozonation membrane was proposed based on the contribution of the Mn(III/IV) redox pair to electron transfer to generate the reactive oxygen species. This innovative two-dimensional confinement catalytic ozonation membrane could act as a nanoreactor and separator to efficiently oxidize organic pollutants and enhance the control of membrane fouling during water purification.

关键词： catalytic membrane reactor     catalytic ozonation     nanoconfinement     two-dimensional manganese oxide    

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Two-phase early prediction method for remaining useful life of lithium-ion batteries based on a neural

《能源前沿（英文）》 doi: 10.1007/s11708-023-0906-4

摘要： Lithium-ion batteries (LIBs) are widely used in transportation, energy storage, and other fields. The prediction of the remaining useful life (RUL) of lithium batteries not only provides a reference for health management but also serves as a basis for assessing the residual value of the battery. In order to improve the prediction accuracy of the RUL of LIBs, a two-phase RUL early prediction method combining neural network and Gaussian process regression (GPR) is proposed. In the initial phase, the features related to the capacity degradation of LIBs are utilized to train the neural network model, which is used to predict the initial cycle lifetime of 124 LIBs. The Pearson coefficient’s two most significant characteristic factors and the predicted normalized lifetime form a 3D space. The Euclidean distance between the test dataset and each cell in the training dataset and validation dataset is calculated, and the shortest distance is considered to have a similar degradation pattern, which is used to determine the initial Dual Exponential Model (DEM). In the second phase, GPR uses the DEM as the initial parameter to predict each test set’s early RUL (ERUL). By testing four batteries under different working conditions, the RMSE of all capacity estimation is less than 1.2%, and the accuracy percentage (AP) of remaining life prediction is more than 98%. Experiments show that the method does not need human intervention and has high prediction accuracy.

关键词： lithium-ion batteries     RUL prediction     double exponential model     neural network     Gaussian process regression (GPR)    

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zirconium-based metal-organic framework-801 films on carbon cloth as shuttle-inhibiting interlayers for lithium-sulfurbatteries

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 511-522 doi: 10.1007/s11705-021-2068-4

摘要： Lithium-sulfur batteries have been regarded as the next-generation rechargeable batteries due to their high theoretical energy density and specific capacity. Nevertheless, the shuttle effect of lithium polysulfides has hindered the development of lithium-sulfur batteries. Herein, a novel zirconium-based metal-organic framework-801 film on carbon cloth was developed as a versatile interlayer for lithium-sulfur batteries. This interlayer has a hierarchical porous structure, suitable for the immobilization of lithium polysulfides and accommodating volume expansion on cycling. Moreover, the MOF-801 material is capable of strongly adsorbing lithium polysulfides and promoting their catalytic conversion, which can be enhanced by the abundant active sites provided by the continuous structure of the MOF-801 films. Based on the above advantages, the lithium-sulfur battery, with the proposed interlayer, delivers an initial discharge capacity of 927 mAh·g–1 at 1 C with an extremely low decay rate of 0.04% over 500 cycles. Additionally, a high area capacity of 4.3 mAh·cm–2 can be achieved under increased S loading.

关键词： lithium-sulfur batteries     metal-organic framework-801 film     interlayer     shuttle effect    

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Promoting Si-graphite composite anodes with SWCNT additives for half and NCM811 full lithium ion batteries

Jingning SHAN, Xiaofang YANG, Chao YAN, Yiguang JU, Lin CHEN, Fang ZHAO

《能源前沿（英文）》 2019年 第13卷 第4期   页码 626-635 doi: 10.1007/s11708-019-0650-y

摘要： Single wall carbon nanotube (SWCNT) additives were formulated into µm-Si-graphite composite electrodes and tested in both half cells and full cells with high nickel cathodes. The critical role of small amount of SWCNT addition (0.2 wt%) was found for significantly improving delithiation capacity, first cycle coulombic efficiency (FCE), and capacity retention. Particularly, Si (10 wt%)-graphite electrode exhibits 560 mAh/g delithiation capacity and 92% FCE at 0.2 C during the first charge-discharge cycle, and 91% capacity retention after 50 cycles (0.5 C) in a half cell. Scanning electron microscope (SEM) was used to illustrate the electrode morphology, compositions and promoting function of the SWCNT additives. In addition, full cells assembled with high nickel-NCM811 cathodes and µm-Si-graphite composite anodes were evaluated for the consistence between half and full cell performance, and the consideration for potential commercial application. Finally, criteria to assess Si-containing anodes are proposed and discussed from an industrial perspective.

关键词： lithium-ion battery     Si anode     Si-graphite composite     single wall carbon nanotube (SWCNT)     NCM811    

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Multi-effect anthraquinone-based polyimide enclosed SnO/reduced graphene oxide composite as high-performanceanode for lithium-ion battery

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1231-1243 doi: 10.1007/s11705-023-2306-z

摘要： The cycling stability of SnO2 anode as lithium-ion battery is poor due to volume expansion. Polyimide coatings can effectively confine the expansion of SnO2. However, linear polyimides are easily dissolved in ester electrolytes and their carbonyls is not fully utilized during charging/discharging process. Herein, the SnO2 enclosed with anthraquinone-based polyimide/reduced graphene oxide composite was prepared by self-assembly. Carbonyls from the anthraquinone unit provide fully available active sites to react with Li+, improving the utilization of carbonyl in the polyimide. More exposed carbonyl active sites promote the conversion of Sn to SnO2 with electrode gradual activation, leading to an increase in reversible capacity during the charge/discharge cycle. In addition, the introduction of reduced graphene oxide cannot only improve the stability of polyimide in the electrolyte, but also build fast ion and electron transport channels for composite electrodes. Due to the multiple effects of anthraquinone-based polyimide and the synergistic effect of reducing graphene oxide, the composite anode exhibits a maximum reversible capacity of 1266 mAh·g−1 at 0.25 A·g−1, and maintains an excellent specific capacity of 983 mAh·g−1 after 200 cycles. This work provides a new strategy for the synergistic modification of SnO2.

关键词： anthraquinone-based polyimide     multi-effect     tin dioxide     reduced graphene oxide     lithium-ion battery    

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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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Fabrication of layered structure VS anchor in 3D graphene aerogels as a new cathode material for lithiumion batteries

《能源前沿（英文）》 2019年 第13卷 第3期   页码 597-602 doi: doi:10.1007/s11708-018-0576-9

摘要： VS4 has gained more and more attention for its high theoretical capacity (449 mAh/g with 3e− transfer) in lithium ion batteries (LIBs). Herein, a layered structure VS4 anchored in graphene aerogels is prepared and first reported as cathode material for LIBs. VS4@GAs composite exhibits an exceptional high initial reversible capacity (511 mAh/g), an excellent high-rate capability (191 mAh/g at the 5 C), and an excellent cyclic stability (239 mAh/g after 15 cycles).

关键词： VS4     graphene aerogels     cathode     lithium storage    

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标题 作者 时间 类型 操作

Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganeseoxide batteries from reactive force field (ReaxFF) based molecular dynamics

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

期刊论文

Preparation of lithium ion-sieve and utilizing in recovery of lithium from seawater

Lu WANG, Changgong MENG, Wei MA

期刊论文

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

期刊论文

下一代锂电池在能源化学工程方面的研究进展

张学强, 赵辰孜, 黄佳琦, 张强

期刊论文

Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

期刊论文

Continuous amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur batteries

期刊论文

Spent rechargeable lithium batteries in e-waste: composition and its implications

Xianlai ZENG,Jinhui LI

期刊论文

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

期刊论文

Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for

期刊论文

Two-phase early prediction method for remaining useful life of lithium-ion batteries based on a neural

期刊论文

zirconium-based metal-organic framework-801 films on carbon cloth as shuttle-inhibiting interlayers for lithium-sulfurbatteries

期刊论文

Promoting Si-graphite composite anodes with SWCNT additives for half and NCM811 full lithium ion batteries

Jingning SHAN, Xiaofang YANG, Chao YAN, Yiguang JU, Lin CHEN, Fang ZHAO

期刊论文

Multi-effect anthraquinone-based polyimide enclosed SnO/reduced graphene oxide composite as high-performanceanode for lithium-ion battery

期刊论文

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

期刊论文

Fabrication of layered structure VS anchor in 3D graphene aerogels as a new cathode material for lithiumion batteries

期刊论文