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nitrogen-doped carbon cladding LiMnO film electrode with enhanced stability for electrochemically selective extractionof lithium ions

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2050-2060 doi: 10.1007/s11705-023-2343-7

摘要： Reducing the dissolution of Mn from LiMn2O4 (LMO) and enhancing the stability of film electrodes are critical and challenging for Li+ ions selective extraction via electrochemically switched ion exchange technology. In this work, we prepared a nitrogen-doped carbon cladding LMO (C-N@LMO) by polymerization of polypyrrole and high-temperature annealing in the N2 gas to achieve the above purpose. The modified C-N@LMO film electrode exhibited lower Mn dissolution and better cyclic stability than the LMO film electrode. The dissolution ratio of Mn from the C-N@LMO film electrode decreased by 42% compared to the LMO film electrode after 10 cycles. The cladding layer not only acted as a protective layer but also functioned as a conductive shell, accelerating the migration rate of Li+ ions. The intercalation equilibrium time of the C-N@LMO film electrode reached within an hour during the extraction of Li+ ions, which was 33% less compared to the pure LMO film electrode. Meanwhile, the C-N@LMO film electrode retained evident selectivity toward Li+ ions, and the separation factor was 118.38 for Li+ toward Mg2+ in simulated brine. Therefore, the C-N@LMO film electrode would be a promising candidate for the recovery of Li+ ions from salt lakes.

关键词： LiMn2O4     lithium extraction     surface coating     cyclic stability     Mn dissolution    

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废锂离子电池中有价金属回收的研究进展 Review

郑晓洪, 朱泽文, 林晓, 张懿, 何艺, 曹宏斌, 孙峙

《工程（英文）》 2018年 第4卷 第3期   页码 361-370 doi: 10.1016/j.eng.2018.05.018

摘要：

近年来，随着锂离子电池在消费电子产品和电动汽车领域应用的快速增长，导致了废旧锂离子电池的数量和重量呈现快速的增长。废旧锂离子电池中不仅含有有害的重金属，还含有有毒的化学物质，这些有害物质会对生态系统和人类健康构成严重的威胁。因此，从环境保护和经济方面考虑，高效地回收废旧锂离子电池受到了广泛的关注。本文综述了废锂离子电池中有价金属回收的工艺现状，介绍了锂离子电池的结构并总结了废锂离子电池回收技术。值得注意的是，预处理过程和金属提取过程在整个回收过程十分重要，其中金属提取过程主要采用的方法有火法冶金、湿法冶金、生物冶金及其他方法等。通过进一步比较不同回收方法，提出了目前废锂离子电池回收处理过程中主要存在的问题和未来的发展方向。

关键词： 废锂离子电池     有价金属     预处理     金属提取     产品制备     回收    

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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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Highly selective and green recovery of lithium ions from lithium iron phosphate powders with ozone

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 749-758 doi: 10.1007/s11705-022-2261-0

摘要： Since lithium iron phosphate cathode material does not contain high-value metals other than lithium, it is therefore necessary to strike a balance between recovery efficiency and economic benefits in the recycling of waste lithium iron phosphate cathode materials. Here, we describe a selective recovery process that can achieve economically efficient recovery and an acceptable lithium leaching yield. Adjusting the acid concentration and amount of oxidant enables selective recovery of lithium ions. Iron is retained in the leaching residue as iron phosphate, which is easy to recycle. The effects of factors such as acid concentration, acid dosage, amount of oxidant, and reaction temperature on the leaching of lithium and iron are comprehensively explored, and the mechanism of selective leaching is clarified. This process greatly reduces the cost of processing equipment and chemicals. This increases the potential industrial use of this process and enables the green and efficient recycling of waste lithium iron phosphate cathode materials in the future.

关键词： lithium iron phosphate powder     stoichiometric number     selective leaching     lithium recovery    

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Capture of carbon dioxide over porous solid adsorbents lithium silicate, lithium aluminate and magnesium

P. V. Korake, A. G. Gaikwad

《化学科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 215-226 doi: 10.1007/s11705-010-1012-9

摘要： The capturing process for carbon dioxide over porous solid adsorbents such as lithium silicate, lithium aluminate, and magnesium aluminate at pre- combustion temperatures was studied. Lithium silicate was prepared by the sol gel and solid fusion methods. The lithium silicate adsorbent was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), nuclear magnetic resonance (NMR), and surface area. The capturing of carbon dioxide over lithium silicate, lithium aluminate, and magnesium aluminate was explored at different experimental conditions such as exposure time, temperature variation, and exposure carbon dioxide pressure. The capturing process for carbon dioxide was investigated over these adsorbents with variation of their metal mole ratios. The effect of the addition of (promoter) sodium, potassium, and cesium in the lithium silicate adsorbent was explored to investigate the variation of the capture of carbon dioxide over these adsorbents.

关键词： capturing CO2     lithium silicate     lithium aluminate     magnesium aluminate    

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Lithium-based draw solute for forward osmosis to treat wastewater discharged from lithium-ion battery

《化学科学与工程前沿（英文）》 2022年 第16卷 第5期   页码 755-763 doi: 10.1007/s11705-022-2137-3

摘要： As draw solute is the core element of forward osmosis (FO) technology, here Li-Bet-Tf2N synthesized from a customized ionic liquid betainium bis(trifluoromethylsulfonyl)imide ([Hbet][Tf2N]) and Li2CO3 recovered from lithium-ion battery (LIB) wastes is proposed as a novel draw solute to treat Li+-containing wastewater from LIB manufacturing through FO filtration. Having high dissociation ability and an extended structure, Li-Bet-Tf2N generates a sufficiently high osmotic pressure to drive the FO filtration efficiently along with insignificant reverse solute diffusion. Li-Bet-Tf2N produces a water flux of 21.3 L·(m2·h)−1 at 1.0 mol∙L–1 against deionized water, surpassing conventional NaCl and MgCl2 draw solutes with a higher water recovery efficiency and a smaller solute loss. Li-Bet-Tf2N induces a more stable and higher water permeation flux with a 10.0% water flux decline than NaCl and MgCl2 for which the water fluxes decline 16.7% and 16.4%, respectively, during the treatment of 2000 mg∙L–1 Li+-containing wastewater for 12 h. More remarkably, unlike other draw solutes which require intensive energy input and complicated processes in recycling, Li-Bet-Tf2N is easily separated from water via solvent extraction. Reproducible results are achieved with the recycled Li-Bet-Tf2N. Li-Bet-Tf2N thus demonstrates a novel class of draw solute with great potentials to treat wastewater economically.

关键词： forward osmosis     lithium-ion battery     draw solution     lithium-containing wastewater     water treatment    

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Entity and relation extraction with rule-guided dictionary as domain knowledge

《工程管理前沿（英文）》   页码 610-622 doi: 10.1007/s42524-022-0226-0

摘要： Entity and relation extraction is an indispensable part of domain knowledge graph construction, which can serve relevant knowledge needs in a specific domain, such as providing support for product research, sales, risk control, and domain hotspot analysis. The existing entity and relation extraction methods that depend on pretrained models have shown promising performance on open datasets. However, the performance of these methods degrades when they face domain-specific datasets. Entity extraction models treat characters as basic semantic units while ignoring known character dependency in specific domains. Relation extraction is based on the hypothesis that the relations hidden in sentences are unified, thereby neglecting that relations may be diverse in different entity tuples. To address the problems above, this paper first introduced prior knowledge composed of domain dictionaries to enhance characters’ dependence. Second, domain rules were built to eliminate noise in entity relations and promote potential entity relation extraction. Finally, experiments were designed to verify the effectiveness of our proposed methods. Experimental results on two domains, including laser industry and unmanned ship, showed the superiority of our methods. The F1 value on laser industry entity, unmanned ship entity, laser industry relation, and unmanned ship relation datasets is improved by +1%, +6%, +2%, and +1%, respectively. In addition, the extraction accuracy of entity relation triplet reaches 83% and 76% on laser industry entity pair and unmanned ship entity pair datasets, respectively.

关键词： entity extraction     relation extraction     prior knowledge     domain rule    

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Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing

Chunlong Zhao, Mingming He, Hongbin Cao, Xiaohong Zheng, Wenfang Gao, Yong Sun, He Zhao, Dalong Liu, Yanling Zhang, Zhi Sun

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 639-650 doi: 10.1007/s11705-019-1806-3

摘要： In the production of lithium-ion batteries (LIBs) and recycling of spent LIBs, a large amount of low-concentration lithium-containing wastewater (LCW) is generated. The recovery of Li from this medium has attracted significant global attention from both the environmental and economic perspectives. To achieve effective Li recycling, the features of impurity removal and the interactions among different ions must be understood. However, it is generally difficult to ensure highly efficient removal of impurity ions while retaining Li in the solution for further recovery. In this study, the removal of typical impurity ions from LCW and the interactions between these species were systematically investigated from the thermodynamic and kinetics aspects. It was found that the main impurities (e.g., Fe , Al , Ca , and Mg ) could be efficiently removed with high Li recovery by controlling the ionic strength of the solution. The mechanisms of Fe , Al , Ca , and Mg removal were investigated to identify the controlling steps and reaction kinetics. It was found that the precipitates are formed by a zero-order reaction, and the activation energies tend to be low with a sequence of fast chemical reactions that reach equilibrium very quickly. Moreover, this study focused on Li loss during removal of the impurities, and the corresponding removal rates of Fe , Al , Ca , and Mg were found to be 99.8%, 99.5%, 99%, and 99.7%, respectively. Consequently, high-purity Li PO was obtained via one-step precipitation. Thus, this research demonstrates a potential route for the effective recovery of Li from low-concentration LCW and for the appropriate treatment of acidic LCW.

关键词： lithium-containing wastewater     lithium phosphate     precipitation     impurity ion    

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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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Primary nucleation of lithium carbonate

Yuzhu SUN, Xingfu SONG, Jin WANG, Yan LUO, Jianguo YU

《化学科学与工程前沿（英文）》 2009年 第3卷 第1期   页码 73-77 doi: 10.1007/s11705-009-0091-y

摘要： A set of laser apparatus was used to explore the induction period and the primary nucleation of lithium carbonate. Results show that the induction period increases with the decrease of supersaturation, temperature and stirring speed. Through the classical theory of primary nucleation, many important properties involved in primary nucleation under different conditions were obtained quantitatively, including the interfacial tension between solid and liquid, contact angle, critical nucleus size, critical nuleation free energy etc.

关键词： lithium carbonate     primary nucleation     reactive crystallization     induction period    

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

《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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Preparation and characterization of lithium

Chang WANG,Yanlong ZHAI,Xi WANG,Ming ZENG

《化学科学与工程前沿（英文）》 2014年 第8卷 第4期   页码 471-477 doi: 10.1007/s11705-014-1449-3

摘要： Lithium -MnO ion-sieves were prepared from spinel LiMn O via treatment with nitric acid. The LiMn O was synthesized by a solid state reaction between LiOH·H O and MnO . The effects of the calcination time and temperature on the preparation of the LiMn O precursor and the lithium ion-sieve were investigated. In addition, the Li extraction ratio, the Mn dissolving ratio and the adsorption properties of the lithium ion-sieve were all measured. The lithium ion-sieve had a high exchange capacity and was selective for Li . Specifically, at pH= 13, the ion exchange capacity of Li was 30.9 mg/g in 10 mmol/L LiCl solution and the lithium extraction ratio and manganese dissolving ratio were 95% and 25%, respectively.

关键词： lithium ion-sieve     solid state reaction     adsorption     LiMn2O4    

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

《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

nitrogen-doped carbon cladding LiMnO film electrode with enhanced stability for electrochemically selective extractionof lithium ions

期刊论文

废锂离子电池中有价金属回收的研究进展

郑晓洪, 朱泽文, 林晓, 张懿, 何艺, 曹宏斌, 孙峙

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

Highly selective and green recovery of lithium ions from lithium iron phosphate powders with ozone

期刊论文

Capture of carbon dioxide over porous solid adsorbents lithium silicate, lithium aluminate and magnesium

P. V. Korake, A. G. Gaikwad

期刊论文

Lithium-based draw solute for forward osmosis to treat wastewater discharged from lithium-ion battery

期刊论文

Entity and relation extraction with rule-guided dictionary as domain knowledge

期刊论文

Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing

Chunlong Zhao, Mingming He, Hongbin Cao, Xiaohong Zheng, Wenfang Gao, Yong Sun, He Zhao, Dalong Liu, Yanling Zhang, Zhi Sun

期刊论文

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

期刊论文

Primary nucleation of lithium carbonate

Yuzhu SUN, Xingfu SONG, Jin WANG, Yan LUO, Jianguo YU

期刊论文

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

期刊论文

Preparation and characterization of lithium

Chang WANG,Yanlong ZHAI,Xi WANG,Ming ZENG

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

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

期刊论文

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

期刊论文