CFD-based structural optimization of suspension drying ovens for lithium-ion batteries to enhance oven performance

The all-solid-state lithium secondary batteries using sulfide-based solid electrolytes are highly anticipated as next generation batteries because of their potential of high power and energy density, long battery life, and higher safety compared with batteries with liquid electrolyte [1]. One of the issues to be solved for the commercialization is the development of a processing technology.Two types of all-solid-state batteries using inorganic solid electrolytes have been studied. One is thin-film batteries and the other is bulk-type batteries. Thin-film batteries consist of electrode and solid electrolyte films. The thickness of the electrode films is usually less than 10 micrometers. Bulk-type batteries consist of composite electrodes with active material and solid electrolyte particles and solid electrolyte separator layer. The bulk-type batteries are further classified into two configurations. One is pellet-type batteries which are constructed using powder compression die. Most of the bulk-type batteries reported heretofore belong to this configuration. The pellet-type batteries are useful for the study of the evaluation of the performance of electrode materials and composite electrode in all-solid-state cells. However, the thickness of the solid electrolyte layer prepared by this process is relatively thick because of the difficulty of the formation of homogeneous and thin solid-electrolyte layer.Sheet-type batteries, which consist of electrode sheets with current collector sheets as shown in Fig. 1, are more practicable battery configuration than pellet-type one. The reports on the sheet-type all-solid-state batteries are still few in number[2, 3]although the research and development of the sheet-type all-solid-state batteries are as important as the materials characterization in the pellet-type batteries.Here we report the practical slurry coating process for the construction of the sheet-type all-solid-state batteries. The charge-discharge performance of the all-solid-state batteries was evaluated.The coarse and small-size solid electrolyte particles were prepared by mechanical milling from crystalline Li2S (Mitsuwa Chemicals) and P2S5 (Aldrich) using heptane as a solvent. Positive and negative electrode sheets were prepared on aluminum or copper foils by coating the slurries consisting of LiNi1/3Co1/3Mn1/3O2 (NCM) or graphite as active materials, 75Li2S·25P2S5 (mol%) glassy solid electrolyte, acetylene black, styrene-butadiene-based binder and aprotic organic solvents. The solid electrolyte sheet was also prepared by slurry coating process.The electrode and electrolyte sheet were stacked and pressed at ca. 300 MPa for cell construction.Cross-sectional SEM images revealed that the electrode and solid electrolyte were inhomogeneously distributed in the electrode sheets prepared using a coarse solid electrolyte particles. The homogeneity in the electrode layer was improved by using smaller-sized solid electrolyte particles. As a result, all-solid-state cell with electrode sheets with the fine solid electrolyte showed higher discharge capacity and rate capability than the cell using the coarse solid electrolyte. The prepared all-solid-state cells are charged and discharged with the capacity of more than 100 mAh g-1 (-NMC) at 30°C. The prepared all-solid-state cell showed the energy density of more than 100 Wh kg-1. Thus, the particle size and its homogeneous distribution play an important role for fabricating sheet-type batteries with improved battery performance. Acknowledgement This research was financially supported by the Japan Science and Technology Agency (JST), Advanced Low Carbon Technology Research and Development Program (ALCA), Specially Promoted Research for Innovative Next Generation Batteries (SPRING) Project.

PurposeLife cycle assessment (LCA) literature evaluating environmental burdens from lithium-ion battery (LIB) production facilities lacks an understanding of how environmental burdens have changed over time due to a transition to large-scale production. The purpose of this study is hence to examine the effect of upscaling LIB production using unique life cycle inventory data representative of large-scale production. A sub-goal of the study is to examine how changes in background datasets affect environmental impacts.MethodWe remodel an often-cited study on small-scale battery production by Ellingsen et al. (2014), representative of operations in 2010, and couple it to updated Ecoinvent background data. Additionally, we use new inventory data to model LIB cell production in a large-scale facility representative of the latest technology in LIB production. The cell manufactured in the small-scale facility is an NMC-1:1:1 (nickel-manganese-cobalt) pouch cell, whereas in the large-scale facility, the cell produced in an NMC-8:1:1 cylindrical cell. We model production in varying carbon intensity scenarios using recycled and exclusively primary materials as input options. We assess environmental pollution–related impacts using ReCiPe midpoint indicators and resource use impacts using the surplus ore method (ReCiPe) and the crustal scarcity indicator.Results and discussionRemodelling of the small-scale factory using updated background data showed a 34% increase in greenhouse gas emissions — linked to updated cobalt sulfate production data. Upscaling production reduced emissions by nearly 45% in the reference scenario (South Korean energy mix) due to a reduced energy demand in cell production. However, the emissions reduce by a further 55% if the energy is sourced from a low-carbon intensity source (Swedish energy mix), shifting almost all burden to upstream supply chain. Regional pollution impacts such as acidification and eutrophication show similar trends. Toxic emissions also reduce, but unlike other impacts, they were already occurring during mining and ore processing. Lastly, nickel, cobalt, and lithium use contribute considerably to resource impacts. From a long-term perspective, copper becomes important from a resource scarcity perspective.ConclusionsUpscaling LIB production shifts environmental burdens to upstream material extraction and production, irrespective of the carbon intensity of the energy source. Thus, a key message for the industry and policy makers is that further reductions in the climate impacts from LIB production are possible, only when the upstream LIB supply chain uses renewable energy source. An additional message to LCA practitioners is to examine the effect of changing background systems when evaluating maturing technologies.

The concentration distributions of binders in dried water-based and organic-based LiCoO2 electrode sheets are studied, and the effects of binder distributions on the physical, electrical and electrochemical properties of electrodes are also discussed. When the LiCoO2 slurry is prepared with an organic-based process, the non-uniform distributions of the binder, poly(vinylidene fluoride), and a conductive agent, graphite, are markedly observed in the dried electrode sheet. Nevertheless, these non-uniform distributions of constituents are less significant for the electrode sheet prepared by a water-based process that uses a blend of styrene butadiene rubber and sodium carboxymethyl cellulose as the binder. Beside the experimental results, the binder distributions in the dried electrodes can be accurately predicted via a theoretical calculation based on a migration-controlled drying kinetics. The calculated results show that the organic-based electrode sheet has much higher non-uniformity of binder distribution than the water-based one. Because of the higher non-uniform distributions of binder, the organic-based electrode sheet displays properties of weaker adhesion and higher electrical resistance. Moreover, the electrochemical performance shows that the IR-drop of the organic-based electrode is larger than the water-based one, which has to be reduced by the compression process of electrode sheets.

Sustainable approach to achieve overall leaching of Li and Co in spent lithium-ion batteries without liberation by overall pyrolysis

Understanding the volume changes in lithium-ion batteries (LIBs) during charge and discharge cycles is crucial for improving battery lifespan and safety. These changes primarily originate from deformations in the electrode sheets, which are expected to be heterogeneous. However, existing methods often lacked spatial resolution and thus are insufficient in mapping this nonuniformity. This study introduced an optical method for mapping thickness changes in electrode sheets through image sharpness evaluation, revealing significant spatial heterogeneity in the expansion and shrinkage of electrode sheets under the operational conditions. The thickness variations of lithium iron phosphate (LFP) and lithium nickel cobalt manganese oxide (NCM) cathodes during cycling were quantitatively investigated. Results demonstrated that the electrode thickness decreased during delithiation and increased during lithiation, corresponding to changes in the crystal structure. Additional factors, such as internal stress accumulated during the manufacturing process, were also identified and analyzed. Results indicate that thickness nonuniformity is influenced by both the state of charge of particles and the evolution of internal stress during cycling. The proposed image-based method offered spatial resolution on the expansion and shrinkage of electrode sheet without interference from gas generation, contributing to a deeper understanding of capacity degradation and the development of strategies to extend the LIB lifespan.

Life Cycle Assessment of Lithium-ion Batteries: A Critical Review

The electrification of transport systems is essential for improved city air quality and reduced noise, may also contribute to enhanced energy security and decreased greenhouse gas emissions. The key enabler of the large-scale uptake of electric vehicles (EVs) are improved lithium-ion batteries (LIBs), offering higher mass specific energies, volumetric energy densities, potential differences and energy efficiencies. Most LIBs used in automotive applications combine nickel-cobalt-manganese (NCM) oxide cathodes with graphite (Gr) anodes intercalating lithium ions from organic electrolyte solutions of lithium salts. Two widely reported modifications include increasing the nickel content in cathodes and introducing silicon-graphite (SiGr) composite anodes, enabling increased energy storage capacities. Technological developments in EVs and LIBs have triggered a growing interest in using Life Cycle Assessment (LCA) to quantify the environmental burdens of electrified mobility (Ellingsen et al., 2014; Kim et al., 2016). Figure 1 compares the global warming potential (GWP) (kg CO2-eq. (battery kW h)- 1) of battery manufacturing at different locations, for reports that allowed the production footprint to be distinguished. The indication that despite the higher coal intensity in its electricity mix, China’s LIB manufacturing has a lower GWP production footprint than other regions is counter-intuitive and raises the need for more detailed analysis. An important additional aim of this work is to consider whether the high environmental burdens of producing LIBs can be counter-balanced by extended EV use periods and the parameters that affect these. Since nickel-rich cathodes and silicon-based anodes are considered the most promising modifications for next-generation LIBs in the near-term, their combined environmental performance is studied. This paper reports on the development of a detailed unit process-based Life Cycle Inventory model, built to assess the production of current and future NCM batteries in China. The definition of the studied product system and LCI model is followed by the introduction of four different battery production scenarios, which were developed to assess the impacts of producing batteries in China, study the introduction of silicon in anodes and examine the effects of two novel cathode chemistries with increased nickel content (NCM622, NCM811). A detailed presentation of the production phase impacts is provided, based on the ReCiPe 1.08 Midpoint characterisation method. The production phase analysis is complemented by the development of a gate-to-gate model, assessing the environmental impact of using a LIB in a passenger vehicle in China. The results indicate that the GWP of producing a LIB in China is 250 kg CO2-eq (battery kW h)-1, which is 40% higher than previously estimated (Ellingsen et al., 2014) and significantly higher than earlier reported values for China (Hao et al., 2017; Yu et al., 2018). The mismatch with the latter two studies is due to the fundamentally different assumptions made when modelling the production phase. This work provides the means to make sensible comparisons, using the same model and assumptions, and accurately benchmark the performance of different scenarios. It is shown that copper production for anode current collectors makes the most important contribution towards all human toxicity and ecotoxicity categories, with the next most important contribution coming from nickel sulfate production for mixed metal oxide cathodes. Furthermore, the manufacturing of next-generation LIBs is estimated to have a slightly increased impact intensity on a per battery pack basis, with the increased nominal energy capacity effectively reducing the impacts on a per kW h basis. The use of LIBs in China primarily affects the GWP, as a result of the high coal intensity of the local electricity mix. References Amarakoon, S., Smith, J., Segal, B., 2013. Application of life-cycle assessment to nanoscale technology: Lithium-ion batteries for electric vehicles. No. EPA 744-R-12-001. Ellingsen, L.A.W., Majeau-Bettez, G., Singh, B., Srivastava, A.K., Valøen, L.O., Strømman, A.H., 2014. Life Cycle Assessment of a Lithium-Ion Battery Vehicle Pack. J. Ind. Ecol. 18, 113–124. Hao, H., Mu, Z., Jiang, S., Liu, Z., Zhao, F., 2017. GHG Emissions from the production of lithium-ion batteries for electric vehicles in China. Sustain. 9. Kim, H.C., Wallington, T.J., Arsenault, R., Bae, C., Ahn, S., Lee, J., 2016. Cradle-to-Gate Emissions from a Commercial Electric Vehicle Li-Ion Battery: A Comparative Analysis. Environ. Sci. Technol. 50, 7715–7722. Majeau-Bettez, G., Hawkins, T.R., StrØmman, A.H., 2011. Life cycle environmental assessment of lithium-ion and nickel metal hydride batteries for plug-in hybrid and battery electric vehicles. Environ. Sci. Technol. 45, 4548–4554. Yu, A., Wei, Y., Chen, W., Peng, N., Peng, L., 2018. Life cycle environmental impacts and carbon emissions: A case study of electric and gasoline vehicles in China. Transp. Res. Part D Transp. Environ. 65, 409–420. Figure 1

Lithium-ion battery (LIB) production as a central part of decarbonisation strategies is driving mineral extraction in countries of the global South, where they exacerbate existing conflicts over the creation and distribution of value. Value, however, is a contested concept. Following the pragmatic sociology of values, we argue that the analysis of value creation and distribution cannot be separated from the intersubjective and normative conflicts over valuation. We examine valuation controversies in Madagascar as a mining dispute by describing the grammar of values on the example of taxation design in Madagascar’s mining reform influenced by LIB production. Empirical evidence from ethnographic fieldwork and expert interviews on negotiations between stakeholders’ different principles of value helped identify conflicting value justifications and finding local compromises. Here, the pervasive nature of neoliberal economisation is monopolised by a specific interpretation of value wired to investors’ expectations and complicated by path-dependent legacies. Our analysis illustrates how asymmetric economic power favours particular economic and operating registers of a ‘green capitalism’ valuation system. Building on the analytical gain of Heinich’s novel pragmatic value approach, we show how the recent mining reform in Madagascar is contested and that compromise around value remains fragile (or impossible) in the current institutional context.

In lithium-ion battery (LIB) production, limp electrodes are handled gently by vacuum-pressure based handling and transport systems, which generate a fluid flow that propagates through the porous electrode coating during handling. To investigate the limits and material-damaging behavior of vacuum pressure-based handling, it is required to understand how process parameters and electrode qualities affect fluid flow. Questions on how fluid flow reduces electrode quality are insufficiently addressed or modeled. Modeling the electrode and handling system interaction requires knowledge of the effective surface geometry and the volumetric flow rate caused by the pressure difference. In this article, flow through porous electrode coatings during handling is modeled. Experiments demonstrate a flow behavior according to the generalized Darcy’s law. Thus, using Darcy’s law, modeling fluid flow through the electrode improves the exploration of the limits and design of vacuum pressure-based handling and transport of electrodes in LIB production.

As the global consumption of lithium-ion batteries (LIBs) continues to accelerate, the need to advance LIB recycling technologies and create a more robust recycling infrastructure has become an important consideration to improve LIB sustainability and recover critical materials to reuse in new LIB production. Battery collection, sorting, diagnostics, and second-life usage all contribute to the LIB logistics network, and developments in each of these areas can improve the ultimate recycling and recovery rate. Recent progress in LIB recycling technology seeks to increase the amount of valuable metal compounds, electrode materials, and other LIB components that are recoverable and that can be redeployed in new LIB production or other markets. This review establishes an overview of these developments and discusses the strengths and weaknesses of each major recycling technology. Of particular note are the differences in recycling technology and infrastructure requirements created by various LIB markets, as well as the techno-economic considerations for different recycling methods based on the evolving LIB formats and component compositions.

The greenhouse gas emissions of automotive lithium-ion batteries: a statistical review of life cycle assessment studies

Lithium ion batteries have received great attention due to emerging electric vehicle market to suppress global climate change issues. Batteries with higher energy density is required to improve driving distance of electric vehicle. As energy density increase, safety become more important point to prevent unexpected accident. Safety issues of current lithium ion battery system mainly comes from the oxide cathode and flammable organic electrolyte. All solid state batteries with non-flammable inorganic solid electrolytes come into the limelight due to its potential for securing higher energy density and safe characteristics over current lithium ion battery system.In this study, composite electrode sheet and cell fabrication technology was examined by slurry mixing coating technique. Cathode electrode sheets were obtained by coating slurries consisting of LiNi0.8Co0.1Mn0.1O2 as the active material, an argyrodite structure Li6PS5Cl solid electrolyte, conductive carbon, butadiene-based binder with solvent on carbon coated aluminum foil as the current collector. Homogeneous mixing and coating conditions were examined by controlling composition, kinds of binder in order to achieve optimal conduction pathway of lithium ion and electron. All solid state batteries were fabricated and evaluated both half-cell and full-cell type. Electrochemical tests were investigated and the detailed results will be discussed in this presentation.

Electric vehicles based on lithium-ion batteries (LIB) have seen rapid growth over the past decade as they are viewed as a cleaner alternative to conventional fossil-fuel burning vehicles, especially for local pollutant (nitrogen oxides [NOx], sulfur oxides [SOx], and particulate matter with diameters less than 2.5 and 10 μm [PM2.5 and PM10]) and CO2 emissions. However, LIBs are known to have their own energy and environmental challenges. This study focuses on LIBs made of lithium nickel manganese cobalt oxide (NMC), since they currently dominate the United States (US) and global automotive markets and will continue to do so into the foreseeable future. The effects of globalized production of NMC, especially LiNi1/3Mn1/3Co1/3O2 (NMC111), are examined, considering the potential regional variability at several important stages of production. This study explores regional effects of alumina reduction and nickel refining, along with the production of NMC cathode, battery cells, and battery management systems. Of primary concern is how production of these battery materials and components in different parts of the world may impact the battery’s life cycle pollutant emissions and total energy and water consumption. Since energy sources for heat and electricity generation are subject to great regional variation, we anticipated significant variability in the energy and emissions associated with LIB production. We configured Argonne National Laboratory’s Greenhouse gases, Regulated Emissions, and Energy use in Transportation (GREET®) model as the basis for this study with key input data from several world regions. In particular, the study examined LIB production in the US, China, Japan, South Korea, and Europe, with details of supply chains and the electrical grid in these regions. Results indicate that 27-kWh automotive NMC111 LIBs produced via a European-dominant supply chain generate 65 kg CO2e/kWh, while those produced via a Chinese-dominant supply chain generate 100 kg CO2e/kWh. Further, there are significant regional differences for local pollutants associated with LIB, especially SOx emissions related to nickel production. We find that no single regional supply chain outperforms all others in every evaluation metric, but the data indicate that supply chains powered by renewable electricity provide the greatest emission reduction potential.

Through investments in automated manufacturing, Quallion will reduce the costs of its domestically produced lithium ion cells and batteries, greatly expanding their potential uses in aerospace, military, and industrial applications.Quallion has demonstrated high quality, long life, and high performance lithium ion battery technology in critical applications such as implantable medical devices and low earth orbit satellites. Quallion’s long life lithium ion cell chemistry was the basis for its selection for a US Government program to build a US based manufacturing capability for space grade lithium ion cells, as well as anode and cathode materials. This vertical integration allows for full configuration control and integration of unique Quallion technologies into large format prismatic cells; however, these materials and cell level advantages remain out of reach of the vast majority of potential applications due to high cost manufacturing associated with custom cell designs and labor intensive processes. Neither Quallion’s small medical cells nor its large satellite cells are cost effective for applications such as military air, sea, and ground vehicles; commercial vehicle applications; or other industrial settings; but new automated manufacturing will enable production of cost effective cells to bring cutting edge lithium ion technology to an expanded pool of users.By leveraging an industrial standard cell design and automating key production processes, Quallion is making its energy storage products more affordable. Quallion’s manufacturing enhancement programs are supported by grants from the State of California, which has opened up additional opportunities to leverage federal matching programs. Quallion targeted the most common industrial battery form factor for its manufacturing program, the cylindrical 18650 cell. Produced in large quantities by Asian industrial giants, the 18650 has a broad base of component and equipment suppliers that reduce the degree of customization of cell design and process, thereby reducing costs. This cell design is also compatible with many Quallion battery pack designs, which have used commercial 18650 cells in conjunction with unique packaging technologies for military and aerospace programs to date.Quallion also automated key manufacturing processes to reduce unit cost and increase production capability, including: winding of electrodes, assembly of 18650 cells, formation and testing of cells, welding of cells into modules, testing of modules and finished batteries, including those with integrated battery management systems. These manufacturing enhancements will reduce direct labor costs per piece, a critical requirement to retain a competitive domestic manufacturing base, enhance factory throughput, and improve product quality through reduced production errors.When completed in 2014, the automated production facility will enable cost competitive, US based production of lithium ion batteries for land, sea, and air applications. These batteries will enable second order cost reductions through weight reduction, fuel savings, and reduced battery replacement compared to legacy Ni-Cd and lead acid batteries. Quallion’s 18650 batteries will feature the same cutting edge technologies that have made Quallion stand out in high reliability medical and space markets, but they will be produced more affordably by leveraging advanced manufacturing techniques. Advanced technologies included in Quallion’s 18650 cells will include a wide operating temperature to enable discharge between -40 to 71C and Zero-Volt deep discharge tolerance which enables a cell to be fully discharged multiple times and stored in that state indefinitely without any reduction in capacity or performance. Cells will also feature Quallion’s long life lithium ion chemistry which demonstrates unrivaled cycle life and calendar life performance.The new manufacturing line will also allow for experimentation and prototyping of new chemistries and cell designs in an industrial setting, and Quallion will make its facilities available to others seeking to demonstrate their electrochemical technology.

The investigation of polymers as binders of Al doped Li4Ti5O12 for Li-ion battery electrode is reported. Polimer binders such as Polyvinylidene fluoride (PVDF), polyvinyl alcohol (PVA), and Polytetrafluoroethylene (PTFE) were used to make electrode sheet. Al doped Lithium Titanate (Al-doped Li4Ti5O12) were used as electrode powders. Al doped Li4Ti5O12 powders were synthesized from LiOH.H2O, TiO2 and Al2O3 via solid state reaction. X-ray diffraction (XRD) was used to analysed phase and size of particle. Electrode sheets were manufactured by used active material, binders, and acetylene black in ratio 85:10:5 wt%. Electrode sheets were cut and assembled into coin cell batteries. Coin cell samples were characterized by EIS, cyclic voltammetry and charge-discharge to get electrochemical performance. XRD result reveals that there are two phases formed from final product such as Li4Ti5O12 and rutile TiO2. EIS diagram showed that sample with PTFE binder has the best conductivity with 3.10−5 S/cm. While, cyclic voltammetry and charge-discharge test showed sample with PVDF binder has the best chemical performance with good redox peaks and highest specific capacity about 110 mAh/g.