Production of high-energy Li-ion batteries comprising silicon-containing anodes and insertion-type cathodes

Eshetu, Gebrekidan Gebresilassie; Zhang, Heng; Judez, Xabier; Adenusi, Henry; Armand, Michel; Passerini, Stefano; Figgemeier, Egbert

doi:10.1038/s41467-021-25334-8

Cited by 222 publications

(172 citation statements)

References 103 publications

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“…In this context, alloy‐type silicon (Si) anode has drawn intensive attention because of the high theoretical specific capacity of 4200 mA h g −1 by forming Li 22 Si 5 , and low working voltage (<0.5 V vs Li + /Li), which satisfies the demands of high energy density storage. [ 16 ] Besides, Si‐based material possesses various merits such as natural abundance, environment‐friendliness, and mature infrastructure for mass production. As early as 1971, Dey began experimenting with silicon as negative electrode.…”

Section: Introductionmentioning

confidence: 99%

Synthetic Methodologies for Si‐Containing Li‐Storage Electrode Materials

Zhou

Lin

2022

Adv Energy and Sustain Res

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Silicon is regarded as the most promising anode candidate for improving the energy density of next‐generation Li‐ion batteries (LIBs) because of the high specific capacity of 4200 mAh g−1, low working voltage, and natural abundance. It is well demonstrated that the serious issues such as huge volume expansion and intrinsic low conductivity of Si anode can be addressed by nanoengineering and compositing strategies. An important step toward fully realizing the practical application of the Si‐containing electrode lies in producing high‐quality materials on large scale. Therefore, a controllable, high‐efficient, low‐cost, and environment‐friendly synthetic methodology is required to fabricate Si‐containing anode materials with high tap density, low specific surface area, high conductivity, chemical and structural stability, and high purity, thus leading to high Coulombic efficiency, high specific capacity, long cycling stability, and superior rate capability. In this review, the effects and bottlenecks of synthetic methodologies for the developments of Si anode are emphasized. The well‐developed physical and chemical synthetic approaches of nano‐ and microstructured Si, Si‐based composites, and Si–graphite hybrid electrode materials are summarized. In each category, the main merits and limitations of different synthetic methods are discussed from both academic and industrial points of view. Finally, this review ends with a conclusion of these synthetic routes, and a brief perspective on the future direction of Si‐containing Li‐storage materials for practical LIBs.

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Section: Introductionmentioning

confidence: 99%

Synthetic Methodologies for Si‐Containing Li‐Storage Electrode Materials

Zhou

Lin

2022

Adv Energy and Sustain Res

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“…8 Even under calendar ageing conditions, SEI formation on Si is more dynamic and less passivating than that formed on graphite, leading to greater levels of degradation. 9,10 Due to these issues, lifetimes of pure Si electrodes are often too short to be relevant for commercial applications. 11 Some of the negative effects of Si-based electrodes can be mitigated though blending silicon or silicon oxides (SiOx) with other materials such as graphite.…”

Section: Introductionmentioning

confidence: 99%

“…[12][13][14] Silicon-graphite (Si-Gr) composite electrodes have been shown to drastically improve cell lifetimes. 10,13 Si-Gr electrodes with various structures and compositions have been explored to avoid the issues of electrical isolation and accelerated SEI growth. 15,16 Due to the slightly higher oxidation potential of silicon vs. graphite in an LIB, the silicon portion of the composite Si-Gr electrode remains lithiated in all but the lowest states-of-charge (SoCs).…”

Section: Introductionmentioning

confidence: 99%

“…15,16 Due to the slightly higher oxidation potential of silicon vs. graphite in an LIB, the silicon portion of the composite Si-Gr electrode remains lithiated in all but the lowest states-of-charge (SoCs). 8,10 This means that cycling a cell at high SoC will largely utilise the graphite content of the NE, whereas cycling at low SoCs will use a greater proportion of the Si content. 16 Hence, the volumetric expansion of the silicon or graphite particles also depends on the SoC cycling range.…”

Section: Introductionmentioning

confidence: 99%

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Lithium-Ion Battery Degradation: Measuring Rapid Loss of Active Silicon in Silicon-Graphite Composite Electrodes

Kirkaldy

Samieian

Offer

et al. 2022

Preprint

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In an effort to increase the specific energy of lithium-ion batteries, silicon additives are often blended with graphite (Gr) in the negative electrode of commercial cells. However, due to the large volumetric expansion of silicon upon lithiation, these Si-Gr composites are prone to faster rates of degradation than conventional graphite electrodes. Understanding the effect of this difference is key to controlling degradation and improving cell lifetimes. Here, we investigate the effects of state of charge and temperature on the ageing of a commercial cylindrical cell with a Si-Gr electrode (LG M50T). Using degradation mode analysis, we were able to quantify the rates of degradation for Si and Gr separately. Loss of active Si is shown to be worse than Gr under all operating conditions, but especially at low state of charge and high temperature, with up to 80% loss in Si capacity after 4 kA h of charge throughput (~400 equivalent full cycles). The results indicate cell lifetimes can be improved by limiting the depth of discharge of cells containing Si-Gr, which suggests Si is not beneficial for all applications. The degradation mode analysis methods developed here provide valuable new insight into the causes of cell ageing by separating the effects of the two active materials in the composite electrode. These methods provide a suitable framework for data analysis of any experimental investigations on cells involving composite electrodes.

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“…Lithium-ion Batteries (LIBs) are currently the most prominent choice for energy storage applications, especially for portable electronic devices, cordless power tools and electric vehicles thanks to their high energy density, long cycle life and low weight, compared to other energy storage technologies [1,2]. However, there is a continuous need to improve the overall electrochemical performance of lithium-ion batteries, as the constant technological advances in the fields of automotive industry and portable communication device industry demand higher specific energy and energy density (>400 Wh/kg and >800 Wh/L) [3] than actually commercially available cells.…”

Section: Introductionmentioning

confidence: 99%

Study of the Role of Void and Residual Silicon Dioxide on the Electrochemical Performance of Silicon Nanoparticles Encapsulated by Graphene

et al. 2021

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Silicon nanoparticles are used to enhance the anode specific capacity for the lithium-ion cell technology. Due to the mechanical deficiencies of silicon during lithiation and delithiation, one of the many strategies that have been proposed consists of enwrapping the silicon nanoparticles with graphene and creating a void area between them so as to accommodate the large volume changes that occur in the silicon nanoparticle. This work aims to investigate the electrochemical performance and the associated kinetics of the hollow outer shell nanoparticles. To this end, we prepared hollow outer shell silicon nanoparticles (nps) enwrapped with graphene by using thermally grown silicon dioxide as a sacrificial layer, ball milling to enwrap silicon particles with graphene and hydro fluorine (HF) to etch the sacrificial SiO2 layer. In addition, in order to offer a wider vision on the electrochemical behavior of the hollow outer shell Si nps, we also prepared all the possible in-between process stages of nps and corresponding electrodes (i.e., bare Si nps, bare Si nps enwrapped with graphene, Si/SiO2 nps and Si/SiO2 nps enwrapped with graphene). The morphology of all particles revealed the existence of graphene encapsulation, void, and a residual layer of silicon dioxide depending on the process of each nanoparticle. Corresponding electrodes were prepared and studied in half cell configurations by means of galvanostatic cycling, cyclic voltammetry and electrochemical impedance spectroscopy. It was observed that nanoparticles encapsulated with graphene demonstrated high specific capacity but limited cycle life. In contrast, nanoparticles with void and/or SiO2 were able to deliver improved cycle life. It is suggested that the existence of the void and/or residual SiO2 layer limits the formation of rich LiXSi alloys in the core silicon nanoparticle, providing higher mechanical stability during the lithiation and delithiation processes.

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Production of high-energy Li-ion batteries comprising silicon-containing anodes and insertion-type cathodes

Cited by 222 publications

References 103 publications

Synthetic Methodologies for Si‐Containing Li‐Storage Electrode Materials

Synthetic Methodologies for Si‐Containing Li‐Storage Electrode Materials

Lithium-Ion Battery Degradation: Measuring Rapid Loss of Active Silicon in Silicon-Graphite Composite Electrodes

Study of the Role of Void and Residual Silicon Dioxide on the Electrochemical Performance of Silicon Nanoparticles Encapsulated by Graphene

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