Towards a Fundamental Understanding of the Improved Electrochemical Performance of Silicon–Carbon Composites

Saint, Juliette; Morcrette, Mathieu; Larcher, Dominique; Laffont, Lydia; Beattie, Shane D.; Pérès, Jean-Paul; Talaga, David; Couzi, M.; Tarascon, Jean‐Marie

doi:10.1002/adfm.200600937

Cited by 277 publications

(221 citation statements)

References 50 publications

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“…Amorphous silicon has been reported to have a characteristic Raman band at ∼480 cm −166 and a very broad 65 or asymmetric 67 Raman peak is observed when silicon crystallites have a significant degree of disorder. For our Si/C composites, the silicon peak is symmetrical, and its shift and width are rather low compared to the ones reported for amorphous silicon, suggesting that the degree of disorder of silicon surface, if any, is insignificant, below detection limit.…”

Section: Resultsmentioning

confidence: 99%

Relationship between the Properties and Cycle Life of Si/C Composites as Performance-Enhancing Additives to Graphite Electrodes for Li-Ion Batteries

Schott

Gómez-Cámer

Novák

et al. 2016

J. Electrochem. Soc.

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With its high theoretical specific charge, silicon is a promising candidate as electrode additive to enhance specific charge of graphite electrodes for high-energy-density Li-ion batteries. We prepared Si/C composites by a two-step procedure: the ballmilling of silicon nanoparticles with a carbon precursor for homogenization, followed by a carbonization step. The effects of the carbon source and the carbonization parameters on the physical and electrochemical composite properties were identified. Longer cycle life was reached for graphite electrodes containing Si/C composites than with silicon nanoparticles simply mixed with carbon black, and the extent of the improvement was dependent on the physical properties of Si/C composite. A carbon host with a larger pore volume -obtained using sucrose precursor, especially at lower heat-treatment temperatures, -enabled a more efficient buffering of the silicon volume changes. However, this did not define good cycling stability. The electrochemical performance was found, instead, being significantly affected by the contact between the silicon nanoparticles and the carbon matrix, and by the structure of the latter. The stacking and in-plane ordering of the graphitic domains in the amorphous carbon -tuned by the precursor nature and the heat-treatment temperature -were crucial for effectiveness of lithiation/delithiation processes. Graphite, due to its very negative reaction potential and its performance stability, is the most common negative electrode material in current lithium-ion batteries. However, limits of its theoretical specific charge (372 mAh g −1 ) have already been reached and, therefore, it is impossible to increase energy density of the battery any further using graphite alone. One promising candidate to replace graphite in negative electrodes is silicon, which has a high theoretical specific charge of 3575 mAh g −1 (forming Li 15 Si 4 ), and whose reactions occur in a potential window similar to graphite. In addition, silicon is abundant, cheap and environmentally friendly, and due to this has attracted a lot of attention in the last twenty years.1-5 However, silicon-containing electrodes suffer from strong performance fading due to significant volume changes of silicon particles during cycling. 2,3,6 These volume changes lead to cracking of the electrode and/or silicon particles, and to disconnection of silicon from the conductive network, which in turn leads to loss of utilizable active material. Moreover, the solid electrolyte interphase (SEI) is damaged after each cycle and grows continuously on the newly exposed surface of silicon, trapping available lithium ions and consuming electrolyte. 7-10Several approaches were suggested in the literature to overcome these challenges. It was demonstrated that electrolyte additives, such as FEC, can prolong the cycle life of silicon-containing electrodes by improving the quality of the SEI on silicon.10-13 The electrode integrity can also be longer maintained if the common PVDF binder is replaced by water-soluble ...

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Section: Resultsmentioning

confidence: 99%

Relationship between the Properties and Cycle Life of Si/C Composites as Performance-Enhancing Additives to Graphite Electrodes for Li-Ion Batteries

Schott

Gómez-Cámer

Novák

et al. 2016

J. Electrochem. Soc.

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“…4 The shortened ion and electron diffusion paths and increased surface area of the electrodes for fast chemical reactions 4,96,97 of nanosized structures also enhance the rate performance. Material compositing, wherein one material component (e.g., Si) is used to store Li, and the other (e.g., carbon) to enhance the overall conductivity and mechanical stability, 61,[98][99][100][101] has also been adopted to improve the electrochemical performance of the electrode materials.…”

Section: Strategies For Mitigating the Electrochemo-mechanical Degradmentioning

confidence: 99%

Chemomechanical modeling of lithiation-induced failure in high-volume-change electrode materials for lithium ion batteries

Zhang

2017

npj Comput Mater

101

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The rapidly increasing demand for efficient energy storage systems in the last two decades has stimulated enormous efforts to the development of high-capacity, high-power, durable lithium ion batteries. Inherent to the high-capacity electrode materials is material degradation and failure due to the large volumetric changes during the electrochemical cycling, causing fast capacity decay and low cycle life. This review surveys recent progress in continuum-level computational modeling of the degradation mechanisms of high-capacity anode materials for lithium-ion batteries. Using silicon (Si) as an example, we highlight the strong coupling between electrochemical kinetics and mechanical stress in the degradation process. We show that the coupling phenomena can be tailored through a set of materials design strategies, including surface coating and porosity, presenting effective methods to mitigate the degradation. Validated by the experimental data, the modeling results lay down a foundation for engineering, diagnosis, and optimization of high-performance lithium ion batteries.

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“…In the literatures, they report that the carbonaceous additives play multiple beneficial roles in Si-based electrodes. [23][24][25][26][27][28][29] Not only are they helpful in limiting the extent to which Si alloys with Li, they also supplement the poor electrical conductivity of Si as well z E-mail: kyuhwan@snu.ac.kr; sehee.lee@colorado.edu as increase the total capacity of the electrode by acting as a secondary Li active material.Electrospinning is a simple and effective method to prepare Si/C composite fiber structures. 14,21,[30][31][32][33] Since the Si/C fibers prepared by electrospinning provide extensive contact areas between the Si and C phase, we can expect many conduction pathways for electron transfer to and from the Si particles.…”

mentioning

confidence: 99%

“…20 One effective strategy to accommodate the extreme volume changes of Si is to limit its extent of alloying with Li by introducing resilient additives into the electrode. [11][12][13][14][21][22][23] These additives encapsulate the Si particles as rigid matrix agents, restricting the particles' free expansion during lithiation, and thereby lowering the number of moles of Li alloying with each Si particle. The restricted lithiation of the Si particles results in a lower specific capacity for the electrode, but this limited capacity can be more reliably maintained with fewer irreversible capacity losses in the subsequent cycles.…”

mentioning

confidence: 99%

Nanostructured Si/C Fibers as a Highly Reversible Anode Material for All-Solid-State Lithium-Ion Batteries

Kim

Dunlap

Han

et al. 2018

J. Electrochem. Soc.

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This study demonstrates the application of Si/C composite fibers as anode materials for all-solid-state lithium-ion batteries. Using polyacrylonitrile as the carbon precursor, Si/C fibers were prepared through electrospinning and subsequent heat-treating processes. To investigate the correlation between fiber diameter and electrochemical performance, we prepared three electrodes (A, B, C), containing Si/C fibers with ∼2 μm, ∼1 μm and ∼0.1 μm diameters, respectively. Our results revealed that although the composition of all three electrodes was nearly the same, the Si/C fiber based electrodes exhibited better capacity retention when their fiber diameters were smaller. Normalized to the total mass of electrode composite, the solid-state half-cell prepared with the smallest diameter (∼0.1 μm) Si/C fibers achieved a reversible specific capacity of ∼700 mAh g −1 (normalized to electrode mass) over 70 cycles. We believe that this report can serve as an informative approach toward the utilization of electrospun Si/C fibers as anode materials for all-solid-state lithium-ion batteries. Lithium-ion batteries (LIBs) have widely been used as portable energy storage devices owing to their great reversibility, long cycle life and high power output without memory effect.1,2 However, current LIBs utilizing conventional organic liquid electrolytes still have significant safety risks, such as operational instability at elevated temperatures, leakage of hazardous solvents and ignition by external damages.3-6 To overcome these safety risks, the development of the all-solid-state lithium-ion battery (SLIB) has attracted considerable attention. [3][4][5][6][7][8][9][10][11] In the SLIB configuration, a highly Li-ion conductive solid-state electrolyte (SSE) layer is deployed between positive and negative electrodes in place of the organic liquid electrolytes typically used in LIBs. This replacement of the liquid electrolyte with a highly conductive ceramic material is expected to improve both the SLIB's thermal and mechanical stabilities.To date, graphite has been extensively used as an anode material in LIBs; however, its limited capacity (372 mAh g −1 ) has been regarded as a drawback to achieving higher energy density LIBs. Silicon is considered to be a promising anode material alternative to graphite due to its large theoretical capacity (3,579 mAh g −1 ), low cost and high earth abundance.9,11-17 To achieve such a high capacity, Si inevitably undergoes a massive volume expansion/contraction process when alloying/de-alloying with Li. 18,19 Since the repeated volume changes of Si particles during cycling causes cracking, pulverization and rapid capacity fading brought on by the electrochemical isolation of active materials, it is believed that an effective accommodation of this Si volume change is essential for achieving acceptable capacity retention in these anodes. 20One effective strategy to accommodate the extreme volume changes of Si is to limit its extent of alloying with Li by introducing resilient additives into the electro...

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Towards a Fundamental Understanding of the Improved Electrochemical Performance of Silicon–Carbon Composites

Cited by 277 publications

References 50 publications

Relationship between the Properties and Cycle Life of Si/C Composites as Performance-Enhancing Additives to Graphite Electrodes for Li-Ion Batteries

Relationship between the Properties and Cycle Life of Si/C Composites as Performance-Enhancing Additives to Graphite Electrodes for Li-Ion Batteries

Chemomechanical modeling of lithiation-induced failure in high-volume-change electrode materials for lithium ion batteries

Nanostructured Si/C Fibers as a Highly Reversible Anode Material for All-Solid-State Lithium-Ion Batteries

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