Case study of N-carboxyanhydrides in silicon-based lithium ion cells as a guideline for systematic electrolyte additive research

Schmiegel, Jan-Patrick; Nölle, Roman; Henschel, Jonas; Quach, Linda; Nowak, Sascha; Winter, Martin; Glorius, Frank; Placke, Tobias

doi:10.1016/j.xcrp.2021.100327

Cited by 19 publications

(45 citation statements)

References 96 publications

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“…The standard electrolyte (STD) used in this work was 1 m LiPF 6 in ethylene carbonate (EC):ethyl methyl carbonate (EMC) 3:7 (by weight; Solvionic; purity: battery grade). Four different separators were used: i) “PP membrane” separator (PP; Celgard 2500; Celgard); ii) “PP fiber” separator (PP; FS2190; Freudenberg); iii) “C‐PET” separator (ceramic‐coated PE terephthalate; Mitsubishi OZ S‐30; Mitsubishi); iv) “C‐PE” separator (ceramic‐coated PE membrane; collected from commercial pouch cells; [ 39 ] Li‐Fun technology). Further details can be found in Table S1, Supporting Information.…”

Section: Methodsmentioning

confidence: 99%

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF₆ on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Klein

Wrogemann

Wickeren

et al. 2021

Advanced Energy Materials

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Section: Methodsmentioning

confidence: 99%

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF₆ on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Klein

Wrogemann

Wickeren

et al. 2021

Advanced Energy Materials

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“…From a series of different analysis techniques, the authors conclude that the additives work by ring‐opening polymerization with decarboxylation and thus generate effective SEI layers. [ 96 ]…”

Section: Electrolyte Interfacing Si‐based Electrodementioning

confidence: 99%

“…For the sake of completeness, reports where FEC is utilized as an electrolyte additive can be found in references [ 45–47,51–55,60–62,67,69,73,75–77,92–125 ] and reports utilizing VC as electrolyte additive can be found in references. [ 40,45,47–49,69,71,73,75–77,98,99,102–104,106,115,119,122,123,126–132 ]…”

Section: Electrolyte Interfacing Si‐based Electrodementioning

confidence: 99%

“…From a series of different analysis techniques, the authors conclude that the additives work by ring-opening polymerization with decarboxylation and thus generate effective SEI layers. [96] Lactide (LAC): Nölle et al designed an additive to combine the beneficial effects of two other additives, one of which was LAC (see lacOCA and DEDC). LAC is able to form effective layers by forming poly(lactic acid) (PLA).…”

Section: Carbonyl-based Additivesmentioning

confidence: 99%

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Interfacing Si‐Based Electrodes: Impact of Liquid Electrolyte and Its Components

Wölke

Sadeghi

Eshetu

et al. 2022

Adv Materials Inter

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As the demand for mobile energy storage devices has steadily increased during the past decades due to the rising popularity of portable electronics as well as the continued implementation of electromobility, energy density has become a crucial metric in the development of modern batteries. It was realized early on that the successful utilization of silicon as negative electrode material in lithium‐ion batteries would be a quantum leap in improving achievable energy densities due to the roughly ten‐fold increase in specific capacity compared to the state‐of‐the‐art graphite material. However, being an alloying type material rather than an intercalation/insertion type, silicon poses numerous obstacles that need to be overcome for its successful implementation as a negative electrode material with the most prominent one being its extreme volume changes on (de‐)lithiation. While, as of today, a plethora of different types of Si‐based electrodes have been reported, a universally common feature is the interface between Si‐based electrode and electrolyte. This review focuses on the knowledge gained thus far on the impact of different liquid electrolyte components/formulations on the interfaces and interphases encountered at Si‐based electrodes.

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“…10 Progressive fracturing and formation of SEI eventually result in disconnection of active Si, degrading the capacity. 11,12 Various strategies have been employed to mitigate fracture and disconnection, such as optimizing electrolyte composition, 13,14 including binders and conductive carbon additives, 15,16 as well as adding protective surface layers encapsulating the silicon. 17,18 Other strategies include changing the Si morphology to nanowires, 19−21 100 nm, 22−24 and introducing porosity to better accommodate volume expansion.…”

Section: ■ Introductionmentioning

confidence: 99%

Beyond Thin Films: Clarifying the Impact of c-Li₁₅Si₄ Formation in Thin Film, Nanoparticle, and Porous Si Electrodes

Woodard

Kalisvaart

Sayed

et al. 2021

ACS Appl. Mater. Interfaces

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The formation of the c-Li15Si4 phase has well-established detrimental effects on the capacity retention of thin film silicon electrodes. However, the role of this crystalline phase with respect to the loss of capacity is somewhat ambiguous in nanoscale morphologies. In this work, three silicon-based morphologies are examined, including planar films, porous planar films, and silicon nanoparticle composite powder electrodes. The cycling conditions are used as the lever to induce, or not induce, the formation of c-Li15Si4 through application of constant-current (CC) or constant-current constant-voltage (CCCV) steps. In this manner, the role of this phase on capacity retention and Coulombic efficiency can be determined with few other convoluting factors such as alteration of the composition or morphology of the silicon electrodes themselves. The results here confirm that the c-Li15Si4 phase increases the rate of capacity decay in planar films but has no major effect on capacity retention in half-cells based on porous silicon films or silicon nanoparticle composite powder electrodes, although this conclusion is nuanced. Besides using a constant-voltage step, formation of the c-Li15Si4 phase is influenced by the dimensions of the Si material and the lithiation cutoff voltage. Porous Si films, which, in this work, comprise primary Si particle sizes that are smaller than those in the preformed Si nanoparticle slurries, do not undergo the formation of c-Li15Si4 at 50 mV, whereas Si nanoparticle slurries are accompanied by the formation of c-Li15Si4 up to 80 mV. The solid-electrolyte interphase (SEI) formed from reaction of the c-Li15Si4 with the carbonate-based electrolyte causes polarization in both nanoparticle and porous film silicon electrodes and lowers the average Coulombic efficiency. A comparison of the cumulative irreversibilities due to SEI formation between different lithiation cutoff voltages in silicon nanoparticle slurry electrodes confirmed the connection between higher SEI buildup and formation of the c-Li15Si4 phase. This work indicates that concerns about the c-Li15Si4 phase in silicon nanoparticles and porous silicon electrodes should mainly focus on the stability of the SEI and a reduction of irreversible electrolyte reactions.

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Case study of N-carboxyanhydrides in silicon-based lithium ion cells as a guideline for systematic electrolyte additive research

Cited by 19 publications

References 96 publications

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF₆ on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF₆ on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Interfacing Si‐Based Electrodes: Impact of Liquid Electrolyte and Its Components

Beyond Thin Films: Clarifying the Impact of c-Li₁₅Si₄ Formation in Thin Film, Nanoparticle, and Porous Si Electrodes

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Case study of N-carboxyanhydrides in silicon-based lithium ion cells as a guideline for systematic electrolyte additive research

Cited by 19 publications

References 96 publications

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF6 on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF6 on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Interfacing Si‐Based Electrodes: Impact of Liquid Electrolyte and Its Components

Beyond Thin Films: Clarifying the Impact of c-Li15Si4 Formation in Thin Film, Nanoparticle, and Porous Si Electrodes

Contact Info

Product

Resources

About

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF₆ on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Understanding the Role of Commercial Separators and Their Reactivity toward LiPF₆ on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells

Beyond Thin Films: Clarifying the Impact of c-Li₁₅Si₄ Formation in Thin Film, Nanoparticle, and Porous Si Electrodes