Lithium-ion battery cell formation: status and future directions towards a knowledge-based process design

Schomburg, Felix; Heidrich, Bastian; Wennemar, Sarah; Drees, Robin; Roth, Thomas; Kurrat, Michael; Heimes, Heiner; Jossen, Andreas; Winter, Martin; Cheong, Jun Young; Röder, Fridolin

doi:10.1039/d3ee03559j

Cited by 15 publications

(1 citation statement)

References 504 publications

(1,065 reference statements)

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“…Lithium oxalate has been proposed as a sacrificial salt [30]. During charging, only Li + and CO 2 are generated, while the gas produced can be extracted by vacuum from the battery system before sealing during the formation process [31]. Because of its theoretical capacity of 545 mAh•g −1 , low cost, remarkable air stability and its lack of decomposition residue, it is an ideal cathode prelithiation additive.…”

Section: Introductionmentioning

confidence: 99%

Electrocatalytic Decomposition of Lithium Oxalate-Based Composite Microspheres as a Prelithiation Additive in Lithium-Ion Batteries

Liu,

Lin,

Yin

et al. 2024

Molecules

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In conventional lithium-ion batteries (LIBs), the active lithium from the lithium-containing cathode is consumed by the formation of a solid electrolyte interface (SEI) at the anode during the first charge, resulting in irreversible capacity loss. Prelithiation additives can provide additional active lithium to effectively compensate for lithium loss. Lithium oxalate is regarded as a promising ideal cathode prelithiation agent; however, the electrochemical decomposition of lithium oxalate is challenging. In this work, a hollow and porous composite microsphere was prepared using a mixture of lithium oxalate, Ketjen Black and transition metal oxide catalyst, and the formulation was optimized. Owing to the compositional and structural merits, the decomposition voltage of lithium oxalate in the microsphere was reduced to 3.93 V; when being used as an additive, there is no noticeable side effect on the performance of the cathode material. With 4.2% of such an additive, the first discharge capacity of the LiFePO4‖graphite full cell increases from 139.1 to 151.9 mAh g−1, and the coulombic efficiency increases from 88.1% to 96.3%; it also facilitates the formation of a superior SEI, leading to enhanced cycling stability. This work provides an optimized formula for developing an efficient prelithiation agent for LIBs.

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Section: Introductionmentioning

confidence: 99%

Electrocatalytic Decomposition of Lithium Oxalate-Based Composite Microspheres as a Prelithiation Additive in Lithium-Ion Batteries

Liu,

Lin,

Yin

et al. 2024

Molecules

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Anions‐Trappable Hollow Mesoporous Nanoparticle Coating Enables High‐Performance and Safe Lithium Metal Batteries

Gao,

Zhang,

et al. 2024

Adv Funct Materials

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Polyolefin separators, such as polypropylene (PP) and polyethylene (PE) separators, are the commonly used separators for lithium batteries, which have good mechanical properties and chemical/electrochemical stability, but their high‐temperature dimensional stability is poor and Li+ transference number (t Li+) is low. Recently, much attention has been paid to developing separators with new substrates, but so far there is no separator to replace the polyolefin separator for large‐scale application. Therefore, the surface modification of the polyolefin separator to enhance its functionality is a simple and effective method. Among many modified layers, the porous modified layer can store the electrolyte and provide enough space for ion transport. In this work, a hollow mesoporous silica nanosphere (mSiO2) is prepared for the PP separator multifunctional coating to improve the electrochemical performance and high‐temperature safety of the PP separator. The experimental and theoretical results show that the mSiO2 coating can not only improve the electrolyte wettability and high‐temperature dimensional stability of the PP separator, but also promote the Li+ transport, so that the mSiO2/PP separator exhibits high ionic conductivity (2.35 mS cm−1) and high t Li+ (0.63). As a result, Li//LiFePO4 cells using mSiO2/PP separators exhibit excellent cycling performance, rate performance, and high‐temperature safety.

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Prelithiated Carbon Nanotube‐Embedded Silicon‐based Negative Electrodes for High‐Energy Density Lithium‐Ion Batteries

Ünal,

Maccio‐Figgemeier,

Haneke

et al. 2024

Adv Materials Inter

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Multi‐walled carbon Nanotubes (MWCNTs) are hailed as beneficial conductive agents in Silicon (Si)‐based negative electrodes due to their unique features enlisting high electronic conductivity and the ability to offer additional space for accommodating the massive volume expansion of Si during (de‐)lithiation. However, both MWCNTs and Siirreversibly consume an enormous amount of Li inventory to principally form a Solid Electrolyte Interphase (SEI) and due to other parasitic reactions, which results in lowering the Coulombic Efficiency (CE), rapid decrease in reversible capacity, and shorter battery life.To tackle these hurdles, electrochemical prelithiation is adopted as a taming strategy to mitigate the large capacity loss (nearly reducing the first irreversible capacity by ≈60%) of MWCNT‐Si/Graphite (Gr) negative electrode‐based full‐cells. In contrast, a yardstick negative electrode utilizing commercially used Super P (Super P‐Si/Gr) showed a reduction of ≈47% after in vitro pre‐doping with lithium, which is considerably smaller compared to that of MWCNTs‐based electrode design. Furthermore, the Initial CE, life cycle, and rate capability are enhanced by prelithiation. Interestingly, prelithiation brings more impact on MWCNTs ‐Si/Gr than with Super P‐Si/Gr design. An in‐depth analysis using X‐ray photoelectron spectroscopy (XPS), RAMAN Spectroscopy, Attenuated Total Reflection Fourier Transform Infrared Spectroscopy (ATR FTIR), laser microscopy, and Scanning Electron Microscopy (SEM) reveal deeper insights into the differences in SEI layer between prelithiated MWCNTs and their Super P‐based electrode counterparts.

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Lithium-ion battery cell formation: status and future directions towards a knowledge-based process design

Abstract: The battery cell formation is one of the most critical process steps in lithium-ion battery (LIB) cell production, because it affects the key battery performance metrics, e.g. rate capability, lifetime...

Cited by 15 publications

References 504 publications

Electrocatalytic Decomposition of Lithium Oxalate-Based Composite Microspheres as a Prelithiation Additive in Lithium-Ion Batteries

Electrocatalytic Decomposition of Lithium Oxalate-Based Composite Microspheres as a Prelithiation Additive in Lithium-Ion Batteries

Anions‐Trappable Hollow Mesoporous Nanoparticle Coating Enables High‐Performance and Safe Lithium Metal Batteries

Prelithiated Carbon Nanotube‐Embedded Silicon‐based Negative Electrodes for High‐Energy Density Lithium‐Ion Batteries

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