Prelithiation Effects in Enhancing Silicon-Based Anodes for Full-Cell Lithium-Ion Batteries Using Stabilized Lithium Metal Particles

dc.citation.firstpage5567en_US
dc.citation.issueNumber10en_US
dc.citation.journalTitleACS Applied Energy Materialsen_US
dc.citation.lastpage5579en_US
dc.citation.volumeNumber6en_US
dc.contributor.authorNguyen, Quan Anhen_US
dc.contributor.authorHaridas, Anulekha K.en_US
dc.contributor.authorTerlier, Tanguyen_US
dc.contributor.authorBiswal, Sibani Lisaen_US
dc.date.accessioned2023-08-01T15:34:06Zen_US
dc.date.available2023-08-01T15:34:06Zen_US
dc.date.issued2023en_US
dc.description.abstractSilicon (Si) has been considered as one of the most promising replacements for graphite anodes in next-generation lithium-ion batteries due to its superior specific capacity. However, the irreversible consumption of lithium (Li) ions in Si-based anodes, which is associated with a large volume expansion upon lithiation and the continuous formation of the solid electrolyte interphase (SEI), is especially detrimental to full-cell batteries, whose Li-ion reserve is limited. This study demonstrates the application of stabilized lithium metal particles (SLMPs) as a prelithiation method for Si anodes that can be readily incorporated into large-scale industrial battery manufacturing. Particularly, a surfactant-stabilized SLMP dispersion was designed to be spray-coated onto prefabricated Si composite anodes, forming a uniformly distributed and well-adhered SLMP layer for in situ prelithiation. In full-cells with lithium iron phosphate (LFP) cathodes, the Si-based anodes demonstrated an improved 1st cycle Coulombic efficiency and cycle life with SLMP prelithiation using capacity-control cycling. However, when cycling over the full potential range, prelithiation with high SLMP loading was found to initially increase battery capacity while inducing accelerated fading in later cycles. This phenomenon was caused by Li trapping in the Li–Si alloy associated with higher SLMP-enabled Li diffusion kinetics. Additionally, cycled Si anodes from full-cells were also examined by surface analysis techniques, X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS), demonstrating SLMP effects in modifying the SEI by increasing the inorganic content, particularly LiF, which had been widely credited with improving SEI morphology and Li-ion diffusion through the interphase. Our findings provide valuable insights into the design of prelithiation and cycling strategies for high-capacity Si-based full-cell batteries to utilize the benefits of SLMP while avoiding the Li trapping phenomenon.en_US
dc.identifier.citationNguyen, Quan Anh, Haridas, Anulekha K., Terlier, Tanguy, et al.. "Prelithiation Effects in Enhancing Silicon-Based Anodes for Full-Cell Lithium-Ion Batteries Using Stabilized Lithium Metal Particles." <i>ACS Applied Energy Materials,</i> 6, no. 10 (2023) American Chemical Society: 5567-5579. https://doi.org/10.1021/acsaem.3c00713.en_US
dc.identifier.doihttps://doi.org/10.1021/acsaem.3c00713en_US
dc.identifier.urihttps://hdl.handle.net/1911/115028en_US
dc.language.isoengen_US
dc.publisherAmerican Chemical Societyen_US
dc.rightsThis work is protected by copyright, and is made available here for research and educational purposes. Permission to reuse, publish, or reproduce the work beyond the bounds of Fair Use or other exemptions to copyright law must be obtained from the copyright holder.en_US
dc.subject.keywordprelithiationen_US
dc.subject.keywordSLMPen_US
dc.subject.keywordlithium trappingen_US
dc.subject.keywordSEIen_US
dc.subject.keywordlithium fluorideen_US
dc.subject.keywordToF-SIMSen_US
dc.titlePrelithiation Effects in Enhancing Silicon-Based Anodes for Full-Cell Lithium-Ion Batteries Using Stabilized Lithium Metal Particlesen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpost-printen_US
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