Silicon Anodes with Improved Calendar Life Enabled By Multivalent Additives

Zhang, Yunya; Li, Xiang; Sivonxay, Eric; Wen, Jianguo; Persson, Kristin A.; Vaughey, John T.; Key, Baris; Dogan, Fulya

doi:10.1002/aenm.202101820

Title: Silicon Anodes with Improved Calendar Life Enabled By Multivalent Additives

Journal Article · 25 August 2021 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.202101820 · OSTI ID:1839391

^[1]; Li, Xiang ^[1]; Sivonxay, Eric ^[2]; Wen, Jianguo ^[3]; Persson, Kristin A. ^[2]; Vaughey, John T. ^[1]; Key, Baris ^[1]; Dogan, Fulya ^[1]

Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials

Silicon is widely recognized as the most promising upgrade for graphite anodes due to its much higher capacity, natural abundance, and ability to be directly applied in the slurry-based, roll-to-roll production lines. However, in addition to the fast capacity decay, silicon anodes also suffer from inferior calendar life in practical applications due to the unstable solid-electrode interface (SEI). Until now, strategies to effectively improve the calendar life by tailored SEIs remain largely unclear, especially in high-Si content, zero-graphite anodes. Here, silicon anodes with superior calendar life are developed by adding small concentrations of multivalent salts into the baseline electrolyte. The Ca additive reacts with the F ions in the electrolyte, forming a layer of nanocrystalline CaF₂ that is closely coated around the silicon particles. The CaF₂-enabled new SEI is strong and dense, which effectively protects the silicon core from side reactions, leading to lower capacity decay after calendar aging at high voltage. More importantly, the Ca additive is effective universally for all available commercial silicon or SiO sources. This study provides a feasible and low-cost solution for developing silicon anodes with long calendar life, paving the way towards commercially viable silicon anodes.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1839391

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 37 Vol. 11; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Silicon Anodes with Improved Calendar Life Enabled By Multivalent Additives

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