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SiO2 Is Wasted Space in Single-Nanometer-Scale Silicon Nanoparticle-Based Composite Anodes for Li-Ion Electrochemical Energy Storage

Journal Article · · ACS Applied Energy Materials
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  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
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The electrode processing conditions of silicon-based composite anodes play a pivotal role in the resulting interfacial chemical speciation and, thus, the electrochemical cycling behavior of the electrode. Systematically investigating how small chemical changes to the surface of the silicon nanoparticle (NP) affect larger, electrode-level properties is a strategy that will inform design principles to maximize electrode energy density and extend electrode lifetime. Here, we incorporate silicon nanoparticles (NPs) with an average diameter of 5.5 nm synthesized from the gas phase through a nonthermal plasma method into composite anode half-cell coin cells. We perform chemistry to functionalize the native hydride-terminated silicon NP surface with N-methylpyrrolidone (NMP) to improve slurry properties and reduce the silicon reactivity prior to composite electrode fabrication. We construct composite electrodes from these silicon NPs and observe an 86% capacity retention over 100 cycles at a rate of C/5, with an initial silicon specific capacity of 2600 mAh/g. We expose the same Si NPs to water that completely oxidizes these small-diameter NPs to SiO2 and find that the SiO2 NPs in the same electrode configuration exhibit no obvious lithium alloying capacity in the electrochemical potential range of lithium silicide alloy formation. As this result stands in contrast to existing literature, we provide a discussion on the origin of the discrepancies.
Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1769862
Report Number(s):
NREL/JA--5900-77402; MainId:26348; UUID:4acf520f-babc-42fa-8a86-ac472f2d789e; MainAdminID:19840
Journal Information:
ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 11 Vol. 3; ISSN 2574-0962
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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25 ENERGY STORAGE
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electrochemical energy storage
lithium-ion battery
silicon
silicon oxide
solid-electrolyte interphase