Investigating the impact of preparation routes on the properties of copper-decorated silicon particles as anode materials for lithium-ion batteries

Araño, Khryslyn G. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:000000018092493X); Armstrong, Beth L. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)]; Tomich, Anton W. [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000222941990); Chambers, Matthew S. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000278939603); Quinn, Joseph [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)]; Meyer III, Harry M. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)]; Kumara, Chanaka [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)]; Huey, Zoey [National Renewable Energy Laboratory (NREL), Golden, CO (United States)]; Jiang, Chun-Sheng [National Renewable Energy Laboratory (NREL), Golden, CO (United States)]; Wang, Chongmin [Argonne National Laboratory (ANL), Argonne, IL (United States)]; Johnson, Christopher S. [Argonne National Laboratory (ANL), Argonne, IL (United States)]; Unocic, Raymond R. [North Carolina State University, Raleigh, NC (United States)]; Veith, Gabriel M. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)]

doi:10.1016/j.nxener.2025.100335

DOE OSTI · 2574695

Investigating the impact of preparation routes on the properties of copper-decorated silicon particles as anode materials for lithium-ion batteries

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Abstract

In recent years, the calendar life of Si has been recognized as a significant issue that must be addressed prior to technology deployment: The carbon conductive additive is a potential source of parasitic side reactions. However, carbon remains essential due to the low electronic conductivity of Si. In this study, we investigate the use of Cu as a conductive additive and potential alternative to carbon. Some Cu-decorated silicon particles (Si Cu ) were prepared using physical vapor deposition (PVD) via sputtering and high-energy milling. Other Si Cu particles were prepared by using a solution method and examined briefly. The milling method caused Cu to appear as island-like features on the Si surface, whereas the PVD method initially produced similar island-like features that gradually developed into a continuous coating around the Si as sputtering time increased. Electrodes fabricated from Si Cu exhibited lower overall resistivity, demonstrating the beneficial effect of Cu in improving electronic percolation through the electrode. Electrochemical tests showed that the milled SiCu exhibited higher capacity retention, improved rate capability, and lower overpotential. Furthermore, Si Cu coupled with an NMC811 cathode exhibited lower leakage currents compared with the baseline silicon, indicating that incorporating Cu provided an additional advantage of minimizing parasitic currents in the cells.

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25 ENERGY STORAGE lithium-ion batteries metal coating milling physical vapor deposition silicon anode sputtering

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Araño, Khryslyn G. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:000000018092493X), Armstrong, Beth L. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Tomich, Anton W. [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000222941990), Chambers, Matthew S. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000278939603), Quinn, Joseph [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)], Meyer III, Harry M. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Kumara, Chanaka [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Huey, Zoey [National Renewable Energy Laboratory (NREL), Golden, CO (United States)], Jiang, Chun-Sheng [National Renewable Energy Laboratory (NREL), Golden, CO (United States)], Wang, Chongmin [Argonne National Laboratory (ANL), Argonne, IL (United States)], Johnson, Christopher S. [Argonne National Laboratory (ANL), Argonne, IL (United States)], Unocic, Raymond R. [North Carolina State University, Raleigh, NC (United States)], Veith, Gabriel M. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)]. 2025-06-18. Investigating the impact of preparation routes on the properties of copper-decorated silicon particles as anode materials for lithium-ion batteries. https://doi.org/10.1016/j.nxener.2025.100335

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