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

Khryslyn G. Araño, Beth L. Armstrong, Anton W. Tomich, Matthew S. Chambers, Joseph Quinn, Harry M. Meyer, Chanaka Kumara, Zoey Huey, Chun Sheng Jiang, Chongmin Wang, Christopher S. Johnson, Raymond R. Unocic, Gabriel M. Veith

Research output: Contribution to journalArticlepeer-review

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 (SiCu) were prepared using physical vapor deposition (PVD) via sputtering and high-energy milling. Other SiCu 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 SiCu 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, SiCu 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.

Original languageEnglish
Article number100335
JournalNext Energy
Volume8
DOIs
StatePublished - Jul 2025

Funding

This research was supported by the US Department of Energy, Vehicle Technologies Office (DOE-VTO) under the Silicon Consortium Project, directed by Nicolas Eidson, Carine Steinway, Thomas Do, and Brian Cunningham, and managed by Anthony Burrell. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with DOE. The publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doepublic-accessplan ). The STEM characterization work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory, which is operated by Battelle for DOE under Contract DE-AC05-76RL01830. STEM-EDS work was performed in part at the Analytical Instrumentation Facility (AIF) at North Carolina State University, which is supported by the State of North Carolina and the National Science Foundation (award number ECCS-2025064). The AIF is a member of the North Carolina Research Triangle Nanotechnology Network, a site in the National Nanotechnology Coordinately Infrastructure. This research was supported by the US Department of Energy, Vehicle Technologies Office (DOE-VTO) under the Silicon Consortium Project, directed by Nicolas Eidson, Carine Steinway, Thomas Do, and Brian Cunningham, and managed by Anthony Burrell. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with DOE. The publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doepublic-accessplan). The STEM characterization work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory, which is operated by Battelle for DOE under Contract DE-AC05-76RL01830. STEM-EDS work was performed in part at the Analytical Instrumentation Facility (AIF) at North Carolina State University, which is supported by the State of North Carolina and the National Science Foundation (award number ECCS-2025064). The AIF is a member of the North Carolina Research Triangle Nanotechnology Network, a site in the National Nanotechnology Coordinately Infrastructure. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( https://www.energy.gov/doe-public-access-plan ).

Keywords

  • Lithium-ion batteries
  • Metal coating
  • Milling
  • Physical vapor deposition
  • Silicon anode
  • Sputtering

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