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Ha DH, Ly T, Caron JM, et al. A General Method for High-Performance Li-Ion Battery Electrodes from Colloidal Nanoparticles without the Introduction of Binders or Conductive-Carbon Additives: The Cases of MnS, Cu(2-x)S, and Ge. ACS Appl Mater Interfaces. 2015;7(45):25053-60doi: 10.1021/acsami.5b03398.
Ha, D. H., Ly, T., Caron, J. M., Zhang, H., Fritz, K. E., & Robinson, R. D. (2015). A General Method for High-Performance Li-Ion Battery Electrodes from Colloidal Nanoparticles without the Introduction of Binders or Conductive-Carbon Additives: The Cases of MnS, Cu(2-x)S, and Ge. ACS applied materials & interfaces, 7(45), 25053-60. https://doi.org/10.1021/acsami.5b03398
Ha, Don-Hyung, et al. "A General Method for High-Performance Li-Ion Battery Electrodes from Colloidal Nanoparticles without the Introduction of Binders or Conductive-Carbon Additives: The Cases of MnS, Cu(2-x)S, and Ge." ACS applied materials & interfaces vol. 7,45 (2015): 25053-60. doi: https://doi.org/10.1021/acsami.5b03398
Ha DH, Ly T, Caron JM, Zhang H, Fritz KE, Robinson RD. A General Method for High-Performance Li-Ion Battery Electrodes from Colloidal Nanoparticles without the Introduction of Binders or Conductive-Carbon Additives: The Cases of MnS, Cu(2-x)S, and Ge. ACS Appl Mater Interfaces. 2015 Nov 18;7(45):25053-60. doi: 10.1021/acsami.5b03398. Epub 2015 Nov 04. PMID: 26535449.
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ACS Appl Mater Interfaces. 2015 Nov 18;7(45):25053-60. doi: 10.1021/acsami.5b03398. Epub 2015 Nov 04.

A General Method for High-Performance Li-Ion Battery Electrodes from Colloidal Nanoparticles without the Introduction of Binders or Conductive-Carbon Additives: The Cases of MnS, Cu(2-x)S, and Ge.

ACS applied materials & interfaces

Don-Hyung Ha, Tiffany Ly, Joseph M Caron, Haitao Zhang, Kevin E Fritz, Richard D Robinson

Affiliations

  1. Department of Materials Science and Engineering, Cornell University , Ithaca, New York 14853, United States.

PMID: 26535449 DOI: 10.1021/acsami.5b03398

Abstract

In this work, we demonstrate a general lithium-ion battery electrode fabrication method for colloidal nanoparticles (NPs) using electrophoretic deposition (EPD). Our process is capable of forming robust electrodes from copper sulfide, manganese sulfide, and germanium NPs without the use of additives such as polymeric binders and conductive agents. After EPD, we show two postprocessing treatments ((NH4)2S and inert atmosphere heating) to effectively remove surfactant ligands and create a linked network of particles. The NP films fabricated by this simple process exhibit excellent electrochemical performance as lithium-ion battery electrodes. Additive-free Cu(2-x)S and MnS NP films show well-defined plateaus at ∼1.7 V, demonstrating potential for use as cathode electrodes. Because of the absence of additives in the NP film, this additive-free NP film is an ideal template for ex situ analyses of the particles to track particle morphology changes and deterioration as a result of Li ion cycling. To this end, we perform a size-dependent investigation of Cu(2-x)S NPs and demonstrate that there is no significant relationship between size and capacity when comparing small (3.8 nm), medium (22 nm), and large (75 nm) diameter Cu(2-x)S NPs up to 50 cycles; however, the 75 nm NPs show higher Coulombic efficiency. Ex situ TEM analysis suggests that Cu(2-x)S NPs eventually break into smaller particles (<10 nm), explaining a weak correlation between size and performance. We also report for the first time on additive-free Ge NP films, which show stable capacities for up to 50 cycles at 750 mAh/g.

Keywords: additive-free; ammonium sulfide; colloidal nanoparticle; copper sulfide; electrophoretic deposition; germanium; manganese sulfide; size-dependent

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