Display options
Cite
Pascal TA, Villaluenga I, Wujcik KH, et al. Liquid Sulfur Impregnation of Microporous Carbon Accelerated by Nanoscale Interfacial Effects. Nano Lett. 2017;17(4):2517-2523doi: 10.1021/acs.nanolett.7b00249.
Pascal, T. A., Villaluenga, I., Wujcik, K. H., Devaux, D., Jiang, X., Wang, D. R., Balsara, N., & Prendergast, D. (2017). Liquid Sulfur Impregnation of Microporous Carbon Accelerated by Nanoscale Interfacial Effects. Nano letters, 17(4), 2517-2523. https://doi.org/10.1021/acs.nanolett.7b00249
Pascal, Tod A, et al. "Liquid Sulfur Impregnation of Microporous Carbon Accelerated by Nanoscale Interfacial Effects." Nano letters vol. 17,4 (2017): 2517-2523. doi: https://doi.org/10.1021/acs.nanolett.7b00249
Pascal TA, Villaluenga I, Wujcik KH, Devaux D, Jiang X, Wang DR, Balsara N, Prendergast D. Liquid Sulfur Impregnation of Microporous Carbon Accelerated by Nanoscale Interfacial Effects. Nano Lett. 2017 Apr 12;17(4):2517-2523. doi: 10.1021/acs.nanolett.7b00249. Epub 2017 Mar 17. PMID: 28290694.
Copy Download .nbib Format: NLM
Share it on

Nano Lett. 2017 Apr 12;17(4):2517-2523. doi: 10.1021/acs.nanolett.7b00249. Epub 2017 Mar 17.

Liquid Sulfur Impregnation of Microporous Carbon Accelerated by Nanoscale Interfacial Effects.

Nano letters

Tod A Pascal, Irune Villaluenga, Kevin H Wujcik, Didier Devaux, Xi Jiang, Dunyang Rita Wang, Nitash Balsara, David Prendergast

Affiliations

  1. Molecular Foundry, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
  2. Department of Chemical and Biomolecular Engineering, University of California , Berkeley, California 94720, United States.
  3. Energy Technologies Area, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
  4. Materials Sciences Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
  5. Department of Materials Science and Engineering, University of California , Berkeley, California 94720, United States.

PMID: 28290694 DOI: 10.1021/acs.nanolett.7b00249

Abstract

Impregnation of porous carbon matrices with liquid sulfur has been exploited to fabricate composite cathodes for lithium-sulfur batteries, aimed at confining soluble sulfur species near conducting carbon to prevent both loss of active material into the electrolyte and parasitic reactions at the lithium metal anode. Here, through extensive computer simulations, we uncover the strongly favorable interfacial free energy between liquid sulfur and graphitic surfaces that underlies this phenomenon. Previously unexplored curvature-dependent enhancements are shown to favor the filling of smaller pores first and effect a quasi-liquid sulfur phase in microporous domains (diameters <2 nm) that persists ∼30° below the expected freezing point. Evidence of interfacial sulfur on carbon is shown to be a 0.3 eV red shift in the simulated and measured interfacial X-ray absorption spectra. Our results elucidate the critical morphology and thermodynamic properties necessary for future cathode design and highlight the importance of molecular-scale details in defining emergent properties of functional nanoscale interfaces.

Keywords: Battery; computer simulation; energy storage; entropy; free energy; molecular dynamics; nanoscale; spectroscopy; sulfur

Publication Types