Regulating Li Nucleation and Growth Heterogeneities via Near-Surface Lithium-Ion Irrigation for Stable Anode-Less Lithium Metal Batteries

Chuyi Xie, Chen Zhao, Heonjae Jeong, Qiang Liu, Tianyi Li, Wenqian Xu, Lei Cheng, Gui Liang Xu, Khalil Amine, Guohua Chen

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

The inhomogeneous nucleation and growth of Li dendrite combined with the spontaneous side reactions with the electrolytes dramatically challenge the stability and safety of Li metal anode (LMA). Despite tremendous endeavors, current success relies on the use of significant excess of Li to compensate the loss of active Li during cycling. Herein, a near-surface Li+ irrigation strategy is developed to regulate the inhomogeneous Li deposition behavior and suppress the consequent side reactions under limited Li excess condition. The conformal polypyrrole (PPy) coating layer on Cu surface via oxidative chemical vapor deposition technique can induce the migration of Li+ to the interregional space between PPy and Cu, creating a near-surface Li+-rich region to smooth diffusion of ion flux and uniform the deposition. Moreover, as evidenced by multiscale characterizations including synchrotron high-energy X-ray diffraction scanning, a robust N-rich solid-electrolyte interface (SEI) is formed on the PPy skeleton to effectively suppress the undesired SEI formation/dissolution process. Strikingly, stable Li metal cycling performance under a high areal capacity of 10 mAh cm−2 at 2.0 mA cm−2 with merely 0.5 × Li excess is achieved. The findings not only resolve the long-standing poor LMA stability/safety issues, but also deepen the mechanism understanding of Li deposition process.

Original languageEnglish
Article number2306868
JournalSmall
Volume20
Issue number12
DOIs
StatePublished - Mar 22 2024
Externally publishedYes

Funding

Research at the Hong Kong Polytechnic University was funded by research grants from Shenzhen Science and Technology Innovation Program (SGDX20190816230615451), the Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515110798), Hong Kong Research Grants Council (GRF, No. 15221719). Research at the Argonne National Laboratory was funded by the US department of Energy (DOE), Vehicle Technologies office. Support from Tien Duong of the US DOE's Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS), an Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. G.X. and K.A. thank the Clean Vehicle Consortium, US, China Clean Energy Research Centre (CERC-CVC2) for support. Research at the Hong Kong Polytechnic University was funded by research grants from Shenzhen Science and Technology Innovation Program (SGDX20190816230615451), the Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515110798), Hong Kong Research Grants Council (GRF, No. 15221719). Research at the Argonne National Laboratory was funded by the US department of Energy (DOE), Vehicle Technologies office. Support from Tien Duong of the US DOE's Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS), an Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE\u2010AC02\u201006CH11357. G.X. and K.A. thank the Clean Vehicle Consortium, US, China Clean Energy Research Centre (CERC\u2010CVC2) for support.

Keywords

  • lithium metal batteries
  • low Li excess
  • oxidative chemical vapor deposition
  • solid-electrolyte interphase
  • synchrotron high-energy X-ray diffraction scanning

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