Modulating reactivity and stability of metallic lithium: Via atomic doping

Ke Lu, Haiping Xu, Haiying He, Siyuan Gao, Xun Li, Chong Zheng, Tao Xu, Yingwen Cheng

Research output: Contribution to journalArticlepeer-review

19 Scopus citations

Abstract

Many approaches have been described to address challenges in metallic Li anodes; but they rarely modulate the inherent chemical reactivities. Here we describe a general approach for modulating Li metal properties and enabling stable metal batteries by doping with ∼0.1 at% Ag or Al. The dopants were atomically dispersed in the vacant face-centered sites of the body-centered cubic Li crystals and pull electrons strongly due to higher electronegativity (Ag: 1.98; Al: 1.61 vs. Li: 0.98). As a result, the doped Li anodes have increased work function with reduced chemical reactivity and remained shiny in dry air for months. They also exhibited enhanced Li+/Li redox kinetics and generated thinner but stronger solid-electrolyte interphases in carbonate electrolytes. The dopant atoms are lithophilic and have stronger binding with Li adatoms, which guide uniform Li deposition and ensures dendrite-free Li interface during battery cycling. Overall, the doped anodes enabled stable operations of not only high current symmetric cells but also practical full cells in which Ni-rich layered cathodes were paired with 30 μm anodes and 7 μL electrolytes. The doping approach is facile and scalable, and opens up new and promising opportunities for designing practical high energy density metal batteries.

Original languageEnglish
Pages (from-to)10363-10369
Number of pages7
JournalJournal of Materials Chemistry A
Volume8
Issue number20
DOIs
StatePublished - May 28 2020
Externally publishedYes

Funding

This work was supported by startup funds provided to Y. C. from Northern Illinois University. Use of the Center for Nano-scale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory. The NMC cathodes were produced at the U.S. Department of Energy's (DOE) CAMP (Cell Analysis, Modeling and Prototyping) Facility, Argonne National Laboratory. The CAMP Facility is fully supported by the DOE Vehicle Technologies Program (VTP) with the core funding of the Applied Battery Research (ABR) for Transportation Program.

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