Improving interfacial stability of ultrahigh-voltage lithium metal batteries with single-crystal Ni-rich cathode via a multifunctional additive strategy

Zhi Zhang; Fangyan Liu; Zeyu Huang; Maoyi Yi; Xinming Fan; Maohui Bai; Bo Hong; Zhian Zhang; Jie Li; Yanqing Lai

doi:10.1016/j.jcis.2021.10.061

Improving interfacial stability of ultrahigh-voltage lithium metal batteries with single-crystal Ni-rich cathode via a multifunctional additive strategy

J Colloid Interface Sci. 2022 Feb 15;608(Pt 2):1471-1480. doi: 10.1016/j.jcis.2021.10.061. Epub 2021 Oct 15.

Authors

Zhi Zhang¹, Fangyan Liu¹, Zeyu Huang¹, Maoyi Yi¹, Xinming Fan¹, Maohui Bai¹, Bo Hong², Zhian Zhang¹, Jie Li¹, Yanqing Lai³

Affiliations

¹ School of Metallurgy and Environment, Central South University, Changsha, 410083 Hunan, China.
² School of Metallurgy and Environment, Central South University, Changsha, 410083 Hunan, China; Engineering Research Centre of Advanced Battery Materials, The Ministry of Education, Changsha, 410083 Hunan, China. Electronic address: bop_hong@163.com.
³ School of Metallurgy and Environment, Central South University, Changsha, 410083 Hunan, China; Engineering Research Centre of Advanced Battery Materials, The Ministry of Education, Changsha, 410083 Hunan, China.

PMID: 34742066
DOI: 10.1016/j.jcis.2021.10.061

Abstract

Electrode (including cathode and anode) /electrolyte interfaces play a vital role in determining battery performance. Especially, high-voltage lithium metal batteries (HVLMBs) with the Ni-rich layered oxide ternary cathode (NCM) can be considered a promising energy storage technology due to their outstanding energy density. However, it is still extremely challenging to address the unstable electrode/electrolyte interface and structural collapse of polycrystalline NCM at high voltage, greatly restraining its practical applications. In this work, a novel electrolyte additive, tris(2-cyanoethyl) borate (TCEB), has been used to construct the robust nitrogen (N) and boron (B)-rich protective films on single-crystal LiNi_0.6Co_0.1Mn_0.3O₂ (SNCM) cathode and lithium metal anode surfaces, which could effectively mitigate parasitic reactions against electrolyte corrosion and retain the structural integrity of electrode. Remarkably, the SNCM||Li metal cell using TCEB-containing electrolyte maintains unprecedentedly superb capacity retention of 80% after 100 cycles at an ultrahigh charging voltage of 4.7 V (versus Li/Li⁺). This finding provides a valuable reference to construct a stable electrode/electrolyte interface for the HVLMBs with achieving high-energy density.

Keywords: Electrode/electrolyte interface; High-voltage, Lithium metal batteries; Single-crystal LiNi(0.6)Co(0.1)Mn(0.3)O(2); Tris(2-cyanoethyl) borate.