The Electrolysis of Anti-Perovskite Li2 OHCl for Prelithiation of High-Energy-Density Batteries

Angew Chem Int Ed Engl. 2021 Jun 1;60(23):13013-13020. doi: 10.1002/anie.202102605. Epub 2021 Apr 28.

Abstract

Anti-perovskite type Li2 OHCl was previously studied as a solid-state Li+ conductor. Here, we report that the Li2 OHCl can be electrolyzed at 3.3 V or 4.0 V, with the creation of O2 /HCl gases and the release of 2 equiv. Li+ via two different decomposition routes, depending on the acidity of electrolyte. In the electrolyte with trace acid, the Li2 OHCl is oxidized at a constant voltage of 3.3 V. In neutral electrolyte, the oxidization of Li2 OHCl starts at 4.0 V, but the produced HCl will increase the acidity of electrolyte and lead to a voltage drop to 3.3 V for the electrolysis of Li2 OHCl. The electrolysis of Li2 OHCl delivers a lithium releasing capacity as high as 810 mAh g-1 , with an equivalent Li-deposition or Li-intercalation on anode, making it a promising candidate as a Li reservoir for prelithiation of anode. Using Li2 OHCl as the lithium source, silicon-carbon (Si@C) composite anode can be effectively prelithiated. The full cells composed of LiNi0.8 Mn0.1 Co0.1 O2 (NMC811) cathode and prelithiated Si@C anode exhibited increased capacities with the increment of prelithiation dosages.

Keywords: anti-perovskite; electrolysis; pre-lithiation; rechargeable batteries; solid-state ionics.