The Raw Mixed Conducting Interphase Affords Effective Prelithiation in Working Batteries

Angew Chem Int Ed Engl. 2022 Jul 18;61(29):e202205697. doi: 10.1002/anie.202205697. Epub 2022 May 25.

Abstract

Contact prelithiation is an important strategy to compensate the initial capacity loss of lithium-ion batteries. However, the dead Li generated from inadequate Li conversion reduces the cycling stability of rechargeable batteries. Herein a mono-solvent dimethyl carbonate (DMC) electrolyte was employed in contact prelithiation for the first time. We discover that the low-organic-content raw electrolyte interphase (REI) induced by this electrolyte on Li source and anode is a mixed ion/electron conductor. Therefore, electron channels can be maintained even when the Li source has been completely wrapped by the DMC-derived REI. As a result, an outstanding Li source utilization of 92.8 % and a negligible dead Li yield can be realized. This strategy renders batteries with a very high initial Coulombic efficiency (90.0 %) and an excellent capacity retention (94.9 %) over 210 cycles, highlighting the significance of REI for effective contact prelithiation.

Keywords: Contact Prelithiation; Electrolyte; Li Source Utilization; Lithium-Ion Batteries; Solid Electrolyte Interphase.