Boosting Properties of 3D Binder‐Free Manganese Oxide Anodes by Preformation of a Solid Electrolyte Interphase

Abstract

Huge irreversible capacity loss prevents the successful use of metal oxide anodes in Li-ion full cells. Here, we focus on the critical prelithiation step and demonstrate the challenge of electrolyte decomposition on a pristine anode in a full cell. Both an electrochemical activation process (54 h) with Li metal and a new electrolytic process (75 min) without Li metal were used to preform complete solid electrolyte interphase (SEI) layers on 3 D binder-free MnOy -based anodes. The preformed SEI layers mitigated the electrolyte decomposition effectively and widened the working voltage for the MnOy /LiMn2 O4 full cell, which resulted in a big boost of the specific energy to 300 and 200 W h kgcathode (-1) , largely improved cycling stability, and much higher specific power (4200 W h kgtotal (-1) ) compared to conventional Li-ion batteries. Detailed characterization, such as cyclic voltammetry, scanning transmission electron microscopy, and FTIR spectroscopy, gives mechanistic insight into SEI preformation. This work provides guidance for the design of anode SEI layers and enables the application of oxides for Li-ion battery full cells.

Carbon Nanosponge Cathode Materials and Graphite-Protected Etched Al Foil Anode for Dual-Ion Hybrid Supercapacitor

“…23 Similar phenomena are also found in the silicon and metal oxide anode of Li-ion battery. 25,26 Recently, Tong et al 27,28 fabricated porous or hollow Al coated with a uniform carbon layer, which provided sufficient space to accommodate volume expansion. Moreover, the outer carbon layer buffered the volume variation effect and to form a passive SEI film during the Al-Li alloying.…”

Li‐Metal‐Free Prelithiation of Si‐Based Negative Electrodes for Full Li‐Ion Batteries

“…It is well known that Li metal also consumes electrolyte reduction products during the cyclingi nt he conventional half-cell configuration, [32] which makes control of the prelithiation more difficult. [34] Hence, in this work, good controllability wasa chieved at ah igh mass-normalized current density (1 Ag Si À1 ), which makes big savings in the prelithiationtime. [7,33] In the electrolytic cell, the influence of the highly reactive Li metal on the SEI formation was excluded, which resulted in better controllability.…”

“…[7,33] In the electrolytic cell, the influence of the highly reactive Li metal on the SEI formation was excluded, which resulted in better controllability. [34] Hence, in this work, good controllability wasa chieved at ah igh mass-normalized current density (1 Ag Si À1 ), which makes big savings in the prelithiationtime.…”

“…Similar work has been well described in our previous literature. [34] Cyclic voltammetry on the electrolytic cell was performed at as can rate of 1mVs À1 with ap otentiostat (Princeton VersaSTAT,U SA), the binder-free Si electrode as the working electrode, the Cu wires as the counter electrode, and Ag/AgCl as the reference electrode. The galvanostatic prelithiation on the binder-free Si electrode was performed at ac urrent density of 1Ag Si À1 on the same potentiostat.…”

Critical Review of Emerging Pre‐metallization Technologies for Rechargeable Metal‐Ion Batteries

“…For the SEI layer, some studies revealed that the initial charge-discharge is sufficient to form the SEI layer and excessive lithiation leads to the loss of active materials and the formation of dendrites. [156][157][158] Based on this simple strategy, both pre-sodiation in SIBs [25] and pre-lithiation in LIBs [159] have achieved good electrochemical performance.…”