Controlled Prelithiation of PbS to Pb/Li₂S for High Initial Coulombic Efficiency in Lithium Ion Batteries

Abstract

PbS nanoparticle aggregates were synthesized in a simple aqueous reaction at room temperature, and were tested as a lithium ion anode material, with a gravimetric capacity of 374 mAh/g at C/2, and a 0.15% capacity loss per cycle. However, its half cell initial Coulombic efficiency (ICE) was only 40%, due to a combination of irreversible Li 2 S and solid electrolyte interface (SEI) formations. A custom controlled prelithiation technique was then applied to the PbS electrodes, converting the active material to Pb/Li 2 S, and consolidating the SEI prior to coin cell assembly. This brought the ICE from 40% to >97%, and allowed for immediate cycling of the electrode at high Coulombic efficiency, without further formation cycles. Upon construction of prelithiated Pb/Li 2 S vs NCM full cells, an 82% ICE was observed, with the majority of the lithium loss from the NCM. The full cells had a combined electrode capacity of 100 mAh/g at C/2.

Prelithiation: A Critical Strategy Towards Practical Application of High‐Energy‐Density Batteries

“…Electrochemical prelithiation is to match the anode against the lithium metal, usually in a half-cell, to conduct the prelithiation process. [82,[144][145][146][147] Kim et al constructed an external short circuit in C-SiO x //Li half-cell, and spontaneous prelithiation occurred driven by the potential difference between the anode material and the lithium metal. When a resistor exists in the [137] Copyright 2019, American Chemical Society.…”

Practical evaluation of prelithiation strategies for next‐generation lithium‐ion batteries

“…134 As shown in Figure 8B, Mullins et al prelithiated a PbS electrode using a galvanostatic charge-discharge approach, converting the active material into Pb/Li 2 S, which increased the ICE from 40% to >97%. 130 Recently, Dou et al developed a thermal passivation strategy for the electrochemically prelithiated SiO x @C anode (Figure 8C). 131 The treatment leaves a robust Li 2 O passivating matrix on the anode surface, promoting its stability in air.…”

Progress and challenges of prelithiation technology for lithium‐ion battery

“…Such a strategy has also been extended to improve the ICE of other anode materials, such as carbon nanospheres, 85 mesocarbon microbeads, 86 and PbS. 87 The commercial graphite (Gr) has a relatively high ICE (typically >90%). Compared to other anode materials, prelithiated graphite is mainly used to improve the energy density and cycling stability of a battery.…”

“…With this strategy, the specific capacity of the LiNi 0.5 Mn 0.5 O 2 /HC full cell increased from 92 to 162 mAh g −1 . Such a strategy has also been extended to improve the ICE of other anode materials, such as carbon nanospheres, 85 mesocarbon microbeads, 86 and PbS 87 …”