Unleashing the Potential of High-Capacity Anodes through an Interfacial Prelithiation Strategy

Helin Wang, Ahu Shao, Ruijun Pan, Wei Tian, Qiurong Jia, Min Zhang, Miao Bai, Zhiqiao Wang, Fu Liu, Ting Liu, Xiaoyu Tang, Shaowen Li, Yue Ma

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

Abstract

The scalable development of an environmentally adaptive and homogeneous Li+ supplementary route remains a formidable challenge for the existing prelithiation technologies, restricting the full potential of high-capacity anodes. In this study, we present a moisture-tolerant interfacial prelithiation approach through casting a hydrophobic poly(vinylidene-co-hexafluoropropylene) membrane blended with a deep-lithiated alloy (Li22Si5@C/PVDF-HFP) onto Si based anodes. This strategy could not only extend to various high-capacity anode systems (SiOx@C, hard carbon) but also align with industrial roll-to-roll assembly processes. By carefully adjusting the thickness of the prelithiation layer, the densely packed Si@C electrode (4.5 mAh cm-2) exhibits significantly improved initial Coulombic efficiency until a close-to-unit value, as well as extreme moisture tolerance (60% relative humidity). Furthermore, it achieves more than 10-fold enhancement of ionic conductivity across the electrode. As pairing the prelithiated Si@C anode with the LiNi0.8Co0.1Mn0.1O2 cathode, the 2 Ah pouch-format prototype balances an energy density of ∼371 Wh kg-1 and an extreme power output of 2450 W kg-1 as well as 83.8% capacity retention for 1000 cycles. The combined operando phase tracking and spatial arrangement analysis of the intermediate alloy elucidate that the enhanced Li utilization derives from the gradient stress dissipation model upon a spontaneous Li+ redistribution process.

Original languageEnglish
Pages (from-to)21850-21864
Number of pages15
JournalACS Nano
Volume17
Issue number21
DOIs
StatePublished - 14 Nov 2023

Keywords

  • Li redistribition
  • interfacial prelithiation strategy
  • moisture tolerance
  • real-time phase tracking
  • stress dissipation

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