Multiple Functional Bonds Integrated Interphases for Long Cycle Sodium-Ion Batteries

Huang, Yongsheng; Zhang, Qingqing; Sun, Xiao‐Guang; Liu, Kai; Sun, Weili; Zhi, Mingyu; Guo, Yayu; Zheng, Shijian; Dai, Sheng

doi:10.1002/anie.202406277

Multiple Functional Bonds Integrated Interphases for Long Cycle Sodium-Ion Batteries

Journal Article · Fri Jun 28 00:00:00 EDT 2024 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202406277· OSTI ID:2438733

Huang, Yongsheng ^[1]; Zhang, Qingqing ^[1]; ^[2]; ^[3]; Sun, Weili ^[1]; Zhi, Mingyu ^[1]; Guo, Yayu ^[3]; Zheng, Shijian ^[1]; ^[4]

Hebei University of Technology, Tianjin (China)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Tianjin Univ. of Technology (China)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Sodium-ion batteries (SIBs) have garnered significant interest as one of the most promising energy suppliers for power grid energy storage. However, the poor electrode/electrolyte interfacial stability leads to continual electrolyte decomposition and transition metal dissolution, resulting in rapid performance degradation of SIBs. In this work, we propose a strategy integrating multiple functional bonds to regulate electrode/electrolyte interphase by triple-coupling of succinonitrile (SN), sodium hexafluorophosphate (NaPF₆) and fluorinated ethylene carbonate (FEC). Theoretical calculation and experiment results show that the solvation structure of Na⁺ and ClO₄^– is effectively reconfigured by the solvated FEC, SN and PF₆^– in PC-based carbonate electrolyte. The newly developed electrolyte demonstrates increased Na⁺-FEC coordination, weakened interaction of Na⁺-PC and participation of SN and PF₆^– anions in solvation, resulting in the formation of a conformal interfacial layer comprising of sodium oxynitrides (NaN_xO_y), sodium fluoride (NaF) and phosphorus oxide compounds (NaP_xO_y). Consequently, a 3 Ah pouch full cell of hard carbon//NaNi_1/3Fe_1/3Mn_1/3O₂ exhibits an excellent capacity retention of 90.4 % after 1000 cycles. Detailed postmortem analysis of interface chemistry is further illustrated by multiple characterization methods. Finally, this study provides a new avenue for developing electrolyte formulations with multiple functional bonds integrated interphases to significantly improve the long-term cycling stability of SIBs.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2438733

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 46 Vol. 63; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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