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<p>Boron-based compounds are known as a class of anion acceptors due to the electron deficiency of the central B atom, which can be designed as electrolyte additives (B-ads) in rechargeable batteries. However, there are still limited systematic investigations into how the electron-deficient properties of B-ads regulate the solvation structures of electrolytes and further impact the electrode-electrolyte interface. In this work, we designed four B-ads for lithium metal batteries (LMBs) and revealed that both the structure of the boron compound and the size of the anion play crucial roles in determining the physicochemical properties of electrolytes. Among these additives, the B atom in tris(hexafluoroisopropyl)borate (THFPB) exhibited the highest electron-deficiency, resulting in the enhanced dissolution of Li<sub>2</sub>O and LiF. This characteristic was found to reduce the interfacial charge transfer resistance of the Li metal anode and enhance the Li<sup>+</sup> diffusion coefficient of Li∥CF<sub><i>x</i></sub> batteries, which ultimately elevated the specific discharge capacity (∼100 mAh g<sup>−1</sup>) and accelerated the kinetic performance of the batteries. Through spectra characterization as well as molecular dynamics (MD) simulations, the addition of THFPB was also confirmed to enhance ion aggregations in the solvation structure, thereby contributing to the formation of robust electrolyte-electrode interphase, especially for high-voltage cathode. Consequently, the Li∥LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> batteries using thin Li anode, high loading cathode, and 0.1 M THFPB added electrolytes maintained 80% of its capacity after 150 cycles. This work demonstrates the versatileness of B-ads that effectively mitigate critical challenges of energy-dense battery systems.</p>

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Designing boron-based anion acceptors as electrolyte additives for energy-dense lithium metal batteries

  • 期刊论文

  • 发表日期：

    2025年4月8日

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  • Kun Li,
  • Jingwei Zhang,
  • Lanqing Wu,
  • Zihang Xi,
  • Jia Li,
  • Zhenyu Fan,
  • Qing Zhao

摘要

Boron-based compounds are known as a class of anion acceptors due to the electron deficiency of the central B atom, which can be designed as electrolyte additives (B-ads) in rechargeable batteries. However, there are still limited systematic investigations into how the electron-deficient properties of B-ads regulate the solvation structures of electrolytes and further impact the electrode-electrolyte interface. In this work, we designed four B-ads for lithium metal batteries (LMBs) and revealed that both the structure of the boron compound and the size of the anion play crucial roles in determining the physicochemical properties of electrolytes. Among these additives, the B atom in tris(hexafluoroisopropyl)borate (THFPB) exhibited the highest electron-deficiency, resulting in the enhanced dissolution of Li2O and LiF. This characteristic was found to reduce the interfacial charge transfer resistance of the Li metal anode and enhance the Li+ diffusion coefficient of Li∥CFx batteries, which ultimately elevated the specific discharge capacity (∼100 mAh g−1) and accelerated the kinetic performance of the batteries. Through spectra characterization as well as molecular dynamics (MD) simulations, the addition of THFPB was also confirmed to enhance ion aggregations in the solvation structure, thereby contributing to the formation of robust electrolyte-electrode interphase, especially for high-voltage cathode. Consequently, the Li∥LiNi0.8Co0.1Mn0.1O2 batteries using thin Li anode, high loading cathode, and 0.1 M THFPB added electrolytes maintained 80% of its capacity after 150 cycles. This work demonstrates the versatileness of B-ads that effectively mitigate critical challenges of energy-dense battery systems.