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Interface-driven and Functionality-oriented Additive Stabilization Design for Ester-based LiPF6 Electrolytes
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DOI：10.1007/s10118-026-3739-x.png)
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Abstract
En 中文
Lithium-ion battery liquid electrolytes serve as the “blood” of the battery, undertaking the critical mission of transporting lithium ions between the cathode and anode. Consequently, the market demand for performance continues to escalate. However, lithium-ion batteries still face substantial challenges in terms of specific energy, safety, and cycle life, with the degradation of ester-based electrolytes being particularly prominent. Therefore, research on multifunctional electrolyte additives has become a focal area, offering promising avenues for effectively addressing these challenges. This study systematically analyzed the degradation mechanisms of ester-based lithium hexafluorophosphate (LiPF6) electrolytes, emphasizing the pivotal role of the inevitably generated hydrogen fluoride and phosphorus pentafluoride (HF and PF5) in electrolyte breakdown. This elucidates the crucial contribution of mechanism-oriented functional groups in stabilizing electrolytes, scavenging HF/PF5, modulating solvation structures, and engineering robust solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI). Furthermore, we developed a high-throughput computational workflow utilizing Gaussian 09, Multiwfn, and VMD to rationally design multifunctional additives through synergistic integration of functional groups and density functional theory (DFT)-guided screening. This approach evaluates HF/PF5 binding energies, frontier orbital energies (HOMO/LUMO) levels (redox activity), chemical hardness, and electrostatic potential interactions. Unlike previous reviews that primarily rely on empirical data summaries, this work innovatively bridges the gap between macroscale electrolyte failure behaviors and the microscale rational design of additives. By establishing a unified framework from HF/PF5 evolution to DFT-driven multi-functional molecular engineering, our study provides a predictive and systematic design guideline to minimize experimental trial and error, thereby accelerating the development of wide-temperature, high-voltage electrolytes with enhanced cycle life and safety.
Keywords:
Ester-based electrolyte additives for lithium-ion batteries
LiPF6 failure mechanisms
Functional groups
Computational chemistry
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4
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3.2K
Citations:
4.7K