Unveiling Mechanisms of SEI Formation and Sodium Loss in Sodium Batteries via Interface Reactor Sampling
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arXiv
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| Autori principali: | , , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2026
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| _version_ | 1866915923952140288 |
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| author | Liu, Zhoulin Wang, Ziliang Chen, Zherui Sha, Jianchun Pan, Fengzijun Zhang, Pingyang Zhang, Yinghe |
| author_facet | Liu, Zhoulin Wang, Ziliang Chen, Zherui Sha, Jianchun Pan, Fengzijun Zhang, Pingyang Zhang, Yinghe |
| contents | The solid electrolyte interphase SEI critically dictates the cyclability and Coulombic efficiency of sodium-metal batteries, yet its dynamic formation mechanisms and atomic-scale evolution during electrochemical cycling remain elusive due to the spatiotemporal limitations of existing techniques. Here, an "Interface Reactor" sampling strategy is proposed to construct a charge-aware neuroevolution potential (qNEP). This approach overcomes the instability bottlenecks of conventional machine learning potentials, enabling stable, first-principles-accurate molecular dynamics simulations of complex electrode-electrolyte interfaces on the hundred-nanosecond scale. Fundamentally distinct SEI formation mechanisms are revealed during the early stage: carbonate-based electrolytes form heterogeneous organic-inorganic matrices via "mixed co-formation," whereas ether-based electrolytes generate dense, self-limiting inorganic barriers through "surface-energy-controlled" NaF crystallization. Metadynamics simulations further elucidate that these compositional disparities govern sodium-ion storage dynamics: NaF-rich SEIs facilitate efficient metallic deposition, while carbonate-dominated interphases induce irreversible sodium trapping and continuous electrolyte decomposition. These findings establish a comprehensive atomic-scale framework linking solvation structure, interfacial reaction networks, and electrochemical performance, providing mechanistic guidelines for rational SEI engineering in next-generation alkali-metal batteries. Crucially, a general and robust computational framework is established for simulating complex interfacial reactions in electrochemical systems. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2604_07077 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Unveiling Mechanisms of SEI Formation and Sodium Loss in Sodium Batteries via Interface Reactor Sampling Liu, Zhoulin Wang, Ziliang Chen, Zherui Sha, Jianchun Pan, Fengzijun Zhang, Pingyang Zhang, Yinghe Materials Science The solid electrolyte interphase SEI critically dictates the cyclability and Coulombic efficiency of sodium-metal batteries, yet its dynamic formation mechanisms and atomic-scale evolution during electrochemical cycling remain elusive due to the spatiotemporal limitations of existing techniques. Here, an "Interface Reactor" sampling strategy is proposed to construct a charge-aware neuroevolution potential (qNEP). This approach overcomes the instability bottlenecks of conventional machine learning potentials, enabling stable, first-principles-accurate molecular dynamics simulations of complex electrode-electrolyte interfaces on the hundred-nanosecond scale. Fundamentally distinct SEI formation mechanisms are revealed during the early stage: carbonate-based electrolytes form heterogeneous organic-inorganic matrices via "mixed co-formation," whereas ether-based electrolytes generate dense, self-limiting inorganic barriers through "surface-energy-controlled" NaF crystallization. Metadynamics simulations further elucidate that these compositional disparities govern sodium-ion storage dynamics: NaF-rich SEIs facilitate efficient metallic deposition, while carbonate-dominated interphases induce irreversible sodium trapping and continuous electrolyte decomposition. These findings establish a comprehensive atomic-scale framework linking solvation structure, interfacial reaction networks, and electrochemical performance, providing mechanistic guidelines for rational SEI engineering in next-generation alkali-metal batteries. Crucially, a general and robust computational framework is established for simulating complex interfacial reactions in electrochemical systems. |
| title | Unveiling Mechanisms of SEI Formation and Sodium Loss in Sodium Batteries via Interface Reactor Sampling |
| topic | Materials Science |
| url | https://arxiv.org/abs/2604.07077 |