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Direct Operando Observation of Double Layer Charging and Early Solid Electrolyte Interphase Formation in Li-Ion Battery Electrolytes.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-05-08 , DOI: 10.1021/acs.jpclett.0c01089
Nataliia Mozhzhukhina 1 , Eibar Flores 2 , Robin Lundström 1 , Ville Nyström 1 , Paul G Kitz 1 , Kristina Edström 1 , Erik J Berg 1, 2
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-05-08 , DOI: 10.1021/acs.jpclett.0c01089
Nataliia Mozhzhukhina 1 , Eibar Flores 2 , Robin Lundström 1 , Ville Nyström 1 , Paul G Kitz 1 , Kristina Edström 1 , Erik J Berg 1, 2
Affiliation
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The solid electrolyte interphase (SEI) is the most critical yet least understood component to guarantee stable and safe operation of a Li-ion cell. Herein, the early stages of SEI formation in a typical LiPF6 and organic carbonate-based Li-ion electrolyte are explored by operando surface-enhanced Raman spectroscopy, on-line electrochemical mass spectrometry, and electrochemical quartz crystal microbalance. The electric double layer is directly observed to charge as Li+ solvated by ethylene carbonate (EC) progressively accumulates at the negatively charged electrode surface. Further negative polarization triggers SEI formation, as evidenced by H2 evolution and electrode mass deposition. Electrolyte impurities, HF and H2O, are reduced early and contribute in a multistep (electro)chemical process to an inorganic SEI layer rich in LiF and Li2CO3. This study is a model example of how a combination of highly surface-sensitive operando characterization techniques offers a step forward to understand interfacial phenomena in Li-ion batteries.
中文翻译:
锂离子电池电解质中双层充电和早期固体电解质中间相形成的直接操作观察。
固态电解质中间相(SEI)是确保锂离子电池稳定和安全运行的最关键但了解最少的组件。在本文中,通过操作表面增强拉曼光谱,在线电化学质谱和电化学石英晶体微量天平,探索了典型的LiPF6和有机碳酸酯基锂离子电解质中SEI形成的早期阶段。当被碳酸亚乙酯(EC)溶剂化的Li +逐渐积累在带负电的电极表面时,直接观察到双电层正在充电。进一步的负极化触发了SEI的形成,如H2的析出和电极质量的沉积所证明。电解质杂质HF和H2O可以尽早还原,并在多步(电)化学过程中有助于形成富含LiF和Li2CO3的无机SEI层。
更新日期:2020-05-01
中文翻译:
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锂离子电池电解质中双层充电和早期固体电解质中间相形成的直接操作观察。
固态电解质中间相(SEI)是确保锂离子电池稳定和安全运行的最关键但了解最少的组件。在本文中,通过操作表面增强拉曼光谱,在线电化学质谱和电化学石英晶体微量天平,探索了典型的LiPF6和有机碳酸酯基锂离子电解质中SEI形成的早期阶段。当被碳酸亚乙酯(EC)溶剂化的Li +逐渐积累在带负电的电极表面时,直接观察到双电层正在充电。进一步的负极化触发了SEI的形成,如H2的析出和电极质量的沉积所证明。电解质杂质HF和H2O可以尽早还原,并在多步(电)化学过程中有助于形成富含LiF和Li2CO3的无机SEI层。