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New Insight on the Role of Electrolyte Additives in Rechargeable Lithium Ion Batteries
ACS Energy Letters ( IF 19.3 ) Pub Date : 2019-10-11 , DOI: 10.1021/acsenergylett.9b01441 Jun Ming 1, 2 , Zhen Cao 3 , Yingqiang Wu 1, 2 , Wandi Wahyudi 1 , Wenxi Wang 1 , Xianrong Guo 4 , Luigi Cavallo 3 , Jang-Yeon Hwang 5 , Atif Shamim 2 , Lain-Jong Li 1 , Yang-Kook Sun 5 , Husam N. Alshareef 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2019-10-11 , DOI: 10.1021/acsenergylett.9b01441 Jun Ming 1, 2 , Zhen Cao 3 , Yingqiang Wu 1, 2 , Wandi Wahyudi 1 , Wenxi Wang 1 , Xianrong Guo 4 , Luigi Cavallo 3 , Jang-Yeon Hwang 5 , Atif Shamim 2 , Lain-Jong Li 1 , Yang-Kook Sun 5 , Husam N. Alshareef 1
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Solid electrolyte interphase (SEI)-forming agents such as vinylene carbonate, sulfone, and cyclic sulfate are commonly believed to be film-forming additives in lithium-ion batteries that help to enhance graphite anode stability. However, we find that the film-forming effect and the resultant SEI may not be the only reasons for the enhanced graphite stability. This is because the as-formed SEI cannot inhibit Li+–solvent co-intercalation once the additive is removed from the electrolyte. Instead, we show that the Li+ solvation structure, which is modified by these additives, plays a critical role in achieving reversible Li+ (de)intercalation within graphite. This discovery is confirmed in both carbonate and ether-based electrolytes. We show that the problem of graphite exfoliation caused by Li+–solvent co-intercalation can be mitigated by adding ethene sulfate to tune the Li+ coordination structure. This work brings new insight into the role of additives in electrolytes, expanding the prevailing thinking over the past 2 decades. In addition, this finding can guide the design of more versatile electrolytes for advanced rechargeable metal-ion batteries.
中文翻译：
电解质添加剂在可充电锂离子电池中的作用的新见解
通常认为，固态电解质相间（SEI）形成剂（例如碳酸亚乙烯酯，砜和环状硫酸盐）是锂离子电池中有助于增强石墨阳极稳定性的成膜添加剂。但是，我们发现成膜效果和生成的SEI可能不是增强石墨稳定性的唯一原因。这是因为一旦从电解质中去除了添加剂，形成的SEI就无法抑制Li +-溶剂的共嵌入。相反，我们证明了由这些添加剂修饰的Li +溶剂化结构在实现可逆Li +中起着关键作用。（脱）插在石墨内。在碳酸盐和基于醚的电解质中均证实了这一发现。我们表明，通过添加硫酸亚乙酯调节Li +配位结构，可以减轻由Li +-溶剂共插层引起的石墨剥落问题。这项工作使人们对添加剂在电解质中的作用有了新的认识，从而扩大了过去20年中流行的思想。此外，这一发现可以指导用于高级可充电金属离子电池的多功能电解质的设计。
更新日期：2019-10-12
中文翻译：
电解质添加剂在可充电锂离子电池中的作用的新见解
通常认为，固态电解质相间（SEI）形成剂（例如碳酸亚乙烯酯，砜和环状硫酸盐）是锂离子电池中有助于增强石墨阳极稳定性的成膜添加剂。但是，我们发现成膜效果和生成的SEI可能不是增强石墨稳定性的唯一原因。这是因为一旦从电解质中去除了添加剂，形成的SEI就无法抑制Li +-溶剂的共嵌入。相反，我们证明了由这些添加剂修饰的Li +溶剂化结构在实现可逆Li +中起着关键作用。（脱）插在石墨内。在碳酸盐和基于醚的电解质中均证实了这一发现。我们表明，通过添加硫酸亚乙酯调节Li +配位结构，可以减轻由Li +-溶剂共插层引起的石墨剥落问题。这项工作使人们对添加剂在电解质中的作用有了新的认识，从而扩大了过去20年中流行的思想。此外，这一发现可以指导用于高级可充电金属离子电池的多功能电解质的设计。
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