TY - JOUR
T1 - Entropy-Driven Liquid Electrolytes for Lithium Batteries
AU - Wang, Qidi
AU - Zhao, Chenglong
AU - Yao, Zhenpeng
AU - Wang, Jianlin
AU - Wu, Fangting
AU - Kumar, Sai Govind Hari
AU - Ganapathy, Swapna
AU - Eustace, Stephen
AU - Wagemaker, Marnix
PY - 2023
Y1 - 2023
N2 - Developing liquid electrolytes with higher kinetics and enhanced interphase stability is one of the key challenges for lithium batteries. However, the poor solubility of lithium salts in solvents sets constraints that compromises the electrolyte properties. Here, it is shown that introducing multiple salts to form a high-entropy solution, alters the solvation structure, which can be used to raise the solubility of specific salts and stabilize electrode–electrolyte interphases. The prepared high-entropy electrolytes significantly enhance the cycling and rate performance of lithium batteries. For lithium-metal anodes the reversibility exceeds 99%, which extends the cycle life of batteries even under aggressive cycling conditions. For commercial batteries, combining a graphite anode with a LiNi0.8Co0.1Mn0.1O2 cathode, more than 1000 charge–discharge cycles are achieved while maintaining a capacity retention of more than 90%. These performance improvements with respect to regular electrolytes are rationalized by the unique features of the solvation structure in high-entropy electrolytes. The weaker solvation interaction induced by the higher disorder results in improved lithium-ion kinetics, and the altered solvation composition leads to stabilized interphases. Finally, the high-entropy, induced by the presence of multiple salts, enables a decrease in melting temperature of the electrolytes and thus enables lower battery operation temperatures without changing the solvents.
AB - Developing liquid electrolytes with higher kinetics and enhanced interphase stability is one of the key challenges for lithium batteries. However, the poor solubility of lithium salts in solvents sets constraints that compromises the electrolyte properties. Here, it is shown that introducing multiple salts to form a high-entropy solution, alters the solvation structure, which can be used to raise the solubility of specific salts and stabilize electrode–electrolyte interphases. The prepared high-entropy electrolytes significantly enhance the cycling and rate performance of lithium batteries. For lithium-metal anodes the reversibility exceeds 99%, which extends the cycle life of batteries even under aggressive cycling conditions. For commercial batteries, combining a graphite anode with a LiNi0.8Co0.1Mn0.1O2 cathode, more than 1000 charge–discharge cycles are achieved while maintaining a capacity retention of more than 90%. These performance improvements with respect to regular electrolytes are rationalized by the unique features of the solvation structure in high-entropy electrolytes. The weaker solvation interaction induced by the higher disorder results in improved lithium-ion kinetics, and the altered solvation composition leads to stabilized interphases. Finally, the high-entropy, induced by the presence of multiple salts, enables a decrease in melting temperature of the electrolytes and thus enables lower battery operation temperatures without changing the solvents.
KW - entropy-driven electrolytes
KW - high-entropy electrolytes
KW - lithium batteries
KW - temperature-dependent electrolytes
KW - weak solvation structures
UR - http://www.scopus.com/inward/record.url?scp=85150838799&partnerID=8YFLogxK
U2 - 10.1002/adma.202210677
DO - 10.1002/adma.202210677
M3 - Article
AN - SCOPUS:85150838799
SN - 0935-9648
VL - 35
JO - Advanced Materials
JF - Advanced Materials
IS - 17
ER -