TY - JOUR

T1 - Constructing LiCl-Rich Solid Electrolyte Interphase by High Amine-Containing 1,2,4,5-Benzenetetramine Tetrahydrochloride Additive

AU - Lin, Zhihua

AU - Bettels, Frederik

AU - Li, Taoran

AU - Satheesh, Sreeja K.

AU - Liu, Yuping

AU - Zhang, Chaofeng

AU - Ding, Fei

AU - Zhang, Lin

PY - 2024/4/9

Y1 - 2024/4/9

N2 - Strategies that aim to achieve highly stable lithium metal batteries (LMBs) are extensively explored. To date, the controlled formation of high-quality inorganic SEI is still quite challenging, which requires a deep understanding and hence the fine-tuning of solvation chemistry by using functional additives in the electrolyte. In this work, a high amine-containing 1,2,4,5-benzenetetramine tetrahydrochloride (BHCL) is developed as a dual-function electrolyte additive for LMBs. The amine group with a high donor number increases the lithium affinity, while the phenyl group with a strong inductive effect prevents the decomposition of solvents, and the free chloride ions replace anions mediating the formation of the rigid inorganic LiCl-rich SEI layer. The experimental results corroborate the theoretical findings. The modified Li||Li symmetric battery is stably cycled for over 2500 h at 1 mA cm−2 current density with an overpotential of ≈45 mV. The performances of the Li||Cu and Li||LFP cells are also significantly enhanced. Therefore, this work provides a promising design principle of multifunctional electrolyte additive.

AB - Strategies that aim to achieve highly stable lithium metal batteries (LMBs) are extensively explored. To date, the controlled formation of high-quality inorganic SEI is still quite challenging, which requires a deep understanding and hence the fine-tuning of solvation chemistry by using functional additives in the electrolyte. In this work, a high amine-containing 1,2,4,5-benzenetetramine tetrahydrochloride (BHCL) is developed as a dual-function electrolyte additive for LMBs. The amine group with a high donor number increases the lithium affinity, while the phenyl group with a strong inductive effect prevents the decomposition of solvents, and the free chloride ions replace anions mediating the formation of the rigid inorganic LiCl-rich SEI layer. The experimental results corroborate the theoretical findings. The modified Li||Li symmetric battery is stably cycled for over 2500 h at 1 mA cm−2 current density with an overpotential of ≈45 mV. The performances of the Li||Cu and Li||LFP cells are also significantly enhanced. Therefore, this work provides a promising design principle of multifunctional electrolyte additive.

KW - 1,2,4,5-benzenetetramine tetrahydrochloride

KW - electrolyte additive

KW - lithium metal anode

KW - solvent sheath

UR - http://www.scopus.com/inward/record.url?scp=85179911582&partnerID=8YFLogxK

U2 - 10.1002/aelm.202300772

DO - 10.1002/aelm.202300772

M3 - Article

AN - SCOPUS:85179911582

VL - 10

JO - Advanced electronic materials

JF - Advanced electronic materials

SN - 2199-160X

IS - 4

M1 - 2300772

ER -