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

N1 - Funding Information: This work was financially supported by the Ministry for Science and Cul-ture of Lower Saxony (MWK), via the Research Training Group “Circular-LIB” and the program “Nanomaterials and Quantum Technology for Dig-ital Transformation” (hsn-digital). Z.H.L acknowledged the support fromthe Chinese Scholarship Council (CSC). Y.L. thanks the research supportfrom the General Program of the National Natural Science Foundation ofChina (22379138), the CAS “Hundred Talents Program B”. C.Z. acknowl-edged the support from Natural Science Foundation of Anhui Provincefor Distinguished Young Scholar (2108085J25), and the Excellent Researchand Innovation Team Project of Anhui Province (2022AH010001)

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 -