TY - JOUR
T1 - Modulating Double-Layer Solvation Structure via Dual-Weak-Interaction for Stable Sodium-Metal Batteries
AU - Shi, Tianze
AU - Hou, Ruilin
AU - Zheng, Linlin
AU - Lu, Hangyu
AU - Xu, Chengrong
AU - Sun, Xinyi
AU - He, Ping
AU - Li, Shukui
AU - Zhou, Haoshen
AU - Guo, Shaohua
N1 - Publisher Copyright:
© 2025 Wiley-VCH GmbH.
PY - 2025/5/27
Y1 - 2025/5/27
N2 - Sodium-metal batteries are the most promising low-cost and high-energy-density new energy storage technology. However, the sodium-metal anode has poor reversibility, which can be optimized by constructing the robust solid electrolyte interphase (SEI). Here, a concept of dual-weak-interaction electrolyte (DWIE) is demonstrated, its double-layer solvation structure is composed of weakly solvated tetrahydrofuran as the inner layer, and dipole interaction are introduced in the outer layer by dibutyl ether. This double-layer solvation structure dominated by contact ion pairs and aggregates can promote to deriving of inorganic-rich SEI film, resulting in smooth and dendrite-free sodium-metal deposition. By adjusting the molecular configuration of dibutyl ether to diisobutyl ether, the dipole interaction is further enhanced, resulting in stronger weakly solvating effect. Thus, the Na||Cu cells using the optimized DWIE achieved a high Coulombic efficiency of 99.22%, surpassing most electrolyte design strategies. Meanwhile, at 5C, the Na3V2(PO4)3 (NVP)||Na cell achieves stable cycling exceeding 3000 cycles. Even under rigorous conditions of ≈8.8 mg cm−2 NVP loading and 50 µm thickness Na, the full cell can achieve a long cycling lifespan of 217 cycles. The pioneering concept paves the way for crafting readily achievable, cost-effective, and eco-friendly electrolytes tailored for SMBs, and offers potential applications in other battery systems.
AB - Sodium-metal batteries are the most promising low-cost and high-energy-density new energy storage technology. However, the sodium-metal anode has poor reversibility, which can be optimized by constructing the robust solid electrolyte interphase (SEI). Here, a concept of dual-weak-interaction electrolyte (DWIE) is demonstrated, its double-layer solvation structure is composed of weakly solvated tetrahydrofuran as the inner layer, and dipole interaction are introduced in the outer layer by dibutyl ether. This double-layer solvation structure dominated by contact ion pairs and aggregates can promote to deriving of inorganic-rich SEI film, resulting in smooth and dendrite-free sodium-metal deposition. By adjusting the molecular configuration of dibutyl ether to diisobutyl ether, the dipole interaction is further enhanced, resulting in stronger weakly solvating effect. Thus, the Na||Cu cells using the optimized DWIE achieved a high Coulombic efficiency of 99.22%, surpassing most electrolyte design strategies. Meanwhile, at 5C, the Na3V2(PO4)3 (NVP)||Na cell achieves stable cycling exceeding 3000 cycles. Even under rigorous conditions of ≈8.8 mg cm−2 NVP loading and 50 µm thickness Na, the full cell can achieve a long cycling lifespan of 217 cycles. The pioneering concept paves the way for crafting readily achievable, cost-effective, and eco-friendly electrolytes tailored for SMBs, and offers potential applications in other battery systems.
KW - dipole interaction
KW - dual-weak-interaction electrolyte
KW - electrode-electrolyte interface
KW - inorganic-rich SEI
KW - sodium-metal batteries
UR - http://www.scopus.com/inward/record.url?scp=85215517836&partnerID=8YFLogxK
U2 - 10.1002/aenm.202405803
DO - 10.1002/aenm.202405803
M3 - Article
AN - SCOPUS:85215517836
SN - 1614-6832
VL - 15
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 20
M1 - 2405803
ER -