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Dynamically Adaptive Interfacial Chemistry via Molecular Programming for Sustainable Zn Batteries
Zelin Chang1, Wenyu Xu1, Hongwei Wang1
1School of Physics and Laboratory of Zhongyuan Light, Zhengzhou University, Zhengzhou 450052, China.
We developed a self-healing ionic liquid interphase for zinc anodes, significantly improving battery lifespan and stability by preventing dendrite growth and corrosion. This breakthrough enhances the practical application of zinc batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Artificial interfacial layers are key for improving zinc (Zn) redox reactions by controlling mass-electron transport.
- However, interface degradation and side reactions limit the long-term stability of Zn batteries.
Purpose of the Study:
- To engineer a mechanically adaptive ionic liquid interphase for enhanced Zn anode stability and performance.
- To suppress dendrite growth and corrosion while maintaining interfacial integrity.
Main Methods:
- Fabrication of a mechanically adaptive ionic liquid interphase using zincophilic coordination and hydrophobic shielding.
- Electrochemical testing of the engineered Zn anode, including cycling stability, rate capability, and long-term operation.
- Operando spectroscopy and theoretical simulations to elucidate the interphase formation mechanism.
- Testing of full battery performance with an iodine (I2) cathode under various conditions, including multiaxial stress in pouch cells.
Main Results:
- The engineered Zn anode demonstrated exceptional cyclability (200 h at 30 mAh cm-2) and high cumulative capacity (5400 mAh at 20 mA cm-2).
- Achieved record-long 4400 h operation at 1 mA cm-2 with low polarization (30 mV) due to superior thermodynamic stability.
- The adaptive architecture improved capacity retention by over 500% in 30 cm2 pouch cells under stress.
- Full batteries retained 86% capacity after 30000 cycles at 10 A g-1.
Conclusions:
- The ionic liquid interphase dynamically self-reconfigures, maintaining structural and functional integrity through zincophilic coordination and hydrophobic shielding.
- Bis(trifluoromethanesulfonyl)imide anions and 1-ethyl-3-methylimidazolium cations play crucial roles in template formation and water blocking, respectively.
- This work presents a viable strategy for developing practical and stable Zn batteries by integrating self-adaptive interfacial layers.
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