High‑Performance Wide‑Temperature Zinc‑Ion Batteries with K+/C3N4 Co‑Intercalated Ammonium Vanadate Cathodes

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High‑Performance Wide‑Temperature Zinc‑Ion Batteries with K+/C3N4 Co‑Intercalated Ammonium Vanadate Cathodes
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High-Performance Wide-Temperature Zinc-Ion Batteries with K+/C3N4 Co-Intercalated Ammonium Vanadate Cathodes - Nano-Micro Letters

NH4V4O10 (NVO) is considered a promising cathode material for aqueous zinc-ion batteries due to its high theoretical capacity. However, its practical application is limited by irreversible deamination, structural collapse, and sluggish reaction kinetics during cycling. Herein, K+ and C3N4 co-intercalated NVO (KNVO-C3N4) nanosheets with expanded interlayer spacing are synthesized for the first time to achieve high-rate, stable, and wide-temperature cathodes. Molecular dynamics and experimental results confirm that there is an optimal C3N4 content to achieve higher reaction kinetics. The synergistic effect of K+ and C3N4 co-intercalation significantly reduces the electrostatic interaction between Zn2+ and the [VOn] layer, improves the specific capacity and cycling stability. Consequently, the KNVO-C3N4 electrode displays outstanding electrochemical performance at room temperature and under extreme environments. It exhibits excellent rate performance (228.4 mAh g−1 at 20 A g−1), long-term cycling stability (174.2 mAh g−1 after 10,000 cycles at 20 A g−1), and power/energy density (210.0 Wh kg−1 at 14,200 W kg−1) at room temperature. Notably, it shows remarkable storage performance at − 20 °C (111.3 mAh g−1 at 20 A g−1) and 60 °C (208.6 mAh g−1 at 20 A g−1). This strategy offers a novel approach to developing high-performance cathodes capable of operating under extreme temperatures.

As demand for safe and low-cost energy storage grows, aqueous zinc-ion batteries (AZIBs) have emerged as promising candidates. However, their practical application is hindered by cathode instability and poor low-temperature performance. Now, researchers from The Hong Kong Polytechnic University and Shenzhen University, led by Professor Zijian Li, have developed a novel K+and C3N4 co-intercalated NH4V4O10 (KNVO-C3N4) cathode that delivers exceptional performance across a wide temperature range.

Why K+/C3N4 Co-Intercalation Matters

  • Enhanced Reaction Kinetics: The synergistic effect of K+ and C3N4 reduces electrostatic interactions and lowers the Zn2+ diffusion barrier.
  • Structural Stability: Expanded interlayer spacing (10.62 Å) and increased oxygen vacancies improve structural integrity during cycling.
  • Wide-Temperature Operation: Delivers 111.3 mAh g-1 at −20 °C and 208.6 mAh g-1 at 60 °C, even at 20 A g-1.
  • Long-Term Durability: Retains 174.2 mAh g-1 after 10,000 cycles at 20 A g-1, with 78.2% capacity retention at 10 A g-1 over 5,000 cycles.

Innovative Design and Features

  • Tunable Interlayer Spacing: Adjusting C3N4 content optimizes ion transport and mechanical flexibility.
  • Synergistic Intercalation: K+ boosts capacity; C3N4 enhances stability—together they outperform single-intercalation strategies.
  • Reversible Phase Transitions: Ex situ XRD, Raman, and XPS confirm reversible Zn2+and H2O co-intercalation without structural collapse.
  • Pouch Cell Viability: Demonstrates stable performance under bending (0–180°) and powers commercial devices like thermometers.

Applications and Future Outlook

  • Extreme Environment Energy Storage: Ideal for cold-climate electronics, wearable devices, and grid storage.
  • Scalable Synthesis: Uses low-cost hydrothermal and stirring methods, suitable for mass production.
  • Next-Gen Cathode Design: Offers a blueprint for co-intercalation strategies in layered vanadates and beyond.
  • Challenges and Opportunities: Future work will explore other co-intercalants and optimize electrolytes for even wider temperature ranges.

This work provides a practical and scalable pathway to high-performance, wide-temperature AZIBs. It underscores the power of synergistic material engineering in overcoming long-standing cathode limitations. Stay tuned for more innovations from Professor Zijian Li and his team!

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Batteries
Physical Sciences > Materials Science > Materials for Energy and Catalysis > Batteries
Electrochemistry
Physical Sciences > Chemistry > Physical Chemistry > Electrochemistry
Reaction Kinetics
Physical Sciences > Chemistry > Physical Chemistry > Reaction Kinetics
Nanoscale Design, Synthesis and Processing
Physical Sciences > Materials Science > Nanotechnology > Nanoscale Design, Synthesis and Processing
Electrocatalysis
Physical Sciences > Materials Science > Materials for Energy and Catalysis > Electrocatalysis
  • Nano-Micro Letters Nano-Micro Letters

    Nano-Micro Letters is a peer-reviewed, international, interdisciplinary and open-access journal that focus on science, experiments, engineering, technologies and applications of nano- or microscale structure and system in physics, chemistry, biology, material science, and pharmacy.