Anionically-Reinforced Nanocellulose Separator Enables Dual Suppression of Zinc Dendrites and Polyiodide Shuttle for Long-Cycle Zn-I2 Batteries

Published in Chemistry and Materials

Anionically-Reinforced Nanocellulose Separator Enables Dual Suppression of Zinc Dendrites and Polyiodide Shuttle for Long-Cycle Zn-I2 Batteries
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Anionically-Reinforced Nanocellulose Separator Enables Dual Suppression of Zinc Dendrites and Polyiodide Shuttle for Long-Cycle Zn-I2 Batteries - Nano-Micro Letters

Zn-I2 batteries have emerged as promising next-generation energy storage systems owing to their inherent safety, environmental compatibility, rapid reaction kinetics, and small voltage hysteresis. Nevertheless, two critical challenges, i.e., zinc dendrite growth and polyiodide shuttle effect, severely impede their commercial viability. To conquer these limitations, this study develops a multifunctional separator fabricated from straw-derived carboxylated nanocellulose, with its negative charge density further reinforced by anionic polyacrylamide incorporation. This modification simultaneously improves the separator’s mechanical properties, ionic conductivity, and Zn2+ ion transfer number. Remarkably, despite its ultrathin 20 μm profile, the engineered separator demonstrates exceptional dendrite suppression and parasitic reaction inhibition, enabling Zn//Zn symmetric cells to achieve impressive cycle life (> 1800 h at 2 mA cm−2/2 mAh cm−2) while maintaining robust performance even at ultrahigh areal capacities (25 mAh cm−2). Additionally, the separator’s anionic characteristic effectively blocks polyiodide migration through electrostatic repulsion, yielding Zn-I2 batteries with outstanding rate capability (120.7 mAh g−1 at 5 A g−1) and excellent cyclability (94.2% capacity retention after 10,000 cycles). And superior cycling stability can still be achieved under zinc-deficient condition and pouch cell configuration. This work establishes a new paradigm for designing high-performance zinc-based energy storage systems through rational separator engineering.

As demand grows for safe and sustainable energy storage, zinc–iodine (Zn–I2) batteries have emerged as a promising candidate due to their fast kinetics and low cost. However, zinc dendrite growth and polyiodide shuttle effects remain major barriers to long-term stability. Now, researchers from Nanjing Forestry University and Nanjing University, led by Prof. Jizhang Chen and Prof. Yagang Yao, have developed a straw-derived, anionically reinforced nanocellulose separator that effectively addresses both challenges.

Why This Separator Matters

  • Dual Functional Design: Simultaneously suppresses zinc dendrite formation and polyiodide migration through electrostatic repulsion and enhanced ion transport.
  • Sustainable & Scalable: Fabricated from renewable straw biomass using a simple solution-casting method—eco-friendly and cost-effective.
  • Ultrathin & Strong: At just 20 μm thick, it offers 147 MPa tensile strength, outperforming conventional glass fiber separators.

Innovative Design and Features

  • TOCN-A Structure: Combines TEMPO-oxidized cellulose nanofibers (TOCN) with anionic polyacrylamide (APAM) to boost negative charge density and mechanical integrity.
  • Enhanced Zn2+ Transport: Achieves a Zn2+ transfer number of 0.45 and ionic conductivity of 14.3 mS cm-1, promoting uniform zinc deposition.
  • Polyiodide Blocking: Strong electrostatic repulsion reduces I3 migration by 81%, significantly improving cathode stability.

Applications and Performance

  • Long Cycle Life: Zn//Zn symmetric cells run for >1800 h at 2 mA cm-2/2 mAh cm-2, and 300 h under extreme conditions (25 mAh cm-2).
  • High Stability: Zn–I2 full cells retain 94.2% capacity after 10,000 cycles at 2 A g-1, with ultralow decay rate of 0.0058‰ per cycle.
  • Pouch Cell Validation: Demonstrates 99.4% capacity retention over 300 cycles and successfully powers LED panels and electronic devices.

Conclusion and Outlook

This work presents a multifunctional, biomass-derived separator that tackles both anode and cathode challenges in Zn–I2 batteries. 

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Batteries
Physical Sciences > Materials Science > Materials for Energy and Catalysis > Batteries
Electrochemistry
Physical Sciences > Chemistry > Physical Chemistry > Electrochemistry
Nanoscale Design, Synthesis and Processing
Physical Sciences > Materials Science > Nanotechnology > Nanoscale Design, Synthesis and Processing
Materials for Energy and Catalysis
Physical Sciences > Materials Science > Materials for Energy and Catalysis
  • 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.