Regularly Arranged Micropore Architecture Enables Efficient Lithium-Ion Transport in SiOx/Artificial Graphite Composite Electrode

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Regularly Arranged Micropore Architecture Enables Efficient Lithium-Ion Transport in SiOx/Artificial Graphite Composite Electrode
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Regularly Arranged Micropore Architecture Enables Efficient Lithium-Ion Transport in SiOx/Artificial Graphite Composite Electrode - Nano-Micro Letters

To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content, it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well. Herein, we suggest an effective approach to control the micropore structure of silicon oxide (SiOx)/artificial graphite (AG) composite electrodes using a perforated current collector. The electrode features a unique pore structure, where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance, leading to a 20% improvement in rate capability at a 5C-rate discharge condition. Using microstructure-resolved modeling and simulations, we demonstrate that the patterned micropore structure enhances lithium-ion transport, mitigating the electrolyte concentration gradient of lithium-ion. Additionally, perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiOx/AG composite electrode, significantly improving adhesion strength. This, in turn, suppresses mechanical degradation and leads to a 50% higher capacity retention. Thus, regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiOx/AG composite electrodes, providing valuable insights into electrode engineering.

As demand rises for fast-charging and high-energy lithium-ion batteries, thick SiOx-based anodes still face slow ion transport and mechanical degradation. Researchers led by Prof. Hongkyung Lee and Prof. Yong Min Lee now report a scalable solution based on a perforated Cu (pCu) current collector, which induces a regularly arranged micropore (RAM) structure. This simple yet powerful design enhances ion diffusion, mechanical stability, and overall electrochemical performance in SiOx/artificial graphite (AG) electrodes.

Why Micropore Regulation Matters

  • Transport bottleneck: Thick SiOx/AG electrodes suffer from tortuous Li-ion pathways and concentration polarization, which limit rate capability.
  • Mechanical degradation: SiOx experiences large volume change, causing cracking, delamination, and rapid capacity loss.
  • Scalability gap: Existing pore-engineering approaches (laser patterning, additives) add complexity; a simple, compatible method is needed for industrial use.

Design Concept: Perforated Cu Induces RAM

  • Perforation mechanism: Chemical etching produces microscale holes in Cu foil. When slurry is cast and calendered, holes fill with active material, producing alternating high-porosity domains (HPds) above perforations and low-porosity domains (LPds) elsewhere.
  • Interface chemistry and mechanics: Etching creates hydroxyl-rich Cu surfaces that enhance wetting and hydrogen-bonding with PAA binder, while the filled holes form an interlocking interface that resists delamination.

Transport Dynamics & Electrochemical Advantages

  • Faster, more uniform ion flux: Microstructure-resolved segmentation and pore-network analysis show larger equivalent pore radii, higher coordination numbers, and lower tortuosity in HPds—facilitating rapid Li-ion access and more homogeneous ion distribution.
  • Reduced polarization at high rates: Pseudo-4D electrochemical simulations show lower overpotential and deeper utilization during fast discharge (e.g., 3C), consistent with experiments.
  • HPd–LPd synergy: HPds act as local ion reservoirs, improving ion supply to adjacent LPds and mitigating localized depletion.

Performance Highlights

  • Rate capability: RAM electrodes deliver higher capacities across 0.2C–5C and recover well when returned to low C-rates.
  • Durability: Slower growth of interfacial resistance, smaller irreversible thickness changes, and minimal delamination yield markedly improved cycle life.
  • Scalability: Double-sided pCu electrodes and 60-mAh pouch cells confirm manufacturing viability.

Practical Benefits & Outlook

  • Energy-density gain: Perforation reduces Cu mass (~32%), raising gravimetric energy density to ~258 Wh kg-1 and volumetric to ~694 Wh L-1.
  • Manufacturing-ready: pCu retains sufficient tensile strength for roll-to-roll processing. Future work should optimize perforation geometry and extend the RAM concept to higher-Si formulations.

This simple, low-cost modification of the current collector provides a practical route to fast-charging, long-life SiOx anodes and advances scalable battery electrode engineering.

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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
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  • 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.