Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Quasi-Solid-State Electrolytes

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Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Quasi-Solid-State Electrolytes
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Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Quasi-Solid-State Electrolytes - Nano-Micro Letters

Quasi-solid-state electrolytes, which integrate the safety characteristics of inorganic materials, the flexibility of polymers, and the high ionic conductivity of liquid electrolytes, represent a transitional solution for high-energy-density lithium batteries. However, the mechanisms by which inorganic fillers enhance multiphase interfacial conduction remain inadequately understood. In this work, we synthesized composite quasi-solid-state electrolytes with high inorganic content to investigate interfacial phenomena and achieve enhanced electrode interface stability. Li1.3Al0.3Ti1.7(PO4)3 particles, through surface anion anchoring, improve Li+ transference numbers and facilitate partial dissociation of solvated Li+ structures, resulting in superior ion transport kinetics that achieve an ionic conductivity of 0.51 mS cm−1 at room temperature. The high mass fraction of inorganic components additionally promotes the formation of more stable interfacial layers, enabling lithium-symmetric cells to operate without short-circuiting for 6000 h at 0.1 mA cm−2. Furthermore, this system demonstrates exceptional stability in 5 V-class lithium metal full cells, maintaining 80.5% capacity retention over 200 cycles at 0.5C. These findings guide the role of inorganic interfaces in composite electrolytes and demonstrate their potential for advancing high-voltage lithium battery technology.

Quasi-solid-state electrolytes promise the safety of ceramics, the flexibility of polymers, and the conductivity of liquids—yet the “how” behind their superior ion transport has remained murky. Now, a joint team from Fudan University and the National Institute for Cryogenic & Isotopic Technologies (Romania), led by Professors Aishui Yu and Tao Huang, delivers a decisive answer in Nano-Micro Letters. Their review, “Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Electrolytes” decodes the hidden chemistry that lets lithium sprint across solid/liquid boundaries.

The Secret Sauce: Acidic Interfaces

  • Selective Anion Anchoring: Acidic LATP surfaces act as Lewis-acid traps for DFOB- anions, loosening Li+ solvation cages and jacking the Li+ transference number from 0.31 → 0.53.
  • Size Matters: Shrinking LATP particles to 200–300 nm boosts specific surface area and pushes ionic conductivity to 51 mS cm-1 at room temperature.
  • Dual-Phase Highways: An “intermediate phase” bridges ceramic and liquid domains, creating 3-D conduction networks that outpace single-phase polymers.

Performance that Speaks Louder than Theory

  • 6000 h non-stop cycling in Li||Li symmetric cells at 0.1 mA cm-2 —no short-circuits.
  • 5 % capacity retention after 200 cycles in a 5 V-class LNMO||Li full cell at 0.5 C.
  • Pouch-cell demo drives LED arrays and mini-motors, proving scalability beyond coin cells.

Design Rules for Tomorrow's Electrolytes

  1. Surface Engineering > Bulk Chemistry: Acidic surface sites are the true catalysts; neutral or basic variants lag by 30 %.
  2. Active Fillers Win: Ion-conductive LATP beats inert alumina, cutting activation energy and sustaining high-rate capability (155 mAh g-1 at 0.1 C vs. 82 mAh g-1).
  3. SEI Self-Defense: LATP-induced decomposition forms a LiF-rich interphase that stops further Ti4+ reduction—self-limiting protection without extra coatings.

Future Outlook

  • Nano-Architected Interfaces: Next-gen electrolytes will leverage tunable surface acidity and hierarchical porosity to push conductivities beyond 1 mS cm-1.
  • High-Loading Cathodes: 14 mg cm-2LNMO cathodes already retain 142 mAh g-1—roadmap to >300 Wh kg-1 pouch cells.
  • Universal Design Toolkit: The acid-base descriptor framework can be ported to sulfides, chlorides, and beyond, fast-tracking the commercial leap from lab to EV.

Stay tuned as the Yu–Huang team turns interfacial chemistry into the next performance revolution for lithium-metal batteries.

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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.