Key Takeaways & Executive Findings
- •• • LATP@C nanofiber network enables dry-processed NCM811 cathodes with areal loading up to 100 mg cm−2, delivering 203 mA h g−1 at 0.1 C and retaining 96.7% capacity after 35 cycles at 0.2 C, demonstrating feasibility for ultra-thick electrodes in high-energy LMBs. • • The integrated ionic-electronic scaffold couples fast Li+ conduction from NASICON core with electron transport via carbon shell, addressing tortuous transport pathways that typically limit dry-processed thick electrodes. • • Pouch cells with 60 mg cm−2 LATP@C cathodes retain 80.5% capacity after 50 cycles, validating scalability and practical viability beyond coin-cell level. • • Mechanically robust fibrous network bridges NCM811 secondary particles, suppressing crack initiation and preserving structural integrity under cycling-induced stress, which is critical for long-term cycling stability.
Abstract
Dry electrode processing offers a solvent-free and scalable pathway toward high-energy lithium metal batteries (LMBs), yet its practical implementation is constrained by tortuous ion/electron transport and weak mechanical cohesion in ultra-thick electrodes. Here, we construct a carbon-coated NASICON-type Li1.3Al0.3Ti1.7(PO4)3 nanofiber network (LATP@C) that serves as an integrated ionic-electronic scaffold within dry-processed Ni-rich cathodes. The one-dimensional LATP@C fibers form a continuous 3D percolation architecture that couples fast Li+ conduction from the NASICON core with efficient electron transport through the conformal carbon shell. Their rough, oxygen-functionalized surfaces further enhance electrolyte affinity, while the mechanically robust fibrous network bridges NCM811 secondary particles, suppressing crack initiation and preserving structural integrity during cycling. Benefiting from these collective effects, the LATP@C cathode with 100 mg cm−2 loading delivers 203 mA h g−1 at 0.1 C and maintains 96.7% capacity over 35 cycles at 0.2 C. Pouch cells incorporating 60 mg cm−2 LATP@C cathodes retain 80.5% capacity after 50 cycles, highlighting the practical viability of this design.
1. Introduction
Conventional slurry-based fabrication of thick cathodes relies on N-methyl-2-pyrrolidone (NMP) and extensive drying, which often induces binder segregation, particle detachment, cracking, and non-uniform porosity in thick electrodes. These processing limitations not only undermine mechanical integrity but also impede ionic and electronic transport, fundamentally restricting the performance of high-loading electrodes. Dry electrode processing, based on shear-induced PTFE fibrillation, has emerged as a scalable and solvent-free alternative capable of supporting ultra-high mass loading. Nevertheless, the intrinsic characteristics of dry-processed thick electrodes introduce new bottlenecks: the insulating PTFE binder forms discontinuous conductive domains, resulting in tortuous electron pathways, while extended Li+ diffusion distance and poor electrolyte infiltration generate severe concentration polarization within the electrode interior.
Attempts to incorporate conductive carbon or inorganic solid electrolytes alleviate part of these issues, but they often suffer from additive agglomeration, limited interfacial contact, and dilution of the active material fraction—offsetting the gains in energy density. Therefore, an integrated conductive network that simultaneously enhances Li+/e− transport, promotes electrolyte wettability, and strengthens mechanical cohesion is essential. This work introduces carbon-coated NASICON-type LATP nanofibers (LATP@C) as a multifunctional hybrid-conductive scaffold, addressing these intrinsic transport and mechanical limitations. The electrospinning-calcination process yields one-dimensional fibers with a fast Li+-conducting LATP core and an amorphous carbon shell, forming a continuous three-dimensional network capable of simultaneously facilitating ionic and electronic transport. The rough, oxygen-functionalized carbon surface enhances electrolyte affinity and infiltration, while the fibrous architecture mechanically bridges NCM811 secondary particles, suppressing crack formation and maintaining electrode cohesion under cycling-induced stress.
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LU Jingshan, ZHANG Yue, SONG Ruifeng, XIONG Xiaoqin, WANG Feng, HUANG Yunhui, XU Henghui (2026). Integrated ionic-electronic LATP@C nanofiber networks enable 100 mg cm−2 dry-processed Ni-rich cathodes for lithium-metal batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3960-0
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Frequently Asked Questions
What is the specific role of the carbon shell in LATP@C nanofibers, and how does it contribute to the electrochemical performance of dry-processed thick cathodes?
The carbon shell provides efficient electron transport pathways, complementing the Li+ conduction from the NASICON core. This integrated ionic-electronic network reduces tortuosity, enabling high areal loadings (100 mg cm−2) to deliver 203 mA h g−1 at 0.1 C and maintain 96.7% capacity after 35 cycles at 0.2 C.
How does the LATP@C scaffold address the mechanical integrity issues commonly observed in dry-processed thick electrodes?
The mechanically robust fibrous network bridges NCM811 secondary particles, suppressing crack initiation and preserving structural integrity during cycling. This is evidenced by stable cycling performance in both coin and pouch cells, with pouch cells retaining 80.5% capacity after 50 cycles at 60 mg cm−2 loading.
What are the scalability prospects of this LATP@C-based dry electrode processing for commercial lithium-metal batteries?
The dry electrode processing is solvent-free and scalable, and the LATP@C scaffold enables high areal loadings up to 100 mg cm−2. Pouch cell demonstration at 60 mg cm−2 with 80.5% capacity retention after 50 cycles indicates practical viability, though further optimization of manufacturing parameters and cost analysis is needed.
How does the LATP@C scaffold improve electrolyte wettability compared to conventional conductive additives like CNT?
The rough, oxygen-functionalized carbon surface enhances electrolyte affinity and infiltration, leading to uniform electrode/electrolyte interface. Ultrasonic imaging showed no blue regions (indicating poor wetting or gas generation) for LATP@C cathodes, unlike CNT+LATP cathodes which exhibited widespread blue regions due to structural inhomogeneity and inadequate electrolyte retention.
What is the impact of LATP@C on the rate capability and long-term cycling stability of Ni-rich cathodes?
The integrated conductive network significantly improves rate capability and long-term structural stability. Specifically, the LATP@C cathode with 100 mg cm−2 loading delivers 203 mA h g−1 at 0.1 C and maintains 96.7% capacity over 35 cycles at 0.2 C, while pouch cells with 60 mg cm−2 retain 80.5% capacity after 50 cycles, demonstrating robust cycling performance.
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