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Pre-Embedded CNTs Architecture Differentiates Carbon Functions for Kinetics Boosting in All-Solid-State Li-S Cathodes
Zeyu Zhu1, Yufei He1, Qinyu Li1
1College of Smart Materials and Future Energy, State Key Laboratory of Advanced Coatings for Equipment, Fudan University, Shanghai, People's Republic of China.
Abstract:
All-solid-state lithium-sulfur batteries (ASSLSBs) are promising high-energy storage systems, yet their performance is severely limited by sluggish cathode kinetics due to the insulating nature of sulfur species and inefficient charge transport within the composite cathode. Herein, a functional-differentiation strategy via a pre-embedded carbon nanotubes (CNTs) framework is proposed to enhance the charge transport in sulfide-based ASSLSB cathodes. The design employs Li6PS5Cl (LPSC) as an ionic conductor, Ketjen black (KB) for sulfur hosting and short-range electron transfer, and pre-embedded CNTs as a long-range electronic conducting skeleton. Compared with conventional loading-type and bridging-type configurations, the framework-type CNTs-based cathode exhibits significantly improved charge transport and electrochemical performance. It delivers a discharge capacity of 1438 mAh g-1 at 1 C (2.5 mA cm-2), with 91.9% capacity retention after 400 cycles, and maintains 404 mAh g-1 under a high sulfur loading of 9 mg cm-2. Electrochemical analyses, local electrical mapping, and theoretical simulations reveal that the enhanced kinetics stem from a more homogeneous electronic network, which suppresses charge accumulation and facilitates Li+ transport. This work highlights that spatial reconstruction and functional differentiation of carbon components can effectively mitigate kinetic barriers in high-energy-density ASSLSBs.
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