Issue 14, 2024

Confined tandem catalytic quasi-solid sulfur reversible conversion for all-solid-state Na–S batteries

Abstract

Controlling the complex, multiphase sulfur/polysulfide redox process is a fundamental pathway to alleviate the cathodic passivation and unlock the high energy potentials of all-solid-state Na–S electrochemistry. Herein, by employing a confined tandem electrocatalytic approach, we successfully tune the polysulfide speciation pathway to enable energetic, low-temperature (80 °C) Na–S systems based on dense Na3Zr2Si2PO12 ceramic membranes. Our design features york–shell structured MnHCF/PPy@MnO2 coaxial nanotubes endowed with a localized and confined environment. These components synergistically catalyze the conversion of encapsulated sulfur/sulfide, with MnO2 effectively directing long-chain polysulfide transition and MnHCF nanoclusters catalyzing low-kinetic Na2S4 to Na2S direct and reversible conversion. This facilitates continuous, fully controllable quasi-solid sulfur conversion, significantly enhancing battery performance. Operando investigations show that, without the mediation of these bi-catalytic centers, the electrodeposited Na2S2/Na2S exhibits a much higher activation energy upon recharging, leading to the accumulation of inactive polysulfide species and exacerbated cathodic passivation. Consequently, our approach enables a low N/P ratio all-solid-state Na–S cell with a high reversible capacity of 1111 mA h gS−1 and an energy output of 880 W h kgcathode−1.

Graphical abstract: Confined tandem catalytic quasi-solid sulfur reversible conversion for all-solid-state Na–S batteries

Supplementary files

Article information

Article type
Paper
Submitted
22 Apr 2024
Accepted
13 Jun 2024
First published
14 Jun 2024

Energy Environ. Sci., 2024,17, 5273-5282

Confined tandem catalytic quasi-solid sulfur reversible conversion for all-solid-state Na–S batteries

W. Zhang, B. Song, M. Wang, T. Miao, X. Huang, E. Zhang, X. Zhan, Y. Yang, H. Zhang and K. Lu, Energy Environ. Sci., 2024, 17, 5273 DOI: 10.1039/D4EE01750A

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