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Combining in situ electrochemistry, operando FTIR and post-mortem analyses to understand Co-Mn-Al spinels on mitigating shuttle effect in lithium-sulfur battery

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Santos, Erick A. ; Anchieta, Chayene G. ; Fernandes, Rodolfo C. ; Pinzon, Manuel J. ; Miranda, Andre N. ; Galantini, Isabela ; Maia, Francisco C. B. ; Doubek, Gustavo ; Rodella, C. B. ; Da Silva, Leonardo M. ; Zanin, Hudson
Total Authors: 11
Document type: Journal article
Source: NANO ENERGY; v. 116, p. 15-pg., 2023-08-28.
Abstract

The spinel oxide Co2Mn0.5Al0.5O4 (CMA) was investigated as an additive onto the cathode of lithium-sulfur batteries. We demonstrate the polysulfide adsorption onto CMA, mitigating the shuttle effect, a well-known failure mechanism. The in situ electrochemical impedance spectroscopy and cyclic voltammetry tests evidenced that CMA facilitates the conversion of short-chain lithium polysulfides (LPS). The CMA reduced the maximum voltammetric current by approximately 20% compared to the AC/S cathode and facilitates the conversion of LPS into solid-liquid-solid species. High conversion efficiencies were verified after 315 cycles, resulting in 89% of capacity retention. Low CMA concentrations of up to 10 wt.% increased battery capacity and showed that CMA has high ionic conductivity, while moderate concentrations of approximately 50 wt.% improved cyclability but increased cell's resistivity. This improvement in cyclability is related to LPS trapped at CMA which is demonstrated by micrographs, X-ray energy dispersive and photoelectron spectra of post-mortem samples. The byproducts formed after cycling until failure, were identified by Raman spectra and diffraction patterns. Fourier transform infrared spectroscopy operando analyses suggested electrolyte decomposition as a relevant cell failure mechanism. In conclusion, we demonstrated how CMA can trap LPS and enhanced initial capacity to 1000 mA h g(sulfur)(-1) cm(-2) and improved cyclability for more than similar to 360 cycles. (AU)

FAPESP's process: 22/02222-0 - Development of prototype pouch cells of lithium-sulfur (Li-S) batteries in solid-liquid state with high stability and advanced scale of technological maturity
Grantee:Érick Alves Santos
Support Opportunities: Scholarships in Brazil - Doctorate
FAPESP's process: 20/04281-8 - Proposal for syntheses, characterization and application of electrodes for Li-S battery like capacitor
Grantee:Érick Alves Santos
Support Opportunities: Scholarships in Brazil - Master
FAPESP's process: 22/02901-4 - Nano-optics of polaritons in two-dimensional crystals and at the metal/dielectric interface in the mid-to-far infrared
Grantee:Francisco Carlos Barbosa Maia
Support Opportunities: Research Grants - Initial Project