Unlocking Four-electron Conversion in Tellurium Cathodes for Advanced Magnesium-based Dual-ion Batteries

Unlocking Four-electron Conversion in Tellurium Cathodes for Advanced Magnesium-based Dual-ion Batteries

2024 | Ahiud Morag, Xingyuan Chu, Maciej Marczewski, Jonas Kunigkei, Christof Neumann, Davood Sabaghi, Grazyna Zofia Zukowska, Jingwei Du, Xiaodong Li, Andrey Turchanin, Eike Brunner, Xinliang Feng, and Minghao Yu
This study addresses the challenge of developing high-performance cathodes for magnesium (Mg) batteries by unlocking the reversible four-electron Te³⁺/Te⁴⁺ conversion in elemental tellurium (Te). The researchers tailored the classic magnesium aluminum chloride complex (MACC) electrolyte by introducing Mg bis(trifluoromethanesulfonyl)imide (Mg(TFSI)), which initiates the Te³⁺/Te⁴⁺ conversion through two distinct charge-storage steps. The Te cathode undergoes a Te/TeCl₄ conversion involving Cl⁻ as charge carriers, with a tellurium subchloride phase as an intermediate. This results in a high specific capacity of 543 mAh/gTe⁻¹ and an energy density of 850 Wh/gTe⁻¹, outperforming most previously reported Mg-based cathodes. The addition of Mg(TFSI)₂ reduces ion-molecule interaction and mitigates ion-solvent aggregation, facilitating Cl⁻ dissociation from the electrolyte. Additionally, Mg(TFSI)₂ acts as a buffer to mitigate corrosion and passivation of Mg anodes caused by the consumption of MgCl₂ in the electrolyte. These findings provide crucial insights for the development of advanced Mg-based dual-ion batteries.This study addresses the challenge of developing high-performance cathodes for magnesium (Mg) batteries by unlocking the reversible four-electron Te³⁺/Te⁴⁺ conversion in elemental tellurium (Te). The researchers tailored the classic magnesium aluminum chloride complex (MACC) electrolyte by introducing Mg bis(trifluoromethanesulfonyl)imide (Mg(TFSI)), which initiates the Te³⁺/Te⁴⁺ conversion through two distinct charge-storage steps. The Te cathode undergoes a Te/TeCl₄ conversion involving Cl⁻ as charge carriers, with a tellurium subchloride phase as an intermediate. This results in a high specific capacity of 543 mAh/gTe⁻¹ and an energy density of 850 Wh/gTe⁻¹, outperforming most previously reported Mg-based cathodes. The addition of Mg(TFSI)₂ reduces ion-molecule interaction and mitigates ion-solvent aggregation, facilitating Cl⁻ dissociation from the electrolyte. Additionally, Mg(TFSI)₂ acts as a buffer to mitigate corrosion and passivation of Mg anodes caused by the consumption of MgCl₂ in the electrolyte. These findings provide crucial insights for the development of advanced Mg-based dual-ion batteries.
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