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 presents a novel magnesium (Mg)-tellurium (Te) dual-ion battery by unlocking the reversible four-electron Te⁰/Te⁴⁺ conversion in elemental Te. The key innovation lies in modifying the classic magnesium aluminum chloride complex (MACC) electrolyte by introducing Mg bis(trifluoromethanesulfonyl)imide (Mg(TFSI)₂), which enables the two-step Te⁰/TeCl₄ conversion. This conversion involves Cl⁻ as charge carriers and generates a tellurium subchloride phase as an intermediate. The Te cathode achieves a high specific capacity of 543 mAh g⁻¹ and an outstanding energy density of 850 Wh kg⁻¹, outperforming most previously reported cathodes. The addition of Mg(TFSI)₂ reduces ion-molecule interactions and mitigates ion-solvent aggregation in the MACC electrolyte, facilitating Cl⁻ dissociation and enabling the Te⁰/Te⁴⁺ conversion. Additionally, Mg(TFSI)₂ acts as an effective buffer to mitigate Mg anode corrosion and passivation caused by electrolyte MgCl₂ consumption. The study also demonstrates that the Te cathode undergoes Te/TeCl₄ conversion with Cl⁻ as charge carriers, and the Te electrode exhibits excellent cyclability when combined with a graphite oxide (GO)-coated separator. The Te electrode achieves a high energy density of 850 Wh kg⁻¹, comparable to the best reported conversion-type S cathode, and significantly higher power density. The study provides crucial insights into the development of advanced Mg-based dual-ion batteries, highlighting the importance of anion charge carriers in enhancing conversion kinetics and battery performance. The findings demonstrate that the Te⁰/Te⁴⁺ conversion is a promising approach for high-performance Mg//Te dual-ion batteries.This study presents a novel magnesium (Mg)-tellurium (Te) dual-ion battery by unlocking the reversible four-electron Te⁰/Te⁴⁺ conversion in elemental Te. The key innovation lies in modifying the classic magnesium aluminum chloride complex (MACC) electrolyte by introducing Mg bis(trifluoromethanesulfonyl)imide (Mg(TFSI)₂), which enables the two-step Te⁰/TeCl₄ conversion. This conversion involves Cl⁻ as charge carriers and generates a tellurium subchloride phase as an intermediate. The Te cathode achieves a high specific capacity of 543 mAh g⁻¹ and an outstanding energy density of 850 Wh kg⁻¹, outperforming most previously reported cathodes. The addition of Mg(TFSI)₂ reduces ion-molecule interactions and mitigates ion-solvent aggregation in the MACC electrolyte, facilitating Cl⁻ dissociation and enabling the Te⁰/Te⁴⁺ conversion. Additionally, Mg(TFSI)₂ acts as an effective buffer to mitigate Mg anode corrosion and passivation caused by electrolyte MgCl₂ consumption. The study also demonstrates that the Te cathode undergoes Te/TeCl₄ conversion with Cl⁻ as charge carriers, and the Te electrode exhibits excellent cyclability when combined with a graphite oxide (GO)-coated separator. The Te electrode achieves a high energy density of 850 Wh kg⁻¹, comparable to the best reported conversion-type S cathode, and significantly higher power density. The study provides crucial insights into the development of advanced Mg-based dual-ion batteries, highlighting the importance of anion charge carriers in enhancing conversion kinetics and battery performance. The findings demonstrate that the Te⁰/Te⁴⁺ conversion is a promising approach for high-performance Mg//Te dual-ion batteries.