TY - JOUR
T1 - Unlocking Four-electron Conversion in Tellurium Cathodes for Advanced Magnesium-based Dual-ion Batteries
AU - Morag, Ahiud
AU - Chu, Xingyuan
AU - Marczewski, Maciej
AU - Kunigkeit, Jonas
AU - Neumann, Christof
AU - Sabaghi, Davood
AU - Żukowska, Grażyna Zofia
AU - Du, Jingwei
AU - Li, Xiaodong
AU - Turchanin, Andrey
AU - Brunner, Eike
AU - Feng, Xinliang
AU - Yu, Minghao
N1 - Publisher Copyright:
© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
PY - 2024/5/6
Y1 - 2024/5/6
N2 - Magnesium (Mg) batteries hold promise as a large-scale energy storage solution, but their progress has been hindered by the lack of high-performance cathodes. Here, we address this challenge by unlocking the reversible four-electron Te0/Te4+ conversion in elemental Te, enabling the demonstration of superior Mg//Te dual-ion batteries. Specifically, the classic magnesium aluminum chloride complex (MACC) electrolyte is tailored by introducing Mg bis(trifluoromethanesulfonyl)imide (Mg(TFSI)2), which initiates the Te0/Te4+ conversion with two distinct charge-storage steps. Te cathode undergoes Te/TeCl4 conversion involving Cl− as charge carriers, during which a tellurium subchloride phase is presented as an intermediate. Significantly, the Te cathode achieves a high specific capacity of 543 mAh gTe−1 and an outstanding energy density of 850 Wh kgTe−1, outperforming most of the previously reported cathodes. Our electrolyte analysis indicates that the addition of Mg(TFSI)2 reduces the overall ion-molecule interaction and mitigates the strength of ion-solvent aggregation within the MACC electrolyte, which implies the facilized Cl− dissociation from the electrolyte. Besides, Mg(TFSI)2 is verified as an essential buffer to mitigate the corrosion and passivation of Mg anodes caused by the consumption of the electrolyte MgCl2 in Mg//Te dual-ion cells. These findings provide crucial insights into the development of advanced Mg-based dual-ion batteries.
AB - Magnesium (Mg) batteries hold promise as a large-scale energy storage solution, but their progress has been hindered by the lack of high-performance cathodes. Here, we address this challenge by unlocking the reversible four-electron Te0/Te4+ conversion in elemental Te, enabling the demonstration of superior Mg//Te dual-ion batteries. Specifically, the classic magnesium aluminum chloride complex (MACC) electrolyte is tailored by introducing Mg bis(trifluoromethanesulfonyl)imide (Mg(TFSI)2), which initiates the Te0/Te4+ conversion with two distinct charge-storage steps. Te cathode undergoes Te/TeCl4 conversion involving Cl− as charge carriers, during which a tellurium subchloride phase is presented as an intermediate. Significantly, the Te cathode achieves a high specific capacity of 543 mAh gTe−1 and an outstanding energy density of 850 Wh kgTe−1, outperforming most of the previously reported cathodes. Our electrolyte analysis indicates that the addition of Mg(TFSI)2 reduces the overall ion-molecule interaction and mitigates the strength of ion-solvent aggregation within the MACC electrolyte, which implies the facilized Cl− dissociation from the electrolyte. Besides, Mg(TFSI)2 is verified as an essential buffer to mitigate the corrosion and passivation of Mg anodes caused by the consumption of the electrolyte MgCl2 in Mg//Te dual-ion cells. These findings provide crucial insights into the development of advanced Mg-based dual-ion batteries.
KW - anion charge carriers
KW - conversion-type cathodes
KW - dual-ion batteries
KW - magnesium batteries
KW - tellurium
UR - http://www.scopus.com/inward/record.url?scp=85188948446&partnerID=8YFLogxK
U2 - 10.1002/anie.202401818
DO - 10.1002/anie.202401818
M3 - Article
C2 - 38465851
AN - SCOPUS:85188948446
SN - 1433-7851
VL - 63
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 19
M1 - e202401818
ER -
