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 Te/Te 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)), which initiates the Te/Te conversion with two distinct charge-storage steps. Te cathode undergoes Te/TeCl 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 g and an outstanding energy density of 850 Wh kg , outperforming most of the previously reported cathodes. Our electrolyte analysis indicates that the addition of Mg(TFSI) 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) is verified as an essential buffer to mitigate the corrosion and passivation of Mg anodes caused by the consumption of the electrolyte MgCl in Mg//Te dual-ion cells. These findings provide crucial insights into the development of advanced Mg-based dual-ion batteries.
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http://dx.doi.org/10.1002/anie.202401818 | DOI Listing |
J Am Chem Soc
January 2025
School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, Beihang University, Beijing 100191, China.
Potassium (K)-based batteries hold great promise for cryogenic applications owing to the small Stokes radius and weak Lewis acidity of K. Nevertheless, energy-dense (>200 W h kg) K batteries under subzero conditions have seldom been reported. Here, an over 400 W h kg K battery is realized at -40 °C via an anode-free and dual-ion strategy, surpassing these state-of-the-art K batteries and even most Li/Na batteries at low temperatures (LTs).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Advanced Energy Storage Technology Research Center, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, 518055, Shenzhen, China.
Organic electrode materials offer multi-electron reactivity, flexible structures, and redox reversibility, but encounter poor conductivity and durability in electrolytes. To overcome above barriers, we propose a dual elongation strategy of π-conjugated motifs with active sites, involving the extended carbazole and electropolymerized polymer, which enhances electronic conductivity by the electronic delocalization of electron-withdrawing conjugated groups, boosts theoretical capacity by increasing redox-active site density, and endows robust electrochemical stability attributed to the nanonetwork feature of polymer structures. As a proof-of-concept, 5,11-dihydridoindolo[3,2-b]carbazole (DHIC) is selected as the model cathode material for a dual-ion battery, with elongated carbazole groups functioning both as redox-active centers and polymerization anchors.
View Article and Find Full Text PDFSmall Methods
December 2024
Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, No.43, Sec. 4, Keelung Road, Taipei, 106, Taiwan.
Dual-ion batteries (DIBs) are garnering immense attention for their capability to operate without the expensive elements required by lithium-ion batteries. Phenylenediamine serves as a versatile and sustainable resource, enabling the efficient preparation of both cathode and anode materials through precise molecular control and straightforward synthesis. The innovative asymmetrical DIBs based on amine-rich poly(phenylenediamine) cathodes and imine-rich poly(phenylenediamine) anodes enable oxidative and reductive states, providing a transition metal-free rechargeable battery.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China.
Using a solid electrolyte is considered to be the most effective strategy to solve the shuttle effect in lithium-sulfur batteries. However, the practical application of solid-state lithium-sulfur batteries (SLSBs) is still far from being realized. This is because SLSBs, like all other solid-state battery systems, also face the dilemma of interface degradation (including both the anode and cathode interfaces), in addition to terrible kinetics due to the nonliquid solid-state electrolytes infiltrating the nonconductive sulfur particles inside the cathode.
View Article and Find Full Text PDFSmall
November 2024
Department of Chemistry and Department of Battery Engineering, Pohang University of Science and Technology (POSTECH), Pohang, 37673, Republic of Korea.
Dual-ion batteries (DIBs) are emerging as promising candidates for fast-charging electric vehicles owing to their ability to intercalate both cations and anions. However, increasing the energy density of DIBs, especially with thick graphite cathodes, remains a challenge due to structural instability during anion intercalation. In this study, a magnetically controlled method is introduced to vertically align graphite particles in thick electrodes, significantly improving the performance of DIBs.
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