Dual-ion batteries are known for anion storage in the cathode coupled to cation incorporation in the anode. We flip the sequence of the anion/cation-storage chemistries of the anode and the cathode in dual-ion batteries (DIBs) by allowing the anode to take in anions and a cation-deficient cathode to host cations, thus operating as a reverse dual-ion battery (RDIB). The anion-insertion anode is a nanocomposite having ferrocene encapsulated inside a microporous carbon, and the cathode is a Zn-insertion Prussian blue, Zn[Fe(CN)]. This unique battery configuration benefits from the usage of a 30 m ZnCl "water-in-salt" electrolyte. This electrolyte minimizes the dissolution of ferrocene; it raises the cation-insertion potential in the cathode, and it depresses the anion-insertion potential in the anode, thus widening the full cell's voltage by 0.35 V compared with a dilute ZnCl electrolyte. RDIBs provide a configuration-based solution to exploit the practicality of cation-deficient cathode materials in aqueous electrolytes.
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http://dx.doi.org/10.1021/jacs.9b00617 | 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 PDFMicromachines (Basel)
October 2024
Department of Chemical, Biological, and Battery Engineering, Gachon University, Seongnam-si 13120, Gyeonggi-do, Republic of Korea.
The demand for safer, sustainable, and economical energy storage devices has motivated the development of lithium dual-ion batteries (Li_DIBs) for large-scale storage applications. For the Li_DIBs, expanded graphite (EG) cathodes are valuable as anion intercalation host frameworks to fabricate safer and more cost-effective devices. In this study, three different carbon cathode materials, including microwave-treated expanded graphite (MW-EG), ball-milled expanded graphite (BM-EG), and high-temperature-carbonized carbon nanoflakes (CNFs), were developed by different synthesis methods.
View Article and Find Full Text PDFAdv Mater
November 2024
Advanced Energy Storage Technology Research Center, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055, China.
Benefiting from the merits of intrinsic safety, high power density, environmental friendliness, and high-output voltage, aqueous dual-ion batteries (ADIBs) have shown broad potential applications in future grid-scale energy storage. However, since the ADIBs require the cathodes to undergo the intercalation reactions through different local structures and mechanisms, causing large structural deformation and cathode failure, their reversible cation-anion intercalation in the cathode remains a major challenge. To address this issue, based on a reasonable selection and theoretical simulation, this work finds that Todorokite manganese dioxide (t-MnO) cathode with a metal-ion stabilized 3 × 3 large-tunnel structure should be suitable for cation-anion intercalation of ADIBs.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Laboratory of Inorganic Materials Chemistry (CMI), University of Namur, 61 rue de Bruxelles, Namur, B-5000, Belgium.
Prussian blue analogues are highly promising electrode materials due to their versatile electrochemical activity and low cost. However, they often suffer from severe structural damage caused by the Jahn-Teller distortion and dissolution of high-spin outer metal ions, resulting in poor cycle life. Material modification and electrolyte regulation have been the common approaches to address this issue, albeit with very limited success.
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