Li-O batteries are recognized for their high theoretical capacity and energy density, positioning them as excellent candidates for next-generation energy storage. This study explores the use of Metal-Organic Frameworks (MOFs) with high specific surface areas and open metal sites as cathode materials to address existing challenges. We developed conductive "cactus-like" composites by employing hydroxylated graphene (G-OH) as a substrate to grow columnar M(HHTP) and MM(HHTP) (M = Cu, Ni) in a one-pot synthesis, enhancing the structure's conductivity and order. The cathode, especially the [CuNi(HHTP)]-(G-OH) composition, demonstrated a specific capacity of up to 12 542 mA h g at a current density of 50 mA g and maintained stability over more than 40 cycles at a limited capacity of 500 mA h g in an O atmosphere. This performance surpasses that of M(HHTP), MM(HHTP), or G-OH alone, highlighting the potential of MOF-based composites in improving the efficiency and durability of Li-O batteries and opening new avenues for cathode material design.
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http://dx.doi.org/10.1039/d5dt00162e | DOI Listing |
Dalton Trans
March 2025
School of Chemistry and Chemical Engineering, Zhejiang Sci-Tech University, Hangzhou 310018, People's Republic of China.
Li-O batteries are recognized for their high theoretical capacity and energy density, positioning them as excellent candidates for next-generation energy storage. This study explores the use of Metal-Organic Frameworks (MOFs) with high specific surface areas and open metal sites as cathode materials to address existing challenges. We developed conductive "cactus-like" composites by employing hydroxylated graphene (G-OH) as a substrate to grow columnar M(HHTP) and MM(HHTP) (M = Cu, Ni) in a one-pot synthesis, enhancing the structure's conductivity and order.
View Article and Find Full Text PDFJ Am Chem Soc
March 2025
Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing 100084, China.
It is desirable for lithium-oxygen batteries (LOBs) to fabricate the cathode catalysts with high catalytic activity and stability. High entropy oxide (HEO) sub-1 nm nanowires (SNWs) with the nearly 100% active site exposure and intrinsic stability are doubtless one of the best candidates. Herein, under a mild solvothermal condition, by incorporating phosphomolybdic acid (PMA) into multimetal oxide reaction system, a series of HEO-PMA SNWs are successfully prepared, where the variety of metal oxides is adjustable from mono component to six components.
View Article and Find Full Text PDFChemphyschem
February 2025
IISER Pune: Indian Institute of Science Education Research Pune, Chemistry, Pashan, 411008, Pune, INDIA.
Polyoligomeric silsesquioxane (POSS) tailored with trifluoromethanesulfonylimide-lithium and solvated in tetraglyme (G4) is a potential electrolyte for Li-ion batteries. Using classical MD simulations, at different G4/POSS(-LiNSO2CF3)8 molar ratios, the interactions of Li+ ions with the oxygen atoms of G4 and, oxygen/nitrogen sites of the pendant tails, the behavior of POSS(--NSO2CF3)8 anion, and the mobility of species are investigated. The RDFs showed that there exist competing interactions of the O(G4), O(POSS), and N(POSS) sites with Li+ ions.
View Article and Find Full Text PDFSmall
February 2025
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China.
Aprotic Li-O batteries exhibit ultra-high energy density through the redox reaction of O. However, their open-structure design makes them prone to water infiltration and electrolyte leakage. Traditionally, dense and thick oxygen-permeable membranes (OPMs) are employed to prevent HO intrusion, but this approach limits O permeance and constrains charge current densities.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2025
School of Energy Science and Engineering, Nanjing Tech University, Nanjing 211816, Jiangsu, China.
The practical development of Li-O batteries is often hindered by poor cycling stability, which arises from volatile liquid electrolytes, an unstable anode/electrolyte interface, and sluggish reaction kinetics related to LiO. In this study, we design a long-life quasi-solid-state Li-O battery by integrating a gel polymer electrolyte (GPE) with a tetramethylpiperidinyloxy (TEMPO) redox mediator anchored in a poly(2,2,6,6-tetramethylpiperidinyloxy-4-methacrylate) (PTMA) cathode. During cycling, the GPE stabilizes the lithium/electrolyte interface and retains the electrolyte, while the TEMPO moieties anchored in the PTMA cathode effectively enhance the catalytic selectivity for LiO formation and decomposition.
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