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Electrochemical capacitors (ECs) have emerged as reliable and fast-charging electrochemical energy storage devices that offer high power densities. Their use is still limited, nevertheless, by their relatively low energy density. Because high specific surface area and electrical conductivity are widely seen as key metrics for improving the energy density and overall performance of ECs, materials that have excellent electrical conductivities but are otherwise nonporous, such as coordination polymers (CPs), are often overlooked. Here, we report a new nonporous CP, Ni(benzenehexathiolate) (NiBHT), which exhibits high electrical conductivity of over 500 S/m. When used as an electrode, NiBHT delivers excellent specific capacitances of 245 F/g and 426 F/cm in nonaqueous electrolytes. Structural and electrochemical studies relate the favorable performance to pseudocapacitive intercalation of Li ions between the 2D layers of NiBHT, a charge-storage mechanism that has thus far been documented only in inorganic materials such as TiO, NbO, and MXenes. This first demonstration of pseudocapacitive ion intercalation in nonporous CPs, a class of materials comprising thousands of members with distinct structures and compositions, provides important motivation for exploring this vast family of materials for nontraditional, high-energy pseudocapacitors.
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http://dx.doi.org/10.1021/jacs.0c10849 | DOI Listing |
Chemistry
December 2024
Ulsan National Institute of Science and Technology, Chemistry, UNIST-gil 50, Bldg.108, Rm901-5, 44919, Ulsan, KOREA, REPUBLIC OF.
Nanographenes and polycyclic aromatic hydrocarbons, both finite forms of graphene, are promising organic semiconducting materials because their optoelectronic and magnetic properties can be modulated through precise control of their molecular peripheries. Several atomically precise edge structures have been prepared by bottom-up synthesis; however, no systematic elucidation of these edge topologies at the molecular level has been reported. Herein, we describe rationally designed modular syntheses of isomeric dibenzoixenes with diverse molecular peripheries, including cove, zigzag, bay, fjord, and gulf structured.
View Article and Find Full Text PDFAdv Mater
December 2024
Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun, 130024, P. R. China.
Ammonium-ion supercapacitors (AISCs) offer considerable potential for future development owing to their low cost, high safety, environmental sustainability, and efficient electrochemical energy storage capabilities. The rapid and efficient charge-transfer process at the AISC can endow them with high capacitive and cycling stabilities. However, the prolonged intercalation/deintercalation of NH in layered and framework materials often results in the cleavage of the active sites and the deconstruction of the framework, which makes it difficult to achieve long-term stable energy storage while maintaining high capacitance in the electrode materials.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
Guangxi Key Laboratory of Low-Carbon Energy Materials, School of Chemistry and Pharmaceutical Sciences, Guangxi Normal University, Guilin 541004, China.
O3-type layered oxides are considered promising cathode materials for next-generation high-energy-density sodium-ion batteries (SIBs). However, they face challenges, such as low rate capacity and poor cycling stability, which arise from structural deformation, sluggish Na diffusion kinetics, and interfacial side reactions. Herein, a synergistic substitution strategy for transitional and interstitial sites was adopted to improve the structure stability and Na diffusion kinetics of the O3-type NaNiFeMnO.
View Article and Find Full Text PDFACS Nano
December 2024
Department of Materials Science and Engineering, Dankook University, 119 Dandae-ro, Cheonan 31116, South Korea.
Crystalline SnS accommodates Na ions through intercalation-conversion-alloying (ICA) reactions, exhibiting a natural potential for high energy storage, while its layered structure facilitates rapid charging. However, these intrinsic advantages are not fully realized in practical battery applications. Herein, utilizing an innovative integration of machine-learning-based thermodynamics, artificial-neural-network-assisted molecular dynamics, and density functional theory, specific solvents are demonstrated to effectively tailor the reaction pathways.
View Article and Find Full Text PDFNanotechnology
December 2024
IMDEA Materials Institute, C/ Eric Kandel 2, Getafe, Madrid, 28906, SPAIN.
Although Mg-Li dual metal-ion batteries are proposed as a superior system that unite safety of Mg-batteries and performance of Li-ion based systems, its practical implantation is limited due to the lack of reliable high performance cathodes. Herein, we report a high-performance Mg-Li dual metal-ion battery system based on highly pseudocapacitive hierarchical TiO2-B nanosheet assembled spheres (NS) cathode. This 2D cathode displayed exceptional pseudocapacitance (a maximum of 93%) specific capacity (303 mAh/g at 25 mA/g), rate performance (210 mAh/g at 1A/g), consistent cycling (retain ~100% capacity for 3000 cycles at 1A/g), coulombic efficiency (nearly 100%) and fast-charging (~12.
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