Metal-sulfur batteries have received great attention for electrochemical energy storage due to high theoretical capacity and low cost, but their further development is impeded by low sulfur utilization, poor electrochemical kinetics, and serious shuttle effect of the sulfur cathode. To avoid these problems, herein, a triple-synergistic small-molecule sulfur cathode is designed by employing N, S co-doped hierarchical porous bamboo charcoal as a sulfur host in an aqueous Cu-S battery. Expect the enhanced conductivity and chemisorption induced by N, S synergistic co-doping, the intrinsic synergy of macro-/meso-/microporous triple structure also ensures space-confined small-molecule sulfur as high utilization reactant and effectively alleviates the volume expansion during conversion reaction. Under a further joint synergy between hierarchical structure and heteroatom doping, the resulting sulfur cathode endows the Cu-S battery with outstanding electrochemical performance. Cycled at 5 A g, it can deliver a high reversible capacity of 2,509.8 mAh g with a good capacity retention of 97.9% after 800 cycles. In addition, a flexible hybrid pouch cell built by a small-molecule sulfur cathode, Zn anode, and gel electrolytes can firmly deliver high average operating voltage of about 1.3 V with a reversible capacity of over 2,500 mAh g under various destructive conditions, suggesting that the triple-synergistic small-molecule sulfur cathode promises energetic metal-sulfur batteries.
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http://dx.doi.org/10.1073/pnas.2312091120 | DOI Listing |
Chem Sci
December 2024
Department of Chemistry, Northeastern University Shenyang 110819 China
Aqueous Zn-S batteries provide competitive energy density for large-scale energy storage systems. However, the cathode active material exhibits poor electrical conductivity especially at the discharged state of ZnS. Its morphology generated in cells thus directly determines the cathode electrochemical activity.
View Article and Find Full Text PDFChemistry
December 2024
Dalian University of Technology, No.2 Linggong Road, Ganjingzi District, Dalian, CHINA.
Sulfur-rich copolymers have gained a great deal of attention as promising cathode materials in Li-S batteries due to their low cost and naturally uniform sulfur dispersion. However, the poor electrical conductivity and shuttle effect cause rapid capacity decay and low sulfur utilization especially under high sulfur loading and low electrolyte/sulfur ratio. Herein, the Fe1-xS/C dispersed and Se-containing sulfur-rich polymer (FSP) was synthesized by one-pot reaction of ferrocene, trithioiynuric acid with SexSy.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Huazhong University of Science and Technology - Main Campus: Huazhong University of Science and Technology, Materials Science and Engineering, CHINA.
Sulfurized polyacrylonitrile (SPAN) presents an opportunity to replace elemental sulfur as a "shuttle-free" cathode for secondary Li-S batteries, which can be an ideal choice for stationary energy storage due to its abundance, low cost, and sustainability. The electrolyte options for the state-of-the-art SPAN batteries have been limited to the flammable carbonate and ether ones, which raises safety concerns. Here, we explored the use of a non-flammable acetonitrile (AN) electrolyte for SPAN battery for the first time and identified the irreversible cleavage of C-S bonds of SPAN as the main reason for the failure of SPAN in AN electrolyte.
View Article and Find Full Text PDFSmall
December 2024
Institute of Photoelectronic Thin Film Devices and Technology, Renewable Energy Conversion and Storage Center, State Key Laboratory of Photovoltaic Materials and Cells, Nankai University, Tianjin, 300350, P. R. China.
Photovoltaic-driven electrochemical (PV-EC) carbon dioxide reduction (COR) coupled with sulfide oxidation (SOR) can efficiently convert the solar energy into chemical energy, expanding its applications. However, developing low-cost electrocatalysts that exhibit high selectivity and efficiency for both COR and SOR remains a challenge. Herein, a bifunctional copper selenide catalyst is developed with copper vacancies (v-CuSe) for the COR-SOR.
View Article and Find Full Text PDFSmall
December 2024
School of Physical Science and Technology, Lanzhou University, 222 South Tianshui Road, Lanzhou, 730000, China.
Well-designed structures of the electrocatalyst provide excellent catalytic activity and high structural stability during the sulfur reduction reaction of Lithium-sulfur batteries (LSBs). In this study, a novel and efficient structure is developed to encapsulate bimetallic FeCo nanoalloy catalysts within N-doped carbon nanotube (NCNT) on carbon nanofibers (FeCo@NCNT/CNFs) using a combination of electrospinning and rapid-cooling techniques. The NCNT matrix with abundant sites not only serves as a high pathway for electron transport during the reaction, but its encapsulation structure also acts as armor to protect the FeCo nanoalloy.
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