“Bowling Collision Effect” of CoMo6 Polyoxometalate Units Enables Wide Temperature Range from ?20 to 60 °C and Dendrite Mitigation Li?S Batteries

The study explores Anderson?type polyoxometalates ([TMMo6O24]n?, TM = Co, Ni, Fe) as modified materials for Li?S battery separators, enhancing performance. CoMo6 units show optimal binding energy and Gibbs free energy, forming strong polar bonds with LiPSs. The resulting Li?S battery exhibits high capacity, excellent cycle life, and stability across ?20 to 60 °C, advancing high?performance, all?weather Li?S batteries.To improve the performance of Lithium?Sulfur (Li?S) batteries, the reaction catalysts of lithium polysulfides (LiPSs) reactions should have the characteristics of large surface area, efficient atomic utilization, high conductivity, small size, good stability, and strong adjustability. Herein, Anderson?type polyoxometalate ([TMMo6O24]n?, TM = Co, Ni, Fe, represented by TMMo6 POMs) are used as the modified materials for Li?S battery separator. By customizing the central metal atoms, this work gains insights into the layer?by?layer electron transfer mechanism between TMMo6 units and LiPSs, similar to the collision effect of a bowling ball. Theoretical analysis and in situ experimental characterization show that the changes of CoMo6 units with moderate binding energy and lowest Gibbs free energy result in the formation of robust polar bonds and prolonged S?S bonds after adsorption. Hence, the representative Li?S battery with CoMo6 and graphene composite modified separator has a high initial capacity of 1588.6 mA h g?1 at 0.2 C, excellent cycle performance of more than 3000 cycles at 5 C, and uniform Li+ transport over 1900 h. More importantly, this work has revealed the inherent contradiction between the kinetics and thermodynamics, achieving a stable cycle in the temperature range of ?20 to 60 °C.

» Publication Date: 03/08/2024

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This project has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement Nº 768737


                   




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