Solid-state Li-CO₂ batteries possess unique merits,including high environmental friendliness,extremely high energy density,and wide operational temperature range.In this work,we used the garnet-type Li₆.₄La₃Zr₁.₄Ta₀.₆...Solid-state Li-CO₂ batteries possess unique merits,including high environmental friendliness,extremely high energy density,and wide operational temperature range.In this work,we used the garnet-type Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂(LLZTO)as the solid electrolyte for Li-CO₂ batteries.By a simple solid-state reaction under vacuum,LLZTO was tightly composited with organic materials.Detailed analysis confirms that a three-in-one effect was achieved,resulting in additional Li⁺ migration pathways,improved mechanical properties of the electrolyte,and more active sites for Li₂CO₃ decomposition.This contributes to accelerated Li⁺ transport and fast CO₂reaction kinetics.A solid-state Li-CO₂ cell was assembled using a Ru@C cathode and an integrated layer of LLZTO@PVDF interfaced with an artificial molten salt.An exceptionally low charging overpotential(below 3.0 V)was achieved,maintaining a charge potential retention rate of over 99%.This work introduces LLZTO as a promising electrolyte for solid-state Li-CO₂ batteries,shedding light on the advancement of next-generation Li-CO₂ battery technologies.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(2232022A-06)National Natural Science Foundation of China(52372001)+1 种基金the Shanghai Natural Science Foundation(22ZR1400300)the Open Fund of Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province.
文摘Solid-state Li-CO₂ batteries possess unique merits,including high environmental friendliness,extremely high energy density,and wide operational temperature range.In this work,we used the garnet-type Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂(LLZTO)as the solid electrolyte for Li-CO₂ batteries.By a simple solid-state reaction under vacuum,LLZTO was tightly composited with organic materials.Detailed analysis confirms that a three-in-one effect was achieved,resulting in additional Li⁺ migration pathways,improved mechanical properties of the electrolyte,and more active sites for Li₂CO₃ decomposition.This contributes to accelerated Li⁺ transport and fast CO₂reaction kinetics.A solid-state Li-CO₂ cell was assembled using a Ru@C cathode and an integrated layer of LLZTO@PVDF interfaced with an artificial molten salt.An exceptionally low charging overpotential(below 3.0 V)was achieved,maintaining a charge potential retention rate of over 99%.This work introduces LLZTO as a promising electrolyte for solid-state Li-CO₂ batteries,shedding light on the advancement of next-generation Li-CO₂ battery technologies.