The“shuttle effect”of lithium polysulfides(LiPSs)is a huge challenge for practical use of high-energydensity lithium-sulfur(Li-S)batteries,and one of the main reasons is the sluggish kinetics of sulfur conversion.Me...The“shuttle effect”of lithium polysulfides(LiPSs)is a huge challenge for practical use of high-energydensity lithium-sulfur(Li-S)batteries,and one of the main reasons is the sluggish kinetics of sulfur conversion.Metal oxides are able to expedite the sulfur electrochemistry,and the structural defects enhance the adsorption-conversion ability of metal oxides for polysulfides.However,a significant research gap still remains regarding the relationship between the oxygen vacancy concentration and the adsorptivecatalytic performance of metal oxides.Herein,we establish a correlation between oxygen vacancy concentration and adsorptive-catalytic properties by using tungsten oxide(WO_(x))as model catalysts.It is revealed that high-concentration oxygen vacancy is beneficial for enhancing the binding between tungsten oxide and LiPSs,reducing the energy barrier of Li_(2)S decomposition,and promoting polysulfide conversion kinetics.Consequently,the Li-S batteries using the tungsten oxide with high-concentration oxygen vacancies deliver high initial discharge capacity of 1169 mA h g^(-1)at 0.2 C and 865 mA h g^(-1)at 2 C,low attenuation rate of 0.064%per cycle over 1100 cycles at 2 C.With a high sulfur area loading of 5.34 mg cm^(-2),the Li-S batteries still exhibit high initial gravimetric capacity of 982 mA h g^(-1)at 0.1 C and areal capacity of 5.92 mA h cm^(-2).This work promotes the feasibility of defect engineering on metal oxides as an effective mean to enhance the practicality of Li-S batteries.展开更多
基金financially supported by National Natural Science Foundation of China(Grant Nos.51972070 and 52062004)Guizhou Provincial High Level Innovative Talents Project(Grant No.QKHPTRC-GCC[2022]013-1)+2 种基金Innovation Team for Advanced Electrochemical Energy Storage Devices and Key Materials of Guizhou Provincial Higher Education Institutions(Grant No.QianJiaoJi[2023]054)Guizhou Provincial Science and Technology Projects(Grant No.QKHJC[2020]1Z042)Cultivation Project of Guizhou University(Grant No.GDPY[2019]01)。
文摘The“shuttle effect”of lithium polysulfides(LiPSs)is a huge challenge for practical use of high-energydensity lithium-sulfur(Li-S)batteries,and one of the main reasons is the sluggish kinetics of sulfur conversion.Metal oxides are able to expedite the sulfur electrochemistry,and the structural defects enhance the adsorption-conversion ability of metal oxides for polysulfides.However,a significant research gap still remains regarding the relationship between the oxygen vacancy concentration and the adsorptivecatalytic performance of metal oxides.Herein,we establish a correlation between oxygen vacancy concentration and adsorptive-catalytic properties by using tungsten oxide(WO_(x))as model catalysts.It is revealed that high-concentration oxygen vacancy is beneficial for enhancing the binding between tungsten oxide and LiPSs,reducing the energy barrier of Li_(2)S decomposition,and promoting polysulfide conversion kinetics.Consequently,the Li-S batteries using the tungsten oxide with high-concentration oxygen vacancies deliver high initial discharge capacity of 1169 mA h g^(-1)at 0.2 C and 865 mA h g^(-1)at 2 C,low attenuation rate of 0.064%per cycle over 1100 cycles at 2 C.With a high sulfur area loading of 5.34 mg cm^(-2),the Li-S batteries still exhibit high initial gravimetric capacity of 982 mA h g^(-1)at 0.1 C and areal capacity of 5.92 mA h cm^(-2).This work promotes the feasibility of defect engineering on metal oxides as an effective mean to enhance the practicality of Li-S batteries.