Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyze...Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyzes the effect of the electrolyte-to-sulfur(E/S) ratios on battery energy density and the challenges for sulfur reduction reactions(SRR) under lean electrolyte conditions. Accordingly, we review the use of various polar transition metal sulfur hosts as corresponding solutions to facilitate SRR kinetics at low E/S ratios(< 10 μL mg~(-1)), and the strengths and limitations of different transition metal compounds are presented and discussed from a fundamental perspective. Subsequently, three promising strategies for sulfur hosts that act as anchors and catalysts are proposed to boost lean electrolyte Li–S battery performance. Finally, an outlook is provided to guide future research on high energy density Li–S batteries.展开更多
Heat is almost everywhere.Unlike electricity,which can be easily manipulated,the current ability to control heat is still highly limited owing to spontaneous thermal dissipation imposed by the second law of thermodyna...Heat is almost everywhere.Unlike electricity,which can be easily manipulated,the current ability to control heat is still highly limited owing to spontaneous thermal dissipation imposed by the second law of thermodynamics.Optical illumination and pressure have been used to switch endothermic/exothermic responses of materials via phase transitions;however,these strategies are less cost-effective and unscalable.Here,we spectroscopically demonstrate the glassy crystal state of 2-amino-2-methyl-1,3-propanediol(AMP)to realize an affordable,easily manageable approach for thermal energy recycling.The supercooled state of AMP is so sensitive to pressure that even several megapascals can induce crystallization to the ordered crystal,resulting in a substantial temperature increase of 48 K within 20 s.Furthermore,we demonstrate a proof-of-concept device capable of programable heating with an extremely high work-to-heat conversion effi-ciency of383.Such delicate and efficient tuning of heat may remarkably facilitate rational utilization of waste heat.展开更多
High sulphur loading and lean electrolyte conditions are important to achieve the high theoretical energy density of lithiumsulphur(Li-S)batteries.However,serious problems such as low sulphur utilization and fast capa...High sulphur loading and lean electrolyte conditions are important to achieve the high theoretical energy density of lithiumsulphur(Li-S)batteries.However,serious problems such as low sulphur utilization and fast capacity fade are typically experienced under low electrolyte/sulphur(E/S)ratios and high sulphur loading conditions.To address these issues,a cobaltcontaining three-dimensional conductive honeycomb(Co@N-HPC)is proposed in this work as a material for sulphur cathodes.The good electrical conductivity and high density of catalytic sites of(Co@N-HPC)allow fast redox kinetics of lithium polysulfide(LiPS)in high-sulphur-loading electrodes.In addition,the hierarchical structure and good wettability by the electrolyte of Co@NHPC facilitates electrolyte penetration and LiPS conversion,leading to a high utilization of sulphur under lean electrolyte conditions.Therefore,at a current density of 0.2 C,a volumetric capacity of 1,410 mAh·cm^(−3)was attained with a sulphur loading of 5.1 mg·cm^(−2)and an E/S ratio of 5μL·mg^(−1).This work provides ideas for the development of lean electrolyte Li-S batteries with a high sulphur loading.展开更多
基金the Research Foundation-Flanders (FWO) for a Research Project (G0B3218N)the financial support by the National Natural Science Foundation of China (22005054)+3 种基金Natural Science Foundation of Fujian Province (2021J01149)State Key Laboratory of Structural Chemistry (20200007)Sichuan Science and Technology Program (project No.: 2022ZYD0016 and 2023JDRC0013)the National Natural Science Foundation of China (project No. 21776120)。
文摘Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyzes the effect of the electrolyte-to-sulfur(E/S) ratios on battery energy density and the challenges for sulfur reduction reactions(SRR) under lean electrolyte conditions. Accordingly, we review the use of various polar transition metal sulfur hosts as corresponding solutions to facilitate SRR kinetics at low E/S ratios(< 10 μL mg~(-1)), and the strengths and limitations of different transition metal compounds are presented and discussed from a fundamental perspective. Subsequently, three promising strategies for sulfur hosts that act as anchors and catalysts are proposed to boost lean electrolyte Li–S battery performance. Finally, an outlook is provided to guide future research on high energy density Li–S batteries.
基金The work conducted in the Institute of Metal Research was supported by the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(grant no.ZDBS-LY-JSC002)the Liaoning Provincial Science Fund for Distinguished Young Scholars(grant no.2023JH6/100500003)+7 种基金the Innovation Fund of Institute of Metal Research,Chinese Academy of Sciences,(grant no.2021-ZD01)the CSNS Consortium on High-performance Materials of the Chinese Academy of Sciences,the Young Innovation Talent Program of Shenyang(grant no.RC210432)the Ministry of Science and Technology of the People’s Republic of China(grant nos.2021YFB3501201,2022YFE0109900,and 2020YFA0406002)the National Natural Science Foundation of China(grant nos.11934007,52001101,and 61974147)the International Partner Program of Chinese Academy of Sciences(grant no.174321KYSB20200008)J.L.and M.W.are grateful for the Research Foundation Flanders(grant no.G0B3218N)J.Luo acknowledges Sichuan Science and Technology Program(grant nos.2022ZYD0016 and 2023JDRC0013)National Natural Science Foundation of China(grant nos.21776120 and 22378270).The authors thank Sucheng Wang and Changji Li for their help with the in situ XRD experiments,Shuai Huang for thermal infrared image measurements,and Bo Huang for sample deuteration.They also thank Prof.Jie Pan and Prof.Si Lan for valuable discussions.
文摘Heat is almost everywhere.Unlike electricity,which can be easily manipulated,the current ability to control heat is still highly limited owing to spontaneous thermal dissipation imposed by the second law of thermodynamics.Optical illumination and pressure have been used to switch endothermic/exothermic responses of materials via phase transitions;however,these strategies are less cost-effective and unscalable.Here,we spectroscopically demonstrate the glassy crystal state of 2-amino-2-methyl-1,3-propanediol(AMP)to realize an affordable,easily manageable approach for thermal energy recycling.The supercooled state of AMP is so sensitive to pressure that even several megapascals can induce crystallization to the ordered crystal,resulting in a substantial temperature increase of 48 K within 20 s.Furthermore,we demonstrate a proof-of-concept device capable of programable heating with an extremely high work-to-heat conversion effi-ciency of383.Such delicate and efficient tuning of heat may remarkably facilitate rational utilization of waste heat.
基金M.W.and J.S.L.acknowledge the Research Foundation-Flanders(FWO)for a Research Project(No.G0B3218N)and a Research Grant(No.1529816N)J.S.L.,Z.B.C.,and M.W.acknowledge the financial support by the National Natural Science Foundation of China(Nos.21776120 and 22005054)H.P.is grateful to the China Scholarship Council.Funding from State Key Laboratory of Structural Chemistry,and the Natural Science Foundation of Fujian Province(No.2021J01149)is also acknowledged.
文摘High sulphur loading and lean electrolyte conditions are important to achieve the high theoretical energy density of lithiumsulphur(Li-S)batteries.However,serious problems such as low sulphur utilization and fast capacity fade are typically experienced under low electrolyte/sulphur(E/S)ratios and high sulphur loading conditions.To address these issues,a cobaltcontaining three-dimensional conductive honeycomb(Co@N-HPC)is proposed in this work as a material for sulphur cathodes.The good electrical conductivity and high density of catalytic sites of(Co@N-HPC)allow fast redox kinetics of lithium polysulfide(LiPS)in high-sulphur-loading electrodes.In addition,the hierarchical structure and good wettability by the electrolyte of Co@NHPC facilitates electrolyte penetration and LiPS conversion,leading to a high utilization of sulphur under lean electrolyte conditions.Therefore,at a current density of 0.2 C,a volumetric capacity of 1,410 mAh·cm^(−3)was attained with a sulphur loading of 5.1 mg·cm^(−2)and an E/S ratio of 5μL·mg^(−1).This work provides ideas for the development of lean electrolyte Li-S batteries with a high sulphur loading.