The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the m...The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the melting point,dominantly limits their applications in solid-state batteries(SSBs).Although the inorganic filler such as CeO_(2)nanoparticle content of composite solid polymer electrolytes(CSPEs)can significantly reduce the enormous charge transfer impedance at the Li metal/SPEs interface,we found that the required content of CeO_(2)nanoparticles in SPEs varies for achieving a decent interfacial charge transfer impedance and the bulk ionic conductivity in CSPEs.In this regard,a sandwich-type composited solid polymer electrolyte with a 10%CeO_(2)CSPEs interlayer sandwiched between two 50%CeO_(2)CSPEs thin layers(sandwiched CSPEs)is constructed to simultaneously achieve low charge transfer impedance and superior ionic conductivity at 30℃.The sandwiched CSPEs allow for stable cycling of Li plating and stripping for 1000 h with 129 mV polarized voltage at 0.1 mA cm^(-2)and 30℃.In addition,the LiFePO_(4)/Sandwiched CSPEs/Li cell also exhibits exceptional cycle performance at 30℃and even elevated120℃without short circuits.Constructing multi-layered CSPEs with optimized contents of the inorganic fillers can be an efficient method for developing all solid-state PEO-based batteries with high performance at a wide range of temperatures.展开更多
Despite being a leading candidate to meet stringent energy targets,lithium(Li) metal batteries(LMBs)face severe challenges at low temperatures such as dramatic increase in impedance,capacity loss and dendrite growth.U...Despite being a leading candidate to meet stringent energy targets,lithium(Li) metal batteries(LMBs)face severe challenges at low temperatures such as dramatic increase in impedance,capacity loss and dendrite growth.Unambiguously fingerprinting rate-limited factors of low-temperature LMBs would encourage targeted approaches to promote performances.Herein,the charge transfer impedance across solid electrolyte interphase(SEI) is identified to restrict battery operation under low temperature,and we propose a facile approach on the basis of ambiently fostering SEI(af-SEI) to facilitate charge transfer.The concept of af-SEI stems from kinetic benefits and structural merits to construct SEI at ambient temperature over low temperature developed SEI that is temporally consuming to achieve steady state and that is structurally defective to incur dendrite growth.The af-SEI allows ionically conductive and morphologically uniform layer on the anode surface,which exhibits a lower resistance and induces an even deposition of Li in the subsequent low temperature battery operation.Armed with af-SEI,the LMBs deliver the improved rate performance and prolonged cycle life when subjected to low temperature cycling.This work unveils the underlying causes that limit low temperature LMB performances,and enlightens the facile test protocols to build up favorable SEI,beyond scope of material and morphology design.展开更多
基金supported by the National Key R&D Program of China(2021YFB2400400)the National Natural Science Foundation of China(Grant No.22379120,22179085)+5 种基金the Key Research and Development Plan of Shanxi Province(China,Grant No.2018ZDXM-GY-135,2021JLM-36)the National Natural Science Foundation of China(Grant No.22108218)the“Young Talent Support Plan”of Xi’an Jiaotong University(71211201010723)the Qinchuangyuan Innovative Talent Project(QCYRCXM-2022-137)the“Young Talent Support Plan”of Xi’an Jiaotong University(HG6J003)the“1000-Plan program”of Shaanxi Province。
文摘The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the melting point,dominantly limits their applications in solid-state batteries(SSBs).Although the inorganic filler such as CeO_(2)nanoparticle content of composite solid polymer electrolytes(CSPEs)can significantly reduce the enormous charge transfer impedance at the Li metal/SPEs interface,we found that the required content of CeO_(2)nanoparticles in SPEs varies for achieving a decent interfacial charge transfer impedance and the bulk ionic conductivity in CSPEs.In this regard,a sandwich-type composited solid polymer electrolyte with a 10%CeO_(2)CSPEs interlayer sandwiched between two 50%CeO_(2)CSPEs thin layers(sandwiched CSPEs)is constructed to simultaneously achieve low charge transfer impedance and superior ionic conductivity at 30℃.The sandwiched CSPEs allow for stable cycling of Li plating and stripping for 1000 h with 129 mV polarized voltage at 0.1 mA cm^(-2)and 30℃.In addition,the LiFePO_(4)/Sandwiched CSPEs/Li cell also exhibits exceptional cycle performance at 30℃and even elevated120℃without short circuits.Constructing multi-layered CSPEs with optimized contents of the inorganic fillers can be an efficient method for developing all solid-state PEO-based batteries with high performance at a wide range of temperatures.
基金supported by the National Natural Science Foundation of China (22379121)Shenzhen Foundation Research Fund granted by the Shenzhen Science and Technology Innovation Committee (JCYJ20220530112812028)+1 种基金Fundamental Research Funds for the Central Universities (G2022KY0606)Zhejiang Province Key Laboratory of Flexible Electronics Open Fund (No. 2023FE005)。
文摘Despite being a leading candidate to meet stringent energy targets,lithium(Li) metal batteries(LMBs)face severe challenges at low temperatures such as dramatic increase in impedance,capacity loss and dendrite growth.Unambiguously fingerprinting rate-limited factors of low-temperature LMBs would encourage targeted approaches to promote performances.Herein,the charge transfer impedance across solid electrolyte interphase(SEI) is identified to restrict battery operation under low temperature,and we propose a facile approach on the basis of ambiently fostering SEI(af-SEI) to facilitate charge transfer.The concept of af-SEI stems from kinetic benefits and structural merits to construct SEI at ambient temperature over low temperature developed SEI that is temporally consuming to achieve steady state and that is structurally defective to incur dendrite growth.The af-SEI allows ionically conductive and morphologically uniform layer on the anode surface,which exhibits a lower resistance and induces an even deposition of Li in the subsequent low temperature battery operation.Armed with af-SEI,the LMBs deliver the improved rate performance and prolonged cycle life when subjected to low temperature cycling.This work unveils the underlying causes that limit low temperature LMB performances,and enlightens the facile test protocols to build up favorable SEI,beyond scope of material and morphology design.