Garnet-based all-solid-state lithium batteries(ASSLBs)were considered as the most promising energy storage device due to their high energy density and good safety.However,interface problems caused by impurities such a...Garnet-based all-solid-state lithium batteries(ASSLBs)were considered as the most promising energy storage device due to their high energy density and good safety.However,interface problems caused by impurities such as Li_(2)CO_(3) on the surface still hinder the practical application of garnet-based ASSLBs.Here,we use a simple ultrasonic spraying method to coat SiO_(2) on the Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)surface,and in-situ construct Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si5 nano-multifunctional interlayer through the high-temperature conversion reaction of SiO_(2).Experiments and density functional theory(DFT)calculations demonstrate that the introduced Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si_(5) nano-multifunctional interlayer at the LLZTO/Li interface can significantly improve the air stability and interface contact of LLZTO/Li.As a result,the interface impedance of Li/SiO_(2)@LLZTO/Li was reduced to 24.2Ωcm^(-2),and it can operate stably over 2400 and 1000 h at current densities of 0.05 and 0.2 mA cm^(−2),respectively.The full cell assembled with LiFePO_(4)(LFP)as cathode(Li/SiO_(2)@LLZTO/LFP)also exhibits excellent cycling performance(capacity retention rate of 95%after 50 cycles at 0.1 C)and rate performance(140 mAh g^(−1) at 0.1 C and 107 mAh g−1 at 1 C).This research provides a strategy to improve interface problems and achieve dendrite-free ASSLBs through in-situ transformation constructed nano-multifunctional interlayers.展开更多
Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prosp...Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prospects of high-entropy materials with high structural disorder and strong component controllability in the field of electrochemical energy storage,herein,a novel high-entropy garnet-type oxide solid electrolyte,Li_(5.75)Ga_(0.25)La_(3)Zr_(0.5)Ti_(0.5)Sn_(0.5)Nb_(0.5)O_(12)(LGLZTSNO)was constructed by partially replacing the Li and Zr sites in Li_(7)La_(3)Zr_(2)O_(12)with Ga and Ti/Sn/Nb elements,respectively.The experimental and density functional theory(DFT)calculation results show that the high-entropy LGLZTSNO electrolyte has preferable room temperature ion conductivity,air stability,interface contact performance with lithium anode,and the ability to suppress lithium dendrites.Thanks to the improvement of electrolyte performance,the critical current density of Li/Ag@LGLZTSNO/Li symmetric cell was increased from 0.42 to 1.57 mA cm^(−2),and the interface area specific impedance(IASR)was reduced from 765.2 to 42.3Ωcm^(2).Meanwhile,the Li/Ag@LGLZTSNO/LFP full cell also exhibits excellent rate performance and cycling performance(148 mA h g^(−1)at 0.1 C and 124 mA h g^(−1)at 0.5 C,capacity retention up to 84.8%after 100 cycles at 0.1 C),showing the application prospects of high-entropy LGLZTSNO solid electrolyte in high-performance all solid state lithium batteries.展开更多
Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment.Herein,a new gel polymer electrolyte(GPE)co...Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment.Herein,a new gel polymer electrolyte(GPE)containing NH_(2)-MIL-53(Al),[PP_(13)][TFSI],LiTFSI,and PVDF-HFP was prepared using a simple method of solution casting.The effects of encapsulating different ratios of ionic liquid([PP_(13)][TFSI])into the micropores of functionalized metal-organic frameworks(NH_(2)-MIL-53(Al))on the electrochemical properties were compared.XRD,SEM,nitrogen adsorption-desorption isotherms,and electrochemical measurements were conducted.This GPE demonstrates a superior ionic conductivity of 8.08×10^(-4)S·cm^(-1)at 60℃and can sustain a discharge specific capacity of 156.6 mA·h·g^(-1)at 0.2 C for over 100 cycles.This work might offer a potential approach to alleviate the solid-solid contact with the solid-state electrolyte and electrodes and broaden a new window for the creation of all-solid-state batteries.展开更多
All-solid-state lithium metal batteries(ASSLMBs)are emerging as a groundbreaking solution,offering higher energy and power densities along with improved safety compared to conventional lithium-ion systems.However,crit...All-solid-state lithium metal batteries(ASSLMBs)are emerging as a groundbreaking solution,offering higher energy and power densities along with improved safety compared to conventional lithium-ion systems.However,critical challenges remain-particularly the instability at the interface between solid-state electrolytes(SSEs)and lithium metal,and the growth of lithium dendrites.展开更多
For all-solid-state lithium batteries(ASSLBs),polymer-blended solid composite electrolytes(SCEs)have drawn wide interest owing to their significance in improving the interfacial solid-solid contacts and inhibiting the...For all-solid-state lithium batteries(ASSLBs),polymer-blended solid composite electrolytes(SCEs)have drawn wide interest owing to their significance in improving the interfacial solid-solid contacts and inhibiting the growth of lithium dendrites.In this work,SCEs based on PVDF-HFP/PMMA matrix containing MOFs(NH2-MIL-53(Al))and LiTFSI were designed and synthesized employing an easy solution casting method.The synthesized samples were examined by XRD,SEM,EDS,and electrochemical tests.It was found that MPP-2 SCE not only has excellent ionic conductivity at 60℃of 5.54×10^(−4)S cm^(−1),but also exhibits superior interfacial compatibility in Li||Li symmetric batteries,which can constantly cycle for about 800 h at 0.1 mA cm^(−2)with no short-circuiting.The assembled Li|MPP-2|LiFePO4 cell exhibited a first discharge specific capacity of up to 157.1 mAh g^(−1)at 60℃and 0.2 C.This work may help to further advance the progress of ASSLBs in the future.展开更多
基金The Key Research and Development Project of Hainan Province(No.ZDYF2022SHFZ093)sHainan Provincial Natural Science Foundation of China(No.120RC455)+1 种基金the Natural Science Foundation of China(No.61901142)the Program of Hainan Association for Science and Technology Plans to Youth R&D Innovation(No.QCXM202014)are acknowledged.
文摘Garnet-based all-solid-state lithium batteries(ASSLBs)were considered as the most promising energy storage device due to their high energy density and good safety.However,interface problems caused by impurities such as Li_(2)CO_(3) on the surface still hinder the practical application of garnet-based ASSLBs.Here,we use a simple ultrasonic spraying method to coat SiO_(2) on the Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)surface,and in-situ construct Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si5 nano-multifunctional interlayer through the high-temperature conversion reaction of SiO_(2).Experiments and density functional theory(DFT)calculations demonstrate that the introduced Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si_(5) nano-multifunctional interlayer at the LLZTO/Li interface can significantly improve the air stability and interface contact of LLZTO/Li.As a result,the interface impedance of Li/SiO_(2)@LLZTO/Li was reduced to 24.2Ωcm^(-2),and it can operate stably over 2400 and 1000 h at current densities of 0.05 and 0.2 mA cm^(−2),respectively.The full cell assembled with LiFePO_(4)(LFP)as cathode(Li/SiO_(2)@LLZTO/LFP)also exhibits excellent cycling performance(capacity retention rate of 95%after 50 cycles at 0.1 C)and rate performance(140 mAh g^(−1) at 0.1 C and 107 mAh g−1 at 1 C).This research provides a strategy to improve interface problems and achieve dendrite-free ASSLBs through in-situ transformation constructed nano-multifunctional interlayers.
基金supported by the Natural Science Foundation of China(61901142)the Key Research and Development Project of Hainan Province(ZDYF2022SHFZ093).
文摘Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prospects of high-entropy materials with high structural disorder and strong component controllability in the field of electrochemical energy storage,herein,a novel high-entropy garnet-type oxide solid electrolyte,Li_(5.75)Ga_(0.25)La_(3)Zr_(0.5)Ti_(0.5)Sn_(0.5)Nb_(0.5)O_(12)(LGLZTSNO)was constructed by partially replacing the Li and Zr sites in Li_(7)La_(3)Zr_(2)O_(12)with Ga and Ti/Sn/Nb elements,respectively.The experimental and density functional theory(DFT)calculation results show that the high-entropy LGLZTSNO electrolyte has preferable room temperature ion conductivity,air stability,interface contact performance with lithium anode,and the ability to suppress lithium dendrites.Thanks to the improvement of electrolyte performance,the critical current density of Li/Ag@LGLZTSNO/Li symmetric cell was increased from 0.42 to 1.57 mA cm^(−2),and the interface area specific impedance(IASR)was reduced from 765.2 to 42.3Ωcm^(2).Meanwhile,the Li/Ag@LGLZTSNO/LFP full cell also exhibits excellent rate performance and cycling performance(148 mA h g^(−1)at 0.1 C and 124 mA h g^(−1)at 0.5 C,capacity retention up to 84.8%after 100 cycles at 0.1 C),showing the application prospects of high-entropy LGLZTSNO solid electrolyte in high-performance all solid state lithium batteries.
基金financially supported by National Natural Science Foundation of China(21701083)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_3137)。
文摘Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment.Herein,a new gel polymer electrolyte(GPE)containing NH_(2)-MIL-53(Al),[PP_(13)][TFSI],LiTFSI,and PVDF-HFP was prepared using a simple method of solution casting.The effects of encapsulating different ratios of ionic liquid([PP_(13)][TFSI])into the micropores of functionalized metal-organic frameworks(NH_(2)-MIL-53(Al))on the electrochemical properties were compared.XRD,SEM,nitrogen adsorption-desorption isotherms,and electrochemical measurements were conducted.This GPE demonstrates a superior ionic conductivity of 8.08×10^(-4)S·cm^(-1)at 60℃and can sustain a discharge specific capacity of 156.6 mA·h·g^(-1)at 0.2 C for over 100 cycles.This work might offer a potential approach to alleviate the solid-solid contact with the solid-state electrolyte and electrodes and broaden a new window for the creation of all-solid-state batteries.
文摘All-solid-state lithium metal batteries(ASSLMBs)are emerging as a groundbreaking solution,offering higher energy and power densities along with improved safety compared to conventional lithium-ion systems.However,critical challenges remain-particularly the instability at the interface between solid-state electrolytes(SSEs)and lithium metal,and the growth of lithium dendrites.
基金supported by National Natural Science Foundation of China(grant Nos.21701083,22179054)The Ministry of Science and Technology of the People's Republic of China(grant No.G2023014022L)Jiangsu Provincial Key Research and Development Program(grant No.BZ2023010).
文摘For all-solid-state lithium batteries(ASSLBs),polymer-blended solid composite electrolytes(SCEs)have drawn wide interest owing to their significance in improving the interfacial solid-solid contacts and inhibiting the growth of lithium dendrites.In this work,SCEs based on PVDF-HFP/PMMA matrix containing MOFs(NH2-MIL-53(Al))and LiTFSI were designed and synthesized employing an easy solution casting method.The synthesized samples were examined by XRD,SEM,EDS,and electrochemical tests.It was found that MPP-2 SCE not only has excellent ionic conductivity at 60℃of 5.54×10^(−4)S cm^(−1),but also exhibits superior interfacial compatibility in Li||Li symmetric batteries,which can constantly cycle for about 800 h at 0.1 mA cm^(−2)with no short-circuiting.The assembled Li|MPP-2|LiFePO4 cell exhibited a first discharge specific capacity of up to 157.1 mAh g^(−1)at 60℃and 0.2 C.This work may help to further advance the progress of ASSLBs in the future.
