The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano i...The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of∼35 nm is designed accurately by magnetron sputtering technology to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously“attacking”the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby significantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of electrolyte/Li anode interface promotes the homogeneous deposition of Li^(+)and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO_(4)|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9%for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs.展开更多
本文利用气体组分及大气气溶胶在线监测系统(MARGA ADI 2080)观测武汉市2018年1月9—26日大气气溶胶中的8种水溶性离子(NH_(4)^(+)、NO_(3)^(-)、SO_(4)^(2-)、Cl^(-)、K^(+)、Ca^(2+)、Na^(+)和Mg^(2+)),结合气象要素数据,使用主成分分...本文利用气体组分及大气气溶胶在线监测系统(MARGA ADI 2080)观测武汉市2018年1月9—26日大气气溶胶中的8种水溶性离子(NH_(4)^(+)、NO_(3)^(-)、SO_(4)^(2-)、Cl^(-)、K^(+)、Ca^(2+)、Na^(+)和Mg^(2+)),结合气象要素数据,使用主成分分析(PCA)、正定矩阵因子分析法(PMF)、HYSPLIT后向轨迹模式、潜在源区贡献(PSCF)和浓度权重轨迹(CWT),对霾污染过程中水溶性离子进行了全面的来源解析,探究了霾不同阶段下来源差异和空间分布特征。结果表明:(1)本次霾污染中的8种水溶性离子和4种污染气体,PCA解析出的源和占比分别为二次源和燃煤源的混合源(41.28%)、工业排放和土壤扬尘混合源(27.73%)和机动车排放源(9.63%),PMF解析出的源和占比分别为燃煤与土壤扬尘混合源(18.57%)、机动车排放源(20.74%)、二次源(18.30%)、光化学污染源(22.24%)和燃煤源(20.15%)。(2)霾在不同阶段下水溶性离子和4种污染气体的来源存在差异,在清洁天和霾消散阶段,光化学的贡献最高,占比分别为31.42%和36.07%;在霾发生阶段燃煤与土壤扬尘源的贡献最高,其贡献为40.94%;在霾发展阶段,最大的控制源为二次源,贡献占比为37.51%。(3)此次武汉市霾污染中PM_(2.5)浓度和NH_(4)^(+)、NO_(3)^(-)和SO_(4)^(2-)的潜在源区为皖豫鄂三省和赣湘鄂三省交界处。霾污染中PM_(2.5)的主要影响范围是武汉市南部和北部省份,NO_(3)^(-)、NH_(4)^(+)和SO_(4)^(2-)的主要影响区域为武汉市东北方向的城市、湖南省和江西省。展开更多
All-solid-state lithium(Li)metal batteries(ASSLMBs)are considered one of the most promising secondary batteries due to their high theoretical capacity and high safety performance.However,low room-temperature ionic con...All-solid-state lithium(Li)metal batteries(ASSLMBs)are considered one of the most promising secondary batteries due to their high theoretical capacity and high safety performance.However,low room-temperature ionic conductivity and poor interfacial stability are two key factors affecting the practical application of ASSLMBs,and our understanding of the mechanisms behind these key problems from microscopic perspective is still limited.In this review,the mechanisms and advanced characterization techniques of ASSLMBs are summarized to correlate the microstructures and properties.Firstly,we summarize the challenges faced by solid polymer electrolytes(SPEs)in ASSLMBs,such as the low roomtemperature ionic conductivity and the poor interfacial stability.Secondly,several typical improvement methods of polymer ASSLMBs are discussed,including composite SPEs,ultra-thin SPEs,SPEs surface modification and Li anode surface modification.Finally,we conclude the characterizations for correlating the microstructures and the properties of SPEs,with emphasis on the use of emerging advanced techniques(e.g.,cryo-transmission electron microscopy)for in-depth analyzing ASSLMBs.The influence of the microstructures on the properties is very important.Until now,it has been difficult for us to understand the microstructures of batteries.However,some recent studies have demonstrated that we have a better understanding of the microstructures of batteries.Then we suggest that in situ characterization,nondestructive characterization and sub-angstrom resolution are the key technologies to help us further understand the batteries'microstructures and promote the development of batteries.And potential investigations to understand the microstructures evolution and the batteries behaviors are also prospected to expect further reasonable theoretical guidance for the design of ASSLMBs with ideal performance.展开更多
基金supported by the National Natural Science Foundation of China(22279116 and U20A20253)the Natural Science Foundationof Zhejiang Province(LD22E020006 and LQ24E020012)+3 种基金the Science and Technology Development of Zhejiang Province(2023C01231 and 2024C01095)the Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation(LBMHD24E020001)the China Postdoctoral Science Foundation(2020M671785 and 2020T130597)the Fundamental Research Funds for the Provincial Universities of Zhejiang(2022YW54).
文摘The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of∼35 nm is designed accurately by magnetron sputtering technology to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously“attacking”the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby significantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of electrolyte/Li anode interface promotes the homogeneous deposition of Li^(+)and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO_(4)|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9%for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs.
文摘本文利用气体组分及大气气溶胶在线监测系统(MARGA ADI 2080)观测武汉市2018年1月9—26日大气气溶胶中的8种水溶性离子(NH_(4)^(+)、NO_(3)^(-)、SO_(4)^(2-)、Cl^(-)、K^(+)、Ca^(2+)、Na^(+)和Mg^(2+)),结合气象要素数据,使用主成分分析(PCA)、正定矩阵因子分析法(PMF)、HYSPLIT后向轨迹模式、潜在源区贡献(PSCF)和浓度权重轨迹(CWT),对霾污染过程中水溶性离子进行了全面的来源解析,探究了霾不同阶段下来源差异和空间分布特征。结果表明:(1)本次霾污染中的8种水溶性离子和4种污染气体,PCA解析出的源和占比分别为二次源和燃煤源的混合源(41.28%)、工业排放和土壤扬尘混合源(27.73%)和机动车排放源(9.63%),PMF解析出的源和占比分别为燃煤与土壤扬尘混合源(18.57%)、机动车排放源(20.74%)、二次源(18.30%)、光化学污染源(22.24%)和燃煤源(20.15%)。(2)霾在不同阶段下水溶性离子和4种污染气体的来源存在差异,在清洁天和霾消散阶段,光化学的贡献最高,占比分别为31.42%和36.07%;在霾发生阶段燃煤与土壤扬尘源的贡献最高,其贡献为40.94%;在霾发展阶段,最大的控制源为二次源,贡献占比为37.51%。(3)此次武汉市霾污染中PM_(2.5)浓度和NH_(4)^(+)、NO_(3)^(-)和SO_(4)^(2-)的潜在源区为皖豫鄂三省和赣湘鄂三省交界处。霾污染中PM_(2.5)的主要影响范围是武汉市南部和北部省份,NO_(3)^(-)、NH_(4)^(+)和SO_(4)^(2-)的主要影响区域为武汉市东北方向的城市、湖南省和江西省。
基金financial support from the National Key R&D Program of China (grant 2022YFB3807700)the National Natural Science Foundation of China (grants 52171225,52102314,52225208,51972285 and U21A20174)the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang (grant 2020R01002)。
文摘All-solid-state lithium(Li)metal batteries(ASSLMBs)are considered one of the most promising secondary batteries due to their high theoretical capacity and high safety performance.However,low room-temperature ionic conductivity and poor interfacial stability are two key factors affecting the practical application of ASSLMBs,and our understanding of the mechanisms behind these key problems from microscopic perspective is still limited.In this review,the mechanisms and advanced characterization techniques of ASSLMBs are summarized to correlate the microstructures and properties.Firstly,we summarize the challenges faced by solid polymer electrolytes(SPEs)in ASSLMBs,such as the low roomtemperature ionic conductivity and the poor interfacial stability.Secondly,several typical improvement methods of polymer ASSLMBs are discussed,including composite SPEs,ultra-thin SPEs,SPEs surface modification and Li anode surface modification.Finally,we conclude the characterizations for correlating the microstructures and the properties of SPEs,with emphasis on the use of emerging advanced techniques(e.g.,cryo-transmission electron microscopy)for in-depth analyzing ASSLMBs.The influence of the microstructures on the properties is very important.Until now,it has been difficult for us to understand the microstructures of batteries.However,some recent studies have demonstrated that we have a better understanding of the microstructures of batteries.Then we suggest that in situ characterization,nondestructive characterization and sub-angstrom resolution are the key technologies to help us further understand the batteries'microstructures and promote the development of batteries.And potential investigations to understand the microstructures evolution and the batteries behaviors are also prospected to expect further reasonable theoretical guidance for the design of ASSLMBs with ideal performance.
