Lithium metal batteries(LMBs)have emerged as pivotal energy storage solutions for electric vehicles and portable electronics.However,their operation under extreme conditions(high-temperature and fast-charging conditio...Lithium metal batteries(LMBs)have emerged as pivotal energy storage solutions for electric vehicles and portable electronics.However,their operation under extreme conditions(high-temperature and fast-charging conditions)faces significant challenges,including accelerated electrolyte decomposition,interfacial instability,and potential thermal runaway risks.To address these challenges,we present a solvation-interphase synergistic regulation strategy using 2-fluorobenzenesulfonamide(2-FBS)as a multifunctional electrolyte additive.The 2-FBS molecule effectively modulates the Li^(+)solvation structure by reducing the coordination of ethylene carbonate(EC)solvent.This transformation suppresses EC-induced parasitic reactions while scavenging superoxide radicals,thereby mitigating gas evolution at electrode interfaces.Upon preferential decomposition,2-FBS further promotes the formation of a robust LiF-Li_(3)N-Li_(2)S-rich interphase with exceptional mechanical strength(Young’s modulus:39.4 GPa).This inorganic-rich hybrid interphase simultaneously enables dendrite-free lithium plating and enhances cathode thermal stability.Consequently,2-FBS-modified electrolyte empowers LiCoO_(2)//Li cells to deliver 82.8%capacity retention after 800 cycles at 55°C and sustain 81.2%capacity retention after 1500 cycles at 4 C.Moreover,practical validation through nail penetration tests confirms the effectiveness of the electrolyte in preventing thermal propagation in fully charged pouch cells.This work establishes a paradigm for enabling reliable battery operation under extreme conditions through synergistic solvation and interphase engineering.展开更多
Ultralow-power non-volatile memristors are key elements in electronics.Generally,power reduction of memristors compromises data retention,a challenge known as the“power-retention dilemma,”due to the stochastic forma...Ultralow-power non-volatile memristors are key elements in electronics.Generally,power reduction of memristors compromises data retention,a challenge known as the“power-retention dilemma,”due to the stochastic formation of conductive dendrites in resistive-switching materials.Here,we report the results of conductive dendrite engineering in single-crystalline two-dimensional(2D)dielectrics in which directional control of filamentary distribution is possible.We find that the single-vacancy density(nSV)of single-crystalline hexagonal boron nitride(h-BN)plays an essential role in regulating conductive dendrite growth,supported by scanning joule expansion microscopy(SJEM).With optimized nSV,random dendrite growth is largely limited,and electrons hop between the neighboring Ag nanoclusters in vertical channels.The corresponding model was established to probe the relationship between nSV and memristor operating voltage.The conductive channel confinement in the vertical orientation contributes to long-retention non-volatile memristors with ultralow switch voltages(set:26 mV;reset:135 mV),excellent power efficiency(4 fW standby and a switching energy of 72 pJ)while keeping a high on/off resistance ratio of 108.Even at a record-low compliance current of 10 nA,memristors retains very robust nonvolatile,multiple resistive states with an operating voltage less than 120 mV(the per-transition power low as 900 pW).展开更多
基金supported by the Key Laboratory of Sichuan Province for Lithium Resources Comprehensive Utilization and New Lithium Based Materials for Advanced Battery Technology(LRMKF202405)the National Natural Science Foundation of China(52402226)the Sichuan Provincial Natural Science Foundation (2024NSFSC1016)
文摘Lithium metal batteries(LMBs)have emerged as pivotal energy storage solutions for electric vehicles and portable electronics.However,their operation under extreme conditions(high-temperature and fast-charging conditions)faces significant challenges,including accelerated electrolyte decomposition,interfacial instability,and potential thermal runaway risks.To address these challenges,we present a solvation-interphase synergistic regulation strategy using 2-fluorobenzenesulfonamide(2-FBS)as a multifunctional electrolyte additive.The 2-FBS molecule effectively modulates the Li^(+)solvation structure by reducing the coordination of ethylene carbonate(EC)solvent.This transformation suppresses EC-induced parasitic reactions while scavenging superoxide radicals,thereby mitigating gas evolution at electrode interfaces.Upon preferential decomposition,2-FBS further promotes the formation of a robust LiF-Li_(3)N-Li_(2)S-rich interphase with exceptional mechanical strength(Young’s modulus:39.4 GPa).This inorganic-rich hybrid interphase simultaneously enables dendrite-free lithium plating and enhances cathode thermal stability.Consequently,2-FBS-modified electrolyte empowers LiCoO_(2)//Li cells to deliver 82.8%capacity retention after 800 cycles at 55°C and sustain 81.2%capacity retention after 1500 cycles at 4 C.Moreover,practical validation through nail penetration tests confirms the effectiveness of the electrolyte in preventing thermal propagation in fully charged pouch cells.This work establishes a paradigm for enabling reliable battery operation under extreme conditions through synergistic solvation and interphase engineering.
基金support from NSFC(92264106,62090034,62104214,62122067,and 62261160574)the Research Grant Council of Hong Kong(CRS_PolyU502/22)+2 种基金the National Key R&D Program(2022YFA1204303)the NSFC of Zhejiang Province(DT23F0401 and DT23F040008)the Young Elite Scientists Sponsorship Program by CAST(2021QNRC001).
文摘Ultralow-power non-volatile memristors are key elements in electronics.Generally,power reduction of memristors compromises data retention,a challenge known as the“power-retention dilemma,”due to the stochastic formation of conductive dendrites in resistive-switching materials.Here,we report the results of conductive dendrite engineering in single-crystalline two-dimensional(2D)dielectrics in which directional control of filamentary distribution is possible.We find that the single-vacancy density(nSV)of single-crystalline hexagonal boron nitride(h-BN)plays an essential role in regulating conductive dendrite growth,supported by scanning joule expansion microscopy(SJEM).With optimized nSV,random dendrite growth is largely limited,and electrons hop between the neighboring Ag nanoclusters in vertical channels.The corresponding model was established to probe the relationship between nSV and memristor operating voltage.The conductive channel confinement in the vertical orientation contributes to long-retention non-volatile memristors with ultralow switch voltages(set:26 mV;reset:135 mV),excellent power efficiency(4 fW standby and a switching energy of 72 pJ)while keeping a high on/off resistance ratio of 108.Even at a record-low compliance current of 10 nA,memristors retains very robust nonvolatile,multiple resistive states with an operating voltage less than 120 mV(the per-transition power low as 900 pW).
