Li-air batteries have attracted extensive attention because of their ultrahigh theoretical energy density. However, the potential safety hazard of flammable organic liquid electrolytes hinders their practical applicat...Li-air batteries have attracted extensive attention because of their ultrahigh theoretical energy density. However, the potential safety hazard of flammable organic liquid electrolytes hinders their practical applications. Replacing liquid electrolytes with solidstate electrolytes(SSEs) is expected to fundamentally overcome the safety issues. In this work, we focus on the development and challenge of solid-state Li-air batteries(SSLABs). The rise of different types of SSEs, interfacial compatibility and verifiability in SSLABs are presented. The corresponding strategies and prospects of SSLABs are also proposed. In particular, combining machine learning method with experiment and in situ(or operando)techniques is imperative to accelerate the development of SSLABs.展开更多
Aprotic lithium-oxygen(Li-O_(2))batteries have a high theoretical energy density,but they face challenges such as cathode blockage,high charge overpotential,and poor cycling stability.These are caused by sluggish reac...Aprotic lithium-oxygen(Li-O_(2))batteries have a high theoretical energy density,but they face challenges such as cathode blockage,high charge overpotential,and poor cycling stability.These are caused by sluggish reaction kinetics and severe parasitic reactions.Enhancing the performance of Li-O_(2) batteries necessitates the development of efficient catalysts.These catalysts not only augment both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)but also inhibit undesirable parasitic reactions.In this work,we demonstrated for the first time a multifunctional soluble catalyst of iridium(III)acetylacetonate(Ir(acac)_(3))that could speed up oxygen electrochemistry.Ir(acac)_(3) regulated the ORR pathway and the reactivity of superoxide radical species by forming a reversible intermediate complex(Ir(acac)_(3)-O_(2)^(−)).During charging,Ir(acac)_(3) acted as a redox mediator and aided in Li_(2)O_(2) decomposition by reacting with superoxide intermediates.Moreover,as demonstrated by operando UV-visible spectroscopy,the lower charge potential significantly reduced the generation of highly reactive singlet oxygen(^(1)O_(2))intermediates.As a result,the Ir(acac)_(3)-mediated Li-O_(2) battery showed low overpotential,large capacity,and stable cyclability.This study offers a new approach to achieving efficient Li-O_(2) batteries and provides an opportunity to suppress parasitic reactions.展开更多
基金supported by National Key Research and Development Program of China (No.2021YFF0500600)NSFC (22279120)Key R&D projects in Henan Province (221111240100)。
文摘Li-air batteries have attracted extensive attention because of their ultrahigh theoretical energy density. However, the potential safety hazard of flammable organic liquid electrolytes hinders their practical applications. Replacing liquid electrolytes with solidstate electrolytes(SSEs) is expected to fundamentally overcome the safety issues. In this work, we focus on the development and challenge of solid-state Li-air batteries(SSLABs). The rise of different types of SSEs, interfacial compatibility and verifiability in SSLABs are presented. The corresponding strategies and prospects of SSLABs are also proposed. In particular, combining machine learning method with experiment and in situ(or operando)techniques is imperative to accelerate the development of SSLABs.
基金supported by the National Natural Science Foundation of China (NSFCgrant no.22202182).
文摘Aprotic lithium-oxygen(Li-O_(2))batteries have a high theoretical energy density,but they face challenges such as cathode blockage,high charge overpotential,and poor cycling stability.These are caused by sluggish reaction kinetics and severe parasitic reactions.Enhancing the performance of Li-O_(2) batteries necessitates the development of efficient catalysts.These catalysts not only augment both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)but also inhibit undesirable parasitic reactions.In this work,we demonstrated for the first time a multifunctional soluble catalyst of iridium(III)acetylacetonate(Ir(acac)_(3))that could speed up oxygen electrochemistry.Ir(acac)_(3) regulated the ORR pathway and the reactivity of superoxide radical species by forming a reversible intermediate complex(Ir(acac)_(3)-O_(2)^(−)).During charging,Ir(acac)_(3) acted as a redox mediator and aided in Li_(2)O_(2) decomposition by reacting with superoxide intermediates.Moreover,as demonstrated by operando UV-visible spectroscopy,the lower charge potential significantly reduced the generation of highly reactive singlet oxygen(^(1)O_(2))intermediates.As a result,the Ir(acac)_(3)-mediated Li-O_(2) battery showed low overpotential,large capacity,and stable cyclability.This study offers a new approach to achieving efficient Li-O_(2) batteries and provides an opportunity to suppress parasitic reactions.