Single-entity collisional electrochemistry(SECE)is a branch of single-entity electrochemistry.It can directly characterize entities/particles with single particle resolution through random collisions between particles...Single-entity collisional electrochemistry(SECE)is a branch of single-entity electrochemistry.It can directly characterize entities/particles with single particle resolution through random collisions between particles and electrodes in a solution,and obtain rich physicochemical information,thus becoming one of the frontiers of electroanalytical chemistry in the past two decades.Interestingly,the(micro/nanoscale)sensing electrodes have evolved from a polarizable liquid/liquid(mercury/liquid)interface to a solid/liquid interface and then to a liquid/liquid interface(i.e.,an interface between twoimmiscible electrolyte solutions,ITIES),as if they have completed a cycle(but in fact they have not).ITIES has become the latest sensing electrode in the booming SECE due to its polarizability(up to 1.1 V at the water/a,a,a-trifluorotoluene interface)and high reproducibility.The four measurement modes(direct electrolysis,mediated electrolysis,current blockade,and charge displacement)developed in the realm of SECE at solid/liquid interfaces have also been fully realized at the miniature ITIES.This article will discuss these four modes at the ITIES from the perspectives of basic concepts,operating mechanisms,and latest developments(e.g.,discovery of ionosomes,blockade effect of Faradaic ion transfer,etc.),and look forward to the future development and direction of this emerging field.展开更多
Lithium-oxygen batteries attract considerable attention due to exceptionally high theoretical energy density,while the development remains in its early stage.As is widely suggested,the solution mechanism induces great...Lithium-oxygen batteries attract considerable attention due to exceptionally high theoretical energy density,while the development remains in its early stage.As is widely suggested,the solution mechanism induces greater discharge capacity,while the surface mechanism induces greater cycle stability.Therefore,battery performance can be improved by adjusting the reaction mechanism.Previous studies predominantly focus on extremely thin or flat electrodes.In contrast,this work utilizes thick electrodes,emphasizing the importance of mass transport.Given that the electrolyte solvent is the main site of mass transport,the effects of two typical solvents on mass transport and battery performance are investigated:dimethyl sulfoxide with low viscosity and a high O_(2) diffusion rate and tetraethylene glycol dimethyl ether with high O_(2) solubility and high Li+transport capability.The results reveal a novel pathway for reaction mechanism induction where the mechanism varies with the spatial position of the electrode.As the spatial distribution of the electrode progresses,a layered appearance of solution mechanism products,transition state products,and surface mechanism products emerges,which is attributed to the increase in the mass transfer resistance.This work presents a distinct perspective on the way solvents influence reaction pathways and offers a new approach to regulating reaction pathways.展开更多
Lithium-ion batteries(LIBs)are an electrochemical energy storage technology that has been widely used for portable electrical devices,electric vehicles,and grid storage,etc.To satisfy the demand for user convenience e...Lithium-ion batteries(LIBs)are an electrochemical energy storage technology that has been widely used for portable electrical devices,electric vehicles,and grid storage,etc.To satisfy the demand for user convenience especially for electric vehicles,the development of a fast-charging technology for LIBs has become a critical focus.In commercial LIBs,the slow kinetics of Li+intercalation into the graphite anode from the electrolyte solution is known as the main restriction for fast-charging.We summarize the recent advances in obtaining fast-charging graphite-based anodes,mainly involving modifications of the electrolyte solution and graphite anode.Specifically,strategies for increasing the ionic conductivity and regulating the Li+solvation/desolvation state in the electrolyte solution,as well as optimizing the fabrication and the intrinsic activity of graphite-based anodes are discussed in detail.This review considers practical ways to obtain fast Li+intercalation kinetics into a graphite anode from the electrolyte as well as analysing progress in the commercialization of fast-charging LIBs.展开更多
基金supported by the National Natural Science Foundation of China(No.21904143).
文摘Single-entity collisional electrochemistry(SECE)is a branch of single-entity electrochemistry.It can directly characterize entities/particles with single particle resolution through random collisions between particles and electrodes in a solution,and obtain rich physicochemical information,thus becoming one of the frontiers of electroanalytical chemistry in the past two decades.Interestingly,the(micro/nanoscale)sensing electrodes have evolved from a polarizable liquid/liquid(mercury/liquid)interface to a solid/liquid interface and then to a liquid/liquid interface(i.e.,an interface between twoimmiscible electrolyte solutions,ITIES),as if they have completed a cycle(but in fact they have not).ITIES has become the latest sensing electrode in the booming SECE due to its polarizability(up to 1.1 V at the water/a,a,a-trifluorotoluene interface)and high reproducibility.The four measurement modes(direct electrolysis,mediated electrolysis,current blockade,and charge displacement)developed in the realm of SECE at solid/liquid interfaces have also been fully realized at the miniature ITIES.This article will discuss these four modes at the ITIES from the perspectives of basic concepts,operating mechanisms,and latest developments(e.g.,discovery of ionosomes,blockade effect of Faradaic ion transfer,etc.),and look forward to the future development and direction of this emerging field.
基金supported by the National Natural Science Foundation of China(52376080 and 52306122)the Anhui Provincial Natural Science Foundation(2308085QE174)+3 种基金the China Postdoctoral Science Foundation(2023TQ0346)the Postdoctoral Fellowship Program of CPSF(GZC20232522)the Fundamental Research Funds for the Central Universities(WK2090000057)the Students’Innovation and Entrepreneurship Foundation of USTC(CY2023C008).
文摘Lithium-oxygen batteries attract considerable attention due to exceptionally high theoretical energy density,while the development remains in its early stage.As is widely suggested,the solution mechanism induces greater discharge capacity,while the surface mechanism induces greater cycle stability.Therefore,battery performance can be improved by adjusting the reaction mechanism.Previous studies predominantly focus on extremely thin or flat electrodes.In contrast,this work utilizes thick electrodes,emphasizing the importance of mass transport.Given that the electrolyte solvent is the main site of mass transport,the effects of two typical solvents on mass transport and battery performance are investigated:dimethyl sulfoxide with low viscosity and a high O_(2) diffusion rate and tetraethylene glycol dimethyl ether with high O_(2) solubility and high Li+transport capability.The results reveal a novel pathway for reaction mechanism induction where the mechanism varies with the spatial position of the electrode.As the spatial distribution of the electrode progresses,a layered appearance of solution mechanism products,transition state products,and surface mechanism products emerges,which is attributed to the increase in the mass transfer resistance.This work presents a distinct perspective on the way solvents influence reaction pathways and offers a new approach to regulating reaction pathways.
文摘Lithium-ion batteries(LIBs)are an electrochemical energy storage technology that has been widely used for portable electrical devices,electric vehicles,and grid storage,etc.To satisfy the demand for user convenience especially for electric vehicles,the development of a fast-charging technology for LIBs has become a critical focus.In commercial LIBs,the slow kinetics of Li+intercalation into the graphite anode from the electrolyte solution is known as the main restriction for fast-charging.We summarize the recent advances in obtaining fast-charging graphite-based anodes,mainly involving modifications of the electrolyte solution and graphite anode.Specifically,strategies for increasing the ionic conductivity and regulating the Li+solvation/desolvation state in the electrolyte solution,as well as optimizing the fabrication and the intrinsic activity of graphite-based anodes are discussed in detail.This review considers practical ways to obtain fast Li+intercalation kinetics into a graphite anode from the electrolyte as well as analysing progress in the commercialization of fast-charging LIBs.
