Lithium-air battery has emerged as a viable electrochemical energy technology;yet a substantial overpotential is typically observed,due to the insulating nature of the discharge product Li_(2)O_(2) that hinders the re...Lithium-air battery has emerged as a viable electrochemical energy technology;yet a substantial overpotential is typically observed,due to the insulating nature of the discharge product Li_(2)O_(2) that hinders the reaction kinetics and device performance.Furthermore,finite solid–solid/-liquid interfaces are formed between Li_(2)O_(2) and catalysts and limit the activity of the electrocatalysts in battery reactions,leading to inadequate electrolytic efficiency.Herein,in-situ doping of Li_(2)O_(2) by select metal ions is found to significantly enhance the lithium-air battery performance,and Co^(2+)stands out as the most effective dopant among the series.This is ascribed to the unique catalytic activity of the resulting Co-O_(x) sites towards oxygen electrocatalysis,rendering the lithium-air battery self-catalytically active.Theoretical studies based on density functional theory calculations show that structural compression occurs upon Co^(2+)doping,which lowers the energy barrier of Li_(2)O_(2) decomposition.Results from this study highlight the significance of in situ electrochemical doping of the discharge product in enhancing the performance of lithium-air battery.展开更多
Regulation of the Li_(2)CO_(3) byproduct is the most critical challenge in the field of non-aqueous Li–O_(2) batteries.Although considerable efforts have been devoted to preventing Li_(2)CO_(3) formation,no approache...Regulation of the Li_(2)CO_(3) byproduct is the most critical challenge in the field of non-aqueous Li–O_(2) batteries.Although considerable efforts have been devoted to preventing Li_(2)CO_(3) formation,no approaches have suggested the ultimate solution of utilizing the clean Li_(2)O_(2) reaction instead of that of Li_(2)CO_(3).Even if extremely pure O_(2) is used in a Li–O_(2) cell,its complete elimination is impossible,eventually generating CO_(2) gas during charge.In this paper,we present the new concept of a CO_(2)-adsorbent spongy electrode(CASE),which is designed to trap the evolved CO_(2) using adsorption materials.Various candidates composed of amine functional groups(–NH2)for capturing CO_(2) were screened,with quadrapurebenzylamine(QPBZA)exhibiting superior CO_(2)-adsorbing ability among the proposed candidates.Accordingly,we fabricated the CASE by sandwiching QPBZA between porous carbon layers,which facilitated the transport of gaseous products.The new electrode was demonstrated to effectively capture the evolved CO_(2) during charge,therefore altering the reaction pathways to the ideal case.It is highly advantageous to mitigate the undesirable CO_(2) incorporation in the next discharge,resulting in improved cyclability.This novel concept of a CO_(2)-sponging electrode provides an alternative route to the realization of practically meaningful Li–O_(2) batteries.展开更多
The aprotic lithium-oxygen battery(Li-O_(2) battery) has attracted much attraction for the future advanced battery technologies due to its ultra-high theoretical energy density that can well meet the ever-growing ener...The aprotic lithium-oxygen battery(Li-O_(2) battery) has attracted much attraction for the future advanced battery technologies due to its ultra-high theoretical energy density that can well meet the ever-growing energy demand of portable electronic products,electric vehicles(EVs),smart grids,and so on [1-5].In principle.展开更多
A facile synthesis of Ag nanocrystals encapsulated in nitrogen-doped carbon fiber(NCF)is proposed,based on the simultaneous reaction between pyrrole and Ag^(+)ions in an aqueous solvent followed by a heat treatment.Th...A facile synthesis of Ag nanocrystals encapsulated in nitrogen-doped carbon fiber(NCF)is proposed,based on the simultaneous reaction between pyrrole and Ag^(+)ions in an aqueous solvent followed by a heat treatment.The as-prepared Ag/NCF demonstrated superior catalytic behavior toward ORR and OER.Besides improved cycling stability,a much lower discharge/charge gap of 0.89 V(vs Li/Li^(+))compared with 1.38 V for NCF cathode with a fixed capacity of 500 m Ah g^(-1)was obtained in lithium oxygen batteries.The introduction of Ag crystals into NCF facilitates the oxygen reduction reaction/oxygen evolution reaction kinetics.X-ray diffraction analysis coupled with Raman spectroscopy confirmed that Ag/NCF cathode could reversibly catalyze Li_(2)O_(2)formation and decomposition.The NCF matrix offers a conductive network to realize rapid mass transfer and the encapsulated Ag nanocrystals supplied effective catalytic active sites.The combined action between both contributes to the superior electrocatalytic performance.展开更多
A series of 20Li_(2)O-30V_(2)O_(5)-(50-x)SiO_(2)-xB_(2)O_(3)(mol.%)(x=10,20,30,40)glasses were prepared by the traditional melt-quenching synthesis.The amorphous nature of the glasses was determined by XRD,DSC and TEM...A series of 20Li_(2)O-30V_(2)O_(5)-(50-x)SiO_(2)-xB_(2)O_(3)(mol.%)(x=10,20,30,40)glasses were prepared by the traditional melt-quenching synthesis.The amorphous nature of the glasses was determined by XRD,DSC and TEM investigations.FTIR measurement revealed the functional group of obtained glasses.And EDS results confirmed the presence and uniform distribution of elements in the glasses.20Li_(2)O-30V_(2)O_(5)-40SiO_(2)-10B_(2)O_(3)(LVSB10)sample with the highest V^(4+) ratio exhibited the best cycling capacity.In order to further improve cycling stability of LVSB10 sample,ball milling was employed to reduce the particle size.The ball milled LVSB10 sample(LVSB10-b)showed an improved first discharge capacity,cycling stability and rate capacity.EIS measurements showed that ball milling can effectively decrease charge transfer impedance and facilitate Li^(+) ion diffusion.This work provides a new way to explore a new type of cathode materials for lithium ion batteries.展开更多
基金This project was supported by the National Natural Science Foundations of China (21771024,and 21871028)China Postdoctoral Science Foundation (2020M680430).
文摘Lithium-air battery has emerged as a viable electrochemical energy technology;yet a substantial overpotential is typically observed,due to the insulating nature of the discharge product Li_(2)O_(2) that hinders the reaction kinetics and device performance.Furthermore,finite solid–solid/-liquid interfaces are formed between Li_(2)O_(2) and catalysts and limit the activity of the electrocatalysts in battery reactions,leading to inadequate electrolytic efficiency.Herein,in-situ doping of Li_(2)O_(2) by select metal ions is found to significantly enhance the lithium-air battery performance,and Co^(2+)stands out as the most effective dopant among the series.This is ascribed to the unique catalytic activity of the resulting Co-O_(x) sites towards oxygen electrocatalysis,rendering the lithium-air battery self-catalytically active.Theoretical studies based on density functional theory calculations show that structural compression occurs upon Co^(2+)doping,which lowers the energy barrier of Li_(2)O_(2) decomposition.Results from this study highlight the significance of in situ electrochemical doping of the discharge product in enhancing the performance of lithium-air battery.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2021R1C1C1003628)the Development Program of Core Industrial Technology,funded by the Ministry of Trade,Industry&Energy of Korea(20012318)the institutional program of the Korea Institute of Science and Technology(2E31001)。
文摘Regulation of the Li_(2)CO_(3) byproduct is the most critical challenge in the field of non-aqueous Li–O_(2) batteries.Although considerable efforts have been devoted to preventing Li_(2)CO_(3) formation,no approaches have suggested the ultimate solution of utilizing the clean Li_(2)O_(2) reaction instead of that of Li_(2)CO_(3).Even if extremely pure O_(2) is used in a Li–O_(2) cell,its complete elimination is impossible,eventually generating CO_(2) gas during charge.In this paper,we present the new concept of a CO_(2)-adsorbent spongy electrode(CASE),which is designed to trap the evolved CO_(2) using adsorption materials.Various candidates composed of amine functional groups(–NH2)for capturing CO_(2) were screened,with quadrapurebenzylamine(QPBZA)exhibiting superior CO_(2)-adsorbing ability among the proposed candidates.Accordingly,we fabricated the CASE by sandwiching QPBZA between porous carbon layers,which facilitated the transport of gaseous products.The new electrode was demonstrated to effectively capture the evolved CO_(2) during charge,therefore altering the reaction pathways to the ideal case.It is highly advantageous to mitigate the undesirable CO_(2) incorporation in the next discharge,resulting in improved cyclability.This novel concept of a CO_(2)-sponging electrode provides an alternative route to the realization of practically meaningful Li–O_(2) batteries.
基金financial support from National Key R&D Program of China(Grant No.2016YFB0100100)the National Natural Science Foundation of China(Grant Nos.21972133 and 21805070)the Newton Advanced Fellowships(NAF/ R2/180603)。
文摘The aprotic lithium-oxygen battery(Li-O_(2) battery) has attracted much attraction for the future advanced battery technologies due to its ultra-high theoretical energy density that can well meet the ever-growing energy demand of portable electronic products,electric vehicles(EVs),smart grids,and so on [1-5].In principle.
基金financial support from an Australian Research Council(ARC)Discovery Project(DP180101453)The Distinguished Young Scientists Program of the National Natural Science Foundation of China(No.51425301)+1 种基金the National Natural Science Foundation of China(No.52002171,No.52002050)the Natural Science Foundation of Jiangsu Province(No.BK20200696,No.BK20200768,No.20KJB430019)are greatly appreciated
文摘A facile synthesis of Ag nanocrystals encapsulated in nitrogen-doped carbon fiber(NCF)is proposed,based on the simultaneous reaction between pyrrole and Ag^(+)ions in an aqueous solvent followed by a heat treatment.The as-prepared Ag/NCF demonstrated superior catalytic behavior toward ORR and OER.Besides improved cycling stability,a much lower discharge/charge gap of 0.89 V(vs Li/Li^(+))compared with 1.38 V for NCF cathode with a fixed capacity of 500 m Ah g^(-1)was obtained in lithium oxygen batteries.The introduction of Ag crystals into NCF facilitates the oxygen reduction reaction/oxygen evolution reaction kinetics.X-ray diffraction analysis coupled with Raman spectroscopy confirmed that Ag/NCF cathode could reversibly catalyze Li_(2)O_(2)formation and decomposition.The NCF matrix offers a conductive network to realize rapid mass transfer and the encapsulated Ag nanocrystals supplied effective catalytic active sites.The combined action between both contributes to the superior electrocatalytic performance.
基金support of National Natural Science Foundation of China(52171215)Tianjin Natural Science Foundation(19JCJQJC62400)Haihe Laboratory of Sustainable Chemical Transformations。
基金supported by the National Natural Science Foundation of China(52006208)the National Innovative Talents Program(GG2090007001)+2 种基金Chinese Academy of Sciences Program(KJ2090130001)USTC Startup Program(KY2090000044)USTC Tang Scholar(KY2090000065)。
基金financially supported by Shenzhen Basic Research Project Funds(JCYJ20170817161127616).
文摘A series of 20Li_(2)O-30V_(2)O_(5)-(50-x)SiO_(2)-xB_(2)O_(3)(mol.%)(x=10,20,30,40)glasses were prepared by the traditional melt-quenching synthesis.The amorphous nature of the glasses was determined by XRD,DSC and TEM investigations.FTIR measurement revealed the functional group of obtained glasses.And EDS results confirmed the presence and uniform distribution of elements in the glasses.20Li_(2)O-30V_(2)O_(5)-40SiO_(2)-10B_(2)O_(3)(LVSB10)sample with the highest V^(4+) ratio exhibited the best cycling capacity.In order to further improve cycling stability of LVSB10 sample,ball milling was employed to reduce the particle size.The ball milled LVSB10 sample(LVSB10-b)showed an improved first discharge capacity,cycling stability and rate capacity.EIS measurements showed that ball milling can effectively decrease charge transfer impedance and facilitate Li^(+) ion diffusion.This work provides a new way to explore a new type of cathode materials for lithium ion batteries.
