With the increasing demand for large-scale battery systems in electric vehicles（EVs） and smart renewable energy grids, organic materials including small molecules and polymers utilized as electrodes in rechargeable ...With the increasing demand for large-scale battery systems in electric vehicles（EVs） and smart renewable energy grids, organic materials including small molecules and polymers utilized as electrodes in rechargeable batteries have received increasing attraction. In recent years, two-dimensional（2D） organic materials possessing planar layered architecture exhibit optional chemical modification, high specific surface area as well as unique electrical/magnetic properties, which have been emerging as the promising functional materials for wide applications in optoelectronics, catalysis, sensing, etc. Integrating with high-density redox-active sites and hierarchical porous structure, significant achievements in 2D organic materials as cathode materials for alkali-metal-ion batteries have been witnessed. In this review, the recent progress in synthetic approaches, structure analyses, electrochemical characterizations of 2D organic materials as well as their application in alkali-metal-ion batteries containing lithium ion battery（LIB）, lithium sulfur battery（LSB）, lithium air battery（LAB） and sodium ion battery（SIB） are summarized systematically,and their current challenges including cycling stability and electron conductivity for cathode materials in battery fields are also discussed.展开更多
Organic cathodes for alkali-metal-ion batteries attract great attentions in recent years,but the ion storage sites are limited to some finite functional groups.This is because an organic cathode must have proper lowes...Organic cathodes for alkali-metal-ion batteries attract great attentions in recent years,but the ion storage sites are limited to some finite functional groups.This is because an organic cathode must have proper lowest unoccupied molecular orbitals(LUMO) to accept electrons at high potential.Herein,a novel type of organophosphate-based cathode has successfully been explored by tuning the LUMO energy level of organophosphates through metal ions with an inert electron pair.For the first time,the P=O of phytate(PA),N,N,N’,N’-ethylenediaminetetrakis(methylene phytate)(EDTMP),and diethylenetriaminepentakis(methyl phytate)(DTPMP) is activated by lead/bismuth(with 6s2electron pair) to storage Li/Na/K ions reversibly.Typically,density functional theory calculations indicate that the LUMO energy of Bi-PA is greatly reduced from-0.99(PA) to-4.61 eV,which shows the first discharge capacity of 173,182 and 206mAh·g-1and the reversibly capacity of 102,102 and 101mAh·g-1with the discharge platform of 2.4,2.1 and 2.4 V for Li/Na/K-ion battery cathodes,respectively.Similarly,with proper LUMO energy level,Pb-PA(-4.63 eV),Pb-EDTMP(-3.71 eV),and Pb-DTPMP(-4.45 eV) all exhibit admirable performance.This unique strategy of organic materials to alkali-metal-ion battery cathodes offers a new avenue for future energy storage systems.展开更多
基金the financial support from the 973 Programs of China(2013CBA01602)NSFC for Excellent Youth Scholars(51722304)+4 种基金NSFC(21720102002,21574080 and 61306018)Shanghai Committee of Science and Technology(15JC1490500,16JC1400703)and Open Project Program of the State Key Laboratory of Supramolecular Structure and Materials(sklssm201732,Jilin University)State Key Laboratory of Inorganic Synthesis and Preparative Chemistry(2016-08,Jilin University)State Key Laboratory for Mechanical Behavior of Materials(20161803,Xi’an Jiaotong University)
文摘With the increasing demand for large-scale battery systems in electric vehicles（EVs） and smart renewable energy grids, organic materials including small molecules and polymers utilized as electrodes in rechargeable batteries have received increasing attraction. In recent years, two-dimensional（2D） organic materials possessing planar layered architecture exhibit optional chemical modification, high specific surface area as well as unique electrical/magnetic properties, which have been emerging as the promising functional materials for wide applications in optoelectronics, catalysis, sensing, etc. Integrating with high-density redox-active sites and hierarchical porous structure, significant achievements in 2D organic materials as cathode materials for alkali-metal-ion batteries have been witnessed. In this review, the recent progress in synthetic approaches, structure analyses, electrochemical characterizations of 2D organic materials as well as their application in alkali-metal-ion batteries containing lithium ion battery（LIB）, lithium sulfur battery（LSB）, lithium air battery（LAB） and sodium ion battery（SIB） are summarized systematically,and their current challenges including cycling stability and electron conductivity for cathode materials in battery fields are also discussed.
基金financially supported by the Science and Technology Commission of Shanghai Municipality (No. 22ZR1471300)the National Science Foundation of China (Nos. 21871008,51922103 and 21801247)+1 种基金the Key Research Program of Chinese Academy of Sciences (No.QYZDJ-SSW-JSC013)China Postdoctoral Science Foundation (Nos.2020M671242 and 2021T140688)。
文摘Organic cathodes for alkali-metal-ion batteries attract great attentions in recent years,but the ion storage sites are limited to some finite functional groups.This is because an organic cathode must have proper lowest unoccupied molecular orbitals(LUMO) to accept electrons at high potential.Herein,a novel type of organophosphate-based cathode has successfully been explored by tuning the LUMO energy level of organophosphates through metal ions with an inert electron pair.For the first time,the P=O of phytate(PA),N,N,N’,N’-ethylenediaminetetrakis(methylene phytate)(EDTMP),and diethylenetriaminepentakis(methyl phytate)(DTPMP) is activated by lead/bismuth(with 6s2electron pair) to storage Li/Na/K ions reversibly.Typically,density functional theory calculations indicate that the LUMO energy of Bi-PA is greatly reduced from-0.99(PA) to-4.61 eV,which shows the first discharge capacity of 173,182 and 206mAh·g-1and the reversibly capacity of 102,102 and 101mAh·g-1with the discharge platform of 2.4,2.1 and 2.4 V for Li/Na/K-ion battery cathodes,respectively.Similarly,with proper LUMO energy level,Pb-PA(-4.63 eV),Pb-EDTMP(-3.71 eV),and Pb-DTPMP(-4.45 eV) all exhibit admirable performance.This unique strategy of organic materials to alkali-metal-ion battery cathodes offers a new avenue for future energy storage systems.
