Despite its potential as a high-capacity battery electrode,magnesium(Mg)metals are highly susceptible to electrolytes,resulting in the formation of unwanted passivation layers,which hinder charge transfer phenomena.He...Despite its potential as a high-capacity battery electrode,magnesium(Mg)metals are highly susceptible to electrolytes,resulting in the formation of unwanted passivation layers,which hinder charge transfer phenomena.Here,we first report an anionic covalent organic framework(a-COF)as an electrostatic molecular rectifier(that can preferentially trap solvent molecules)to stabilize Mg metal electrodes.Compared to a neutral COF(n-COF)as a control sample,the a-COF enhances Mg^(2+)transport by facilitating the desolvation of Mg^(2+)-solvent complexes and cationic mobility through its negatively charged one-dimensional columns,thereby achieving an ionic conductivity eight times higher than that of the n-COF.In addition,the anionic porous frameworks in contact with Mg metal electrodes enable a uniform Mg^(2+)flux and interfacial stability with Mg metal electrodes.Consequently,the a-COF exhibited reversible Mg plating/stripping cyclability on Mg metal electrodes compared to the n-COF,demonstrating the electrochemical viability of the anionic frameworks for Mg metal electrode stabilization.展开更多
基金supported by the Technology Innovation Program(grant no.20012216)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by the Basic Science Research Program(grant nos.22021R1A2B5B03001615,2018M3D1A1058744)through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT and future Planning.
文摘Despite its potential as a high-capacity battery electrode,magnesium(Mg)metals are highly susceptible to electrolytes,resulting in the formation of unwanted passivation layers,which hinder charge transfer phenomena.Here,we first report an anionic covalent organic framework(a-COF)as an electrostatic molecular rectifier(that can preferentially trap solvent molecules)to stabilize Mg metal electrodes.Compared to a neutral COF(n-COF)as a control sample,the a-COF enhances Mg^(2+)transport by facilitating the desolvation of Mg^(2+)-solvent complexes and cationic mobility through its negatively charged one-dimensional columns,thereby achieving an ionic conductivity eight times higher than that of the n-COF.In addition,the anionic porous frameworks in contact with Mg metal electrodes enable a uniform Mg^(2+)flux and interfacial stability with Mg metal electrodes.Consequently,the a-COF exhibited reversible Mg plating/stripping cyclability on Mg metal electrodes compared to the n-COF,demonstrating the electrochemical viability of the anionic frameworks for Mg metal electrode stabilization.
