Understanding the microscopic structure and thermodynamic properties of electrode/electrolyte interfaces is central to the rational design of electric-double-layer capacitors(EDLCs).Whereas practical applications ofte...Understanding the microscopic structure and thermodynamic properties of electrode/electrolyte interfaces is central to the rational design of electric-double-layer capacitors(EDLCs).Whereas practical applications often entail electrodes with complicated pore structures,theoretical studies are mostly restricted to EDLCs of simple geometry such as planar or slit pores ignoring the curvature effects of the electrode surface.Significant gaps exist regarding the EDLC performance and the interfacial structure.Herein the classical density functional theory(CDFT)is used to study the capacitance and interfacial behavior of spherical electric double layers within a coarse-grained model.The capacitive performance is associated with electrode curvature,surface potential,and electrolyte concentration and can be correlated with a regression-tree(RT)model.The combination of CDFT with machine-learning methods provides a promising quantitative framework useful for the computational screening of porous electrodes and novel electrolytes.展开更多
基金sponsored by the National Natural Science Foundation of China(Nos.91834301,21908053,and 21808055)Shanghai Sailing Program(19YF1411700)financial support from the Fluid Interface Reactions,Structures and Transport(FIRST)Center,an Energy Frontier Research Center funded by the U.S.Department of Energy,Office of Basic Energy Sciences。
文摘Understanding the microscopic structure and thermodynamic properties of electrode/electrolyte interfaces is central to the rational design of electric-double-layer capacitors(EDLCs).Whereas practical applications often entail electrodes with complicated pore structures,theoretical studies are mostly restricted to EDLCs of simple geometry such as planar or slit pores ignoring the curvature effects of the electrode surface.Significant gaps exist regarding the EDLC performance and the interfacial structure.Herein the classical density functional theory(CDFT)is used to study the capacitance and interfacial behavior of spherical electric double layers within a coarse-grained model.The capacitive performance is associated with electrode curvature,surface potential,and electrolyte concentration and can be correlated with a regression-tree(RT)model.The combination of CDFT with machine-learning methods provides a promising quantitative framework useful for the computational screening of porous electrodes and novel electrolytes.
