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Raman probing carbon&aqueous electrolytes interfaces and molecular dynamics simulations towards understanding electrochemical properties under polarization conditions in supercapacitors

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Journal of Energy Chemistry 2021年第9期30卷 279-292页

作者： Rafael Vicentini Leonardo M.Da Silva Débora V.Franco Willian G.Nunes juliane fiates Gustavo Doubek Luís F.M.Franco Renato G.Freitas Cristiano Fantini Hudson Zanin Advanced Energy Storage Division Carbon Sci-Tech LabsUniversity of CampinasAv Albert Einstein 400CampinasSP 13083-852Brazil Department of Chemistry Federal University of Jequitinhonha and Mucuri’s ValleyRodovia MGT 367km 5835000Alto da Jacuba39.100-000 DiamantinaMGBrazil Advanced Energy Storage Division Center for Innovation on New EnergiesLaboratory of Advanced BatteriesSchool of Chemical EngineeringUniversity of Campinas(UNICAMP)CampinasSP 13083-852Brazil Department of Chemistry Federal University of Mato GrossoICET-UFMT78060-900 CuiabáMTBrazil Departamento de Física ICExUniversidade Federal de Minas GeraisBelo HorizonteMG 31270-901Brazil

Raman probing of carbon electrode and electrolyte under dynamic conditions is performed here using different aqueous electrolytes to elucidate the fundamental events occurring in electrochemical supercapacitor during charge–discharge processes.The areal capacitance ranges from 1.54 to 2.31μF cm^(-2)μm and it is determined using different techniques.These findings indicate that the Helmholtz capacitance governs the overall charge-storage process instead of the space charge(quantum)capacitance commonly verified for HOPG electrodes in the range of~3 to 7μF cm^(-2).Molecular dynamics simulations are employed to elucidate the origin of the reversible Raman spectral changes during the charge–discharge processes.A correlation is verified between the reversible Raman shift and the surface excesses of the different ionic species.A theoretical framework is presented to relate the effect of the applied potential on the Raman shift and its correlation with the surface ionic charge.It is proposed that the Raman shift is governed by the interaction of solvated cations with graphite promoted by polarization conditions.It is the first time that a comparative study on different aqueous electrolyte p H and cation ion size has been performed tracking the Raman spectra change under dynamic polarization conditions and contrasting with comprehensive electrochemistry and dynamic molecular simulations studies.This study shines lights onto the charge-storage mechanism with evidence of Kohn anomaly reduction in the carbon electrode during the reversible adsorption/desorption and insertion/extraction of ionic species.

关键词： Defect reorganization in graphite Surface excess of charge Operando Raman studies Electrical double-layer capacitors

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