Oxygen functional groups (OFGs) in graphene oxide (GO) are responsible for its different properties and peculiar reactivity in water and different solvents. A detailed assignment, both theoretical and experimental, of OFGs is still missing, and a full reconstruction of GO electrochemical behavior remains unreached. The spatial localization of OFGs is expected to play an important role in the reduction process, but so far, this important aspect remains undisclosed in the literature. Here, the nature and interactions of adjacent OFGs have been investigated, shedding light on the energetics of their electrochemical reduction. GO chemical modifications upon modulated and controlled electrochemical reduction conditions have been studied, in order to excite and reveal the contribution from single reactive OFGs. The characterization has been conducted via X-ray photoelectron spectroscopic analysis supported by theoretical modelling, to compose a detailed picture of the various local environments participating to the rich chemistry of GO. As a result, the interplay between XPS, cyclic voltammetry and DFT computation allowed for a consistent parallel assessment of both the C 1s ionization energy and the electrochemical reduction potential of the various carbonaceous species of GO.
Understanding the nature of graphene oxide functional groups by modulation of the electrochemical reduction: a combined experimental and theoretical approach / Ferrari, Irene; Motta, Alessandro; Zanoni, Robertino; Scaramuzzo, FRANCESCA ANNA; Amato, Francesco; Dalchiele, Enrique A.; Marrani, Andrea Giacomo. - In: CARBON. - ISSN 0008-6223. - 203:(2022), pp. 29-38. [10.1016/j.carbon.2022.11.052]
Understanding the nature of graphene oxide functional groups by modulation of the electrochemical reduction: a combined experimental and theoretical approach
Irene Ferrari;Alessandro Motta;Robertino Zanoni;Francesca Anna Scaramuzzo;Francesco Amato;Andrea Giacomo Marrani
2022
Abstract
Oxygen functional groups (OFGs) in graphene oxide (GO) are responsible for its different properties and peculiar reactivity in water and different solvents. A detailed assignment, both theoretical and experimental, of OFGs is still missing, and a full reconstruction of GO electrochemical behavior remains unreached. The spatial localization of OFGs is expected to play an important role in the reduction process, but so far, this important aspect remains undisclosed in the literature. Here, the nature and interactions of adjacent OFGs have been investigated, shedding light on the energetics of their electrochemical reduction. GO chemical modifications upon modulated and controlled electrochemical reduction conditions have been studied, in order to excite and reveal the contribution from single reactive OFGs. The characterization has been conducted via X-ray photoelectron spectroscopic analysis supported by theoretical modelling, to compose a detailed picture of the various local environments participating to the rich chemistry of GO. As a result, the interplay between XPS, cyclic voltammetry and DFT computation allowed for a consistent parallel assessment of both the C 1s ionization energy and the electrochemical reduction potential of the various carbonaceous species of GO.File | Dimensione | Formato | |
---|---|---|---|
Ferrari_nature of graphene_2022.pdf
solo gestori archivio
Tipologia:
Documento in Post-print (versione successiva alla peer review e accettata per la pubblicazione)
Licenza:
Tutti i diritti riservati (All rights reserved)
Dimensione
1.79 MB
Formato
Adobe PDF
|
1.79 MB | Adobe PDF | Contatta l'autore |
I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.