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electrochemical route to holey graphene nanosheets

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D.F. Carrasco, J.I. Paredes, S. Villar-Rodil et al. Carbon 195 (2022) 57e68 power density of ~600 W kg1 (see corresponding cyclic voltam- mograms and galvanostatic profiles in Fig. S10). This behavior was most likely due to the particular electrode configuration used for the present measurements, in which the holey graphene materials were heavily compacted under high pressure to a density of ~1.6 g cm3. Such an extensive compaction acts as a barrier to the transport of ions within the electrode, even in the presence of holes in the NSs, thus yielding limited performance metrics. Still, the benefits of using the electrochemically derived holey graphene over its Hummers-based counterpart were made apparent even with this electrode configuration. Future work in our laboratory will focus on exploiting such benefits for the development of high performance electrodes, e.g., by processing the electrochemical holey graphene into lower density, three-dimensional aerogels. 4. Conclusions For the first time, highly oxidized graphene obtained by an electrochemical exfoliation approach was shown to be a convenient alternative to the more prevalent standard graphene oxides derived from common oxidation strategies (e.g., Hummers method) as a precursor for the preparation of holey graphene NSs. Comparison of two different highly oxidized graphenes, made by the electro- chemical and Hummers routes but having the same extent of oxidation, revealed the former route to afford NSs with larger ar- omatic areas and, consequently, with smaller and denser oxidized domains. When these two graphenes were used to generate holey NSs based on the selective etching of their oxidized domains, such structural differences led to holey products with distinct charac- teristics, namely, the created holes tended to be smaller and more uniform in the electrochemically derived material. As an electrode for electrochemical charge storage, this new type of holey graphene exhibited some advantages relative to its standard graphene oxide- based counterpart, which translated into improved capacity and energy density values. Finally, it is anticipated that applications other than electrochemical charge storage can benefit from the present electrochemically derived holey graphene. For example, the ability to generate holes in the NSs with more uniform di- mensions could be exploited in (bio)molecular separation mem- branes that outperform those based on standard graphene oxides. CRediT authorship contribution statement D.F. Carrasco: Investigation, Data curation, Validation. J.I. Par- edes: Funding acquisition, Resources, Project administration, Su- pervision, Conceptualization, Methodology, Validation, Writing e original draft, Writing e review & editing. S. Villar-Rodil: Investi- gation, Data curation, Validation, Formal analysis, Visualization, Writing e review & editing. F. Suarez-García: Funding acquisition, Resources, Investigation, Data curation, Formal analysis. A. Martí- nez-Alonso: Funding acquisition, Resources. J.M.D. Tascon: Fund- ing acquisition, Resources. Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Acknowledgements Funding by the Spanish Ministerio de Ciencia, Innovacion y Universidades (MICINN), Agencia Estatal de Investigacion (AEI) and the European Regional Development Fund (ERDF) through project RTI2018-100832-B-I00, as well as by Plan de Ciencia, Tecnología e Innovacion (PCTI) 2013e2017 and 2018e2022 del Principado de Asturias and the ERDF (projects IDI/2018/000233 and IDI/2021/ 000037) is gratefully acknowledged. Appendix A. 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