Experimental and density functional theory studies of laminar double-oxidized graphene oxide nanofiltration membranes

Solmaz Valizadeh, Leila Naji*, Mohammad Karimi, Saeedeh Sarabadani Tafreshi, Bas Heijman, Nora H. de Leeuw

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

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The type and loading level of oxygen-containing functional groups on graphene oxide (GO) nanosheets significantly affect the size and alignment of nanochannels formed between the GO nanosheets and the separation performance of laminar GO membranes. Here, we demonstrate how double-oxidation of GO leads to the higher surface charge of GO nanosheets, the formation of highly stable water-based GO solution, more-ordered deposition of GOs on the polyethersulfone membrane through the pressure-assisted self-assembly method, and the formation of highly durable GO membranes possessing smoother surface morphology and higher antifouling properties. A multi-technique investigation was applied to follow the physicochemical difference between GO and double-oxidized GO, and the physical stability and separation performance of the corresponding membranes using experimental and computational studies. The double-oxidized GO-based membranes provided a significantly high water flux of 230 L/(m2.h) in 2.5 bar transmembrane pressure, excellent rejection of 99.9% for methylene blue (MB) dye, and outstanding separation performance stability over time. In contrast, GO membranes showed rejection of 81.5% for MB, and their separation performance diminished significantly over time. The antifouling properties of double-oxidized GO membranes were substantially higher (∼ four times) due to their higher negative surface charge and smoother surface morphology. The density functional theory (DFT) was used to gain insight into the interactions between the functional groups and the reasoning for the higher mechanical stability of double-oxidized GO membranes. Results revealed that the formation energy of GO decreases by increasing the number density of functional groups. It was also found that a higher number of carboxyl groups at the edges of the double-oxidized GO leads to higher hydrogen bonding, higher binding energy, and a more stable GO-membrane structure.

Original languageEnglish
Pages (from-to)590-606
Number of pages17
JournalChemical Engineering Research and Design
Publication statusPublished - 2022

Bibliographical note

Green Open Access added to TU Delft Institutional Repository 'You share, we take care!' - Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.


  • Density Functional Theory (DFT)
  • Graphene oxide
  • Membrane separation
  • Morphology
  • Oxidation level

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