Ion effects on molecular interaction between graphene oxide and organic molecules

Zilong Liu*, Tatiana Rios-Carvajal, Martin P. Andersson, Marcel Ceccato, Susan L. S. Stipp, Tue Hassenkam

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Interactions between graphene oxide (GO) and organic molecules play a role in processes such as environmental remediation and water treatment. However, little is known about underlying molecular level processes with the presence of ions. In this study, we utilized atomic force microscopy (AFM) in chemical force mapping (CFM) mode to directly probe their adhesion interactions. AFM tips were functionalised to serve as models for nonpolar and polar organic molecules, i.e. with alkyl, -CH3, and carboxyl, -COO(H). For experiments with -COO(H) tips, adhesion between GO and tips decreased in the order: Ba2+ > Ca2+ > Mg2+ > Na+, whereas for the -CH3 tips, ion dependent adhesion was relatively low but followed the same: Ba2+ > Ca2+ > Mg2+ ≈ Na+. Calculations with Derjaguin-Landau-Verwey-Overbeek (DLVO) theory and the Schulze-Hardy rule could not account for the observations. We propose that ion bridging plays a definitive role in adhesion between -COO(H) tips and the GO surface. This is consistent with proposed models with density functional theory (DFT) calculations. Adhesion of -CH3 tips is a response to the hydrophilic interactions and the ion dependent part is suggested to arise from ion bridging between slightly negative charged -CH3 tips and the GO surface. High pH had a notable influence on the adhesion of the -COO(H) tip but a negligible effect on the -CH3 tip. These results offer important insights into interactions between solutions and mineral surfaces with adsorbed organic molecules.

Original languageEnglish
JournalEnvironmental Science: Nano
Volume6
Issue number7
Pages (from-to)2281-2291
ISSN2051-8153
DOIs
Publication statusPublished - 2019

Cite this

Liu, Zilong ; Rios-Carvajal, Tatiana ; Andersson, Martin P. ; Ceccato, Marcel ; Stipp, Susan L. S. ; Hassenkam, Tue. / Ion effects on molecular interaction between graphene oxide and organic molecules. In: Environmental Science: Nano. 2019 ; Vol. 6, No. 7. pp. 2281-2291.
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abstract = "Interactions between graphene oxide (GO) and organic molecules play a role in processes such as environmental remediation and water treatment. However, little is known about underlying molecular level processes with the presence of ions. In this study, we utilized atomic force microscopy (AFM) in chemical force mapping (CFM) mode to directly probe their adhesion interactions. AFM tips were functionalised to serve as models for nonpolar and polar organic molecules, i.e. with alkyl, -CH3, and carboxyl, -COO(H). For experiments with -COO(H) tips, adhesion between GO and tips decreased in the order: Ba2+ > Ca2+ > Mg2+ > Na+, whereas for the -CH3 tips, ion dependent adhesion was relatively low but followed the same: Ba2+ > Ca2+ > Mg2+ ≈ Na+. Calculations with Derjaguin-Landau-Verwey-Overbeek (DLVO) theory and the Schulze-Hardy rule could not account for the observations. We propose that ion bridging plays a definitive role in adhesion between -COO(H) tips and the GO surface. This is consistent with proposed models with density functional theory (DFT) calculations. Adhesion of -CH3 tips is a response to the hydrophilic interactions and the ion dependent part is suggested to arise from ion bridging between slightly negative charged -CH3 tips and the GO surface. High pH had a notable influence on the adhesion of the -COO(H) tip but a negligible effect on the -CH3 tip. These results offer important insights into interactions between solutions and mineral surfaces with adsorbed organic molecules.",
author = "Zilong Liu and Tatiana Rios-Carvajal and Andersson, {Martin P.} and Marcel Ceccato and Stipp, {Susan L. S.} and Tue Hassenkam",
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Liu, Z, Rios-Carvajal, T, Andersson, MP, Ceccato, M, Stipp, SLS & Hassenkam, T 2019, 'Ion effects on molecular interaction between graphene oxide and organic molecules', Environmental Science: Nano, vol. 6, no. 7, pp. 2281-2291. https://doi.org/10.1039/c9en00274j

Ion effects on molecular interaction between graphene oxide and organic molecules. / Liu, Zilong; Rios-Carvajal, Tatiana; Andersson, Martin P.; Ceccato, Marcel; Stipp, Susan L. S.; Hassenkam, Tue.

In: Environmental Science: Nano, Vol. 6, No. 7, 2019, p. 2281-2291.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Ion effects on molecular interaction between graphene oxide and organic molecules

AU - Liu, Zilong

AU - Rios-Carvajal, Tatiana

AU - Andersson, Martin P.

AU - Ceccato, Marcel

AU - Stipp, Susan L. S.

AU - Hassenkam, Tue

PY - 2019

Y1 - 2019

N2 - Interactions between graphene oxide (GO) and organic molecules play a role in processes such as environmental remediation and water treatment. However, little is known about underlying molecular level processes with the presence of ions. In this study, we utilized atomic force microscopy (AFM) in chemical force mapping (CFM) mode to directly probe their adhesion interactions. AFM tips were functionalised to serve as models for nonpolar and polar organic molecules, i.e. with alkyl, -CH3, and carboxyl, -COO(H). For experiments with -COO(H) tips, adhesion between GO and tips decreased in the order: Ba2+ > Ca2+ > Mg2+ > Na+, whereas for the -CH3 tips, ion dependent adhesion was relatively low but followed the same: Ba2+ > Ca2+ > Mg2+ ≈ Na+. Calculations with Derjaguin-Landau-Verwey-Overbeek (DLVO) theory and the Schulze-Hardy rule could not account for the observations. We propose that ion bridging plays a definitive role in adhesion between -COO(H) tips and the GO surface. This is consistent with proposed models with density functional theory (DFT) calculations. Adhesion of -CH3 tips is a response to the hydrophilic interactions and the ion dependent part is suggested to arise from ion bridging between slightly negative charged -CH3 tips and the GO surface. High pH had a notable influence on the adhesion of the -COO(H) tip but a negligible effect on the -CH3 tip. These results offer important insights into interactions between solutions and mineral surfaces with adsorbed organic molecules.

AB - Interactions between graphene oxide (GO) and organic molecules play a role in processes such as environmental remediation and water treatment. However, little is known about underlying molecular level processes with the presence of ions. In this study, we utilized atomic force microscopy (AFM) in chemical force mapping (CFM) mode to directly probe their adhesion interactions. AFM tips were functionalised to serve as models for nonpolar and polar organic molecules, i.e. with alkyl, -CH3, and carboxyl, -COO(H). For experiments with -COO(H) tips, adhesion between GO and tips decreased in the order: Ba2+ > Ca2+ > Mg2+ > Na+, whereas for the -CH3 tips, ion dependent adhesion was relatively low but followed the same: Ba2+ > Ca2+ > Mg2+ ≈ Na+. Calculations with Derjaguin-Landau-Verwey-Overbeek (DLVO) theory and the Schulze-Hardy rule could not account for the observations. We propose that ion bridging plays a definitive role in adhesion between -COO(H) tips and the GO surface. This is consistent with proposed models with density functional theory (DFT) calculations. Adhesion of -CH3 tips is a response to the hydrophilic interactions and the ion dependent part is suggested to arise from ion bridging between slightly negative charged -CH3 tips and the GO surface. High pH had a notable influence on the adhesion of the -COO(H) tip but a negligible effect on the -CH3 tip. These results offer important insights into interactions between solutions and mineral surfaces with adsorbed organic molecules.

U2 - 10.1039/c9en00274j

DO - 10.1039/c9en00274j

M3 - Journal article

AN - SCOPUS:85069051426

VL - 6

SP - 2281

EP - 2291

JO - Environmental Science: Nano

JF - Environmental Science: Nano

SN - 2051-8153

IS - 7

ER -