Dynamics of Micropollutant Adsorption to Polystyrene Surfaces Probed by Angle-Resolved Second Harmonic Scattering

William T. S. Cole; Haoyun Wei; Son C. Nguyen; Charles B. Harris; Daniel J. Miller; Richard J. Saykally

doi:10.1021/acs.jpcc.9b01146

Dynamics of Micropollutant Adsorption to Polystyrene Surfaces Probed by Angle-Resolved Second Harmonic Scattering

William T. S. Cole, Haoyun Wei, Son C. Nguyen, Charles B. Harris, Daniel J. Miller, Richard J. Saykally

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

Angle-resolved second harmonic scattering is used to probe the adsorption dynamics of aqueous cationic and anionic dye molecules onto polystyrene surfaces. The adsorptions of malachite green to negatively charged polystyrene and naphthol yellow S to positively charged polystyrene are both highly favorable, with Î"GAds values of -10.9 ± 0.2 and -10.27 ± 0.09 kcal/mol, respectively. A competitive displacement methodology was employed to obtain values for the adsorption free energies of various smaller neutral organic molecules, including the important micropollutant ascorbic acid, caffeine, and pentoxifylline. For charged adsorbers, electrostatic interactions appear to significantly contribute to adsorption behavior. However, electrostatic repulsion does not necessarily deter the adsorption of molecules with large uncharged moieties (e.g., surfactants). In these cases, the mechanism of adsorption is dominated by van der Waals interactions, with the surface charge playing a relatively minor role.

Original language	English (US)
Pages (from-to)	14362-14369
Number of pages	8
Journal	The Journal of Physical Chemistry C
Volume	123
Issue number	23
DOIs	https://doi.org/10.1021/acs.jpcc.9b01146
State	Published - May 22 2019
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2021-03-12
Acknowledged KAUST grant number(s): OSR-2016-CRG5-2992
Acknowledgements: This work was supported by the Director, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (DOE) under contract no. DE-AC02-05CH11231 through the Chemical Sciences Division of the Lawrence Berkeley National Laboratory (LBNL), by the National Natural Science Foundation of China (NSFC) under grant no. 61775114, by KAUST under grant OSR-2016-CRG5-2992, and by CALSOLV (an affiliate of RESOLV) under Fund #56475. of the U.S. Department of Energy under Award Number DE-SC000493.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

ASJC Scopus subject areas

Surfaces, Coatings and Films
General Energy
Physical and Theoretical Chemistry
Electronic, Optical and Magnetic Materials

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10.1021/acs.jpcc.9b01146

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title = "Dynamics of Micropollutant Adsorption to Polystyrene Surfaces Probed by Angle-Resolved Second Harmonic Scattering",

abstract = "Angle-resolved second harmonic scattering is used to probe the adsorption dynamics of aqueous cationic and anionic dye molecules onto polystyrene surfaces. The adsorptions of malachite green to negatively charged polystyrene and naphthol yellow S to positively charged polystyrene are both highly favorable, with {\^I}{"}GAds values of -10.9 ± 0.2 and -10.27 ± 0.09 kcal/mol, respectively. A competitive displacement methodology was employed to obtain values for the adsorption free energies of various smaller neutral organic molecules, including the important micropollutant ascorbic acid, caffeine, and pentoxifylline. For charged adsorbers, electrostatic interactions appear to significantly contribute to adsorption behavior. However, electrostatic repulsion does not necessarily deter the adsorption of molecules with large uncharged moieties (e.g., surfactants). In these cases, the mechanism of adsorption is dominated by van der Waals interactions, with the surface charge playing a relatively minor role.",

author = "Cole, {William T. S.} and Haoyun Wei and Nguyen, {Son C.} and Harris, {Charles B.} and Miller, {Daniel J.} and Saykally, {Richard J.}",

note = "KAUST Repository Item: Exported on 2021-03-12 Acknowledged KAUST grant number(s): OSR-2016-CRG5-2992 Acknowledgements: This work was supported by the Director, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (DOE) under contract no. DE-AC02-05CH11231 through the Chemical Sciences Division of the Lawrence Berkeley National Laboratory (LBNL), by the National Natural Science Foundation of China (NSFC) under grant no. 61775114, by KAUST under grant OSR-2016-CRG5-2992, and by CALSOLV (an affiliate of RESOLV) under Fund #56475. of the U.S. Department of Energy under Award Number DE-SC000493. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

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AU - Miller, Daniel J.

AU - Saykally, Richard J.

N1 - KAUST Repository Item: Exported on 2021-03-12 Acknowledged KAUST grant number(s): OSR-2016-CRG5-2992 Acknowledgements: This work was supported by the Director, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (DOE) under contract no. DE-AC02-05CH11231 through the Chemical Sciences Division of the Lawrence Berkeley National Laboratory (LBNL), by the National Natural Science Foundation of China (NSFC) under grant no. 61775114, by KAUST under grant OSR-2016-CRG5-2992, and by CALSOLV (an affiliate of RESOLV) under Fund #56475. of the U.S. Department of Energy under Award Number DE-SC000493. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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N2 - Angle-resolved second harmonic scattering is used to probe the adsorption dynamics of aqueous cationic and anionic dye molecules onto polystyrene surfaces. The adsorptions of malachite green to negatively charged polystyrene and naphthol yellow S to positively charged polystyrene are both highly favorable, with Î"GAds values of -10.9 ± 0.2 and -10.27 ± 0.09 kcal/mol, respectively. A competitive displacement methodology was employed to obtain values for the adsorption free energies of various smaller neutral organic molecules, including the important micropollutant ascorbic acid, caffeine, and pentoxifylline. For charged adsorbers, electrostatic interactions appear to significantly contribute to adsorption behavior. However, electrostatic repulsion does not necessarily deter the adsorption of molecules with large uncharged moieties (e.g., surfactants). In these cases, the mechanism of adsorption is dominated by van der Waals interactions, with the surface charge playing a relatively minor role.

AB - Angle-resolved second harmonic scattering is used to probe the adsorption dynamics of aqueous cationic and anionic dye molecules onto polystyrene surfaces. The adsorptions of malachite green to negatively charged polystyrene and naphthol yellow S to positively charged polystyrene are both highly favorable, with Î"GAds values of -10.9 ± 0.2 and -10.27 ± 0.09 kcal/mol, respectively. A competitive displacement methodology was employed to obtain values for the adsorption free energies of various smaller neutral organic molecules, including the important micropollutant ascorbic acid, caffeine, and pentoxifylline. For charged adsorbers, electrostatic interactions appear to significantly contribute to adsorption behavior. However, electrostatic repulsion does not necessarily deter the adsorption of molecules with large uncharged moieties (e.g., surfactants). In these cases, the mechanism of adsorption is dominated by van der Waals interactions, with the surface charge playing a relatively minor role.

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Dynamics of Micropollutant Adsorption to Polystyrene Surfaces Probed by Angle-Resolved Second Harmonic Scattering

Abstract

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