Effects of ion adsorption on graphene oxide films and interfacial water structure: A molecular-scale description

Carr, Amanda J.; Kumal, Raju R.; Bu, Wei; Uysal, Ahmet

doi:10.1016/j.carbon.2022.03.077

Title: Effects of ion adsorption on graphene oxide films and interfacial water structure: A molecular-scale description

Journal Article · 01 April 2022 · Carbon

DOI: https://doi.org/10.1016/j.carbon.2022.03.077 · OSTI ID:1962094

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^[1]; Bu, Wei ^[2];

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Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Chicago, IL (United States)

Herein we discuss graphene oxide as a promising, emerging separation material, as it is durable, dispersible in water, and has naturally forming functional groups. Bulk studies using graphene oxide flakes have demonstrated impressive metal adsorption. However, little interfacial information about water and metal organization near graphene oxide is available. A mechanistic understanding of water and ions interactions with graphene oxide films is critical toward advanced separations, including improved sorption efficiency and membrane regeneration. We study metal ion and local water organization near graphene oxide thin films formed at the air/water interface. These films are not typical membranes and allow us to determine nanoscale information about the graphene oxide-water interface. We accomplish this with x-ray reflectivity (XR), x-ray fluorescence near total reflection (XFNTR), and vibrational sum frequency generation spectroscopy (SFG). These interface-specific techniques provide the electron density profile normal to the interface, number of adsorbed ions, and information about the orientational ordering and hydrogen-bonding network of interfacial water, respectively. Via XFNTR and SFG, we find that trivalent yttrium ions preferentially adsorb to graphene oxide and affect its structure, compared to divalent strontium and monovalent cesium ions. Two different interfacial water populations can be described, based on their hydrogen bonding strength, and the adsorbed ions affect these populations differently. These results provide fundamental information about ion and water organization at the interface and help address the large computational-experimental agreement gap for graphene oxide systems. Additionally, they are relevant for improved soft-scaffold graphene oxide membranes and downstream applications.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1962094

Journal Information:: Carbon, Journal Name: Carbon Vol. 195; ISSN 0008-6223

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Ion adsorption
Graphene oxide
Air-water interface
X-ray reflectivity
X-ray fluorescence near total reflection
Sum frequency generation spectroscopy

Title: Effects of ion adsorption on graphene oxide films and interfacial water structure: A molecular-scale description

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