Convenient Confinement: Interplay of Solution Conditions and Graphene Oxide Film Structure on Rare Earth Separations

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

doi:10.1021/acsami.2c16156

Title: Convenient Confinement: Interplay of Solution Conditions and Graphene Oxide Film Structure on Rare Earth Separations

Journal Article · Mon Dec 19 00:00:00 EST 2022 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.2c16156· OSTI ID:2290270

^[1]; Lee, Seung Eun ^[1];

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

Graphene oxide (GO) membranes are excellent candidates for a range of separation applications, including rare earth segregation and radionuclide decontamination. Understanding nanoscale water and ion behavior near interfacial GO is critical for groundbreaking membrane advances, including improved selectivity and permeability. Here, we experimentally examine the impact of solution conditions on water and lanthanide interactions with interfacial GO films and connect these results to GO membrane performance. The investigation of the confined films at the air–water interface with a combination of surface-specific spectroscopy and X-ray scattering techniques allows us to understand water and ion behaviors separately. Sum frequency generation spectroscopy reveals a dramatic change in interfacial water organization because of graphene oxide film deprotonation. Interfacial X-ray fluorescence measurements show a 17× increase in adsorbed lanthanide to the GO film from subphase pH 3 to pH 9. Liquid surface X-ray reflectivity data show an additional 2.7 $e^–$ per Å² for GO films at pH 9 versus pH 3 as well. These results are connected to GO membrane performance, which show increased selectivity and decreased flux for membranes filtering pH 9 solutions. We posit insoluble lanthanide hydroxides form at higher pHs. Taken together, these results highlight the importance of interfacial experiments on model GO systems.

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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 (CSGB); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; CHE-1834750

OSTI ID:: 2290270

Journal Information:: ACS Applied Materials and Interfaces, Vol. 14, Issue 51; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Convenient Confinement: Interplay of Solution Conditions and Graphene Oxide Film Structure on Rare Earth Separations

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