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

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

Journal Article · Sun Dec 18 23:00:00 EST 2022 · ACS Applied Materials and Interfaces

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

^[1]; Lee, Seung Eun ^[1]; ^[1]; ^[2]; ^[1]

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.

View Accepted Manuscript (DOE)

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

OSTI ID:: 2290270

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (55)

Spontaneous Adsorption of Graphene Oxide to Oil–Water and Air–Water Interfaces by Adsorption of Hydrotropes Turpin, Geosmin A.; Holt, Stephen A.; Scofield, Joel M. P. Advanced Materials Interfaces, Vol. 7, Issue 9 https://doi.org/10.1002/admi.201901810	journal	March 2020
Molecular Structure and Dynamics of Water at the Water-Air Interface Studied with Surface-Specific Vibrational Spectroscopy Bonn, Mischa; Nagata, Yuki; Backus, Ellen H. G. Angewandte Chemie International Edition, Vol. 54, Issue 19 https://doi.org/10.1002/anie.201411188	journal	April 2015
Synthesis and characterization of semi-permeable graphene/graphene oxide membranes for water desalination Romaniak, Grzegorz; Dybowski, Konrad; Jeziorna, Agata Journal of Materials Science, Vol. 55, Issue 23 https://doi.org/10.1007/s10853-020-04648-w	journal	April 2020
Selective sorption of uranium from aqueous solution by graphene oxide-modified materials Mohamud, H.; Ivanov, P.; Russell, B. C. Journal of Radioanalytical and Nuclear Chemistry, Vol. 316, Issue 2 https://doi.org/10.1007/s10967-018-5741-4	journal	February 2018
Liquid Surface X-Ray Scattering Bera, Mrinal K.; Bu, Wei; Uysal, Ahmet Physical Chemistry of Gas-Liquid Interfaces https://doi.org/10.1016/B978-0-12-813641-6.00007-8	book	June 2018
Graphene oxide membranes for ion separation: Detailed studies on the effects of fabricating conditions Hou, Jingke; Bao, Chenlu; Qu, Shaoyi Applied Surface Science, Vol. 459 https://doi.org/10.1016/j.apsusc.2018.07.207	journal	November 2018
New insights into the mechanism of graphene oxide and radionuclide interaction Kuzenkova, Anastasiia S.; Romanchuk, Anna Yu; Trigub, Alexander L. Carbon, Vol. 158 https://doi.org/10.1016/j.carbon.2019.10.003	journal	March 2020
Effects of ion adsorption on graphene oxide films and interfacial water structure: A molecular-scale description Carr, Amanda J.; Kumal, Raju R.; Bu, Wei Carbon, Vol. 195 https://doi.org/10.1016/j.carbon.2022.03.077	journal	August 2022
Self-crosslinking of graphene oxide sheets by dehydration Huang, Haiyue; Park, Hun; Huang, Jiaxing Chem, Vol. 8, Issue 9 https://doi.org/10.1016/j.chempr.2022.05.016	journal	September 2022
The behavior of graphene oxide trapped at the air water interface López-Diaz, David; Merchán, M. Dolores; Velázquez, M. Mercedes Advances in Colloid and Interface Science, Vol. 286 https://doi.org/10.1016/j.cis.2020.102312	journal	December 2020
Defective graphene nanosheets for drinking water purification: Adsorption mechanism, performance, and recovery Khaliha, Sara; Marforio, Tainah D.; Kovtun, Alessandro FlatChem, Vol. 29 https://doi.org/10.1016/j.flatc.2021.100283	journal	September 2021
pKa determination of graphene-like materials: Validating chemical functionalization Orth, Elisa S.; Ferreira, José G. L.; Fonsaca, Jéssica E. S. Journal of Colloid and Interface Science, Vol. 467 https://doi.org/10.1016/j.jcis.2016.01.013	journal	April 2016
La3+ and Y3+ interactions with the carboxylic acid moiety at the liquid/vapor interface: Identification of binding complexes, charge reversal, and detection limits Sthoer, Adrien; Adams, Ellen M.; Sengupta, Sanghamitra Journal of Colloid and Interface Science, Vol. 608 https://doi.org/10.1016/j.jcis.2021.10.052	journal	February 2022
Rapid and highly efficient removal of Eu(III) from aqueous solutions using graphene oxide Hu, Baowei; Hu, Qingyuan; Li, Xue Journal of Molecular Liquids, Vol. 229 https://doi.org/10.1016/j.molliq.2016.12.030	journal	March 2017
Preparation and characterization of oxidized graphene for actinides and rare earth elements removal in nitric acid solutions from nuclear wastes Ali, Imran; Zakharchenko, E. A.; Myasoedova, G. V. Journal of Molecular Liquids, Vol. 335 https://doi.org/10.1016/j.molliq.2021.116260	journal	August 2021
Vibrational Spectroscopy and Dynamics of Water Perakis, Fivos; De Marco, Luigi; Shalit, Andrey Chemical Reviews, Vol. 116, Issue 13 https://doi.org/10.1021/acs.chemrev.5b00640	journal	April 2016
Surface Complexation Modeling of Eu(III) and U(VI) Interactions with Graphene Oxide Xie, Yu; Helvenston, Edward M.; Shuller-Nickles, Lindsay C. Environmental Science & Technology, Vol. 50, Issue 4 https://doi.org/10.1021/acs.est.5b05307	journal	January 2016
Thermodynamic Signatures of the Origin of Anti -Hofmeister Selectivity for Phosphate at Aqueous Interfaces Grooms, Alexander J.; Neal, Jennifer F.; Ng, Ka Chon The Journal of Physical Chemistry A, Vol. 124, Issue 27 https://doi.org/10.1021/acs.jpca.0c02515	journal	May 2020
Surface pK_a of Saturated Carboxylic Acids at the Air/Water Interface: A Quantum Chemical Approach Vysotsky, Yuri B.; Kartashynska, Elena S.; Vollhardt, Dieter The Journal of Physical Chemistry C, Vol. 124, Issue 25 https://doi.org/10.1021/acs.jpcc.0c03785	journal	June 2020
Chemical Potential Driven Reorganization of Anions between Stern and Diffuse Layers at the Air/Water Interface Kumal, Raju R.; Nayak, Srikanth; Bu, Wei The Journal of Physical Chemistry C, Vol. 126, Issue 2 https://doi.org/10.1021/acs.jpcc.1c06925	journal	January 2022
Probing the Structure of Water at the Interface with Graphene Oxide Using Sum Frequency Generation Vibrational Spectroscopy Hong, Yongming; He, Jiali; Zhang, Cuiyun The Journal of Physical Chemistry C, Vol. 126, Issue 3 https://doi.org/10.1021/acs.jpcc.1c08328	journal	January 2022
Heavy Anionic Complex Creates a Unique Water Structure at a Soft Charged Interface Rock, William; Qiao, Baofu; Zhou, Tiecheng The Journal of Physical Chemistry C, Vol. 122, Issue 51 https://doi.org/10.1021/acs.jpcc.8b08419	journal	November 2018
The Role of Specific Ion Effects in Ion Transport: The Case of Nitrate and Thiocyanate Lovering, Kaitlin; Nayak, Srikanth; Bu, Wei The Journal of Physical Chemistry C, Vol. 124, Issue 1 https://doi.org/10.1021/acs.jpcc.9b09288	journal	December 2019
Increased Acid Dissociation at the Quartz/Water Interface Parashar, Shivam; Lesnicki, Dominika; Sulpizi, Marialore The Journal of Physical Chemistry Letters, Vol. 9, Issue 9 https://doi.org/10.1021/acs.jpclett.8b00686	journal	April 2018
Understanding the Role of Oxidative Debris on the Structure of Graphene Oxide Films at the Air–Water Interface: A Neutron Reflectivity Study López-Dı́az, David; Merchán, M. Dolores; Velázquez, M. Mercedes ACS Applied Materials & Interfaces, Vol. 12, Issue 22 https://doi.org/10.1021/acsami.0c05649	journal	May 2020
Enhanced Sorption of Radionuclides by Defect-Rich Graphene Oxide Boulanger, Nicolas; Kuzenkova, Anastasiia S.; Iakunkov, Artem ACS Applied Materials & Interfaces, Vol. 12, Issue 40 https://doi.org/10.1021/acsami.0c11122	journal	September 2020
Origins of Clustering of Metalate–Extractant Complexes in Liquid–Liquid Extraction Nayak, Srikanth; Kumal, Raju R.; Liu, Zhu ACS Applied Materials & Interfaces, Vol. 13, Issue 20 https://doi.org/10.1021/acsami.0c23158	journal	April 2021
Tuning the Charge and Hydrophobicity of Graphene Oxide Membranes by Functionalization with Ionic Liquids at Epoxide Sites Tan, Shuai; Zhang, Difan; Nguyen, Manh-Thuong ACS Applied Materials & Interfaces, Vol. 14, Issue 16 https://doi.org/10.1021/acsami.2c02366	journal	April 2022
Linear Free Energy Relationship for Actinide Sorption to Graphene Oxide Xie, Yu; Powell, Brian A. ACS Applied Materials & Interfaces, Vol. 10, Issue 38 https://doi.org/10.1021/acsami.8b08478	journal	August 2018
Bioinspired Graphene Oxide Membranes with pH-Responsive Nanochannels for High-Performance Nanofiltration Zhang, Zhijie; Xiao, Xiao; Zhou, Yihao ACS Nano, Vol. 15, Issue 8 https://doi.org/10.1021/acsnano.1c02719	journal	July 2021
Organization of Water and Atmospherically Relevant Ions and Solutes: Vibrational Sum Frequency Spectroscopy at the Vapor/Liquid and Liquid/Solid Interfaces Jubb, Aaron M.; Hua, Wei; Allen, Heather C. Accounts of Chemical Research, Vol. 45, Issue 1 https://doi.org/10.1021/ar200152v	journal	November 2011
Vibrational Sum Frequency Spectroscopy Studies of the Influence of Solutes and Phospholipids at Vapor/Water Interfaces Relevant to Biological and Environmental Systems Johnson, C. Magnus; Baldelli, Steven Chemical Reviews, Vol. 114, Issue 17 https://doi.org/10.1021/cr4004902	journal	January 2014
Graphene Oxide Sheets at Interfaces Kim, Jaemyung; Cote, Laura J.; Kim, Franklin Journal of the American Chemical Society, Vol. 132, Issue 23 https://doi.org/10.1021/ja102777p	journal	June 2010
Langmuir−Blodgett Assembly of Graphite Oxide Single Layers Cote, Laura J.; Kim, Franklin; Huang, Jiaxing Journal of the American Chemical Society, Vol. 131, Issue 3 https://doi.org/10.1021/ja806262m	journal	January 2009
High-Yield Spreading of Water-Miscible Solvents on Water for Langmuir–Blodgett Assembly Nie, Hua-Li; Dou, Xuan; Tang, Zhihong Journal of the American Chemical Society, Vol. 137, Issue 33 https://doi.org/10.1021/jacs.5b06052	journal	August 2015
Graphene Oxide as a Pb(II) Separation Medium: Has Part of the Story Been Overlooked? Nguyen, Manh-Thuong; Zhang, Jun; Prabhakaran, Venkateshkumar JACS Au, Vol. 1, Issue 6 https://doi.org/10.1021/jacsau.0c00075	journal	April 2021
X-ray Studies of Interfacial Strontium–Extractant Complexes in a Model Solvent Extraction System Bu, Wei; Mihaylov, Miroslav; Amoanu, Daniel The Journal of Physical Chemistry B, Vol. 118, Issue 43 https://doi.org/10.1021/jp508430e	journal	October 2014
Graphene Oxide Thin Films: Influence of Chemical Structure and Deposition Methodology Hidalgo, R. S.; López-Díaz, D.; Velázquez, M. Mercedes Langmuir, Vol. 31, Issue 9 https://doi.org/10.1021/la5029178	journal	February 2015
Structure and chemistry of graphene oxide in liquid water from first principles Mouhat, Félix; Coudert, François-Xavier; Bocquet, Marie-Laure Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15381-y	journal	March 2020
Controlling covalent chemistry on graphene oxide Guo, Shi; Garaj, Slaven; Bianco, Alberto Nature Reviews Physics, Vol. 4, Issue 4 https://doi.org/10.1038/s42254-022-00422-w	journal	February 2022
Graphene-based membranes Liu, Gongping; Jin, Wanqin; Xu, Nanping Chemical Society Reviews, Vol. 44, Issue 15 https://doi.org/10.1039/C4CS00423J	journal	January 2015
Increase in the reduction potential of uranyl upon interaction with graphene oxide surfaces Bliznyuk, V. N.; Conroy, N. A.; Xie, Y. Physical Chemistry Chemical Physics, Vol. 20, Issue 3 https://doi.org/10.1039/C7CP04197G	journal	January 2018
How exfoliated graphene oxide nanosheets organize at the water interface: evidence for a spontaneous bilayer self-assembly Bonatout, Nathalie; Muller, François; Fontaine, Philippe Nanoscale, Vol. 9, Issue 34 https://doi.org/10.1039/C7NR03403B	journal	January 2017
Reactive events at the graphene oxide–water interface David, Rolf; Kumar, Revati Chemical Communications, Vol. 57, Issue 88 https://doi.org/10.1039/D1CC04589J	journal	January 2021
Graphene oxide for effective radionuclide removal Romanchuk, Anna Yu.; Slesarev, Alexander S.; Kalmykov, Stepan N. Physical Chemistry Chemical Physics, Vol. 15, Issue 7 https://doi.org/10.1039/c2cp44593j	journal	January 2013
Salt concentration, pH and pressure controlled separation of small molecules through lamellar graphene oxide membranes Huang, Hubiao; Mao, Yiyin; Ying, Yulong Chemical Communications, Vol. 49, Issue 53 https://doi.org/10.1039/c3cc41953c	journal	January 2013
Elucidation of molecular structures at buried polymer interfaces and biological interfaces using sum frequency generation vibrational spectroscopy Zhang, Chi; Myers, John N.; Chen, Zhan Soft Matter, Vol. 9, Issue 19 https://doi.org/10.1039/c3sm27710k	journal	January 2013
Trivalent ion overcharging on electrified graphene Carr, Amanda J.; Lee, Sang Soo; Uysal, Ahmet Journal of Physics: Condensed Matter, Vol. 34, Issue 14 https://doi.org/10.1088/1361-648X/ac4a58	journal	January 2022
Stochastic fitting of specular X-ray reflectivity data using StochFit Danauskas, Stephen M.; Li, Dongxu; Meron, Mati Journal of Applied Crystallography, Vol. 41, Issue 6 https://doi.org/10.1107/S0021889808032445	journal	November 2008
Realizing small-flake graphene oxide membranes for ultrafast size-dependent organic solvent nanofiltration Nie, Lina; Goh, Kunli; Wang, Yu Science Advances, Vol. 6, Issue 17 https://doi.org/10.1126/sciadv.aaz9184	journal	April 2020
Unimpeded Permeation of Water Through Helium-Leak-Tight Graphene-Based Membranes Nair, R. R.; Wu, H. A.; Jayaram, P. N. Science, Vol. 335, Issue 6067, p. 442-444 https://doi.org/10.1126/science.1211694	journal	January 2012
Precise and Ultrafast Molecular Sieving Through Graphene Oxide Membranes Joshi, R. K.; Carbone, P.; Wang, F. C. Science, Vol. 343, Issue 6172 https://doi.org/10.1126/science.1245711	journal	February 2014
Graphene Oxide Membranes for Ionic and Molecular Sieving Mi, B. Science, Vol. 343, Issue 6172 https://doi.org/10.1126/science.1250247	journal	February 2014
Second Harmonic Generation, Sum Frequency Generation, and χ ⁽³⁾ : Dissecting Environmental Interfaces with a Nonlinear Optical Swiss Army Knife Geiger, Franz M. Annual Review of Physical Chemistry, Vol. 60, Issue 1 https://doi.org/10.1146/annurev.physchem.59.032607.093651	journal	May 2009
The Removal of Phosphate from Aqueous Solution through Chemical Filtration Using a Sponge Filter Yang, Shengjiong; Chen, Xiaotian; Zhang, Zhenya Chemistry Letters, Vol. 47, Issue 1 https://doi.org/10.1246/cl.170915	journal	January 2018

Figures / Tables (7)

Similar Records

Heavy Versus Light Lanthanide Selectivity for Graphene Oxide Films is Concentration Dependent

Journal Article · Fri Jul 14 00:00:00 EDT 2023 · Journal of Physical Chemistry. C · OSTI ID:2367267

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
air-liquid interface
confinement
graphene oxide
ion adsorption
sum frequency generation spectroscopy (SFG)
x-ray fluorescence near total reflection (XFNTR)
x-ray reflectivity (XR)

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

Citation Formats

References (55)

Figures / Tables (7)

Similar Records

Related Subjects