Graphene Oxide as a Pb(II) Separation Medium: Has Part of the Story Been Overlooked?

Manh Thuong Nguyen; Jun Zhang; Venkateshkumar Prabhakaran; Shuai Tan; Eric T. Baxter; Vaithiyalingam Shutthanandan; Grant E. Johnson; Roger Rousseau; Vassiliki Alexandra Glezakou

doi:10.1021/jacsau.0c00075

Graphene Oxide as a Pb(II) Separation Medium: Has Part of the Story Been Overlooked?

Manh Thuong Nguyen, Jun Zhang, Venkateshkumar Prabhakaran, Shuai Tan, Eric T. Baxter, Vaithiyalingam Shutthanandan, Grant E. Johnson, Roger Rousseau, Vassiliki Alexandra Glezakou

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

13 Scopus citations

Abstract

A key problem associated with the design of graphene oxide (GO) materials and their tuning for nanoscale separations is how specific functional groups influence the competitive adsorption of solvated ions and water at liquid/graphene interfaces. Computation accompanied by experiment shows that OH and COOH exert an influence on water adsorption properties stronger than that of O and H functional groups. The COO^-anions, following COOH deprotonation, stabilize Pb(II) through strong electrostatic interactions. This suggests that, among the functional groups under study, COOH offers the best Pb(II) adsorption capacity and the ability to regenerate the sorbent through a pH swing. In line with computation, striking experimental observations revealed that a substantial increase in Pb(II) adsorption occurs with increasing pH. Our findings provide a systematic framework for controlled design and implementation of regenerable C-based sorbents used in separations and desalination.

Original language	English
Pages (from-to)	766-776
Number of pages	11
Journal	JACS Au
Volume	1
Issue number	6
DOIs	https://doi.org/10.1021/jacsau.0c00075
State	Published - Jun 28 2021
Externally published	Yes

Funding

This work was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, project 72353 (Interfacial Structure and Dynamics in Ion Separations). Part of this work was performed using EMSL, a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated for DOE by Battelle for the U.S. Department of Energy under Contract DE-AC05-76RL01830. Computer resources were provided by Research Computing at Pacific Northwest National Laboratory, and the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231.

Keywords

AIMD
Graphene oxide
adsorption
desorption
ion transport
lead removal
membrane separation
pH

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/jacsau.0c00075

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title = "Graphene Oxide as a Pb(II) Separation Medium: Has Part of the Story Been Overlooked?",

abstract = "A key problem associated with the design of graphene oxide (GO) materials and their tuning for nanoscale separations is how specific functional groups influence the competitive adsorption of solvated ions and water at liquid/graphene interfaces. Computation accompanied by experiment shows that OH and COOH exert an influence on water adsorption properties stronger than that of O and H functional groups. The COO-anions, following COOH deprotonation, stabilize Pb(II) through strong electrostatic interactions. This suggests that, among the functional groups under study, COOH offers the best Pb(II) adsorption capacity and the ability to regenerate the sorbent through a pH swing. In line with computation, striking experimental observations revealed that a substantial increase in Pb(II) adsorption occurs with increasing pH. Our findings provide a systematic framework for controlled design and implementation of regenerable C-based sorbents used in separations and desalination.",

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author = "Nguyen, {Manh Thuong} and Jun Zhang and Venkateshkumar Prabhakaran and Shuai Tan and Baxter, {Eric T.} and Vaithiyalingam Shutthanandan and Johnson, {Grant E.} and Roger Rousseau and Glezakou, {Vassiliki Alexandra}",

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AU - Tan, Shuai

AU - Baxter, Eric T.

AU - Shutthanandan, Vaithiyalingam

AU - Johnson, Grant E.

AU - Rousseau, Roger

AU - Glezakou, Vassiliki Alexandra

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N2 - A key problem associated with the design of graphene oxide (GO) materials and their tuning for nanoscale separations is how specific functional groups influence the competitive adsorption of solvated ions and water at liquid/graphene interfaces. Computation accompanied by experiment shows that OH and COOH exert an influence on water adsorption properties stronger than that of O and H functional groups. The COO-anions, following COOH deprotonation, stabilize Pb(II) through strong electrostatic interactions. This suggests that, among the functional groups under study, COOH offers the best Pb(II) adsorption capacity and the ability to regenerate the sorbent through a pH swing. In line with computation, striking experimental observations revealed that a substantial increase in Pb(II) adsorption occurs with increasing pH. Our findings provide a systematic framework for controlled design and implementation of regenerable C-based sorbents used in separations and desalination.

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KW - AIMD

KW - Graphene oxide

KW - adsorption

KW - desorption

KW - ion transport

KW - lead removal

KW - membrane separation

KW - pH

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Graphene Oxide as a Pb(II) Separation Medium: Has Part of the Story Been Overlooked?

Abstract

Funding

Keywords

UN SDGs

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