Selective single-atom adsorption for precision separation of lead ions in tap water via capacitive deionization

Zhenwei Gao; Luqing Wang; Xingkang Huang; Chris Benmore; Haihui Pu; Jianguo Wen; Wen Zhuang; Maria K.Y. Chan; Junhong Chen

doi:10.1016/j.watres.2024.122665

Selective single-atom adsorption for precision separation of lead ions in tap water via capacitive deionization

Zhenwei Gao, Luqing Wang, Xingkang Huang, Chris Benmore, Haihui Pu, Jianguo Wen, Wen Zhuang, Maria K.Y. Chan, Junhong Chen^*

^*Corresponding author for this work

MRC - Materials Research Center

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

8 Scopus citations

Abstract

Capacitive deionization (CDI) offers a cost-effective and low-energy method for selective removal of Pb²⁺ from drinking water. Modifying CDI electrode surfaces with functional groups presents a versatile approach to enhancing selective ion adsorption capacity. However, a comprehensive understanding of the selectivity and removal efficiency of Pb²⁺ among diverse functional groups remains unexplored. Here, we investigated the effects of different functional groups (-SH, -COOH, and -NH₂) attached to the graphene oxide (GO) electrode surfaces on Pb²⁺ selectivity and removal efficiency. Surprisingly, GO-COOH demonstrated single-atom adsorption of Pb²⁺, displaying superior removal efficiency and selectivity compared with -SH and -NH₂, although -SH possesses significant chelation capability for Pb²⁺. Both density functional theory (DFT) calculations and X-ray pair distribution function (PDF) analyses confirmed that Pb²⁺ exhibits a theoretically higher affinity to -COOH. This research deepens our understanding of the interactions between functional groups and heavy metal ions, enabling selective and rapid separation of target cations for water purification.

Original language	English (US)
Article number	122665
Journal	Water Research
Volume	268
DOIs	https://doi.org/10.1016/j.watres.2024.122665
State	Published - Jan 1 2025

Funding

The authors are grateful for the support received from the UChicago Joint Task Force Initiative and the National Science Foundation's Major Research Instrumentation Program (No. 2117896). The authors would like to gratefully acknowledge Dr. Seth B. Darling and Dr. Jeffrey Elam at Argonne National Laboratory for the use of ICP and XPS, and the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. Work performed at the Center for Nanoscale Materials and Advanced Photon Source (beamline 4-ID-D), both U.S. Department of Energy Office of Science User Facilities, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.

Keywords

Capacitive deionization
Computational modeling
Functionalized graphene oxide
Lead removal
Water remediation

ASJC Scopus subject areas

Environmental Engineering
Civil and Structural Engineering
Ecological Modeling
Water Science and Technology
Waste Management and Disposal
Pollution

UN SDGs

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

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10.1016/j.watres.2024.122665

Cite this

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title = "Selective single-atom adsorption for precision separation of lead ions in tap water via capacitive deionization",

abstract = "Capacitive deionization (CDI) offers a cost-effective and low-energy method for selective removal of Pb2+ from drinking water. Modifying CDI electrode surfaces with functional groups presents a versatile approach to enhancing selective ion adsorption capacity. However, a comprehensive understanding of the selectivity and removal efficiency of Pb2+ among diverse functional groups remains unexplored. Here, we investigated the effects of different functional groups (-SH, -COOH, and -NH2) attached to the graphene oxide (GO) electrode surfaces on Pb2+ selectivity and removal efficiency. Surprisingly, GO-COOH demonstrated single-atom adsorption of Pb2+, displaying superior removal efficiency and selectivity compared with -SH and -NH2, although -SH possesses significant chelation capability for Pb2+. Both density functional theory (DFT) calculations and X-ray pair distribution function (PDF) analyses confirmed that Pb2+ exhibits a theoretically higher affinity to -COOH. This research deepens our understanding of the interactions between functional groups and heavy metal ions, enabling selective and rapid separation of target cations for water purification.",

keywords = "Capacitive deionization, Computational modeling, Functionalized graphene oxide, Lead removal, Water remediation",

author = "Zhenwei Gao and Luqing Wang and Xingkang Huang and Chris Benmore and Haihui Pu and Jianguo Wen and Wen Zhuang and Chan, \{Maria K.Y.\} and Junhong Chen",

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year = "2025",

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doi = "10.1016/j.watres.2024.122665",

language = "English (US)",

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AU - Gao, Zhenwei

AU - Wang, Luqing

AU - Huang, Xingkang

AU - Benmore, Chris

AU - Pu, Haihui

AU - Wen, Jianguo

AU - Zhuang, Wen

AU - Chan, Maria K.Y.

AU - Chen, Junhong

PY - 2025/1/1

Y1 - 2025/1/1

N2 - Capacitive deionization (CDI) offers a cost-effective and low-energy method for selective removal of Pb2+ from drinking water. Modifying CDI electrode surfaces with functional groups presents a versatile approach to enhancing selective ion adsorption capacity. However, a comprehensive understanding of the selectivity and removal efficiency of Pb2+ among diverse functional groups remains unexplored. Here, we investigated the effects of different functional groups (-SH, -COOH, and -NH2) attached to the graphene oxide (GO) electrode surfaces on Pb2+ selectivity and removal efficiency. Surprisingly, GO-COOH demonstrated single-atom adsorption of Pb2+, displaying superior removal efficiency and selectivity compared with -SH and -NH2, although -SH possesses significant chelation capability for Pb2+. Both density functional theory (DFT) calculations and X-ray pair distribution function (PDF) analyses confirmed that Pb2+ exhibits a theoretically higher affinity to -COOH. This research deepens our understanding of the interactions between functional groups and heavy metal ions, enabling selective and rapid separation of target cations for water purification.

AB - Capacitive deionization (CDI) offers a cost-effective and low-energy method for selective removal of Pb2+ from drinking water. Modifying CDI electrode surfaces with functional groups presents a versatile approach to enhancing selective ion adsorption capacity. However, a comprehensive understanding of the selectivity and removal efficiency of Pb2+ among diverse functional groups remains unexplored. Here, we investigated the effects of different functional groups (-SH, -COOH, and -NH2) attached to the graphene oxide (GO) electrode surfaces on Pb2+ selectivity and removal efficiency. Surprisingly, GO-COOH demonstrated single-atom adsorption of Pb2+, displaying superior removal efficiency and selectivity compared with -SH and -NH2, although -SH possesses significant chelation capability for Pb2+. Both density functional theory (DFT) calculations and X-ray pair distribution function (PDF) analyses confirmed that Pb2+ exhibits a theoretically higher affinity to -COOH. This research deepens our understanding of the interactions between functional groups and heavy metal ions, enabling selective and rapid separation of target cations for water purification.

KW - Capacitive deionization

KW - Computational modeling

KW - Functionalized graphene oxide

KW - Lead removal

KW - Water remediation

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Selective single-atom adsorption for precision separation of lead ions in tap water via capacitive deionization

Abstract

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Keywords

ASJC Scopus subject areas

UN SDGs

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