Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewater

Abstract Heavy metals complexed with organic ligands are among the most critical carcinogens threatening global water safety. The challenge of efficiently and cost-effectively removing and recovering these metals has long eluded existing technologies. Here, we show a strategy of coordinating mediato...

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Main Authors: Wei Shi, Jiayi Li, Fei Gao, Lijun Meng, Xiao Su, Zhiwei Wang
Format: Article
Language:English
Published: Nature Portfolio 2024-12-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55174-1
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author Wei Shi
Jiayi Li
Fei Gao
Lijun Meng
Xiao Su
Zhiwei Wang
author_facet Wei Shi
Jiayi Li
Fei Gao
Lijun Meng
Xiao Su
Zhiwei Wang
author_sort Wei Shi
collection DOAJ
description Abstract Heavy metals complexed with organic ligands are among the most critical carcinogens threatening global water safety. The challenge of efficiently and cost-effectively removing and recovering these metals has long eluded existing technologies. Here, we show a strategy of coordinating mediator-based electro-reduction (CMBER) for the single-step recovery of heavy metals from wastewater contaminated with heavy metal-organic complexes. In CMBER, amidoxime with superior coordinating abilities over traditional ligands is immobilized by an amidoximation reaction onto a flow-through electrode that concurrently functions as a filtration device. This unique process spontaneously captures heavy metal ions at the -N-OH and -NH2 groups of the amidoxime from their complexes without external energy input (ΔG of amidoxime mediator with Cu(II): −6.59 eV), followed by direct in situ electro-reduction for metal recovery. The reduction of captured Cu(II) to Cu(0) regenerates the amidoxime’s active sites, enabling continuous capture of Cu(II). Operating at a voltage of 3 V and a water flux of 250 L m−2 h−1, the CMBER system achieves a Cu(II) recovery rate of 97.6% and demonstrates an energy efficiency of 340.1 g kWh−1. This energy efficiency significantly outperforms existing technologies, showing a nearly fivefold improvement. CMBER creates a new dimension for cost-effective resource recovery and water purification.
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publishDate 2024-12-01
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spelling doaj-art-99d718812aab44b58ed9d3f4ae71203b2025-01-05T12:35:27ZengNature PortfolioNature Communications2041-17232024-12-0115111010.1038/s41467-024-55174-1Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewaterWei Shi0Jiayi Li1Fei Gao2Lijun Meng3Xiao Su4Zhiwei Wang5State Key Laboratory of Pollution Control and Resource Reuse, Tongji UniversitySchool of Environmental Science and Engineering, Tongji UniversitySchool of Environmental Science and Engineering, Tongji UniversitySchool of Environmental Science and Engineering, Tongji UniversityDepartment of Chemical and Biomolecular Engineering, University of Illinois Urbana-ChampaignState Key Laboratory of Pollution Control and Resource Reuse, Tongji UniversityAbstract Heavy metals complexed with organic ligands are among the most critical carcinogens threatening global water safety. The challenge of efficiently and cost-effectively removing and recovering these metals has long eluded existing technologies. Here, we show a strategy of coordinating mediator-based electro-reduction (CMBER) for the single-step recovery of heavy metals from wastewater contaminated with heavy metal-organic complexes. In CMBER, amidoxime with superior coordinating abilities over traditional ligands is immobilized by an amidoximation reaction onto a flow-through electrode that concurrently functions as a filtration device. This unique process spontaneously captures heavy metal ions at the -N-OH and -NH2 groups of the amidoxime from their complexes without external energy input (ΔG of amidoxime mediator with Cu(II): −6.59 eV), followed by direct in situ electro-reduction for metal recovery. The reduction of captured Cu(II) to Cu(0) regenerates the amidoxime’s active sites, enabling continuous capture of Cu(II). Operating at a voltage of 3 V and a water flux of 250 L m−2 h−1, the CMBER system achieves a Cu(II) recovery rate of 97.6% and demonstrates an energy efficiency of 340.1 g kWh−1. This energy efficiency significantly outperforms existing technologies, showing a nearly fivefold improvement. CMBER creates a new dimension for cost-effective resource recovery and water purification.https://doi.org/10.1038/s41467-024-55174-1
spellingShingle Wei Shi
Jiayi Li
Fei Gao
Lijun Meng
Xiao Su
Zhiwei Wang
Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewater
Nature Communications
title Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewater
title_full Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewater
title_fullStr Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewater
title_full_unstemmed Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewater
title_short Strongly coordinating mediator enables single-step resource recovery from heavy metal-organic complexes in wastewater
title_sort strongly coordinating mediator enables single step resource recovery from heavy metal organic complexes in wastewater
url https://doi.org/10.1038/s41467-024-55174-1
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