Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering
Abstract Utilizing ligand-mediated homogeneous catalysis to enhance oxidant-driven pollutant removal efficiency presents significant research value while posing substantial challenges. This study utilized ethylenediaminetetraacetic acid (EDTA) to alter the coordination environment of ferrate(VI), th...
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| Format: | Article |
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Nature Portfolio
2025-07-01
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| Series: | npj Clean Water |
| Online Access: | https://doi.org/10.1038/s41545-025-00488-w |
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| author | Zhi Gao Yu-Lei Liu Zhuang-Song Huang Xiao-Na Zhao Xian-Shi Wang Zi-Yi Han Chong-Wei Cui Jun Ma Lu Wang |
| author_facet | Zhi Gao Yu-Lei Liu Zhuang-Song Huang Xiao-Na Zhao Xian-Shi Wang Zi-Yi Han Chong-Wei Cui Jun Ma Lu Wang |
| author_sort | Zhi Gao |
| collection | DOAJ |
| description | Abstract Utilizing ligand-mediated homogeneous catalysis to enhance oxidant-driven pollutant removal efficiency presents significant research value while posing substantial challenges. This study utilized ethylenediaminetetraacetic acid (EDTA) to alter the coordination environment of ferrate(VI), thereby steering electron transfer and the phenoxylation pathways to enhance the pollutant removal, which is realized by the complexation-mediated regulation for kinetics and thermodynamics. For example, the introduction of EDTA increased the rate constant of ferrate(VI) oxidizing phenol by four times (from 50.79 M−1 s−1 to 208 M−1 s−1) and the stoichiometric ratio (∆[phenol]/∆[K2FeO4]) from 0.17:1 to 0.22:1. Theoretical calculation and experimental characterization proved that the in-situ formed metastable Fe(VI)-EDTA complex facilitates the electron transfer from Fe(VI) to benzene ring and the phenoxylation pathways. Consequently, the related polymerization products were produced in greater quantities (about 5 times) and with broader diversity than Fe(VI) alone. In the application to real water, the introduction of EDTA reduced more than half of ferrate(VI)’s dosage previously required for completely removing phenol. This study presents a novel strategy for optimizing ferrate(VI) oxidizing pollutants in water treatment, which presents notable environmental benefits by minimizing ferrate(VI) consumption and enhancing pollutant removal efficiency. |
| format | Article |
| id | doaj-art-72897ab32e674e5fb8bb88ec9d5f0c2a |
| institution | DOAJ |
| issn | 2059-7037 |
| language | English |
| publishDate | 2025-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Clean Water |
| spelling | doaj-art-72897ab32e674e5fb8bb88ec9d5f0c2a2025-08-20T03:03:20ZengNature Portfolionpj Clean Water2059-70372025-07-01811910.1038/s41545-025-00488-wTailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steeringZhi Gao0Yu-Lei Liu1Zhuang-Song Huang2Xiao-Na Zhao3Xian-Shi Wang4Zi-Yi Han5Chong-Wei Cui6Jun Ma7Lu Wang8State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyState Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of TechnologyAbstract Utilizing ligand-mediated homogeneous catalysis to enhance oxidant-driven pollutant removal efficiency presents significant research value while posing substantial challenges. This study utilized ethylenediaminetetraacetic acid (EDTA) to alter the coordination environment of ferrate(VI), thereby steering electron transfer and the phenoxylation pathways to enhance the pollutant removal, which is realized by the complexation-mediated regulation for kinetics and thermodynamics. For example, the introduction of EDTA increased the rate constant of ferrate(VI) oxidizing phenol by four times (from 50.79 M−1 s−1 to 208 M−1 s−1) and the stoichiometric ratio (∆[phenol]/∆[K2FeO4]) from 0.17:1 to 0.22:1. Theoretical calculation and experimental characterization proved that the in-situ formed metastable Fe(VI)-EDTA complex facilitates the electron transfer from Fe(VI) to benzene ring and the phenoxylation pathways. Consequently, the related polymerization products were produced in greater quantities (about 5 times) and with broader diversity than Fe(VI) alone. In the application to real water, the introduction of EDTA reduced more than half of ferrate(VI)’s dosage previously required for completely removing phenol. This study presents a novel strategy for optimizing ferrate(VI) oxidizing pollutants in water treatment, which presents notable environmental benefits by minimizing ferrate(VI) consumption and enhancing pollutant removal efficiency.https://doi.org/10.1038/s41545-025-00488-w |
| spellingShingle | Zhi Gao Yu-Lei Liu Zhuang-Song Huang Xiao-Na Zhao Xian-Shi Wang Zi-Yi Han Chong-Wei Cui Jun Ma Lu Wang Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering npj Clean Water |
| title | Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering |
| title_full | Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering |
| title_fullStr | Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering |
| title_full_unstemmed | Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering |
| title_short | Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering |
| title_sort | tailoring fe vi coordination microenvironment for high efficiency oxidation ligand driven electron transfer and polymerization steering |
| url | https://doi.org/10.1038/s41545-025-00488-w |
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