Dynamic Geminal‐Atom Coordination for Highly Efficient Photo‐Fenton Catalysis

Understanding and leveraging non-reactive species in natural environments to modulate the active centers of geminal-atom catalysts (GACs) is crucial for enhancing their catalytic performance. Here, we develop a two-coordinated copper geminal-atom catalyst and reveal that the ubiquitous yet inert carbonate ions (CO<sub>3</sub> <sup>2-</sup>) in seawater dynamically reorganize the coordination environment of active copper sites, thereby enhancing photo-Fenton reactivity. Control experiments, in situ spectroscopy and theoretical modeling demonstrate that CO<sub>3</sub> <sup>2-</sup> induces reversible coordination transformations that modulate the electronic structure and facilitate interfacial charge transfer, resulting in a 17-fold increase in hydroxyl radical production. This effect enables efficient degradation of diverse marine pollutants, including effective Chlorella decomposition under natural sunlight. Life-cycle and technoeconomic assessments further demonstrate the environmental benefits and economic feasibility of this approach. Overall, this work establishes a generalizable strategy for active geminal-atom catalysts via environmentally abundant species, offering mechanistic insights and scalable pathways toward large-scale and sustainable aquatic pollution remediation.

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Publication Details

Journal
Advanced Materials
Published
2025-12-19
DOI
https://doi.org/10.1002/adma.202518940
Primary Topic
Advanced oxidation water treatment
Type
article
Field-Weighted Citation Impact
0.00

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article

Dynamic Geminal‐Atom Coordination for Highly Efficient Photo‐Fenton Catalysis

Chrystelle Salameh, Damien Voiry, Jieru Zhang, Lanlu Lu et al.
Advanced Materials
Advanced oxidation water treatment
article

Dynamic Geminal‐Atom Coordination for Highly Efficient Photo‐Fenton Catalysis

Chrystelle Salameh, Damien Voiry, Jieru Zhang, Lanlu Lu, Kun Qi, Feng Zhou, Fuxiang Zhang, Keqiang Chen, Dantong Zhang, Jiangpeng Li, Wenjun Jiang, Xinzhe Li, Qiuchen He, Yang Zhang, Jingyuan Ma, Yuchen Qiao, Su Zhan
article en

Abstract

Understanding and leveraging non-reactive species in natural environments to modulate the active centers of geminal-atom catalysts (GACs) is crucial for enhancing their catalytic performance. Here, we develop a two-coordinated copper geminal-atom catalyst and reveal that the ubiquitous yet inert carbonate ions (CO<sub>3</sub> <sup>2-</sup>) in seawater dynamically reorganize the coordination environment of active copper sites, thereby enhancing photo-Fenton reactivity. Control experiments, in situ spectroscopy and theoretical modeling demonstrate that CO<sub>3</sub> <sup>2-</sup> induces reversible coordination transformations that modulate the electronic structure and facilitate interfacial charge transfer, resulting in a 17-fold increase in hydroxyl radical production. This effect enables efficient degradation of diverse marine pollutants, including effective Chlorella decomposition under natural sunlight. Life-cycle and technoeconomic assessments further demonstrate the environmental benefits and economic feasibility of this approach. Overall, this work establishes a generalizable strategy for active geminal-atom catalysts via environmentally abundant species, offering mechanistic insights and scalable pathways toward large-scale and sustainable aquatic pollution remediation.

Advanced MaterialsVol. 38(8)
Qiqihar University (CN), Centre National de la Recherche Scientifique (FR), Dalian Institute of Chemical Physics (CN), Chinese Academy of Sciences (CN), Université de Montpellier (FR), China University of Geosciences (CN), Shanghai Advanced Research Institute (CN), Dalian National Laboratory for Clean Energy (CN), Institut Européen des Membranes (FR), Dalian Maritime University (CN), Xi'an Jiaotong University (CN)
Salt Science Research Foundation, National Natural Science Foundation of China, Chinese Academy of Sciences, Natural Science Foundation of Shaanxi Province, Dalian Institute of Chemical Physics, Young Scientists Fund, National Key Research and Development Program of China
Openalex Percentile: Top 62%
Advanced oxidation water treatment
DOIOpen Access PDFOpenAlex
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