Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction of emerging contaminants

Highlights

● Cu-C-MSNs are developed via a co-doping step of Cu with L(+)-ascorbic acid.

● Cu-C-MSNs show superb performance in removing contaminants and purifying wastewater.

● The performance is owing to the polarization electric field and cation-π structures.

● The biological toxicity of bisphenol A is considerably weakened after the reaction.

Abstract

Effective removal of emerging contaminants (ECs) to minimize their impacts on human health and the natural environment is a global priority. For the removal of ECs in water, we fabricated a seaweed spherical microsphere catalyst with Cu cation-π structures by in situ doping of Cu species and ascorbic acid in mesoporous silica (Cu-C-MSNs) via a hydrothermal method. The results indicate that bisphenol A (BPA) is substantially degraded within 5 min under natural conditions, with its biological toxicity considerably weakened. Moreover, industrial wastewater could also be effectively purified by Cu-C-MSNs/H₂O₂ system. The presence of metal sites and the complexation of ECs via cation-π interaction and π-π stacking on the catalyst surface were directly responsible for the polarization distribution of electrons, thus activating H₂O₂ and dissolved oxygen (DO). The removal of contaminants could be attributed primarily to 1) the activation of H₂O₂ into ^•OH to attack the contaminants and 2) self-cleavage because of the transfer of electrons from the contaminants to the catalysts. This study provides an innovative solution for the effective treatment of ECs and has positive implications for easing global environmental crises.

Graphical abstract

Keywords

Cation-π structures / Polarization electric field / Fenton-like process / Contaminants cleavage

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CRediT Authorship Contribution Statement

Yuhang Liu: Design experiments, Methodology Data curation, Formal analysis, Writing original draft. Wenxuan Deng & Xiaojun Wu: Investigation, Performing experiments. Hu Chun & Lai Lyu: Conceptualization, Visualization, Formal analysis, Writing - review and editing, Supervision, Validation, Resources, Funding acquisition, Project administration.

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 52122009, 52070046, and 51838005), the Introduced Innovative R&D Team Project under the “Pearl River Talent Recruitment Program” of Guangdong Province (China) (No. 2019ZT08L387), and the Basic and Applied Basic Research Project of Guangzhou (China) (No. 202201020163).

Declaration of Competing Interests

The author Lai Lyu is a Youth Editorial Board Member of Frontiers of Environmental Science & Engineering. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Data Availability

Data will be made available on request.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-024-1804-7 and is accessible for authorized users.

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