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Effective degradation of tetracycline via recyclable free-standing three-dimensional copper-based graphene as a persulfate catalyst

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Abstract

Water pollution by antibiotics is a serious and growing problem. Given this challenge, a free-standing three-dimensional (3D) reduced graphene oxide foam supported copper oxide nanoparticles (3D-rGO-CuxO) was synthesized using GO as a precursor and applied as an efficient persulfate activator for tetracycline (TC) degradation. The influences of CuxO mass, solution pH, persulfate dosage, and common anions on the TC degradation were investigated in detail. Analytical techniques indicated that the 3D-rGO-CuxO showed a cross-linking three-dimensional network structure, and CuxO particles with irregular shapes were uniformly loaded on graphene pore walls. The XPS and Auger spectra of Cu confirmed that Cu2O was the main component in solid copper compounds. The addition of CuxO was vitally important for the activation of the oxidation system, and the removal rate reached 98% with a CuxO load of 7:1. The pH showed little influence on the activation effect on TC degradation. For common anions, Cl− and CO32− had little influence on the system, while humic acid had a great inhibitory effect. The EPR test and quenching experiment revealed that the active substances in the oxidative degradation process mainly include SO4−·, ·OH, 1O2, and reactive Cu(III). Additionally, the 3D-rGO-CuxO material proved highly stable according to the replicated test results and was promising for the remediation of antibiotic-contaminated water.

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The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.

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Funding

This research was funded by the National Natural Science Foundation (41703120), the Project Tackling of Key Scientific and Technical Problems of Henan Province, China (222102320200), the Geological Survey Program of the CGS, China (DD20221782), and the Basic Ability Improvement Project for Young and Middle-Aged Teachers in Guangxi Province (No.2019KY0187).

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Authors and Affiliations

  1. School of Materials and Environment, Guangxi Key Laboratory of Advanced Structural Materials and Carbon Neutralization, Guangxi Colleges and Universities Key Laboratory of Environmental-Friendly Materials and New Technology For Carbon Neutralization, Guangxi Minzu University, Guangxi Nanning, 530006, China

    Chuanqi Zhao, Liying Liang & Qin Shi

  2. Zhengzhou Institute of Multipurpose Utilization of Mineral Resources, CAGS, Zhengzhou, 450006, China

    Hui **a

  3. Key Lab of Eco-Restoration of Regional Contaminated Environment, Ministry of Education, Shenyang University, Shenyang, 110044, China

    Chaofan Li

  4. School of Artificial Intelligence, Shenyang University of Technology, Shenyang, 110870, China

    Junguan Ma

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  1. Chuanqi Zhao
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  2. Liying Liang
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  3. Qin Shi
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  4. Hui **a
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  5. Chaofan Li
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Contributions

Chuanqi Zhao: writing—original draft, conceptualization, funding acquisition, investigation. Junguan Ma: methodology, software. Chaofan Li: writing—review and editing. Liying Liang: data curation, investigation. Qin Shi: resources, funding acquisition. Hui **a: resources, funding acquisition.

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Correspondence to Chuanqi Zhao.

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Highlights

• The 3D-rGO-CuxO was synthesized and applied as PDS activator for TC degradation.

• CuxO particles were distributed on 3D-rGO surface, and Cu2O was the main component.

• The 3D-rGO-CuxO showed a high catalytic activation effect on PDS in a wide pH range.

• The degradation of TC was completed by SO4−·, ·OH, 1O2 and reactive Cu(III).

The original online version of this article was revised: Equations 7, 9 and 10 contain Chinese characters.

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Zhao, C., Liang, L., Shi, Q. et al. Effective degradation of tetracycline via recyclable free-standing three-dimensional copper-based graphene as a persulfate catalyst. Environ Sci Pollut Res 30, 62410–62421 (2023). https://doi.org/10.1007/s11356-023-26407-5

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