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Research Article

Synergy enhancement of Co single atoms and asymmetric sub-nanoclusters for Fenton-like activation

Ming Ma1Zhiyi Sun2Ziwei Deng2Xiang Li1( )Fang Zhang3Wenxing Chen2( )
School of Materials, Key Laboratory of Cluster Science Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Advanced Technologies Research Institute (Jinan), Advanced Research Institute of Multidisciplinary Science, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
Energy and Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Analysis and Testing Center, Beijing Institute of Technology, Beijing Institute of Technology, Beijing 100081, China
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Abstract

As a new water treatment technology, Fenton-like reaction has great potential. In this study, we successfully prepared an excellent Fenton-like catalyst, which is composed of cobalt monoatoms and asymmetric subnanoclusters (labeled CoSA/Clu-C2N), and exhibits excellent peroxymonosulfate (PMS) activation reactivity. By directly comparing the catalytic properties of CoSA-C2N and CoSA/Clu-C2N, the synergistic effects of coasymmetric Co subclusters and Co atoms on the activation of PMS and degradation of organic micropollutants were investigated. The results showed that CoSA/Clu-C2N had higher degradation rates of carbamazepine (CBZ), antipyrine (AT) and chlorobenzoic acid (CA) when combined with active oxidant PMS. The cyclic frequency of CBZ was 5.4 min−1, which was twice as high as the catalytic constant of CoSA-C2N (2.4 min−1). The results show that CoSA/Clu-C2N cobalt subnanoclusters and cobalt single atom can synergistically improve the catalytic performance of activated PMS oxidation of micropollutants in water. In addition, electron paramagnetic resonance (EPR) technology has proved that the introduction of Co subnano clusters in CoSA/Clu-C2N is conducive to the production of singlet oxygen (1O2), thereby improving the efficiency of pollutant oxidation. This work lays a solid foundation for the future design of advanced multifunctional catalysts by carefully regulating and combining monmetallic atoms and metal subnanoclusters.

Graphical Abstract

As a new water treatment technology, Fenton-like reaction has great potential. In this study, we successfully prepared an excellent Fenton-like catalyst, which is composed of cobalt monoatoms and asymmetric subnanoclusters (labeled CoSA/Clu-C2N), and exhibits excellent peroxymonosulfate (PMS) activation reactivity. By directly comparing the catalytic properties of CoSA-C2N and CoSA/Clu-C2N, the synergistic effects of coasymmetric Co subclusters and Co atoms on the activation of PMS and degradation of organic micropollutants were investigated. The results showed that CoSA/Clu-C2N had higher degradation rates of carbamazepine (CBZ), antipyrine (AT) and chlorobenzoic acid (CA) when combined with active oxidant PMS. The cyclic frequency of CBZ was 5.4 min−1, which was twice as high as the catalytic constant of CoSA-C2N (2.4 min−1). The results show that CoSA/Cul-C2N cobalt subnanoclusters and cobalt single atom can synergistically improve the catalytic performance of activated PMS oxidation of micropollutants in water. In addition, electron paramagnetic resonance (EPR) technology has proved that the introduction of Co subnano clusters in CoSA/Cu-C2N is conducive to the production of 1O2, thereby improving the efficiency of pollutant oxidation. This work lays a solid foundation for the future design of advanced multifunctional catalysts by carefully regulating and combining monmetallic atoms and metal subnanoclusters.

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Nano Research
Pages 7935-7944

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Cite this article:
Ma M, Sun Z, Deng Z, et al. Synergy enhancement of Co single atoms and asymmetric sub-nanoclusters for Fenton-like activation. Nano Research, 2024, 17(9): 7935-7944. https://doi.org/10.1007/s12274-024-6792-1
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Received: 03 April 2024
Revised: 20 May 2024
Accepted: 28 May 2024
Published: 29 June 2024
© Tsinghua University Press 2024