Intrinsic nanoparticle-single-atom interplays steering radical versus nonradical pathways in catalytic ozonation
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Date
2025
Authors
Liu, Y.
Yang, J.
Wang, Y.
Zhu, W.
Hu, K.
Liu, Z.
Yeung, K.
Zhu, Z.-S.
Chen, C.
Duan, X.
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Journal article
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Nature Communications, 2025; 16(1):8790-1-8790-16
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Ya Liu, Jiajia Yang, Yuxian Wang, Wanli Zhu, Kunsheng Hu, Zhang Liu, Kinglun Yeung, Zhong-Shuai Zhu, Chunmao Chen, Xiaoguang Duan, Shaobin Wang
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Abstract
Compositional heterogeneity in metal/nitrogen-doped carbons (M-N-Cs) complicates the fundamental elucidation of the intricate interplay between the active metal species that rule the reactivity of single atomic catalysts (SACs). This study unveils the electronic disruptions of cobalt nanoparticles (Co NPs) to the catalytic behaviors of cobalt single-atom (Co SA). The intense electronic communications between high-density Co NPs and Co SA sites lead to dissociation O3 on the high-spin Co SA sites to generate surface-confined hydroxyl radicals (•OH). However, the tandem electron transfer yields superoxide radical (O₂•–) with low reactivity and remarkably reduce ozone utilization efficiency (OUE). In contrast, independent Co SA sites far or free from adjacent Co NPs induce a nonradical O₃ activation regime, which markedly improves electron utilization efficiency (~2.9-fold), OUE ( ~ 3.0-fold), and turnover frequency (TOF, ~2.5-fold) of Co SA. The nonradical catalytic ozonation process demonstrates high adaptability to complex water matrices and maintains long-term stability in the treatment of real petrochemical wastewater. The deciphered electronic interplays between metal nanoparticles and single atom sites advance a new paradigm to regulate the selectivity of single atom catalysis.
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© The Author(s) 2025. This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http:// creativecommons.org/licenses/by-nc-nd/4.0/.