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Tailoring d-band center of high-valent metal-oxo species for pollutant removal via complete polymerization

Author

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  • Hong-Zhi Liu

    (University of Science and Technology of China)

  • Xiao-Xuan Shu

    (University of Science and Technology of China)

  • Mingjie Huang

    (University of Science and Technology of China
    Huazhong University of Science and Technology)

  • Bing-Bing Wu

    (University of Science and Technology of China)

  • Jie-Jie Chen

    (University of Science and Technology of China)

  • Xi-Sheng Wang

    (University of Science and Technology of China)

  • Hui-Lin Li

    (University of Science and Technology of China)

  • Han-Qing Yu

    (University of Science and Technology of China)

Abstract

Polymerization-driven removal of pollutants in advanced oxidation processes (AOPs) offers a sustainable way for the simultaneous achievement of contamination abatement and resource recovery, supporting a low-carbon water purification approach. However, regulating such a process remains a great challenge due to the insufficient microscopic understanding of electronic structure-dependent reaction mechanisms. Herein, this work probes the origin of catalytic pollutant polymerization using a series of transition metal (Cu, Ni, Co, and Fe) single-atom catalysts and identifies the d-band center of active site as the key driver for polymerization transfer of pollutants. The high-valent metal-oxo species, produced via peroxymonosulfate activation, are found to trigger the pollutant removal via polymerization transfer. Phenoxyl radicals, identified by the innovative spin-trapping and quenching approaches, act as the key intermediate in the polymerization reactions. More importantly, the oxidation capacity of high-valent metal-oxo species can be facilely tuned by regulating their binding strength for peroxymonosulfate through d-band center modulation. A 100% polymerization transfer ratio is achieved by lowering the d-band center. This work presents a paradigm to dynamically modulate the electronic structure of high-valent metal-oxo species and optimize pollutant removal from wastewater via polymerization.

Suggested Citation

  • Hong-Zhi Liu & Xiao-Xuan Shu & Mingjie Huang & Bing-Bing Wu & Jie-Jie Chen & Xi-Sheng Wang & Hui-Lin Li & Han-Qing Yu, 2024. "Tailoring d-band center of high-valent metal-oxo species for pollutant removal via complete polymerization," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46739-1
    DOI: 10.1038/s41467-024-46739-1
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    1. Yan Meng & Yu-Qin Liu & Chao Wang & Yang Si & Yun-Jie Wang & Wen-Qi Xia & Tian Liu & Xu Cao & Zhi-Yan Guo & Jie-Jie Chen & Wen-Wei Li, 2024. "Nanoconfinement steers nonradical pathway transition in single atom fenton-like catalysis for improving oxidant utilization," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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