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

Hong-Zhi Liu, Xiao-Xuan Shu, Mingjie Huang (), Bing-Bing Wu, Jie-Jie Chen (), Xi-Sheng Wang, Hui-Lin Li and Han-Qing Yu ()
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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
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

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-46739-1

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