Dynamic active-site induced by host-guest interactions boost the Fenton-like reaction for organic wastewater treatment

Dongpeng Zhang, Yanxiao Li, Pengfei Wang, Jinyong Qu, Yi Li () and Sihui Zhan ()
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Dongpeng Zhang: Nankai University
Yanxiao Li: Nankai University
Pengfei Wang: Hebei University of Technology
Jinyong Qu: Nankai University
Yi Li: Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Sihui Zhan: Nankai University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract In heterogeneous catalysis, uncovering the dynamic evolution of active sites in the working conditions is crucial to realizing increased activity and enhanced stability of catalyst in Fenton-like activation. Herein, we capture the dynamic changes in the unit cell of Co/La-SrTiO3 catalyst during the exemplary peroxymonosulfate activation process using X-ray absorption spectroscopy and in situ Raman spectroscopy, revealing the substrate tuned its structural evolution, which is the reversible stretching vibration of O-Sr-O and Co/Ti-O bonds in different orientations. This process effectively promotes the generation of key SO5* intermediates, which is beneficial to the formation of 1O2 and SO4•− from persulfate on the Co active site. Density functional theory and X-ray absorption spectroscopy show that the optimized structural distortion enhanced the metal-oxygen bond strength by tuning the eg orbitals and increased the number of transferred electrons to peroxymonosulfate by about 3-fold, achieving excellent efficiency and stability in removing organic pollutants.

Date: 2023
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DOI: 10.1038/s41467-023-39228-4

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