Harnessing air-water interface to generate interfacial ROS for ultrafast environmental remediation

Ruijie Xie, Kaiheng Guo, Yong Li, Yingguang Zhang, Huanran Zhong, Dennis Y. C. Leung and Haibao Huang ()
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Ruijie Xie: Sun Yat-sen University
Kaiheng Guo: Sun Yat-sen University
Yong Li: University of Bremen
Yingguang Zhang: The University of Hong Kong
Huanran Zhong: Sun Yat-sen University
Dennis Y. C. Leung: The University of Hong Kong
Haibao Huang: Sun Yat-sen University

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

Abstract: Abstract The air-water interface of microbubbles represents a crucial microenvironment that can dramatically accelerate reactive oxidative species (ROS) reactions. However, the dynamic nature of microbubbles presents challenges in probing ROS behaviors at the air-water interface, limiting a comprehensive understanding of their chemistry and application. Here we develop an approach to investigate the interfacial ROS via coupling microbubbles with a Fenton-like reaction. Amphiphilic single-Co-atom catalyst (Co@SCN) is employed to efficiently transport the oxidant peroxymonosulfate (PMS) from the bulk solution to the microbubble interface. This triggers an accelerated generation of interfacial sulfate radicals (SO4•−), with 20-fold higher concentration (4.48 × 10−11 M) than the bulk SO4•−. Notably, the generated SO4•− is preferentially situated at the air-water interface due to its lowest free energy and the strong hydrogen bonding interactions with H3O+. Moreover, it exhibits the highest oxidation reactivity toward gaseous pollutants like toluene, with a rate constant of 1010 M−1 s−1-over 100 times greater than bulk reactions. This work demonstrates a promising strategy to harness the air-water interface for accelerating ROS-induced reactions, highlighting the importance of interfacial ROS and its potential application.

Date: 2024
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DOI: 10.1038/s41467-024-53289-z

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