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Research Article

Generating 1O2 and CoIV=O through efficient peroxymonosulfate activation by ZnCo2O4 nanosheets for pollutant control

Xiaoke Zhang1,§, Yangyang Zhang1,§, Jiaqi Tian1, Yadan Guo3, Zhongkui Zhou3, Zhongyi Liu1,2( ), Zaiwang Zhao5, Bin Liu4, Jun Li1( )
College of Chemistry, Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou 450052, China
State Key Laboratory of Coking Coal Resources Green Exploitation, Zhengzhou University, Zhengzhou 450001, China
School of Water Resources and Environmental Engineering, East China University of Technology, Nanchang 330013, China
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China
College of Energy Materials and Chemistry, College of Chemistry and Chemical Engineering, InnerMongolia University, Hohhot 010070, China

§ Xiaoke Zhang and Yangyang Zhang contributed equally to this work.

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Graphical Abstract

A series of surface Co defect-rich spinel ZnCo2O4 porous nanosheets were successfully synthesized, and employed for peroxymonosulfate activation to generate ≡CoIV=O and 1O2 over a wide pH range. This work demonstrates a functional catalyst with high activity and stability, paving the way for the design of highly efficient heterogeneous catalysts for phenolic pollutant degradation.

Abstract

Heterogeneous advanced oxidation processes (AOPs) based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH range. Herein, we fabricate surface Co defect-rich spinel ZnCo2O4 porous nanosheets, which can generate ≡CoIV=O and 1O2 over a wide pH range of 3.81–10.96 by the formation of amphoteric ≡Zn(OH)2 in peroxymonosulfate (PMS) activation process. Density functional theory (DFT) calculations show Co defect-rich ZnCo2O4 possesses much stronger adsorption ability and more electron transfer to PMS. Moreover, the adsorption mode changes from terminal oxygen Co–O–Co to Co–O, accelerating the polarization of adjacent oxygen, which is beneficial to the generation of ≡CoIV=O and 1O2. Co defect-rich ZnCo2O4 porous nanosheets exhibit highly active PMS activation activity and stability in p-nitrophenol (PNP) degradation, whose toxicity of degradation intermediates is significant reduction. The Co defect-rich ZnCo2O4 nanosheet catalyst sponge/PMS system achieved stable and efficient removal of PNP with a removal efficiency higher than 93% over 10 h. This work highlights the development of functional catalyst and provides an atomic-level understanding into non-radical PMS activation process in wastewater treatment.

Keywords

advanced oxidation processesZnCo2O4 nanosheetsperoxymonosulfate activationCoIV=Owastewater treatment

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Nano Research
Volume 17 Issue 9,
September 2024
Pages 8025-8035
DOI: 10.1007/s12274-024-6836-6
Cite this article:
Zhang X, Zhang Y, Tian J, et al. Generating 1O2 and CoIV=O through efficient peroxymonosulfate activation by ZnCo2O4 nanosheets for pollutant control. Nano Research, 2024, 17(9): 8025-8035. https://doi.org/10.1007/s12274-024-6836-6
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Received: 22 April 2024
Revised: 03 June 2024
Accepted: 22 June 2024
Published: 25 July 2024
© Tsinghua University Press 2024
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