Activation of peroxymonosulfate by Cu-Ni-Fe layered double oxides for degradation of butyl 4-hydroxybenzoate: Synergistic effect of oxygen vacancy and Cu(I)

Huiwang Dai; Jingyi Zhu; Fanxu Meng; Daohui Lin; Wenjun Zhou; Dingjiang Chen; Ming Zhang; Qingqing Wang

doi:10.1016/j.chemosphere.2023.140253

Activation of peroxymonosulfate by Cu-Ni-Fe layered double oxides for degradation of butyl 4-hydroxybenzoate: Synergistic effect of oxygen vacancy and Cu(I)

Chemosphere. 2023 Dec:343:140253. doi: 10.1016/j.chemosphere.2023.140253. Epub 2023 Sep 21.

Authors

Huiwang Dai¹, Jingyi Zhu², Fanxu Meng², Daohui Lin¹, Wenjun Zhou³, Dingjiang Chen⁴, Ming Zhang⁵, Qingqing Wang⁶

Affiliations

¹ Zhejiang Ecological Civilization Academy, Anji, Zhejiang, 310058, China; Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang, 310058, China.
² Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang, 310058, China.
³ Zhejiang Ecological Civilization Academy, Anji, Zhejiang, 310058, China; Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang, 310058, China. Electronic address: wenjunzhou@zju.edu.cn.
⁴ Zhejiang Ecological Civilization Academy, Anji, Zhejiang, 310058, China; Institute of Soil and Water Resources and Environmental Science, Zhejiang University, Hangzhou, Zhejiang, 310058, China.
⁵ Department of Environment Engineering, China Jiliang University, Hangzhou, 310018, China.
⁶ DeQing Environmental Monitoring Station, Huzhou, Zhejiang, 313200, China.

PMID: 37741373
DOI: 10.1016/j.chemosphere.2023.140253

Abstract

In this study, Cu hybridization coupling oxygen defect engineering was adopted to synthesis of CuNiFe layered double oxides (CuNiFe-LDOs) in peroxymonosulfate (PMS) activation for degradation of methyl 4-hydroxybenzoate. The morphology and crystal structure of CuNiFe-LDOs was characterized in detail, which exhibited regular layered-structure at a Cu:Ni doping ratio of 1:1 and annealing temperature of 400 °C, and presented the crystal of Cu_xO@Fe₃O₄-NiO. Besides, the X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) results demonstrated that abundant oxygen vacancies (OVs) and low oxidation state Cu species were composed in CuNiFe-LDOs400. The Cu_1·5Ni_1·5Fe₁-LDOs400/PMS system showed excellent catalytic performance toward the degradation of butyl 4-hydroxybenzoate (BuP), and resistant to the effect of pH value and background inorganic anions. Based on quenching experiments and EPR measurements, singlet oxygen (¹O₂) was identified as the dominant active species during the heterogeneous catalytic process, which was generated by the synergistic interaction between OVs-Cu(I) site and PMS. In this process, the electron-drawing property of OVs promoted the adsorption of PMS molecule on Cu(I) site, followed by the accumulation of electron and cleavage of O-O bond to generate intermediate oxygen radical species, which donated one electron to eventually generate singlet oxygen.

Keywords: Layered double oxides; Oxygen vacancies; Peroxymonosulfate activation; Singlet oxygen.

MeSH terms

Oxides*
Oxygen*
Peroxides / chemistry
Singlet Oxygen

Substances

peroxymonosulfate
Oxygen
Oxides
4-hydroxybenzoic acid
Singlet Oxygen
Peroxides
butylparaben