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Uniform Mesoporous Amorphous Cobalt-Inherent Silicon Oxide as a Highly Active Heterogeneous Catalyst in the Activation of Peroxymonosulfate for Rapid Oxidation of 2,4-Dichlorophenol: The Important Role of Inherent Cobalt in the Catalytic Mechanism

  • Qiyu Lian
    Qiyu Lian
    Department of Civil Engineering, University of Louisiana at Lafayette, P.O. Box 43598, Lafayette, Louisiana 70504, United States
    Center for Environmental Technology, The Energy Institute of Louisiana, P.O. Box 43597, Lafayette, Louisiana 70504, United States
    More by Qiyu Lian
  • Amitava Roy
    Amitava Roy
    The J. Bennett Johnston, Sr., Center for Advanced Microstructures and Devices (CAMD), Baton Rouge, Louisiana 70806, United States
    More by Amitava Roy
  • Orhan Kizilkaya
    Orhan Kizilkaya
    The J. Bennett Johnston, Sr., Center for Advanced Microstructures and Devices (CAMD), Baton Rouge, Louisiana 70806, United States
  • Daniel Dianchen Gang*
    Daniel Dianchen Gang
    Department of Civil Engineering, University of Louisiana at Lafayette, P.O. Box 43598, Lafayette, Louisiana 70504, United States
    Center for Environmental Technology, The Energy Institute of Louisiana, P.O. Box 43597, Lafayette, Louisiana 70504, United States
    *Email: [email protected]. Phone (+1) 337-482-5184.
  • William Holmes
    William Holmes
    Center for Environmental Technology, The Energy Institute of Louisiana, P.O. Box 43597, Lafayette, Louisiana 70504, United States
    Department of Chemical Engineering, University of Louisiana at Lafayette, P.O. Box 43675, Lafayette, Louisiana 70504, United States
  • Mark E. Zappi
    Mark E. Zappi
    Department of Civil Engineering, University of Louisiana at Lafayette, P.O. Box 43598, Lafayette, Louisiana 70504, United States
    Center for Environmental Technology, The Energy Institute of Louisiana, P.O. Box 43597, Lafayette, Louisiana 70504, United States
    Department of Chemical Engineering, University of Louisiana at Lafayette, P.O. Box 43675, Lafayette, Louisiana 70504, United States
  • Xu Zhang
    Xu Zhang
    Beijing International Scientific and Technological Cooperation Base of Water Pollution Control Techniques for Antibiotics and Resistance Genes, School of Civil Engineering, Beijing Jiaotong University, 3 Shangyuancun, Beijing 100044, P. R. China
    More by Xu Zhang
  • , and 
  • Hong Yao
    Hong Yao
    Beijing International Scientific and Technological Cooperation Base of Water Pollution Control Techniques for Antibiotics and Resistance Genes, School of Civil Engineering, Beijing Jiaotong University, 3 Shangyuancun, Beijing 100044, P. R. China
    More by Hong Yao
Cite this: ACS Appl. Mater. Interfaces 2020, 12, 51, 57190–57206
Publication Date (Web):December 8, 2020
https://doi.org/10.1021/acsami.0c20341
Copyright © 2020 American Chemical Society
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Abstract

Amorphous cobalt-inherent silicon oxide (Co-SiOx) was synthesized for the first time and employed as a highly active catalyst in the activation of peroxymonosulfate (PMS) for the rapid oxidation of 2,4-dichlorophenol (2,4-DCP). The characterization results revealed that the 0.15Co-SiOx possessed a high specific surface area of 607.95 m2/g with a uniform mesoporous structure (24.33 nm). The X-ray diffraction patterns indicate that the substituted cobalt atoms enlarge the unit cell parameter of the original SiO2, and the selected area electron diffraction pattern confirmed the amorphous nature of Co-SiOx. More bulk oxygen vacancies (Ov) existing in the Co-SiOx were identified to be one of the primary contributors to the significantly enhanced catalytic activation of PMS. The cobalt substitution both creates and stabilizes the surficial Ov and forms the adequately active Co(II)–Ov pairs which engine the electron transfer process during the catalytic activities. The active Co(II)–Ov pairs weaken the average electronegativity of Co/Si and Co/O sites, resulting in the prevalent changes in final state energy, which is the main driving cause of the binding energy shifts in the X-ray photoelectron spectroscopy (XPS) spectra of Si and O among all samples. The increase of the relative proportion of Co(III) in the spent Co-SiOx probably causes the binding energy shifts of the Co XPS spectrum compared to that of the Co-SiOx. The amorphous Co-SiOx outperforms stable and quick 2,4-DCP degradation, achieving a much higher kinetic rate of 0.7139 min–1 at pH = 7.02 than others via sulfate radical advanced oxidation processes (AOPs), photo-Fenton AOPs, H2O2 reagent AOPs, and other AOP approaches. The efficient degradation performance makes the amorphous Co-SiOx as a promising catalyst in removing 2,4-DCP or organic-rich pollutants.

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Cited By


This article is cited by 4 publications.

  1. Leiduo Lai, Peng Zhou, Hongyu Zhou, Minglu Sun, Yue Yuan, Yang Liu, Gang Yao, Bo Lai. Heterogeneous Fe(III)/Fe(II) circulation in FeVO4 by coupling with dithionite towards long-lasting peroxymonosulfate activation: Pivotal role of vanadium as electron shuttles. Applied Catalysis B: Environmental 2021, 297 , 120470. https://doi.org/10.1016/j.apcatb.2021.120470
  2. Qiyu Lian, Fahrin Islam, Zaki Uddin Ahmad, Xiaobo Lei, Dilip Depan, Mark Zappi, Daniel D. Gang, William Holmes, Hui Yan. Enhanced adsorption of resorcinol onto phosphate functionalized graphene oxide synthesized via Arbuzov Reaction: A proposed mechanism of hydrogen bonding and π-π interactions. Chemosphere 2021, 280 , 130730. https://doi.org/10.1016/j.chemosphere.2021.130730
  3. Liang Wang, Yangyang Wang, Lili Zhang, Tong Li, Min Yang, Chun Hu. CoO anchored on boron nitride nanobelts for efficient removal of water contaminants by peroxymonosulfate activation. Chemical Engineering Journal 2021, 12 , 132915. https://doi.org/10.1016/j.cej.2021.132915
  4. Lihong Wang, Haodan Xu, Ning Jiang, Suyan Pang, Jin Jiang, Tao Zhang. Effective activation of peroxymonosulfate with natural manganese-containing minerals through a nonradical pathway and the application for the removal of bisphenols. Journal of Hazardous Materials 2021, 417 , 126152. https://doi.org/10.1016/j.jhazmat.2021.126152