Skip to main content
Log in

Superior degradation of phenolic contaminants in different water matrices via non-radical Fenton-like mechanism mediated by surface-disordered WO3

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Heterogeneous Fenton-like catalysis mediated by solid catalyst is a promising oxidation technology for water purification. The redox reactivity, cost-effectiveness, and environmental compatibility of solid catalyst play governing roles in oxidant activation, radical generation, and pollutant degradation. Herein, the surface-disordered WO3 (D-WO3) functionally engineered by the unique crystalline-amorphous core–shell structure is proven to be a superior solid catalyst of heterogeneous Fenton-like catalysis for peroxymonosulfate (PMS) activation and pollutant degradation in various water matrices. Six typical phenolic and dye pollutants are effectively and selectively degraded in the D-WO3/PMS system with much reduced matrix effects. Both radical identifying and scavenging tests elucidate the important role of non-radical 1O2 and mediated electron transfer during PMS activation on the D-WO3 surface. The superior Fenton-like activity of D-WO3 can be mainly attributed to the surface and sub-surface distorted lattice sites with finely tailored atomic and electronic structures and surface chemistry. These distorted lattice sites can thermodynamically serve as the key reactive centers of dissociative adsorption and catalytic activation for both PMS and pollutant, with high adsorption energy, strong structural activation, and smooth electron transfer. Our findings provide a new chance for heterogeneous Fenton-like catalysis mediated by transition metal oxides with high capacity, low cost, and no toxicity for promising water purification.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Scheme 1

Similar content being viewed by others

Data availability

The data sets used during the current study are available from the corresponding author on reasonable request.

References

  • Ahn Y-Y, Yun E-T, Seo J-W, Lee C, Kim SH, Kim J-H, Lee J (2016) Activation of peroxymonosulfate by surface-loaded noble metal nanoparticles for oxidative degradation of organic compounds. Environ Sci Technol 50:10187–10197

    Article  CAS  Google Scholar 

  • Anantharaj S, Noda S (2020) Amorphous catalysts and electrochemical water splitting: an untold story of harmony. Small 16:1905779

    Article  CAS  Google Scholar 

  • Anipsitakis GP, Dionysiou DD (2004) Radical generation by the interaction of transition metals with common oxidants. Environ Sci Technol 38:3705–3712

    Article  CAS  Google Scholar 

  • Antonopoulou M, Evgenidou E, Lambropoulou D, Konstantinou I (2014) A review on advanced oxidation processes for the removal of taste and odor compounds from aqueous media. Water Res 53:215–234

    Article  CAS  Google Scholar 

  • Awfa D, Ateia M, Fuji M, Johnson MS, Yoshimura C (2018) Photodegradation of pharmaceuticals and personal care products in water treatment using carbonaceous-TiO2 composites: a critical review of recent literature. Water Res 142:26–45

    Article  CAS  Google Scholar 

  • Behara DK, Ummireddi AK, Aragonda V, Gupta PK, Pala RGS, Sivakumar S (2016) Coupled optical absorption, charge carrier separation, and surface electrochemistry in surface disordered/hydrogenated TiO2 for enhanced PEC water splitting reaction. Phys Chem Chem Phys 188:364–8377

    Google Scholar 

  • Duan XG, Sun HQ, Kang J, Wang YX, Indrawirawan S, Wang SB (2015a) Insights into heterogeneous catalysis of persulfate activation on dimensional-structured nanocarbons. ACS Catal 5:4629–4636

    Article  CAS  Google Scholar 

  • Duan XG, Sun HQ, Wang SB (2018) Metal-free carbocatalysis in advanced oxidation reactions. Acc Chem Res 51:678–687

    Article  CAS  Google Scholar 

  • Duan XG, Sun HQ, Wang YX, Kang J, Wang SB (2015b) N-doping-induced nonradical reaction on single-walled carbon nanotubes for catalytic phenol oxidation. ACS Catal 5:553–559

    Article  CAS  Google Scholar 

  • Guan CT, Jiang J, Pang SY, Luo CW, Ma J, Zhou Y, Yang Y (2017) Oxidation kinetics of bromophenols by nonradical activation of peroxydisulfate in the presence of carbon nanotube and formation of brominated polymeric products. Environ Sci Technol 51:10718–10728

    Article  CAS  Google Scholar 

  • Huang KZ, Zhang HC (2019) Direct electron-transfer-based peroxymonosulfate activation by iron-doped manganese oxide (δ-MnO2) and the development of galvanic oxidation processes. Environ Sci Technol 53:12610–12620

    Article  CAS  Google Scholar 

  • Huang Y, Kong MH, Coffin S, Cochran KH, Westerman DC, Schlenk D, Richardson SD, Lei LC, Dionysiou DD (2020) Degradation of contaminants of emerging concern by UV/H2O2 for water reuse: kinetics, mechanisms, and cytotoxicity analysis. Water Res 174:115587

    Article  CAS  Google Scholar 

  • Hu PD, Su HR, Chen ZY, Yu CY, Li QL, Zhou BX, Alvarez PJJ, Long MC (2017) Selective degradation of organic pollutants using an efficient metal-free catalyst derived from carbonized polypyrrole via peroxymonosulfate activation. Environ Sci Technol 51:11288–11296

    Article  CAS  Google Scholar 

  • Kim J, Lee CW, Choi W (2010) Platinized WO3 as an environmental photocatalyst that generates OH radicals under visible light. Environ Sci Technol 44:6849–6854

    Article  CAS  Google Scholar 

  • Koo MS, Chen XF, Cho K, An TC, Choi W (2019) In situ photoelectrochemical chloride activation using a WO3 electrode for oxidative treatment with simultaneous H2 evolution under visible light. Environ Sci Technol 53:9926–9936

    Article  CAS  Google Scholar 

  • Lee H, Kim H-i, Weon S, Choi W, Hwang YS, Seo J, Lee C, Kim J-H (2016) Activation of persulfates by graphitized nanodiamonds for removal of organic compounds. Environ Sci Technol 50:10134–10142

    Article  CAS  Google Scholar 

  • Lee H, Lee H-J, Jeong J, Lee J, Park N-B, Lee C (2015) Activation of persulfates by carbon nanotubes: oxidation of organic compounds by nonradical mechanism. Chem Eng J 266:28–33

    Article  CAS  Google Scholar 

  • Li XT, Ma JZ, Yang L, He GZ, Zhang CB, Zhang RD, He H (2018) Oxygen vacancies induced by transition metal doping in γ-MnO2 for highly efficient ozone decomposition. Environ Sci Technol 52:12685–12696

    Article  CAS  Google Scholar 

  • Lindsey ME, Tarr MA (2000) Inhibition of hydroxyl radical reaction with aromatics by dissolved natural organic matter. Environ Sci Technol 34:444–449

    Article  CAS  Google Scholar 

  • Liu C, Min Y, Zhang A-Y, Si Y, Chen J-J, Yu H-Q (2019) Electrochemical treatment of phenol-containing wastewater by facet-tailored TiO2: efficiency, characteristics and mechanisms. Water Res 165:114980

    Article  CAS  Google Scholar 

  • Liu Z, Ren BX, Ding HJ, He H, Deng HP, Zhao C, Wang P, Dionysiou DD (2020) Simultaneous regeneration of cathodic activated carbon fiber and mineralization of desorbed contaminations by electro-peroxydisulfate process: advantages and limitations. Water Res 171:115456

    Article  CAS  Google Scholar 

  • Luo XB, Deng F, Min LJ, Luo SL, Guo B, Zeng GS, Au C (2013) Facile one-step synthesis of inorganic-framework molecularly imprinted TiO2/WO3 nanocomposite and its molecular recognitive photocatalytic degradation of target contaminant. Environ Sci Technol 47:7404–7412

    Article  CAS  Google Scholar 

  • Miao J, Geng W, Alvarez PJJ, Long MC (2020) 2D N-doped porous carbon derived from polydopamine-coated graphitic carbon nitride for efficient nonradical activation of peroxymonosulfate. Environ Sci Technol 54:8473–8481

    Article  CAS  Google Scholar 

  • Ren W, Xiong LL, Yuan XH, Yu ZW, Zhang H, Duan XG, Wang SB (2019) Activation of peroxydisulfate on carbon nanotubes: electron-transfer mechanism. Environ Sci Technol 53:14595–14603

    Article  CAS  Google Scholar 

  • Sun ZQ, Zhao L, Liu CH, Zhen YF, Ma J (2019) Catalytic ozonation of ketoprofen with in situ N-doped carbon: a novel synergetic mechanism of hydroxyl radical oxidation and an intra-electron-transfer nonradical reaction. Environ Sci Technol 53:10342–10351

    Article  CAS  Google Scholar 

  • Westerhoff P, Aiken G, Amy G, Debroux J (1999) Relationships between the structure of natural organic matter and its reactivity towards molecular ozone and hydroxyl radicals. Water Res 33:2265–2276

    Article  CAS  Google Scholar 

  • Yang ZC, Qian JS, Yu AQ, Pan BC (2019) Singlet oxygen mediated iron-based Fenton-like catalysis under nanoconfinement. Proc Natl Acad Sci USA 116:6659–6664

    Article  CAS  Google Scholar 

  • Yao JY, Yu Y, Qu RJ, Chen J, Huo ZL, Zhu F, Wang ZY (2020) Fe-activated peroxymonosulfate enhances the degradation of dibutyl phthalate on ground quartz sand. Environ Sci Technol 54:9052–9061

    Article  CAS  Google Scholar 

  • Yun E-T, Lee JH, Kim J, Park H-D, Lee J (2018) Identifying the nonradical mechanism in the peroxymonosulfate activation process: singlet oxygenation versus mediated electron transfer. Environ Sci Technol 52:7032–7042

    Article  CAS  Google Scholar 

  • Yun E-T, Yoo H-Y, Bae H, Kim H-I, Lee J (2017) Exploring the role of persulfate in the activation process: radical precursor versus electron acceptor. Environ Sci Technol 51:10090–10099

    Article  CAS  Google Scholar 

  • Zhang A-Y, He Y-Y, Chen Y-P, Feng J-W, Huang N-H, Lian F (2020a) Degradation of organic pollutants by Co3O4-mediated peroxymonosulfate oxidation: roles of high-energy {001}-exposed TiO2 support. Chem Eng J 334:1430–1439

    Article  CAS  Google Scholar 

  • Zhang A-Y, Zhao P-C, He Y-Y, Zhou Y, Feng J-W (2020b) Non-radical activation of H2O2 by surface-disordered WO3 for efficient and selective pollutants degradation with weak matrix effects. Environ Sci Poll Res 27:1898–1911

    Article  CAS  Google Scholar 

  • Zhang T, Chen Y, Wang YR, Roux JL, Yang Y, Croué J-P (2014) Efficient peroxydisulfate activation process not relying on sulfate radical generation for water pollutant degradation. Environ Sci Technol 48:5868–5875

    Article  CAS  Google Scholar 

  • Zhu SS, Huang XC, Ma F, Wang L, Duan XG, Wang SB (2018) Catalytic removal of aqueous contaminants on N-doped graphitic biochars: inherent roles of adsorption and nonradical mechanisms. Environ Sci Technol 52:8649–8658

    Article  CAS  Google Scholar 

Download references

Funding

This work is supported by the National Natural Science Foundation of China (21876040, 22076036), the Fundamental Research Funds for the Central Universities (PA2021KCPY0031), and the Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (No. ESK202105).

Author information

Authors and Affiliations

Authors

Contributions

AYZ, SX, and PCZ conceptualized and conducted the experiment. AYZ, HL, and JFW wrote the manuscript. AYZ and HL supervised the work. JWF and PCZ conducted the literature review and compiled the overall manuscript.

Corresponding authors

Correspondence to Ai-Yong Zhang or Heng Liang.

Ethics declarations

Ethics approval

Not applicable.

Consent to participate

Not applicable.

Consent for publication

Not applicable.

Competing interests

The authors declare no competing interests.

Additional information

Responsible Editor: Ricardo A. Torres-Palma

Publisher's note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 2668 KB)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, AY., Xu, S., Feng, JW. et al. Superior degradation of phenolic contaminants in different water matrices via non-radical Fenton-like mechanism mediated by surface-disordered WO3. Environ Sci Pollut Res 29, 18259–18270 (2022). https://doi.org/10.1007/s11356-021-17088-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-021-17088-z

Keywords

Navigation