Insights into Heterogeneous Catalysis of Persulfate Activation on Dimensional-Structured Nanocarbons
Abstract
A variety of dimensional-structured nanocarbons were applied for the first time as metal-free catalysts to activate persulfate (PS) for catalytic oxidation of phenolics and dyes as well as their degradation intermediates. Single-walled carbon nanotubes (SWCNTs), reduced graphene oxide (rGO), and mesoporous carbon (CMK-8) demonstrated superior catalytic activities for heterogeneous PS activation, whereas fullerene (C 60 ), nanodiamonds, and graphitic carbon nitride (g-C 3 N 4 ) presented low efficiencies. Moreover, the carbocatalysts presented even better catalytic performances than activated carbon and metal oxides, such as Fe 3 O 4, CuO, Co 3 O 4, and MnO 2 . The activity of prepared rGO-900 was further competing to the most efficient electron donor of zerovalent iron (ZVI). Both characterization and oxidation results suggested that the catalytic performances of the nanocarbons are determined by the intrinsic atom arrangements of carbon hybridization, pore structure, defective sites, and functional groups (especially the carbonyl groups). Electron paramagnetic resonance (EPR) spectra revealed that carbocatalysts might act as an excellent electron bridge in activation of PS to oxidize adsorbed water directly to generate hydroxyl radicals, distinct from homogeneous and metal-based catalytic activation. This study discovers several efficient nanocarbons for heterogeneous PS activation, and it presents new insights into the catalytic activation processes, providing a fascinating strategy to develop metal-free catalysts for green remediation.
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Molecular arrangement of carbon materials is typically associated with adsorption capacity towards organic compounds, following the order 0D (fullerene and nanodiamonds) < 1D (single-walled or multi-walled carbon nanotubes) < 2D (graphene and graphitic carbon nitride) < 3D (cubic mesoporous carbon, AC, and biochar).
“Molecular arrangement of carbon materials are typically associated with adsorption capacity towards organic compounds, which sequentially follows 0D (fullerene and nanodiamonds) < 1D (single-walled or multi-walled carbon nanotubes) < 2D (graphene and graphitic carbon nitride) <3D (cubic mesoporous carbon, AC, and biochar).1”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [1]
Nanodiamonds with a sp3-hybridized core coated with amorphous carbon layer are ineffective for electron abstraction in PDS activation, whereas rGO-900 with sp2-hybridized lattices and plentiful defective sites, non-hexagonal units, and RAMs demonstrates superior electroactive performance for catalytic reactions.
“Previously, nanodiamonds that possesses a sp 3 -hybridized core and coated with amorphous carbon layer were found to be ineffective for electron abstraction in PDS activation, while rGO-900 with sp 2 -hybridized lattices and plentiful defective sites, non-hexagonal units, and RAMs demonstrated superior electroactive performance for catalytic reactions.1”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [1]
Highly conductive graphitic carbonaceous interfaces such as fullerene and graphitic carbon nitride are ineffective at initiating electron-based carbocatalysis.
“Nonetheless, the highly conductive graphitic carbonaceous interfaces such as fullerene and graphitic carbon nitride were ineffective to initiate the electron-based carbocatalysis, 1”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [1]
Since Wang et al. reported superior catalytic performance of various nanocarbons that primarily stemmed from open sp2-hybridized carbon matrices with rich zigzag/armchair edges and vacancy defects, structural engineering with reactive defective sites has been an emerging technique applied in the carbon-involved environmental field.
“Since Wang et al. reported the superior catalytic performance of various nanocarbons, which primarily stemmed from the open sp 2 -hybridized carbon matrices with rich zigzag/armchain edges and vacancy defects, 1 structural engineering with reactive defective sites has been an emerging technique applied in carbon-involved environmental field.”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [1]
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Self-citation
- Authors
- Duan, X., Sun, H., Kang, J., Wang, Y., Indrawirawan, S., & Wang, S.
- Affiliations
- Curtin University (AU)
- Corresponding author
- Sun, Hongqi
- Wang, Shaobin
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-07-07
- Volume
- 5
- Issue
- 8
- Pages
- 4629-4636
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2266953687
- Cited by
- 799
- References
- 40
- Citations by year
- 2026: 42 · 2025: 66 · 2024: 61 · 2023: 100 · 2022: 113 · 2021: 101 · 2020: 103 · 2019: 83 · 2018: 63 · 2017: 42 · 2016: 21 · 2015: 3
- FWCI
- 28.47
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- ACS Catalysis (publishedVersion)
- Adelaide Research & Scholarship (AR&S) (University of Adelaide) (submittedVersion)
- eSpace (Curtin University) (submittedVersion)
- Funders
- Australian Research Council (DP130101319)
- Curtin University of Technology
- Topics
- Physical Sciences › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
- Physical Sciences › Engineering › Biomedical Engineering › Environmental remediation with nanomaterials
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
- Keywords
- persulfate activation, heterogeneous catalysis, metal-free catalysts, single-walled carbon nanotubes, reduced graphene oxide, mesoporous carbon, C60, nanodiamonds, graphitic carbon nitride, phenolic compounds, dye degradation, hydroxyl radicals, electron transfer, carbonyl compounds, carbon defects, zero-valent iron, water remediation
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