Key Role of Persistent Free Radicals in Hydrogen Peroxide Activation by Biochar: Implications to Organic Contaminant Degradation
Abstract
We investigated the activation of hydrogen peroxide (H2O2) by biochars (produced from pine needles, wheat, and maize straw) for 2-chlorobiphenyl (2-CB) degradation in the present study. It was found that H2O2 can be effectively activated by biochar, which produces hydroxyl radical ((•)OH) to degrade 2-CB. Furthermore, the activation mechanism was elucidated by electron paramagnetic resonance (EPR) and salicylic acid (SA) trapping techniques. The results showed that biochar contains persistent free radicals (PFRs), typically ∼ 10(18) unpaired spins/gram. Higher trapped [(•)OH] concentrations were observed with larger decreases in PFRs concentration, when H2O2 was added to biochar, indicating that PFRs were the main contributor to the formation of (•)OH. This hypothesis was supported by the linear correlations between PFRs concentration and trapped [(•)OH], as well as kobs of 2-CB degradation. The correlation coefficients (R(2)) were 0.723 and 0.668 for PFRs concentration vs trapped [(•)OH], and PFRs concentration vs kobs, respectively, when all biochars pyrolyzed at different temperatures were included. For the same biochar washed by different organic solvents (methanol, hexane, dichloromethane, and toluene), the correlation coefficients markedly increased to 0.818-0.907. Single-electron transfer from PFRs to H2O2 was a possible mechanism for H2O2 activation by biochars, which was supported by free radical quenching studies. The findings of this study provide a new pathway for biochar implication and insight into the mechanism of H2O2 activation by carbonaceous materials (e.g., activated carbon and graphite).
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The mechanistic route is predominantly controlled by one-electron transfer from EPFRs towards H2O2 molecules, confirmed by a linear correlation among EPFRs density, •OH characteristic signal intensity, and pollutant degradation rate constant.
“The mechanistic route was predominantly controlled by one-electron transfer from EPFRs towards H2O2 molecules, which was confirmed by a linear correlation among EPFRs density, • OH characteristic signal intensity, as well as pollutant degradation rate constant.”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [128]
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- Authors
- Fang, G., Gao, J., Liu, C., Dionysiou, D. D., Wang, Y., & Zhou, D.
- Affiliations
- Chinese Academy of Sciences (CN)
- University of Cincinnati (US)
- Corresponding author
- Zhou, Dongmei
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-01-21
- Volume
- 48
- Issue
- 3
- Pages
- 1902-1910
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2031933809
- Cited by
- 802
- References
- 67
- Citations by year
- 2026: 62 · 2025: 79 · 2024: 96 · 2023: 107 · 2022: 90 · 2021: 96 · 2020: 94 · 2019: 70 · 2018: 42 · 2017: 29 · 2016: 18 · 2015: 12 · 2014: 4
- FWCI
- 15.82
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Environmental Science & Technology (publishedVersion)
- PubMed (publishedVersion)
- Funders
- National Science Foundation
- National Natural Science Foundation of China
- National Key Research and Development Program of China
- Topics
- Physical Sciences › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
- Physical Sciences › Environmental Science › Water Science and Technology › Adsorption and biosorption for pollutant removal
- Physical Sciences › Engineering › Biomedical Engineering › Environmental remediation with nanomaterials
- Keywords
- biochar, hydrogen peroxide activation, persistent free radicals, hydroxyl radicals, 2-chlorobiphenyl, organic pollutant degradation, wheat straw biochar, maize straw biochar, pyrolysis temperature, single electron transfer, free radical quenching, advanced oxidation processes
- MeSH terms
- Biphenyl Compounds, Charcoal, Zea mays, Electron Spin Resonance Spectroscopy, Environmental Pollutants, Free Radicals, Hydrogen Peroxide, Triticum, Hydroxyl Radical, Pinus
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