Edge-nitrogenated biochar for efficient peroxydisulfate activation: An electron transfer mechanism
Abstract
N-doped biochars (NBCs) were prepared by pyrolyzing corncob biomass and urea in different proportion which manifested superior catalytic performance of peroxydisulfate (PDS) activation for sulfadiazine (SDZ) degradation. Through both dynamic fitting and density functional theory (DFT) calculations, the critical role of edge nitrogenation in biochar (BC) structure was revealed for the first time. The incorporation of edge nitrogen configurations (pyridinic N and pyrrolic N rather than graphitic N) generated reactive sites for the PDS activation. Additionally, a thorough investigation was conducted to explicate the PDS activation mechanism by NBC through chemical quenching experiments, electron spin resonance (ESR) detection, oxidant consumption monitoring and electrochemical analysis. Different from the well-reported singlet oxygen (1 O 2) dominated nonradical mechanism, an electron transfer pathway involving surface-bound reactive complexes was proved to play a major role in the NBC/PDS system. Benefit from the electron transfer mechanism, the NBC/PDS system not only has wide pH adaptation for real application, but also shows high resistance to the inorganic anions in aquatic environment. We believe this study will deepen the understanding of the carbon-driven persulfate activation mechanism and provide strong technical support for the BC-mediated persulfate activation in practical applications.
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Urea-derived N functionalization of biochar preferentially introduced pyrrolic N and pyridinic N, with no regularity found for graphitic N.
“Nevertheless, opposite findings were observed that urea-derived N functionalization for biochar led to preferential introduction of pyrrolic N and pyridinic N while no regularity was found for graphitic N. 35”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [35]
Edge-nitrogenated biochar functionalized with large amounts of pyrrolic N and pyridinic N can evolve formation of surface-bound reactive PDS complexes followed by direct electron abstraction to degrade pollutants.
“The edge-nitrogenated biochar functionalized with large amount of pyrrolic N and pyridinic N was able to evolve the formation of surface-bound reactive PDS complexes followed with a direct electron abstraction process to degrade pollutants.”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [35]
Irrespective of specific N dopants, both edge-nitrogenated biochar with pyrrolic N and pyridinic N and N-doped biochar functionalized with graphitic N prompt generation of surface-bound reactive complexes that subsequently attack organic pollutants via a direct electron transfer regime along the graphitic carbon lattice.
“Irrespective of the specific N dopants, both the edge-nitrogenated (pyrrolic N and pyridinic N) biochar and the N-doped biochar functionalized with graphitic N were testified to prompt the generation of surface-bound reactive complexes that subsequently attacked organic pollutants via a direct electron transfer regime along the graphitic carbon lattice.34,35”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [35]
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- Authors
- Wang, H., Guo, W., Liu, B., Wu, Q., Luo, H., Zhao, Q., Si, Q., Sseguya, F., & Ren, N.
- Affiliations
- Harbin Institute of Technology (CN)
- Corresponding author
- Guo, Wanqian
- Venue
- Water Research
- Publisher
- Elsevier BV
- Published
- 2019-09
- Volume
- 160
- Pages
- 405-414
- ISSN
- 0043-1354 (ISSN-L)
- OpenAlex
- W2946447261
- Cited by
- 914
- References
- 59
- Citations by year
- 2026: 91 · 2025: 144 · 2024: 156 · 2023: 166 · 2022: 181 · 2021: 113 · 2020: 52 · 2019: 11
- FWCI
- 32.29
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Water Research (publishedVersion)
- PubMed (publishedVersion)
- Funders
- National Natural Science Foundation of China of China (51678188)
- State Key Laboratory of Urban Water Resource and Environment (2015TS06)
- Topics
- Physical Sciences › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
- Physical Sciences › Engineering › Biomedical Engineering › Environmental remediation with nanomaterials
- Physical Sciences › Environmental Science › Health, Toxicology and Mutagenesis › Water Treatment and Disinfection
- Keywords
- N-doped biochar, persulfate activation, sulfadiazine degradation, electron transfer mechanism, pyridinic nitrogen, pyrrolic nitrogen, anion resistance, pH adaptation, antibiotic removal
- MeSH terms
- Catalysis, Charcoal, Electrons, Graphite
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