Catalytic Removal of Aqueous Contaminants on N-Doped Graphitic Biochars: Inherent Roles of Adsorption and Nonradical Mechanisms
Abstract
Environmentally friendly and low-cost catalysts are important for the rapid mineralization of organic contaminants in powerful advanced oxidation processes (AOPs). In this study, we reported N-doped graphitic biochars (N-BCs) as low-cost and efficient catalysts for peroxydisulfate (PDS) activation and the degradation of diverse organic pollutants in water treatment, including Orange G, phenol, sulfamethoxazole, and bisphenol A. The biochars at high annealing temperatures (>700 °C) presented highly graphitic nanosheets, large specific surface areas (SSAs), and rich doped nitrogen. In particular, N-BC derived at 900 °C (N-BC900) exhibited the highest degradation rate, which was 39-fold and 6.5-fold of that on N-BC400 and pristine biochar, respectively, and the N-BC900 surpassed most popular metal or nanocarbon catalysts. Different from the radical-based oxidation in N-BC400/PDS via the persistent free radicals (PFRs), singlet oxygen and nonradical pathways (surface-confined activated persulfate-carbon complexes) were discovered to dominate the oxidation processes in N-BC900/PDS. Moreover, the adsorption of organics was determined to be the key step determining reaction rate, revealing that the pre-adsorption of reactants significantly accelerated the nonradical oxidation pathway. This study not only provides robust and cheap carbonaceous materials for environmental remediation but also enables the first insight into the graphitic biochar-based nonradical catalysis.
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Zhu et al. managed to fabricate a highly graphitized biochar with tailored defective degree under 900 °C pyrolysis.
“Typically, Zhu et al. managed to fabricate a highly graphitized biochar with tailored defective degree under 900 °C pyrolysis.This work revealed the reinforced adsorption capacity towards reactants associated with greater defective level could accelerate the formation of electrophilic oxyanion-carbon complexes oxidative to pollutants.36”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [36]
Zhu et al.'s work revealed the reinforced adsorption capacity towards reactants associated with greater defective level could accelerate the formation of electrophilic oxyanion-carbon complexes oxidative to pollutants.
“Typically, Zhu et al. managed to fabricate a highly graphitized biochar with tailored defective degree under 900 °C pyrolysis.This work revealed the reinforced adsorption capacity towards reactants associated with greater defective level could accelerate the formation of electrophilic oxyanion-carbon complexes oxidative to pollutants.36”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [36]
N-doped graphitic biochar derived from co-pyrolysis of reed mixed with urea under 900 °C displayed an increased graphitic N level that enhanced non-radical activation of PDS via a two-electron process.
“Recently, N-doped graphitic biochar derived from co-pyrolysis of reed mixed with urea under 900 ℃ displayed an increased graphitic N level to enhance the non-radical activation of PDS via a two-electron process.36”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [36]
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- Authors
- Zhu, S., Huang, X., Ma, F., Wang, L., Duan, X., & Wang, S.
- Affiliations
- Harbin Institute of Technology (CN)
- Curtin University (AU)
- Corresponding author
- Wang, Li
- Duan, Xiaoguang
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-07-20
- Volume
- 52
- Issue
- 15
- Pages
- 8649-8658
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2885002054
- Cited by
- 1,179
- References
- 64
- Citations by year
- 2026: 81 · 2025: 142 · 2024: 172 · 2023: 190 · 2022: 220 · 2021: 166 · 2020: 125 · 2019: 76 · 2018: 7
- FWCI
- 40.89
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Environmental Science & Technology (publishedVersion)
- PubMed (publishedVersion)
- Adelaide Research & Scholarship (AR&S) (University of Adelaide) (submittedVersion)
- eSpace (Curtin University) (submittedVersion)
- Funders
- Ministry of Science and Technology of the People's Republic of China (2016YFC0401105)
- National Natural Science Foundation of China (31570505)
- Nanqi Ren Studio, Harbin institute of Technology (HSCJ201708)
- State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (QAK201808)
- 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 › Environmental Chemistry › Per- and polyfluoroalkyl substances research
- Keywords
- persulfate activation, advanced oxidation processes, organic pollutant degradation, adsorption, persistent free radicals, singlet oxygen, Orange G, phenols, sulfamethoxazole, bisphenol A, annealing temperature, water treatment
- MeSH terms
- Adsorption, Catalysis, Charcoal, Graphite
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