Radical and non-radical cooperative degradation in metal-free electro-Fenton based on nitrogen self-doped biochar
(2022) In Journal of Hazardous Materials 435.- Abstract
To achieve sustainable metal-free electron-Fenton, N self-doped biochar air-cathode (BCAC) was prepared by pyrolyzing coffee residues. During the pyrolysis process, the endogenous N transformed from edge-doping to graphite-doping. Particularly, N vacancies started to evolve when the peak temperature exceeded 700 °C. A high Tetracycline removal rate of 70.42% was obtained on the BCAC at the current density of 4 mA cm−2. Quenching tests incorporated with ESR spectroscopy were adopted to identify the specific oxidants produced on the cathode. The results showed that •OH (37.36%), •O2- (29.67%) and 1O2 (24.17%) played comparable role in the tetracycline removal, suggesting the coexist... (More)
To achieve sustainable metal-free electron-Fenton, N self-doped biochar air-cathode (BCAC) was prepared by pyrolyzing coffee residues. During the pyrolysis process, the endogenous N transformed from edge-doping to graphite-doping. Particularly, N vacancies started to evolve when the peak temperature exceeded 700 °C. A high Tetracycline removal rate of 70.42% was obtained on the BCAC at the current density of 4 mA cm−2. Quenching tests incorporated with ESR spectroscopy were adopted to identify the specific oxidants produced on the cathode. The results showed that •OH (37.36%), •O2- (29.67%) and 1O2 (24.17%) played comparable role in the tetracycline removal, suggesting the coexist of radical and non-radical oxidants in our electro-Fenton system. According to the structure characterization and the DFT calculation, graphitic N was suggested as the critical site for H2O2 generation, and both graphitic N and pyridinic N were electroactive sites for H2O2 activation to •OH. Graphitic N and N vacancies with stronger capabilities in O2 adsorption and electron-trapping were proposed as the electroactive sites for 1O2 and •O2- formation. This work predicts a novel electro-Fenton process with cooperative radical and non-radical degradation on N self-doped carbonaceous catalysts at a mild condition, which is extremely meaningful for boosting sustainable electro-Fenton technology.
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- author
- Zhang, Ting ; Sun, Lu ; Sun, Xiaohong ; Dong, Heng ; Yu, Han LU and Yu, Hongbing
- organization
- publishing date
- 2022-08-05
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- Metal-free electro-Fenton, N self-doped biochar, N vacancy, Reactive oxygen species, Singlet oxygen
- in
- Journal of Hazardous Materials
- volume
- 435
- article number
- 129063
- publisher
- Elsevier
- external identifiers
-
- scopus:85129714821
- pmid:35650745
- ISSN
- 0304-3894
- DOI
- 10.1016/j.jhazmat.2022.129063
- language
- English
- LU publication?
- yes
- id
- c75863b2-c2ca-4b76-841f-7dd0fbead49e
- date added to LUP
- 2022-12-27 15:42:47
- date last changed
- 2024-10-19 12:09:28
@article{c75863b2-c2ca-4b76-841f-7dd0fbead49e, abstract = {{<p>To achieve sustainable metal-free electron-Fenton, N self-doped biochar air-cathode (BCAC) was prepared by pyrolyzing coffee residues. During the pyrolysis process, the endogenous N transformed from edge-doping to graphite-doping. Particularly, N vacancies started to evolve when the peak temperature exceeded 700 °C. A high Tetracycline removal rate of 70.42% was obtained on the BCAC at the current density of 4 mA cm<sup>−2</sup>. Quenching tests incorporated with ESR spectroscopy were adopted to identify the specific oxidants produced on the cathode. The results showed that •OH (37.36%), •O<sub>2</sub><sup>-</sup> (29.67%) and <sup>1</sup>O<sub>2</sub> (24.17%) played comparable role in the tetracycline removal, suggesting the coexist of radical and non-radical oxidants in our electro-Fenton system. According to the structure characterization and the DFT calculation, graphitic N was suggested as the critical site for H<sub>2</sub>O<sub>2</sub> generation, and both graphitic N and pyridinic N were electroactive sites for H<sub>2</sub>O<sub>2</sub> activation to •OH. Graphitic N and N vacancies with stronger capabilities in O<sub>2</sub> adsorption and electron-trapping were proposed as the electroactive sites for <sup>1</sup>O<sub>2</sub> and •O<sub>2</sub><sup>-</sup> formation. This work predicts a novel electro-Fenton process with cooperative radical and non-radical degradation on N self-doped carbonaceous catalysts at a mild condition, which is extremely meaningful for boosting sustainable electro-Fenton technology.</p>}}, author = {{Zhang, Ting and Sun, Lu and Sun, Xiaohong and Dong, Heng and Yu, Han and Yu, Hongbing}}, issn = {{0304-3894}}, keywords = {{Metal-free electro-Fenton; N self-doped biochar; N vacancy; Reactive oxygen species; Singlet oxygen}}, language = {{eng}}, month = {{08}}, publisher = {{Elsevier}}, series = {{Journal of Hazardous Materials}}, title = {{Radical and non-radical cooperative degradation in metal-free electro-Fenton based on nitrogen self-doped biochar}}, url = {{http://dx.doi.org/10.1016/j.jhazmat.2022.129063}}, doi = {{10.1016/j.jhazmat.2022.129063}}, volume = {{435}}, year = {{2022}}, }