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Eine Plattform für die Wissenschaft: Bauingenieurwesen, Architektur und Urbanistik
Enhanced Mediated Electron Transfer Pathway of Peroxymonosulfate Activation Dominated with Graphitic‑N for the Efficient Degradation of Various Organic Contaminants in Multiple Solutions
https://orcid.org/0000-0001-8511-8347
https://orcid.org/0000-0003-3873-6059
https://orcid.org/0000-0002-4466-2474
https://orcid.org/0000-0002-9027-6857
https://orcid.org/0000-0003-0225-1690
https://orcid.org/0000-0002-9118-9990
Persulfate activated by carbon catalysts raised tremendous attention as a promising approach for degrading organic contaminants because the nonradical species produced can resist the interference of background substances. However, due to the complex and diverse structures of carbon catalysts, the reported peroxymonosulfate (PMS) activation mechanisms are varied. Herein, we used fabricated N-doped carbon nanotubes with a simple one-dimensional structure as a model catalyst to reveal the nature of PMS activation by carbon catalysts. The graphitic-N was identified as the active center to play a dominant role via structure–activity relationship analysis and density functional theory (DFT). Moreover, electron paramagnetic resonance, radical scavenging tests, and in situ Raman spectra demonstrated that the generated common reactive oxygen species did not contribute to carbamazepine (CBZ) degradation, but the electron transfer process directly oxidized the organic. Fortunately, the direct electron transfer pathway could quickly and simultaneously degrade various organics (including CBZ, sulfamethoxazole, bisphenol A, diclofenac, and tetracycline). In addition, the nature of degradation differences of various organics was revealed through the Fukui function calculated by DFT. This work revealed the mechanism of PMS activation by graphitic-N to produce mediated electron transfer pathways and provided an insight into the decomposition difference of various organic contaminants.
This work elucidated the intrinsic mechanism of mediated electron transfer oxidation and degradation difference of various organic contaminants with the carbon catalysts/PMS system.
Enhanced Mediated Electron Transfer Pathway of Peroxymonosulfate Activation Dominated with Graphitic‑N for the Efficient Degradation of Various Organic Contaminants in Multiple Solutions
https://orcid.org/0000-0001-8511-8347
https://orcid.org/0000-0003-3873-6059
https://orcid.org/0000-0002-4466-2474
https://orcid.org/0000-0002-9027-6857
https://orcid.org/0000-0003-0225-1690
https://orcid.org/0000-0002-9118-9990
Persulfate activated by carbon catalysts raised tremendous attention as a promising approach for degrading organic contaminants because the nonradical species produced can resist the interference of background substances. However, due to the complex and diverse structures of carbon catalysts, the reported peroxymonosulfate (PMS) activation mechanisms are varied. Herein, we used fabricated N-doped carbon nanotubes with a simple one-dimensional structure as a model catalyst to reveal the nature of PMS activation by carbon catalysts. The graphitic-N was identified as the active center to play a dominant role via structure–activity relationship analysis and density functional theory (DFT). Moreover, electron paramagnetic resonance, radical scavenging tests, and in situ Raman spectra demonstrated that the generated common reactive oxygen species did not contribute to carbamazepine (CBZ) degradation, but the electron transfer process directly oxidized the organic. Fortunately, the direct electron transfer pathway could quickly and simultaneously degrade various organics (including CBZ, sulfamethoxazole, bisphenol A, diclofenac, and tetracycline). In addition, the nature of degradation differences of various organics was revealed through the Fukui function calculated by DFT. This work revealed the mechanism of PMS activation by graphitic-N to produce mediated electron transfer pathways and provided an insight into the decomposition difference of various organic contaminants.
This work elucidated the intrinsic mechanism of mediated electron transfer oxidation and degradation difference of various organic contaminants with the carbon catalysts/PMS system.
Enhanced Mediated Electron Transfer Pathway of Peroxymonosulfate Activation Dominated with Graphitic‑N for the Efficient Degradation of Various Organic Contaminants in Multiple Solutions
https://orcid.org/0000-0001-8511-8347
https://orcid.org/0000-0003-3873-6059
https://orcid.org/0000-0002-4466-2474
https://orcid.org/0000-0002-9027-6857
https://orcid.org/0000-0003-0225-1690
https://orcid.org/0000-0002-9118-9990
Persulfate activated by carbon catalysts raised tremendous attention as a promising approach for degrading organic contaminants because the nonradical species produced can resist the interference of background substances. However, due to the complex and diverse structures of carbon catalysts, the reported peroxymonosulfate (PMS) activation mechanisms are varied. Herein, we used fabricated N-doped carbon nanotubes with a simple one-dimensional structure as a model catalyst to reveal the nature of PMS activation by carbon catalysts. The graphitic-N was identified as the active center to play a dominant role via structure–activity relationship analysis and density functional theory (DFT). Moreover, electron paramagnetic resonance, radical scavenging tests, and in situ Raman spectra demonstrated that the generated common reactive oxygen species did not contribute to carbamazepine (CBZ) degradation, but the electron transfer process directly oxidized the organic. Fortunately, the direct electron transfer pathway could quickly and simultaneously degrade various organics (including CBZ, sulfamethoxazole, bisphenol A, diclofenac, and tetracycline). In addition, the nature of degradation differences of various organics was revealed through the Fukui function calculated by DFT. This work revealed the mechanism of PMS activation by graphitic-N to produce mediated electron transfer pathways and provided an insight into the decomposition difference of various organic contaminants.
This work elucidated the intrinsic mechanism of mediated electron transfer oxidation and degradation difference of various organic contaminants with the carbon catalysts/PMS system.
Enhanced Mediated Electron Transfer Pathway of Peroxymonosulfate Activation Dominated with Graphitic‑N for the Efficient Degradation of Various Organic Contaminants in Multiple Solutions
Liu, Shuan (Autor:in) / Pan, Qixin (Autor:in) / Li, Juan (Autor:in) / Wang, Min (Autor:in) / Zhang, Jian (Autor:in) / Song, Yunqian (Autor:in) / Zhao, Chun (Autor:in) / Shi, Jun (Autor:in) / Deng, Huiping (Autor:in)
ACS ES&T Water ; 2 ; 817-829
13.05.2022
Aufsatz (Zeitschrift)
Elektronische Ressource
Englisch
| British Library Online Contents | 2018
| British Library Online Contents | 2019