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Tunneling Electron-Mediated Electrochemical Activation of Peroxydisulfate for the Removal of Refractory Pollutants
https://orcid.org/0000-0002-4320-6039
https://orcid.org/0000-0001-8178-9418
In the SO4 •– radical-based advanced oxidation processes (AOPs), activation of peroxydisulfate (PS) is an effective method for the removal of refractory organic pollutants. Within this context, we report a novel electrochemical activation of PS (E-PS) by solvated electrons generated via the electron tunneling effect. The results demonstrated that the sulfamethoxazole (SMX) could be completely degraded (∼100% degradation efficiency) within 30 min (k = 0.0957 min–1) at the pH-neutral conditions when n+Si/Al2O3 was employed as the cathode. Further investigations based on electron paramagnetic resonance (EPR) and scavenger tests indicated that both SO4 •– and •OH were responsible for SMX degradation. Electrochemiluminescence (ECL) and current–voltage (I–V) characterization fitted by the tunneling models revealed the dominance of the direct electron tunneling effect at negative potential on the metal oxide semiconductor (MOS)-structured n+Si/Al2O3 cathode. The tunneling electrons were accepted by the lowest unoccupied orbital energy level (LUMO) of the water molecule to produce solvated electrons (esolv –) for subsequent PS activation and SMX removal. This study represents a paradigm shift to advance the electrochemical advanced oxidation process by creating an electron tunneling effect.
Tunneling Electron-Mediated Electrochemical Activation of Peroxydisulfate for the Removal of Refractory Pollutants
https://orcid.org/0000-0002-4320-6039
https://orcid.org/0000-0001-8178-9418
In the SO4 •– radical-based advanced oxidation processes (AOPs), activation of peroxydisulfate (PS) is an effective method for the removal of refractory organic pollutants. Within this context, we report a novel electrochemical activation of PS (E-PS) by solvated electrons generated via the electron tunneling effect. The results demonstrated that the sulfamethoxazole (SMX) could be completely degraded (∼100% degradation efficiency) within 30 min (k = 0.0957 min–1) at the pH-neutral conditions when n+Si/Al2O3 was employed as the cathode. Further investigations based on electron paramagnetic resonance (EPR) and scavenger tests indicated that both SO4 •– and •OH were responsible for SMX degradation. Electrochemiluminescence (ECL) and current–voltage (I–V) characterization fitted by the tunneling models revealed the dominance of the direct electron tunneling effect at negative potential on the metal oxide semiconductor (MOS)-structured n+Si/Al2O3 cathode. The tunneling electrons were accepted by the lowest unoccupied orbital energy level (LUMO) of the water molecule to produce solvated electrons (esolv –) for subsequent PS activation and SMX removal. This study represents a paradigm shift to advance the electrochemical advanced oxidation process by creating an electron tunneling effect.
Tunneling Electron-Mediated Electrochemical Activation of Peroxydisulfate for the Removal of Refractory Pollutants
https://orcid.org/0000-0002-4320-6039
https://orcid.org/0000-0001-8178-9418
In the SO4 •– radical-based advanced oxidation processes (AOPs), activation of peroxydisulfate (PS) is an effective method for the removal of refractory organic pollutants. Within this context, we report a novel electrochemical activation of PS (E-PS) by solvated electrons generated via the electron tunneling effect. The results demonstrated that the sulfamethoxazole (SMX) could be completely degraded (∼100% degradation efficiency) within 30 min (k = 0.0957 min–1) at the pH-neutral conditions when n+Si/Al2O3 was employed as the cathode. Further investigations based on electron paramagnetic resonance (EPR) and scavenger tests indicated that both SO4 •– and •OH were responsible for SMX degradation. Electrochemiluminescence (ECL) and current–voltage (I–V) characterization fitted by the tunneling models revealed the dominance of the direct electron tunneling effect at negative potential on the metal oxide semiconductor (MOS)-structured n+Si/Al2O3 cathode. The tunneling electrons were accepted by the lowest unoccupied orbital energy level (LUMO) of the water molecule to produce solvated electrons (esolv –) for subsequent PS activation and SMX removal. This study represents a paradigm shift to advance the electrochemical advanced oxidation process by creating an electron tunneling effect.
Tunneling Electron-Mediated Electrochemical Activation of Peroxydisulfate for the Removal of Refractory Pollutants
Liu, Guoshuai (author) / Mao, Xuelian (author) / Wang, Lu (author) / Zhang, Jian (author) / Zou, Hua (author) / Zhang, Jinna (author) / You, Shijie (author)
ACS ES&T Engineering ; 4 ; 797-806
2024-04-12
Article (Journal)
Electronic Resource
English
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