Modulating the electronic structure of Mn promotes singlet oxygen generation from electrochemical oxidation of H₂O via O-O coupling
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Autor:in (Körperschaft)
Publikationsdatum
12/2024
Typ der Arbeit
Studiengang
Sammlung
Typ
01A - Beitrag in wissenschaftlicher Zeitschrift
Herausgeber:innen
Herausgeber:in (Körperschaft)
Betreuer:in
Übergeordnetes Werk
Chemical Engineering Journal
Themenheft
DOI der Originalpublikation
Link
Reihe / Serie
Reihennummer
Jahrgang / Band
502
Ausgabe / Nummer
Seiten / Dauer
Patentnummer
Verlag / Herausgebende Institution
Elsevier
Verlagsort / Veranstaltungsort
Auflage
Version
Programmiersprache
Abtretungsempfänger:in
Praxispartner:in/Auftraggeber:in
Zusammenfassung
Selectively catalytic conversion H₂O into singlet oxygen (¹O₂) without additional oxidants is considered as an economic-efficient method for organic pollutants degradation. However, H₂O are more consistent with the spin state of ¹O₂ than common oxygen (O₂), retarding the kinetics of spin transition-induced reaction between O₂ and ¹O₂. Herein, we report an unprecedented ¹O₂ mediated electrocatalytic oxidation process, which allows O–O coupling for ¹O₂ evolution from H₂O over CrMn@C anode. The electron occupancy (eg) of CrMn@C (0.89) is very close to the optimal eg (0.95) of manganese-based materials reported in the literature, which facilitates the activation of H₂O on surface. Mn(Mn0.193Cr1.808)O₄-Mn in CrMn@C electrode significantly promotes the activation of H₂O to produce *O, followed by coupling of *O at adjacent sites to produce *OO, which further spontaneously forms ¹O₂. And H₂¹⁸O isotope experiments provide direct evidence for the production of ¹O₂ directly from H₂O. Consequently, the production of ¹O₂ is enhanced with the yield of 785.6 μmol·L⁻¹. Such ¹O₂-dominated electrocatalytic oxidation system can achieve efficient removal of electron-rich pollutant (bisphenol A) and improve the biodegradability of pharmaceutical wastewater (from 0.17 to 0.39).
Schlagwörter
Fachgebiet (DDC)
Veranstaltung
Startdatum der Ausstellung
Enddatum der Ausstellung
Startdatum der Konferenz
Enddatum der Konferenz
Datum der letzten Prüfung
ISBN
ISSN
1385-8947
1873-3212
1873-3212
Sprache
Englisch
Während FHNW Zugehörigkeit erstellt
Ja
Zukunftsfelder FHNW
Publikationsstatus
Veröffentlicht
Begutachtung
Peer-Review der ganzen Publikation
Open Access-Status
Closed
Lizenz
Zitation
Chen, H., Hou, Z., Yue, J., Wang, J., Wang, Y., Li, A., & Corvini, P. (2024). Modulating the electronic structure of Mn promotes singlet oxygen generation from electrochemical oxidation of H₂O via O-O coupling. Chemical Engineering Journal, 502. https://doi.org/10.1016/j.cej.2024.157947