title: Partial-Redox-Promoted Mn Cycling of Mn(II)-Doped Heterogeneous Catalyst for Efficient H2O2-Mediated Oxidation.
abstract: The development of a heterogeneous catalyst with high catalytic activity and durability for H2O2-mediated oxidation is one of the most important industrial and environmental issues. In this study, a Mn(II)-doped TiO2heterogeneous catalyst was developed for H2O2-mediated oxidation. The TiO2substrate-dependent partial-redox behavior of Mn was identified on the basis of our density functional theory simulations. This unique redox cycle was induced by a moderate electron transfer from Ti to Mn, which compensated for the electron loss of Mn and finally resulted in a high-efficiency cycling of Mn between its oxidized and reduced forms. In light of the theoretical results, a Mn(II)-doped TiO2composite with well-defined morphology and large surface area (153.3 m2g-1) was elaborately fabricated through incorporating Mn(II) ions into a TiO2nanoflower, and further tested as the catalyst for oxidative degradation of organic pollutants in the presence of H2O2. Benefiting from the remarkable textural features and excellent Mn cycling property, this composite exhibited superior catalytic performance for organic pollutant degradation. Moreover, it could retain 98.40% of its initial activity even in the fifth cycle. Our study provides an effective strategy for designing heterogeneous catalytic systems for H2O2-mediated oxidations.
authors.affiliation: Department of Chemistry, Faculty of Material Science and Chemistry, China University of Geosciences , Wuhan 430074, P. R. China.
authors.forename: Hai-Tao
authors.initials: HT
authors.lastname: Li
authors.affiliation: Department of Chemistry, Faculty of Material Science and Chemistry, China University of Geosciences , Wuhan 430074, P. R. China.
authors.forename: Qiang
authors.identifier: http://orcid.org/0000-0002-9750-5923
authors.initials: Q
authors.lastname: Gao
authors.affiliation: Sustainable Energy Laboratory, Faculty of Material Science and Chemistry, China University of Geosciences , Wuhan 430074, P. R. China.
authors.forename: Bo
authors.identifier: http://orcid.org/0000-0002-8472-3294
authors.initials: B
authors.lastname: Han
authors.affiliation: Department of Chemistry, Faculty of Material Science and Chemistry, China University of Geosciences , Wuhan 430074, P. R. China.
authors.forename: Zheng-Hui
authors.initials: ZH
authors.lastname: Ren
authors.affiliation: Sustainable Energy Laboratory, Faculty of Material Science and Chemistry, China University of Geosciences , Wuhan 430074, P. R. China.
authors.forename: Kai-Sheng
authors.initials: KS
authors.lastname: Xia
authors.affiliation: Sustainable Energy Laboratory, Faculty of Material Science and Chemistry, China University of Geosciences , Wuhan 430074, P. R. China.
authors.forename: Cheng-Gang
authors.identifier: http://orcid.org/0000-0002-3148-0188
authors.initials: CG
authors.lastname: Zhou
keywords: H2O2-mediated oxidation; Mn(II)-doped TiO2; heterogeneous catalyst; high catalytic activity and durability; partial redox