标題: Mn-Fe Dual-Metal Assemblages on Carbon-Coated Al₂O₃ Spheres for Catalytic Ozonation Oxidation: Structure, Performance, and Reaction Mechanism

作者: Xu, T (Xu, Tao); Jiang, MH (Jiang, Meihui); Mo, SY (Mo, Siyu); Wang, XH (Wang, Xianhui); Ren, TL (Ren, Tianlin); Liu, ZC (Liu, Zhichen); Wang, ZC (Wang, Zhicheng); Qiu, YC (Qiu, Yicheng); Gu, LY (Gu, Lingying); Wang, X (Wang, Xu); Mao, XH (Mao, Xuhui)

來源出版物: CHEMSUSCHEM  DOI: 10.1002/cssc.202401837  Early Access Date: NOV 2024  Published Date: 2024 NOV 7  

摘要: Catalysts with high catalytic activity and low production cost are important for industrial application of heterogeneous catalytic ozonation (HCO). In this study, we designed a carbon-coated aluminum oxide carrier (C-Al2O3) and reinforced it with Mn-Fe bimetal assemblages to prepare a high-performance catalyst Mn-Fe/C-Al2O3. The results showed that the carbon embedding significantly improved the abundance of surface oxygen functional groups, conductivity, and adsorption capacity of gamma-Al2O3, while preserving its exceptional mechanical strength as a carrier. The prepared Mn-Fe/C-Al2O3 catalyst exhibited satisfactory catalytic ozonation activity and stability in the degradation of p-nitrophenol (PNP). Electron paramagnetic resonance (EPR) and quenching experiments reveal that radical ( & sdot; OH and & sdot; O-2 & sdot; ) and nonradical oxidation (O-1(2)) dominated the PNP degradation process. Theoretical calculations corroborated that the anchored atomic Fe and Mn sites regulated the local electronic structure of the catalyst. This modulation effectively promoted the activation of O-3 molecules, resulting in the generation of atomic oxygen species (AOS) and reactive oxygen species (ROS). The economic analysis on Mn-Fe/C-Al2O3 revealed that it was a cost-competitive catalyst for HCO. This study not only deepens the understanding on the reaction mechanism of HCO with transition metal/carbon composite catalysts, also provides a high-performance and cost-competitive ozone catalyst for prospective application.

作者關鍵詞: Heterogeneous catalytic ozonation; Supported metal catalysts; Carbon-coated-Al2O3; Life cycle cost

KeyWords Plus: NANOPARTICLES; ADSORPTION

地址: [Xu, Tao; Jiang, Meihui; Wang, Xianhui; Ren, Tianlin; Liu, Zhichen; Wang, Zhicheng; Qiu, Yicheng; Wang, Xu; Mao, Xuhui] Wuhan Univ, Sch Resource & Environm Sci, Dept Environm Sci & Engn, Hubei Key Lab Biomass Resource Chem & Environm Bio, Wuhan 430079, Peoples R China.

[Mo, Siyu] Wuhan Univ, Coll Chem & Mol Sci, Wuhan, Peoples R China.

[Gu, Lingying] Hubei Prov Fibre Inspect Bur, Wuhan, Peoples R China.

通訊作者地址: Wang, X; Mao, XH (通訊作者)，Wuhan Univ, Sch Resource & Environm Sci, Dept Environm Sci & Engn, Hubei Key Lab Biomass Resource Chem & Environm Bio, Wuhan 430079, Peoples R China.

電子郵件地址: xu.wang@whu.edu.cn; clab@whu.edu.cn

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