标题: Catalytic ozonation with gamma-Al2O3 sphere supported highly dispersed iron species: Preparation, performance and catalytic mechanism

作者: Wang, ZC (Wang, Zhicheng); Xu, T (Xu, Tao); Tang, DD (Tang, Dingding); Zhou, Y (Zhou, Yan); Zheng, BJ (Zheng, Bijuan); Qiu, YC (Qiu, Yicheng); He, DK (He, Dongkai); Zeng, X (Zeng, Xiang); Jiang, R (Jiang, Rui); Mao, XH (Mao, Xuhui)

来源出版物: COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS 卷: 658 文献号: 130560 DOI: 10.1016/j.colsurfa.2022.130560 出版年: FEB 5 2023

摘要: Maximizing the number of active sites is important to obtain an excellent catalytic activity for supported metal catalysts. Herein, citric acid-modified Al2O3 spheres in millimeter scale were employed as the porous support for loading iron species by a impregnation-calcination method using Fe(NO3)(3)center dot 9 H2O as the metal precursor. A good dispersion of the iron species inside the Al2O3 spheres was achieved, and the characterizations revealed that Fe sites were incorporated into the framework of Al2O3 in the form of -[Al-O-Fe-III]- structure. The obtained Fe-III/CA-Al2O3 catalyst was found to have a significantly increased amount of surface Lewis acid sites (LAS), showing a better performance than the counterpart catalyst Fe2O3/Al2O3 for p-nitrophenol (PNP) degradation. It was found that the presence of both oxidizable organic pollutants (as electron donator) and ozone was the prerequisite for observing the transformation from surface-ferric (equivalent to Fe-III) to surface-ferrous (equivalent to Fe-II) iron on the surface of Fe-III/CA-Al2O3 catalyst. In comparison with Fe2O3/Al2O3 catalyst, the Fe-III/CA-Al2O3 catalyst also demonstrated a higher level of equivalent to Fe-II during the catalytic reaction, suggesting that it had more iron active centers for the catalytic reaction. The cycle of the redox couple equivalent to Fe-III and equivalent to Fe-II played an important role for producing the reactive oxygen species. This study confirms that the modification of gamma-Al2O3 spheres with citric acid enabled a highly homogeneous dispersion of iron within the support matrix, providing a feasible route for the synthesis of high-performance and low-cost iron-bearing catalysts for industrial application.

作者关键词: Catalytic ozonation; Supported metal catalysts; gamma-Al2O3; Iron

地址: [Wang, Zhicheng; Xu, Tao; Qiu, Yicheng; He, Dongkai; Jiang, Rui; Mao, Xuhui] Wuhan Univ, Sch Resources & Environm Sci, Hubei Key Lab Biomass Resource Chem & Environm Bio, Wuhan 430079, Peoples R China.

[Tang, Dingding; Zhou, Yan; Zheng, Bijuan] China Construct Third Bur Green Ind Investment Co, Wuhan 430064, Peoples R China.

[Zeng, Xiang] Guangdong Cimoen Co Ltd, Zhongshan 528437, Guangdong, Peoples R China.

通讯作者地址: Mao, XH (通讯作者)，Wuhan Univ, Sch Resources & Environm Sci, Hubei Key Lab Biomass Resource Chem & Environm Bio, Wuhan 430079, Peoples R China.

电子邮件地址: clab@whu.edu.cn

影响因子：5.518