Magnéli phases TinO2n-1 as novel ozonation catalysts for effective mineralization of phenol

doi:10.1016/j.cjche.2018.01.011

Chinese Journal of Chemical Engineering ›› 2018, Vol. 26 ›› Issue (9): 1978-1984.DOI: 10.1016/j.cjche.2018.01.011

• Energy, Resources and Environmental Technology • 上一篇下一篇

Magnéli phases Ti_nO_2n-1 as novel ozonation catalysts for effective mineralization of phenol

Xian Mao, Fanglu Yuan, Anqi Zhou, Wenheng Jing

State Key Laboratory of Materials-Oriented Chemical Engineering, National Engineering Research Center for Special Separation Membrane, College of Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China

收稿日期:2017-10-30 修回日期:2017-12-06 出版日期:2018-09-28 发布日期:2018-10-17
通讯作者: Wenheng Jing,E-mail address:jingwh@njtech.edu.cn
基金资助:
Supported by the National Natural Science Foundation of China (21676139), the Higher Education Natural Science Foundation of Jiangsu Province (15KJA530001), the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), and the Research Fund of State Key Laboratory of MaterialsOriented Chemical Engineering (ZK201604).

Magnéli phases Ti_nO_2n-1 as novel ozonation catalysts for effective mineralization of phenol

Xian Mao, Fanglu Yuan, Anqi Zhou, Wenheng Jing

State Key Laboratory of Materials-Oriented Chemical Engineering, National Engineering Research Center for Special Separation Membrane, College of Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China

Received:2017-10-30 Revised:2017-12-06 Online:2018-09-28 Published:2018-10-17
Contact: Wenheng Jing,E-mail address:jingwh@njtech.edu.cn
Supported by:
Supported by the National Natural Science Foundation of China (21676139), the Higher Education Natural Science Foundation of Jiangsu Province (15KJA530001), the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), and the Research Fund of State Key Laboratory of MaterialsOriented Chemical Engineering (ZK201604).

摘要/Abstract

摘要： Magnéli phases Ti_nO_2n-1 have been demonstrated as promising environmentally friendly materials in advanced oxidation processes. In this study, Magnéli phases Ti_nO_2n-1 have been used as catalysts for the ozonation of phenol in aqueous solution for the first time. The materials exhibited excellent catalytic ozonation activities both in phenol degradation and mineralization. When Ti₄O₇ was added, the reaction rate was six-fold higher than that of with ozone alone, while the total organic carbon removal rate was substantially elevated from around 19.2% to 92%. By virtue of the good chemical stability of the materials, a low metal leaching of less than 0.15 mg·L^-1 could effectively avoid the secondary pollution by metal ions. Radical quenching tests revealed ·O₂^- and ¹O₂ to be active oxygen species for phenol degradation at pH 5. As semiconductor catalysts, Ti_nO_2n-1 materials show electronic transfer capability. Ozone adsorbed at B-acid sites of the catalyst surface can capture an electron from the conversion of Ti(Ⅲ) to Ti(IV), and is thereby broken into the active oxygen species. It was interesting to observe that Ti_nO_2n-1 exhibit better catalytic activity for phenol degradation and mineralization with lower n value. The difference in electrical conductivity can be considered as a major factor for the catalytic performances. More highly conductive catalysts show a faster electron-transfer rate and better catalytic activity. Thus, significant evidences have been obtained for a single-electron-transfer mechanism of catalytic ozonation with Magnéli phases Ti_nO_2n-1.

关键词: Ti_nO_2n-1, Catalytic ozonation, Conductivity, B-acid sites, Single-electron-transfer

Abstract: Magnéli phases Ti_nO_2n-1 have been demonstrated as promising environmentally friendly materials in advanced oxidation processes. In this study, Magnéli phases Ti_nO_2n-1 have been used as catalysts for the ozonation of phenol in aqueous solution for the first time. The materials exhibited excellent catalytic ozonation activities both in phenol degradation and mineralization. When Ti₄O₇ was added, the reaction rate was six-fold higher than that of with ozone alone, while the total organic carbon removal rate was substantially elevated from around 19.2% to 92%. By virtue of the good chemical stability of the materials, a low metal leaching of less than 0.15 mg·L^-1 could effectively avoid the secondary pollution by metal ions. Radical quenching tests revealed ·O₂^- and ¹O₂ to be active oxygen species for phenol degradation at pH 5. As semiconductor catalysts, Ti_nO_2n-1 materials show electronic transfer capability. Ozone adsorbed at B-acid sites of the catalyst surface can capture an electron from the conversion of Ti(Ⅲ) to Ti(IV), and is thereby broken into the active oxygen species. It was interesting to observe that Ti_nO_2n-1 exhibit better catalytic activity for phenol degradation and mineralization with lower n value. The difference in electrical conductivity can be considered as a major factor for the catalytic performances. More highly conductive catalysts show a faster electron-transfer rate and better catalytic activity. Thus, significant evidences have been obtained for a single-electron-transfer mechanism of catalytic ozonation with Magnéli phases Ti_nO_2n-1.

Key words: Ti_nO_2n-1, Catalytic ozonation, Conductivity, B-acid sites, Single-electron-transfer

Xian Mao, Fanglu Yuan, Anqi Zhou, Wenheng Jing. Magnéli phases Ti_nO_2n-1 as novel ozonation catalysts for effective mineralization of phenol[J]. Chinese Journal of Chemical Engineering, 2018, 26(9): 1978-1984.

Xian Mao, Fanglu Yuan, Anqi Zhou, Wenheng Jing. Magnéli phases Ti_nO_2n-1 as novel ozonation catalysts for effective mineralization of phenol[J]. Chin.J.Chem.Eng., 2018, 26(9): 1978-1984.

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Magnéli phases Ti_nO_2n-1 as novel ozonation catalysts for effective mineralization of phenol

Magnéli phases Ti_nO_2n-1 as novel ozonation catalysts for effective mineralization of phenol

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