Preparation of Co-MnOx/GAC catalyst by high-gravity technology and its mechanism for synergistic catalytic ozone degradation of phenol

doi:10.1016/j.cjche.2024.12.007

Chinese Journal of Chemical Engineering ›› 2025, Vol. 81 ›› Issue (5): 208-218.DOI: 10.1016/j.cjche.2024.12.007

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Preparation of Co-MnO_x/GAC catalyst by high-gravity technology and its mechanism for synergistic catalytic ozone degradation of phenol

Cibin Wang¹, Kangrui Nie¹, Zhiwei Zhao¹, Yan Xue², Tong Zhao², Fuming Miao¹, Youzhi Liu¹, Weizhou Jiao¹

1. Shanxi Province Key Laboratory of Chemical Process Intensification, State Key Laboratory of Coal and CBM Co-Mining, School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China;
2. Shanxi Xinhua Chemical Protection Equipment Research Institute Co. Ltd., Taiyuan 030008, China

Received:2024-11-11 Revised:2024-12-04 Accepted:2024-12-15 Online:2025-02-27 Published:2025-05-28
Contact: Weizhou Jiao,E-mail:zbdxjwz@nuc.edu.cn
Supported by:
This research was supported by the National Natural Science Foundation of China (U23A20676), Key Research & Development Plan of Shanxi Province (202202040201011), Shanxi Scholarship Council of China (2023-128), Small and medium-sized oriented scientific and technological enterprises innovation ability improvement project of Shandong Province (2023TSGC0004) and the Graduate Student Innovation Project of Shanxi Province(2023SJ205), Local Funds for Science and Technology Development Guided by the Central Finance (YDZJSX20231A030).

Preparation of Co-MnO_x/GAC catalyst by high-gravity technology and its mechanism for synergistic catalytic ozone degradation of phenol

Cibin Wang¹, Kangrui Nie¹, Zhiwei Zhao¹, Yan Xue², Tong Zhao², Fuming Miao¹, Youzhi Liu¹, Weizhou Jiao¹

1. Shanxi Province Key Laboratory of Chemical Process Intensification, State Key Laboratory of Coal and CBM Co-Mining, School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China;
2. Shanxi Xinhua Chemical Protection Equipment Research Institute Co. Ltd., Taiyuan 030008, China

通讯作者: Weizhou Jiao,E-mail:zbdxjwz@nuc.edu.cn
基金资助:
This research was supported by the National Natural Science Foundation of China (U23A20676), Key Research & Development Plan of Shanxi Province (202202040201011), Shanxi Scholarship Council of China (2023-128), Small and medium-sized oriented scientific and technological enterprises innovation ability improvement project of Shandong Province (2023TSGC0004) and the Graduate Student Innovation Project of Shanxi Province(2023SJ205), Local Funds for Science and Technology Development Guided by the Central Finance (YDZJSX20231A030).

Abstract

Abstract: The impregnation method for preparing catalysts often faces challenges such as prolonged preparation times and poor dispersion of active components due to the limited mobility of the impregnation liquid. The rotating packed bed (RPB) can break the precursor solution into fine droplets, enabling dynamic impregnation of active components onto the surface of activated carbon. This approach facilitates the uniform distribution of active components on the carrier and enhances the stability and performance of the catalyst. In this study, activated carbon catalysts were prepared using high-gravity technology. It was found that the preparation time for Co-MnO_x/GAC using the RPB method was reduced by 98%, the catalytic activity increased by 6.62%, and the loadings of active components increased by 13% and 17%, the catalytic activity remained stable after five cycles, with a significantly lower rate of metal dissolution. A suite of complementary analytical techniques demonstrates that Co-MnO_x/GAC(RPB) has higher homogeneity and dispersion. X-ray photoelectron spectroscopy (XPS) results indicate that Co(II) and Mn(IV)/Mn(III) are the primary active sites during the catalytic decomposition of ozone, elucidating the mechanism of synergistic catalytic ozonation by dual-active components. Finally, electron paramagnetic resonance (EPR) confirmed that hydroxyl radicals (·OH) were the predominant reactive species in the reaction.

Key words: High-gravity technology, Dynamic impregnation, Co-MnO_x/GAC, Uniform distribution, Stability, Synergy catalytic

摘要： The impregnation method for preparing catalysts often faces challenges such as prolonged preparation times and poor dispersion of active components due to the limited mobility of the impregnation liquid. The rotating packed bed (RPB) can break the precursor solution into fine droplets, enabling dynamic impregnation of active components onto the surface of activated carbon. This approach facilitates the uniform distribution of active components on the carrier and enhances the stability and performance of the catalyst. In this study, activated carbon catalysts were prepared using high-gravity technology. It was found that the preparation time for Co-MnO_x/GAC using the RPB method was reduced by 98%, the catalytic activity increased by 6.62%, and the loadings of active components increased by 13% and 17%, the catalytic activity remained stable after five cycles, with a significantly lower rate of metal dissolution. A suite of complementary analytical techniques demonstrates that Co-MnO_x/GAC(RPB) has higher homogeneity and dispersion. X-ray photoelectron spectroscopy (XPS) results indicate that Co(II) and Mn(IV)/Mn(III) are the primary active sites during the catalytic decomposition of ozone, elucidating the mechanism of synergistic catalytic ozonation by dual-active components. Finally, electron paramagnetic resonance (EPR) confirmed that hydroxyl radicals (·OH) were the predominant reactive species in the reaction.

关键词: High-gravity technology, Dynamic impregnation, Co-MnO_x/GAC, Uniform distribution, Stability, Synergy catalytic

Cibin Wang, Kangrui Nie, Zhiwei Zhao, Yan Xue, Tong Zhao, Fuming Miao, Youzhi Liu, Weizhou Jiao. Preparation of Co-MnO_x/GAC catalyst by high-gravity technology and its mechanism for synergistic catalytic ozone degradation of phenol[J]. Chinese Journal of Chemical Engineering, 2025, 81(5): 208-218.

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Preparation of Co-MnO_x/GAC catalyst by high-gravity technology and its mechanism for synergistic catalytic ozone degradation of phenol

Preparation of Co-MnO_x/GAC catalyst by high-gravity technology and its mechanism for synergistic catalytic ozone degradation of phenol

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