The high catalytic activity and strong stability of 3%Fe/AC catalysts for catalytic wet peroxide oxidation of m-cresol: The role of surface functional groups and FeOx particles

doi:10.1016/j.cjche.2021.04.040

中国化学工程学报 ›› 2022, Vol. 44 ›› Issue (4): 105-114.DOI: 10.1016/j.cjche.2021.04.040

The high catalytic activity and strong stability of 3%Fe/AC catalysts for catalytic wet peroxide oxidation of m-cresol: The role of surface functional groups and FeO_x particles

Peiwei Han¹, Chunhua Xu², Yamin Wang³, Chenglin Sun³, Huangzhao Wei³, Haibo Jin¹, Ying Zhao³, Lei Ma¹

1 Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology/College of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing 102617, China;
2 Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Qingdao 266237, China;
3 Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

收稿日期:2020-10-16 修回日期:2020-12-04 出版日期:2022-04-28 发布日期:2022-06-18
通讯作者: Ying Zhao,E-mail:zying@dicp.ac.cn;Lei Ma,E-mail:malei@bipt.edu.cn
基金资助:
This research was funded by the National Natural Science Foundation of China (52100072), the Beijing Natural Science Foundation (8214056), the special fund of Beijing Key Laboratory of Clean Fuels and Efficient Catalytic Emission Reduction Technology, the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21021101), the National Key Research and Development Program of China (2019YFA0705803), Scientific Research Common Program of Beijing Municipal Commission of Education (KM202010017006).

The high catalytic activity and strong stability of 3%Fe/AC catalysts for catalytic wet peroxide oxidation of m-cresol: The role of surface functional groups and FeO_x particles

Peiwei Han¹, Chunhua Xu², Yamin Wang³, Chenglin Sun³, Huangzhao Wei³, Haibo Jin¹, Ying Zhao³, Lei Ma¹

1 Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology/College of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing 102617, China;
2 Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Qingdao 266237, China;
3 Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

Received:2020-10-16 Revised:2020-12-04 Online:2022-04-28 Published:2022-06-18
Contact: Ying Zhao,E-mail:zying@dicp.ac.cn;Lei Ma,E-mail:malei@bipt.edu.cn
Supported by:
This research was funded by the National Natural Science Foundation of China (52100072), the Beijing Natural Science Foundation (8214056), the special fund of Beijing Key Laboratory of Clean Fuels and Efficient Catalytic Emission Reduction Technology, the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21021101), the National Key Research and Development Program of China (2019YFA0705803), Scientific Research Common Program of Beijing Municipal Commission of Education (KM202010017006).

摘要/Abstract

摘要： FeO supported on activated carbon (AC) has been shown to be an ideal catalyst for catalytic wet peroxide oxidation (CWPO) due to its high CWPO reaction activity and stability. Although there have been some studies on the mechanism of Fe/AC catalysis in CWPO, the specific contribution of each component (surface oxygen groups and FeO_x on AC) inside an Fe/AC catalyst and their corresponding reaction mechanism remain unclear, and the reaction stability of CWPO catalysts has rarely been discussed. Then the optimal CWPO catalyst in our laboratory, 3%Fe/AC, was selected. (1) By removing certain components on the AC through heat treatment, its contribution to the reaction and the corresponding reaction mechanism were investigated. With the aid of temperature-programmed desorption–mass spectrometry (TPD–MS) and the CWPO reaction, the normalized catalytic contributions of components were shown to be: 37.3% (carboxylic groups), 5.3% (anhydride), 19.3% (ether/hydroxyl), -71.4% (carbonyl groups) and 100% (FeO_x), respectively. DFT calculation and EPR analysis confirmed that carboxylic groups and Fe₂O₃ are able to activate the H₂O₂ to generate ·OH. (2) The catalysts at were characterized at different reaction times (0 h, 450 h, 900 h, 1350 h, and 1800 h) by TPD–MS and Mössbauer spectroscopy. Results suggested that the number of carboxylic goups gradually increased and the size of paramagnetic Fe₂O₃ particle crystallites gradually increased as the reactions progressed. The occurrence of strong interactions between metal oxides and AC was also confirmed. Due to these effects, the strong stability of 3%Fe/AC was further improved. Therefore, the reasons for the high activity and strong stability of 3%Fe/AC in CWPO were clearly shown. We believe that this work provides an idea of the removal of cresols from wastewater into the introduction to show the potential applications of CWPO.

关键词: Catalytic wet peroxide oxidation, Fe/AC catalyst, Surface functional groups, Reaction mechanism

Abstract: FeO supported on activated carbon (AC) has been shown to be an ideal catalyst for catalytic wet peroxide oxidation (CWPO) due to its high CWPO reaction activity and stability. Although there have been some studies on the mechanism of Fe/AC catalysis in CWPO, the specific contribution of each component (surface oxygen groups and FeO_x on AC) inside an Fe/AC catalyst and their corresponding reaction mechanism remain unclear, and the reaction stability of CWPO catalysts has rarely been discussed. Then the optimal CWPO catalyst in our laboratory, 3%Fe/AC, was selected. (1) By removing certain components on the AC through heat treatment, its contribution to the reaction and the corresponding reaction mechanism were investigated. With the aid of temperature-programmed desorption–mass spectrometry (TPD–MS) and the CWPO reaction, the normalized catalytic contributions of components were shown to be: 37.3% (carboxylic groups), 5.3% (anhydride), 19.3% (ether/hydroxyl), -71.4% (carbonyl groups) and 100% (FeO_x), respectively. DFT calculation and EPR analysis confirmed that carboxylic groups and Fe₂O₃ are able to activate the H₂O₂ to generate ·OH. (2) The catalysts at were characterized at different reaction times (0 h, 450 h, 900 h, 1350 h, and 1800 h) by TPD–MS and Mössbauer spectroscopy. Results suggested that the number of carboxylic goups gradually increased and the size of paramagnetic Fe₂O₃ particle crystallites gradually increased as the reactions progressed. The occurrence of strong interactions between metal oxides and AC was also confirmed. Due to these effects, the strong stability of 3%Fe/AC was further improved. Therefore, the reasons for the high activity and strong stability of 3%Fe/AC in CWPO were clearly shown. We believe that this work provides an idea of the removal of cresols from wastewater into the introduction to show the potential applications of CWPO.

Key words: Catalytic wet peroxide oxidation, Fe/AC catalyst, Surface functional groups, Reaction mechanism

Peiwei Han, Chunhua Xu, Yamin Wang, Chenglin Sun, Huangzhao Wei, Haibo Jin, Ying Zhao, Lei Ma. The high catalytic activity and strong stability of 3%Fe/AC catalysts for catalytic wet peroxide oxidation of m-cresol: The role of surface functional groups and FeO_x particles[J]. 中国化学工程学报, 2022, 44(4): 105-114.

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The high catalytic activity and strong stability of 3%Fe/AC catalysts for catalytic wet peroxide oxidation of m-cresol: The role of surface functional groups and FeO_x particles

The high catalytic activity and strong stability of 3%Fe/AC catalysts for catalytic wet peroxide oxidation of m-cresol: The role of surface functional groups and FeO_x particles

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