Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of Chlorobenzene
Abstract Chlorinated volatile organic compounds (CVOCs) are a class of hazardous pollutants that severely threaten environmental safety and human health. Although the catalytic oxidation technique for CVOCs elimination is effective, enhancing the catalytic efficiency and simultaneously inhibiting th...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2023-01-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202205054 |
| _version_ | 1797943398465798144 |
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| author | Xiaoxiao Duan Ting Zhao Ben Niu Zheng Wei Ganggang Li Zhongshen Zhang Jie Cheng Zhengping Hao |
| author_facet | Xiaoxiao Duan Ting Zhao Ben Niu Zheng Wei Ganggang Li Zhongshen Zhang Jie Cheng Zhengping Hao |
| author_sort | Xiaoxiao Duan |
| collection | DOAJ |
| description | Abstract Chlorinated volatile organic compounds (CVOCs) are a class of hazardous pollutants that severely threaten environmental safety and human health. Although the catalytic oxidation technique for CVOCs elimination is effective, enhancing the catalytic efficiency and simultaneously inhibiting the production of organic byproducts is still of great challenge. Herein, Ru‐substituted LaMn(Ru)O3+δ perovskite with Ru–O–Mn structure and weakened Mn–O bond strength has been developed for catalytic oxidation of chlorobenzene (CB). The formed Ru–O–Mn structure serves as favorable sites for CB adsorption and activation, while the weakening of Mn–O bond strength facilitates the formation of active oxygen species and improves oxygen mobility and catalyst reducibility. Therefore, LaMn(Ru)O3+δ exhibits superior low‐temperature activity with the temperature of 90% CB conversion decreasing by over 90 °C compared with pristine perovskite, and the deep oxidation of chlorinated byproducts produced in low temperature is also accelerated. Furthermore, the introduction of water vapor into reaction system triggers the process of hydrolysis oxidation that promotes CB destruction and inhibits the generation of chlorinated byproducts, due to the higher‐activity *OOH species generated from the dissociated H2O reacting with adsorbed oxygen. This work can provide a unique, high‐efficiency, and facile strategy for CVOCs degradation and environmental improvement. |
| first_indexed | 2024-04-10T20:23:33Z |
| format | Article |
| id | doaj.art-ccc2eddad5444b838218853d8b045562 |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-04-10T20:23:33Z |
| publishDate | 2023-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-ccc2eddad5444b838218853d8b0455622023-01-25T13:47:49ZengWileyAdvanced Science2198-38442023-01-01103n/an/a10.1002/advs.202205054Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of ChlorobenzeneXiaoxiao Duan0Ting Zhao1Ben Niu2Zheng Wei3Ganggang Li4Zhongshen Zhang5Jie Cheng6Zhengping Hao7National Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaNational Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaNational Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaNational Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaNational Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaNational Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaNational Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaNational Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing 101408 P. R. ChinaAbstract Chlorinated volatile organic compounds (CVOCs) are a class of hazardous pollutants that severely threaten environmental safety and human health. Although the catalytic oxidation technique for CVOCs elimination is effective, enhancing the catalytic efficiency and simultaneously inhibiting the production of organic byproducts is still of great challenge. Herein, Ru‐substituted LaMn(Ru)O3+δ perovskite with Ru–O–Mn structure and weakened Mn–O bond strength has been developed for catalytic oxidation of chlorobenzene (CB). The formed Ru–O–Mn structure serves as favorable sites for CB adsorption and activation, while the weakening of Mn–O bond strength facilitates the formation of active oxygen species and improves oxygen mobility and catalyst reducibility. Therefore, LaMn(Ru)O3+δ exhibits superior low‐temperature activity with the temperature of 90% CB conversion decreasing by over 90 °C compared with pristine perovskite, and the deep oxidation of chlorinated byproducts produced in low temperature is also accelerated. Furthermore, the introduction of water vapor into reaction system triggers the process of hydrolysis oxidation that promotes CB destruction and inhibits the generation of chlorinated byproducts, due to the higher‐activity *OOH species generated from the dissociated H2O reacting with adsorbed oxygen. This work can provide a unique, high‐efficiency, and facile strategy for CVOCs degradation and environmental improvement.https://doi.org/10.1002/advs.202205054active siteschlorinated volatile organic compounds (CVOCs) eliminationhydrolysis oxidationMn–O bond strengthperovskite oxides |
| spellingShingle | Xiaoxiao Duan Ting Zhao Ben Niu Zheng Wei Ganggang Li Zhongshen Zhang Jie Cheng Zhengping Hao Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of Chlorobenzene Advanced Science active sites chlorinated volatile organic compounds (CVOCs) elimination hydrolysis oxidation Mn–O bond strength perovskite oxides |
| title | Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of Chlorobenzene |
| title_full | Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of Chlorobenzene |
| title_fullStr | Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of Chlorobenzene |
| title_full_unstemmed | Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of Chlorobenzene |
| title_short | Simultaneously Constructing Active Sites and Regulating Mn–O Strength of Ru‐Substituted Perovskite for Efficient Oxidation and Hydrolysis Oxidation of Chlorobenzene |
| title_sort | simultaneously constructing active sites and regulating mn o strength of ru substituted perovskite for efficient oxidation and hydrolysis oxidation of chlorobenzene |
| topic | active sites chlorinated volatile organic compounds (CVOCs) elimination hydrolysis oxidation Mn–O bond strength perovskite oxides |
| url | https://doi.org/10.1002/advs.202205054 |
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