Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like Reaction
Abstract Improving the utilization of active sites in carbon catalysts is significant for various catalytic reactions, but still challenging, mainly due to the lack of strategies for controllable introduction of active dopants. Herein, a novel “Ar plasma etching‐NH3 annealing” strategy is developed...
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| Format: | Article |
| Language: | English |
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Wiley
2024-11-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202404958 |
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| author | Huajie Zhong Zeyu Gong Jiaxing Yu Yu Hou Yuan Tao Qi Fu Huangsheng Yang Xinzhe Xiao Xingzhong Cao Junhui Wang Gangfeng Ouyang |
| author_facet | Huajie Zhong Zeyu Gong Jiaxing Yu Yu Hou Yuan Tao Qi Fu Huangsheng Yang Xinzhe Xiao Xingzhong Cao Junhui Wang Gangfeng Ouyang |
| author_sort | Huajie Zhong |
| collection | DOAJ |
| description | Abstract Improving the utilization of active sites in carbon catalysts is significant for various catalytic reactions, but still challenging, mainly due to the lack of strategies for controllable introduction of active dopants. Herein, a novel “Ar plasma etching‐NH3 annealing” strategy is developed to regulate the position of active N sites, while maintaining the same nitrogen species and contents. Theoretical and experimental results reveal that the edge‐hosted‐N doped carbon nanotubes (E‐N‐CNT), with only 0.29 at.% N content, show great affinity to peroxymonosulfate (PMS), and exhibit excellent Fenton‐like activity by generating singlet oxygen (1O2), which can reach as high as 410 times higher than the pristine CNT. The remarkable utilization of edge‐hosted nitrogen atom is further verified by the edge‐hosted‐N enriched carbocatalyst, which shows superior capability for 4‐chlorophenol degradation with a turnover frequency (TOF) value as high as 3.82 min−1, and the impressive TOF value can even surpass those of single‐atom catalysts. This work proposes a controllable position regulation of active sites to improve atom utilization, which provides a new insight into the design of excellent Fenton‐like catalysts with remarkable atom utilization efficiency. |
| format | Article |
| id | doaj-art-4dcf5f34ae48453b97930ea205f4810d |
| institution | OA Journals |
| issn | 2198-3844 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-4dcf5f34ae48453b97930ea205f4810d2025-08-20T02:12:24ZengWileyAdvanced Science2198-38442024-11-011141n/an/a10.1002/advs.202404958Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like ReactionHuajie Zhong0Zeyu Gong1Jiaxing Yu2Yu Hou3Yuan Tao4Qi Fu5Huangsheng Yang6Xinzhe Xiao7Xingzhong Cao8Junhui Wang9Gangfeng Ouyang10School of Chemical Engineering and Technology Sun Yat‐Sen University Zhuhai Guangdong 519082 P. R. ChinaSchool of Chemical Engineering and Technology Sun Yat‐Sen University Zhuhai Guangdong 519082 P. R. ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry/KLGHEI of Environment and Energy Chemistry School of Chemistry Sun Yat‐Sen University Guangzhou Guangdong 510275 P. R. ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry/KLGHEI of Environment and Energy Chemistry School of Chemistry Sun Yat‐Sen University Guangzhou Guangdong 510275 P. R. ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry/KLGHEI of Environment and Energy Chemistry School of Chemistry Sun Yat‐Sen University Guangzhou Guangdong 510275 P. R. ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry/KLGHEI of Environment and Energy Chemistry School of Chemistry Sun Yat‐Sen University Guangzhou Guangdong 510275 P. R. ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry/KLGHEI of Environment and Energy Chemistry School of Chemistry Sun Yat‐Sen University Guangzhou Guangdong 510275 P. R. ChinaSchool of Chemical Engineering and Technology Sun Yat‐Sen University Zhuhai Guangdong 519082 P. R. ChinaInstitute of High Energy Physics Chinese Academy of Sciences Beijing 100049 P. R. ChinaSchool of Chemical Engineering and Technology Sun Yat‐Sen University Zhuhai Guangdong 519082 P. R. ChinaSchool of Chemical Engineering and Technology Sun Yat‐Sen University Zhuhai Guangdong 519082 P. R. ChinaAbstract Improving the utilization of active sites in carbon catalysts is significant for various catalytic reactions, but still challenging, mainly due to the lack of strategies for controllable introduction of active dopants. Herein, a novel “Ar plasma etching‐NH3 annealing” strategy is developed to regulate the position of active N sites, while maintaining the same nitrogen species and contents. Theoretical and experimental results reveal that the edge‐hosted‐N doped carbon nanotubes (E‐N‐CNT), with only 0.29 at.% N content, show great affinity to peroxymonosulfate (PMS), and exhibit excellent Fenton‐like activity by generating singlet oxygen (1O2), which can reach as high as 410 times higher than the pristine CNT. The remarkable utilization of edge‐hosted nitrogen atom is further verified by the edge‐hosted‐N enriched carbocatalyst, which shows superior capability for 4‐chlorophenol degradation with a turnover frequency (TOF) value as high as 3.82 min−1, and the impressive TOF value can even surpass those of single‐atom catalysts. This work proposes a controllable position regulation of active sites to improve atom utilization, which provides a new insight into the design of excellent Fenton‐like catalysts with remarkable atom utilization efficiency.https://doi.org/10.1002/advs.202404958atom utilizationcarbon defectcarbon nanomaterialsFenton‐like reaction |
| spellingShingle | Huajie Zhong Zeyu Gong Jiaxing Yu Yu Hou Yuan Tao Qi Fu Huangsheng Yang Xinzhe Xiao Xingzhong Cao Junhui Wang Gangfeng Ouyang Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like Reaction Advanced Science atom utilization carbon defect carbon nanomaterials Fenton‐like reaction |
| title | Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like Reaction |
| title_full | Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like Reaction |
| title_fullStr | Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like Reaction |
| title_full_unstemmed | Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like Reaction |
| title_short | Remarkable Active Site Utilization in Edge‐Hosted‐N Doped Carbocatalysts for Fenton‐Like Reaction |
| title_sort | remarkable active site utilization in edge hosted n doped carbocatalysts for fenton like reaction |
| topic | atom utilization carbon defect carbon nanomaterials Fenton‐like reaction |
| url | https://doi.org/10.1002/advs.202404958 |
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