Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworks
Abstract Covalent organic frameworks (COFs) have been well developed in electrocatalytic systems owing to their controllable skeletons, porosities, and functions. However, the catalytic process in COFs remains underexplored, hindering an in‐depth understanding of the catalytic mechanism. In this wor...
| Main Authors: | , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2023-06-01
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| Series: | SusMat |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/sus2.125 |
| _version_ | 1797796641353236480 |
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| author | Shuai Yang Lanlu Lu Ji Li Qingqing Cheng Bingbao Mei Xuewen Li Jianing Mao Panzhe Qiao Fanfei Sun Jingyuan Ma Qing Xu Zheng Jiang |
| author_facet | Shuai Yang Lanlu Lu Ji Li Qingqing Cheng Bingbao Mei Xuewen Li Jianing Mao Panzhe Qiao Fanfei Sun Jingyuan Ma Qing Xu Zheng Jiang |
| author_sort | Shuai Yang |
| collection | DOAJ |
| description | Abstract Covalent organic frameworks (COFs) have been well developed in electrocatalytic systems owing to their controllable skeletons, porosities, and functions. However, the catalytic process in COFs remains underexplored, hindering an in‐depth understanding of the catalytic mechanism. In this work, uniform Pt–N1O1Cl4 sites chelated via C–N and C=O bonds along the one‐dimensional and open channels of TP–TTA–COF were established. Different from conventional single‐metal sites constructed for the near‐free platinum for hydrogen evolution, the as‐constructed PtCl–COF showed 2e− oxygen reduction for H2O2 production. We tracked the dynamic evolution process of atomic Pt sites in which Pt–N1O1Cl4 was transformed into Pt–N1O1(OH)2 using in situ X‐ray adsorption. The theoretical calculations revealed that the strong Pt–support interaction in Pt–N1O1(OH)2 facilitated *OOH formation and thus led to higher selectivity and activity for the oxygen reduction reaction in the 2e− pathway. This work can expand the applications of COFs through the regulation of their local electronic states for the manipulation of the metal center. |
| first_indexed | 2024-03-13T03:37:06Z |
| format | Article |
| id | doaj.art-142f615839b14bfd88c6709395d3c843 |
| institution | Directory Open Access Journal |
| issn | 2692-4552 |
| language | English |
| last_indexed | 2024-03-13T03:37:06Z |
| publishDate | 2023-06-01 |
| publisher | Wiley |
| record_format | Article |
| series | SusMat |
| spelling | doaj.art-142f615839b14bfd88c6709395d3c8432023-06-23T16:06:27ZengWileySusMat2692-45522023-06-013337938910.1002/sus2.125Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworksShuai Yang0Lanlu Lu1Ji Li2Qingqing Cheng3Bingbao Mei4Xuewen Li5Jianing Mao6Panzhe Qiao7Fanfei Sun8Jingyuan Ma9Qing Xu10Zheng Jiang11Shanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Institute of Applied Physics Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaShanghai Advanced Research Institute Chinese Academy of Sciences ShanghaiChinaAbstract Covalent organic frameworks (COFs) have been well developed in electrocatalytic systems owing to their controllable skeletons, porosities, and functions. However, the catalytic process in COFs remains underexplored, hindering an in‐depth understanding of the catalytic mechanism. In this work, uniform Pt–N1O1Cl4 sites chelated via C–N and C=O bonds along the one‐dimensional and open channels of TP–TTA–COF were established. Different from conventional single‐metal sites constructed for the near‐free platinum for hydrogen evolution, the as‐constructed PtCl–COF showed 2e− oxygen reduction for H2O2 production. We tracked the dynamic evolution process of atomic Pt sites in which Pt–N1O1Cl4 was transformed into Pt–N1O1(OH)2 using in situ X‐ray adsorption. The theoretical calculations revealed that the strong Pt–support interaction in Pt–N1O1(OH)2 facilitated *OOH formation and thus led to higher selectivity and activity for the oxygen reduction reaction in the 2e− pathway. This work can expand the applications of COFs through the regulation of their local electronic states for the manipulation of the metal center.https://doi.org/10.1002/sus2.125covalent organic frameworkoxygen reduction reactionsingle‐atom catalysis |
| spellingShingle | Shuai Yang Lanlu Lu Ji Li Qingqing Cheng Bingbao Mei Xuewen Li Jianing Mao Panzhe Qiao Fanfei Sun Jingyuan Ma Qing Xu Zheng Jiang Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworks SusMat covalent organic framework oxygen reduction reaction single‐atom catalysis |
| title | Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworks |
| title_full | Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworks |
| title_fullStr | Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworks |
| title_full_unstemmed | Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworks |
| title_short | Boosting hydrogen peroxide production via establishment and reconstruction of single‐metal sites in covalent organic frameworks |
| title_sort | boosting hydrogen peroxide production via establishment and reconstruction of single metal sites in covalent organic frameworks |
| topic | covalent organic framework oxygen reduction reaction single‐atom catalysis |
| url | https://doi.org/10.1002/sus2.125 |
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