Engineering β-ketoamine covalent organic frameworks for photocatalytic overall water splitting
Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β -ketoamine COFs by systematically en...
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| Published in | Nature communications Vol. 14; no. 1; pp. 593 - 10 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
03.02.2023
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of
β
-ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H
2
and O
2
evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers.
Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution. Here, the authors report a β-ketoamine COF by systematically engineering N-sites, architecture, and morphology for improved water splitting activity. |
|---|---|
| AbstractList | Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β-ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H
and O
evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers. Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β -ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H 2 and O 2 evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers. Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution. Here, the authors report a β-ketoamine COF by systematically engineering N-sites, architecture, and morphology for improved water splitting activity. Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β-ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H2 and O2 evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers.Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution. Here, the authors report a β-ketoamine COF by systematically engineering N-sites, architecture, and morphology for improved water splitting activity. Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β-ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H2 and O2 evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers.Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β-ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H2 and O2 evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers. Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β -ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H 2 and O 2 evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers. Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution. Here, the authors report a β-ketoamine COF by systematically engineering N-sites, architecture, and morphology for improved water splitting activity. |
| ArticleNumber | 593 |
| Author | Lan, Ya-Qian Lu, Meng Yang, Yan Yang, Zhao-Di Zhang, Rui Liu, Yu-Han Zhang, Hong-Yu Chu, Xiaoyu Zhang, Feng-Ming |
| Author_xml | – sequence: 1 givenname: Yan surname: Yang fullname: Yang, Yan organization: Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology – sequence: 2 givenname: Xiaoyu surname: Chu fullname: Chu, Xiaoyu organization: Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology – sequence: 3 givenname: Hong-Yu surname: Zhang fullname: Zhang, Hong-Yu organization: Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology – sequence: 4 givenname: Rui surname: Zhang fullname: Zhang, Rui organization: Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology – sequence: 5 givenname: Yu-Han surname: Liu fullname: Liu, Yu-Han organization: Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology – sequence: 6 givenname: Feng-Ming orcidid: 0000-0002-2738-306X surname: Zhang fullname: Zhang, Feng-Ming email: zhangfm80@163.com organization: Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology – sequence: 7 givenname: Meng orcidid: 0000-0003-4502-7517 surname: Lu fullname: Lu, Meng organization: School of Chemistry, South China Normal University – sequence: 8 givenname: Zhao-Di surname: Yang fullname: Yang, Zhao-Di email: yangzhaodi@163.com organization: Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology – sequence: 9 givenname: Ya-Qian orcidid: 0000-0002-2140-7980 surname: Lan fullname: Lan, Ya-Qian email: yqlan@m.scnu.edu.cn organization: School of Chemistry, South China Normal University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/36737616$$D View this record in MEDLINE/PubMed |
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| DOI | 10.1038/s41467-023-36338-x |
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| Snippet | Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting... Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution. Here, the authors report a β-ketoamine... |
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| SubjectTerms | 639/638/77/890 639/638/911 Catalysts Covalence Electron transfer Evolution Humanities and Social Sciences Hydrogen Hydrogen evolution Morphology multidisciplinary Nanoparticles Photocatalysis Photocatalysts Platinum Science Science (multidisciplinary) Splitting Water splitting |
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| Title | Engineering β-ketoamine covalent organic frameworks for photocatalytic overall water splitting |
| URI | https://link.springer.com/article/10.1038/s41467-023-36338-x https://www.ncbi.nlm.nih.gov/pubmed/36737616 https://www.proquest.com/docview/2772194275 https://www.proquest.com/docview/2773113557 https://pubmed.ncbi.nlm.nih.gov/PMC9898260 https://doaj.org/article/084b57e236f04391a5c50f6a315d621e |
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