Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis
Abstract Two-dimensional (2D) covalent organic frameworks (COFs) and their derivatives have been widely applied as electrocatalysts owing to their unique nanoscale pore configurations, stable periodic structures, abundant coordination sites and high surface area. This work aims to construct a non-th...
| Main Authors: | , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-03-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-46872-x |
| _version_ | 1797247150501920768 |
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| author | Ziqi Zhang Zhe Zhang Cailing Chen Rui Wang Minggang Xie Sheng Wan Ruige Zhang Linchuan Cong Haiyan Lu Yu Han Wei Xing Zhan Shi Shouhua Feng |
| author_facet | Ziqi Zhang Zhe Zhang Cailing Chen Rui Wang Minggang Xie Sheng Wan Ruige Zhang Linchuan Cong Haiyan Lu Yu Han Wei Xing Zhan Shi Shouhua Feng |
| author_sort | Ziqi Zhang |
| collection | DOAJ |
| description | Abstract Two-dimensional (2D) covalent organic frameworks (COFs) and their derivatives have been widely applied as electrocatalysts owing to their unique nanoscale pore configurations, stable periodic structures, abundant coordination sites and high surface area. This work aims to construct a non-thermodynamically stable Pt-N2 coordination active site by electrochemically modifying platinum (Pt) single atoms into a fully conjugated 2D COF as conductive agent-free and pyrolysis-free electrocatalyst for the hydrogen evolution reaction (HER). In addition to maximizing atomic utilization, single-atom catalysts with definite structures can be used to investigate catalytic mechanisms and structure-activity relationships. In this work, in-situ characterizations and theoretical calculations reveal that a nitrogen-rich graphene analogue COF not only exhibits a favorable metal-support effect for Pt, adjusting the binding energy between Pt sites to H* intermediates by forming unique Pt-N2 instead of the typical Pt-N4 coordination environment, but also enhances electron transport ability and structural stability, showing both conductivity and stability in acidic environments. |
| first_indexed | 2024-04-24T19:54:07Z |
| format | Article |
| id | doaj.art-ae62ca027674472aab449a637de69060 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-04-24T19:54:07Z |
| publishDate | 2024-03-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-ae62ca027674472aab449a637de690602024-03-24T12:26:31ZengNature PortfolioNature Communications2041-17232024-03-0115111310.1038/s41467-024-46872-xSingle-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysisZiqi Zhang0Zhe Zhang1Cailing Chen2Rui Wang3Minggang Xie4Sheng Wan5Ruige Zhang6Linchuan Cong7Haiyan Lu8Yu Han9Wei Xing10Zhan Shi11Shouhua Feng12State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityAdvanced Membranes and Porous Materials Center, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology (KAUST)State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityElectron Microscopy Center, South China University of TechnologyState Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of SciencesState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityAbstract Two-dimensional (2D) covalent organic frameworks (COFs) and their derivatives have been widely applied as electrocatalysts owing to their unique nanoscale pore configurations, stable periodic structures, abundant coordination sites and high surface area. This work aims to construct a non-thermodynamically stable Pt-N2 coordination active site by electrochemically modifying platinum (Pt) single atoms into a fully conjugated 2D COF as conductive agent-free and pyrolysis-free electrocatalyst for the hydrogen evolution reaction (HER). In addition to maximizing atomic utilization, single-atom catalysts with definite structures can be used to investigate catalytic mechanisms and structure-activity relationships. In this work, in-situ characterizations and theoretical calculations reveal that a nitrogen-rich graphene analogue COF not only exhibits a favorable metal-support effect for Pt, adjusting the binding energy between Pt sites to H* intermediates by forming unique Pt-N2 instead of the typical Pt-N4 coordination environment, but also enhances electron transport ability and structural stability, showing both conductivity and stability in acidic environments.https://doi.org/10.1038/s41467-024-46872-x |
| spellingShingle | Ziqi Zhang Zhe Zhang Cailing Chen Rui Wang Minggang Xie Sheng Wan Ruige Zhang Linchuan Cong Haiyan Lu Yu Han Wei Xing Zhan Shi Shouhua Feng Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis Nature Communications |
| title | Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis |
| title_full | Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis |
| title_fullStr | Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis |
| title_full_unstemmed | Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis |
| title_short | Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis |
| title_sort | single atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis |
| url | https://doi.org/10.1038/s41467-024-46872-x |
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