Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer
Abstract The rational design of carbon-supported transition-metal single-atom catalysts requires the precise arrangement of heteroatoms within the single-atom catalysts. However, achieving this design is challenging due to the collapse of the structure during the pyrolysis. Here, we introduce a topo...
| 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/s41467-024-47061-6 |
| _version_ | 1797233493226291200 |
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| author | Sheng Qian Feng Xu Yu Fan Ningyan Cheng Huaiguo Xue Ye Yuan Romain Gautier Tengfei Jiang Jingqi Tian |
| author_facet | Sheng Qian Feng Xu Yu Fan Ningyan Cheng Huaiguo Xue Ye Yuan Romain Gautier Tengfei Jiang Jingqi Tian |
| author_sort | Sheng Qian |
| collection | DOAJ |
| description | Abstract The rational design of carbon-supported transition-metal single-atom catalysts requires the precise arrangement of heteroatoms within the single-atom catalysts. However, achieving this design is challenging due to the collapse of the structure during the pyrolysis. Here, we introduce a topological heteroatom-transfer strategy to prevent the collapse and accurately control the P coordination in carbon-supported single-atom catalysts. As an illustration, we have prepared self-assembled helical fibers with encapsulated cavities. Within these cavities, adjustable functional groups can chelate metal ions (Nx···Mn+···Oy), facilitating the preservation of the structure during the pyrolysis based phosphidation. This process allows for the transfer of heteroatoms from the assembly into single-atom catalysts, resulting in the precise coordination tailoring. Notably, the Co–P2N2–C catalyst exhibits electrocatalytic performance as a non-noble metal single-atom catalyst for alkaline hydrogen evolution, attaining a current density of 100 mA cm−2 with an overpotential of only 131 mV. |
| first_indexed | 2024-04-24T16:17:03Z |
| format | Article |
| id | doaj.art-daf335d93f4643988c61297928614146 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-04-24T16:17:03Z |
| publishDate | 2024-03-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-daf335d93f4643988c612979286141462024-03-31T11:24:36ZengNature PortfolioNature Communications2041-17232024-03-0115111110.1038/s41467-024-47061-6Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transferSheng Qian0Feng Xu1Yu Fan2Ningyan Cheng3Huaiguo Xue4Ye Yuan5Romain Gautier6Tengfei Jiang7Jingqi Tian8School of Chemistry and Chemical Engineering, Yangzhou UniversitySchool of Chemistry and Chemical Engineering, Yangzhou UniversitySchool of Chemistry and Chemical Engineering, Yangzhou UniversityInformation Materials and Intelligent Sensing Laboratory of Anhui Province, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Institutes of Physical Science and Information Technology, Anhui UniversitySchool of Chemistry and Chemical Engineering, Yangzhou UniversityKey Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education, Faculty of Chemistry, Northeast Normal UniversityNantes Université, CNRS, Institut des Matériaux de Nantes Jean Rouxel, IMNSchool of Chemistry and Chemical Engineering, Yangzhou UniversitySchool of Chemistry and Chemical Engineering, Yangzhou UniversityAbstract The rational design of carbon-supported transition-metal single-atom catalysts requires the precise arrangement of heteroatoms within the single-atom catalysts. However, achieving this design is challenging due to the collapse of the structure during the pyrolysis. Here, we introduce a topological heteroatom-transfer strategy to prevent the collapse and accurately control the P coordination in carbon-supported single-atom catalysts. As an illustration, we have prepared self-assembled helical fibers with encapsulated cavities. Within these cavities, adjustable functional groups can chelate metal ions (Nx···Mn+···Oy), facilitating the preservation of the structure during the pyrolysis based phosphidation. This process allows for the transfer of heteroatoms from the assembly into single-atom catalysts, resulting in the precise coordination tailoring. Notably, the Co–P2N2–C catalyst exhibits electrocatalytic performance as a non-noble metal single-atom catalyst for alkaline hydrogen evolution, attaining a current density of 100 mA cm−2 with an overpotential of only 131 mV.https://doi.org/10.1038/s41467-024-47061-6 |
| spellingShingle | Sheng Qian Feng Xu Yu Fan Ningyan Cheng Huaiguo Xue Ye Yuan Romain Gautier Tengfei Jiang Jingqi Tian Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer Nature Communications |
| title | Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer |
| title_full | Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer |
| title_fullStr | Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer |
| title_full_unstemmed | Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer |
| title_short | Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer |
| title_sort | tailoring coordination environments of single atom electrocatalysts for hydrogen evolution by topological heteroatom transfer |
| url | https://doi.org/10.1038/s41467-024-47061-6 |
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