Revealing the Mechanism of sp-N Doping in Graphdiyne for Developing Site-Defined Metal-Free Catalysts

Revealing the Mechanism of sp-N Doping in Graphdiyne for Developing Site-Defined Metal-Free Catalysts

© 2022 Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 50 vom: 11. Dez., Seite e2206450
1. Verfasser: Liu, Baokun (VerfasserIn)
Weitere Verfasser: Zhan, Shuhui, Du, Jiang, Yang, Xin, Zhao, Yasong, Li, Lulu, Wan, Jiawei, Zhao, Zhi-Jian, Gong, Jinlong, Yang, Nailiang, Yu, Ranbo, Wang, Dan
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2023
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article 2D materials N doping carbon materials graphdiyne sp-N
Beschreibung
Zusammenfassung:© 2022 Wiley-VCH GmbH.
Due to the limited reserves of metals, scientists are devoted to exploring high-performance metal-free catalysts based on carbon materials to solve environment-related issues. Doping would build up inhomogeneous charge distribution on surface, which is an efficient approach for boosting the catalytic performance. However, doping sites are difficult to control in traditional carbon materials, thus hindering their development. Taking the advantage of unique sp-C in graphdiyne (GDY), a new N doping configuration of sp-hybridized nitrogen (sp-N), bringing a Pt-comparable catalytic activity in oxygen reduction reaction is site-defined introduced. However, the reaction intermediate of this process is never captured, hindering the understanding of the mechanism and the precise synthesis of metal-free catalysts. After the four-year study, the fabrication of intermediate-like molecule is realized, and finally sp-N doped GDY via the pericyclic reaction is obtained. Compared with GDY doped with other N configurations, the designed sp-N GDY shows much higher catalytic activity in electroreduction of CO2 toward CH4 production, owing to the unique electronic structure introduced by sp-N, which is more favorable in stabilizing the intermediate. Thus, besides opening the black-box for the site-defined doping, this work reveals the relationship between doping configuration and products of CO2 reduction
Beschreibung:Date Revised 14.12.2023
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202206450