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| Revealing the Mechanism of sp-N Doping in Graphdiyne for Developing Site-Defined Metal-Free Catalysts | |
| Liu, Baokun1,2,3; Zhan, Shuhui1,4; Du, Jiang2,3; Yang, Xin2,3; Zhao, Yasong1; Li, Lulu5,6; Wan, Jiawei1,4; Zhao, Zhi-Jian5,6; Gong, Jinlong5,6; Yang, Nailiang1,4; Yu, Ranbo7,8; Wang, Dan1,4 | |
| 2022-11-02 | |
| Source Publication | ADVANCED MATERIALS
 |
| ISSN | 0935-9648 |
| Pages | 7 |
| Abstract | 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. |
| Keyword | carbon materials graphdiyne N doping sp-N 2D materials |
| DOI | 10.1002/adma.202206450 |
| Language | 英语 |
| WOS Keyword | REDUCTION ; CO2 |
| Funding Project | National Key R&D Program of China[2018YFA0703504] ; National Key R&D Program of China[2021YFB3802600] ; National Natural Science Foundation of China[51932001] ; National Natural Science Foundation of China[21971244] ; National Natural Science Foundation of China[21820102002] ; National Natural Science Foundation of China[21971245] |
| WOS Research Area | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
| WOS Subject | Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter |
| Funding Organization | National Key R&D Program of China ; National Natural Science Foundation of China |
| WOS ID | WOS:000877954800001 |
| Publisher | WILEY-V C H VERLAG GMBH |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.ipe.ac.cn/handle/122111/55401 |
| Collection | 中国科学院过程工程研究所 |
| Corresponding Author | Yang, Nailiang; Yu, Ranbo; Wang, Dan |
| Affiliation | 1.Chinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing 100190, Peoples R China 2.Zhengzhou Univ, Sch Mat Sci & Engn, Henan Prov Ind Technol Res Inst Resources & Mat, Green Catalysis Ctr, Zhengzhou 450001, Peoples R China 3.Zhengzhou Univ, Coll Chem, Zhengzhou 450001, Peoples R China 4.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China 5.Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China 6.Collaborat Innovat Ctr Chem Sci & Engn, Tianjin 300072, Peoples R China 7.Univ Sci & Technol Beijing, Dept Phys Chem, 30 Xueyuan Rd, Beijing 100083, Peoples R China 8.Univ Sci & Technol Beijing, Sch Met & Ecol Engn, 30 Xueyuan Rd, Beijing 100083, Peoples R China |
| Recommended Citation GB/T 7714 | Liu, Baokun,Zhan, Shuhui,Du, Jiang,et al. Revealing the Mechanism of sp-N Doping in Graphdiyne for Developing Site-Defined Metal-Free Catalysts[J]. ADVANCED MATERIALS,2022:7. |
| APA | Liu, Baokun.,Zhan, Shuhui.,Du, Jiang.,Yang, Xin.,Zhao, Yasong.,...&Wang, Dan.(2022).Revealing the Mechanism of sp-N Doping in Graphdiyne for Developing Site-Defined Metal-Free Catalysts.ADVANCED MATERIALS,7. |
| MLA | Liu, Baokun,et al."Revealing the Mechanism of sp-N Doping in Graphdiyne for Developing Site-Defined Metal-Free Catalysts".ADVANCED MATERIALS (2022):7. |
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