Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis
文献类型：期刊论文
| 作者 | Zhao, Yasong1,2; Wan, Jiawei1; Yao, Huiying3; Zhang, Lijuan1; Lin, Kaifeng2; Wang, Lei4; Yang, Nailiang1; Liu, Daobin5; Song, Li5; Zhu, Jia3 |
| 刊名 | NATURE CHEMISTRY
 |
| 出版日期 | 2018-09-01 |
| 卷号 | 10期号:9页码:924-931 |
| ISSN号 | 1755-4330 |
| DOI | 10.1038/s41557-018-0100-1 |
| 英文摘要 | The oxygen reduction reaction (ORR) is a fundamental reaction for energy storage and conversion. It has mainly relied on platinum-based electrocatalysts, but the chemical doping of carbon-based materials has proven to be a promising strategy for preparing metal-free alternatives. Nitrogen doping in particular provides a diverse range of nitrogen forms. Here, we introduce a new form of nitrogen doping moieties - sp-hybridized nitrogen (sp-N) atoms into chemically defined sites of ultrathin graphdiyne, through pericyclic replacement of the acetylene groups. The as-prepared sp-N-doped graphdiyne catalyst exhibits overall good ORR performance, in particular with regards to peak potential, half-wave potential and current density. Under alkaline conditions it was comparable to commercial Pt/C, and showed more rapid kinetics. And although its performances are a bit lower than those of Pt/C in acidic media they surpass those of other metal-free materials. Taken together, experimental data and density functional theory calculations suggest that the high catalytic activity originates from the sp-N dopant, which facilitates O-2 adsorption and electron transfer on the surface of the catalyst. This incorporation of chemically defined sp-N atoms provides a new synthetic route to high-performance carbon-based and other metal-free catalysts. |
| 语种 | 英语 |
| 出版者 | NATURE PUBLISHING GROUP |
| WOS记录号 | WOS:000442395200006 |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/42389]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Yang, Nailiang; Zhu, Jia; Li, Yuliang; Wang, Dan |
| 作者单位 | 1.Chinese Acad Sci, Inst Proc Engn, CAS Ctr Excellence Nanosci, State Key Lab Biochem Engn, Beijing, Peoples R China 2.Harbin Inst Technol, Sch Chem & Chem Engn, MIIT Key Lab Crit Mat Technol New Energy Convers, Harbin, Heilongjiang, Peoples R China 3.Beijing Normal Univ, Dept Chem, Key Lab Theoret & Computat Photochem, Minist Educ, Beijing, Peoples R China 4.Qiangdao Univ Sci & Technol, 53 Zhengzhou Rd, Qingdao, Shandong, Peoples R China 5.Univ Sci & Technol China, CAS Ctr Excellence Nanosci, Natl Synchrotron Radiat Lab, Hefei, Anhui, Peoples R China 6.Chinese Acad Sci, Inst Phys, Beijing, Peoples R China 7.Tsinghua Univ, Dept Chem, Beijing, Peoples R China 8.Griffith Univ, Ctr Clean Environm & Energy, Gold Coast Campus, Southport, Qld, Australia 9.Chinese Acad Sci, Beijing Natl Lab Mol Sci, Inst Chem, CAS Key Lab Organ Solids, Beijing, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zhao, Yasong,Wan, Jiawei,Yao, Huiying,et al. Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis[J]. NATURE CHEMISTRY,2018,10(9):924-931. |
| APA | Zhao, Yasong.,Wan, Jiawei.,Yao, Huiying.,Zhang, Lijuan.,Lin, Kaifeng.,...&Wang, Dan.(2018).Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis.NATURE CHEMISTRY,10(9),924-931. |
| MLA | Zhao, Yasong,et al."Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis".NATURE CHEMISTRY 10.9(2018):924-931. |
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来源：化学研究所
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