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Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis
Zhao, Yasong1,2; Wan, Jiawei1; Yao, Huiying3; Zhang, Lijuan1; Lin, Kaifeng2; Wang, Lei4; Yang, Nailiang1; Liu, Daobin5; Song, Li5; Zhu, Jia3; Gu, Lin6; Liu, Lei7; Zhao, Huijun8; Li, Yuliang9; Wang, Dan1,4,8
2018-09-01
Source PublicationNATURE CHEMISTRY
ISSN1755-4330
Volume10Issue:9Pages:924-931
Abstract

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.

DOI10.1038/s41557-018-0100-1
Language英语
WOS KeywordMetal-free Electrocatalysts ; Fuel-cells ; Evolution Reactions ; Mesoporous Carbons ; Graphene Oxide ; Free Catalysts ; Performance ; Batteries ; Pyrolysis ; Size
Funding ProjectNational Science Fund for Distinguished Young Scholars[21325105] ; National Natural Science Foundation of China[21590795] ; National Natural Science Foundation of China[21401199] ; National Natural Science Foundation of China[21790050] ; National Natural Science Foundation of China[21790051] ; National Key Research and Development Program of China[2016YFB0600903] ; National Key Research and Development Program of China[2016YFA0200104] ; Chinese Academy of Sciences (CAS) Interdisciplinary Innovation Team ; Australian Research Council (ARC) Discovery Project[160104817] ; Foundation for State Key Laboratory of Biochemical Engineering
WOS Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
Funding OrganizationNational Science Fund for Distinguished Young Scholars ; National Natural Science Foundation of China ; National Key Research and Development Program of China ; Chinese Academy of Sciences (CAS) Interdisciplinary Innovation Team ; Australian Research Council (ARC) Discovery Project ; Foundation for State Key Laboratory of Biochemical Engineering
WOS IDWOS:000442395200006
PublisherNATURE PUBLISHING GROUP
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/25631
Collection中国科学院过程工程研究所
Corresponding AuthorYang, Nailiang; Zhu, Jia; Li, Yuliang; Wang, Dan
Affiliation1.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
Recommended Citation
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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