Direct Growth of Carbon Nanotubes Doped with Single Atomic Fe-N-4 Active Sites and Neighboring Graphitic Nitrogen for Efficient and Stable Oxygen Reduction Electrocatalysis

Xia, Dongsheng1; Yang, Xin1; Xie, Lin2; Wei, Yinping1; Jiang, Wulv1; Dou, Miao1; Li, Xuning3; Li, Jia1; Gan, Lin1; Kang, Feiyu1

2019-09-12

10.1002/adfm.201906174

ADVANCED FUNCTIONAL MATERIALS   影响因子和分区

1616-301X

1616-3028

Single atomic Fe-N-x moieties embedded on a high surface area carbon (Fe-N/C) represents one of the most promising nonprecious metal electrocatalysts for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells. While significant progress has been made in the preparation of Fe-N/C catalysts with high-density Fe-N-x sites, key structural descriptors determining the intrinsic activity of the Fe center remain elusive, and effective ways to enhance the intrinsic activity are still lacking. Moreover, most Fe-N/C catalysts developed to date are built on carbons with rather low graphitization degree, which suffer from relatively severe carbon corrosion and thereby poor stability. The direct growth of carbon nanotubes doped with high-density Fe-N-x sites neighbored with graphitic-nitrogen-rich environment is reported here, which are successfully applied as a both active and stable ORR electrocatalyst in fuel cells. Combining both experiments and density functional theory calculations, it is revealed that the neighboring graphitic nitrogen can effectively induce higher filling degree of d-orbitals and simultaneously decrease on-site magnetic moment (namely, lowered spin) of the Fe center, which can optimize the binding energies of ORR intermediates and thereby substantially enhance intrinsic ORR activity.

carbon nanotubes graphitic nitrogen oxygen reduction reaction single atomic FeN4 stability

SCI ; EI

英语

NI期刊 ; NI论文

其他

Basic Research Project of Shenzhen, China[JCYJ20170817161445322] ; Basic Research Project of Shenzhen, China[JCYJ20170412171430026]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000486257900001

WILEY-V C H VERLAG GMBH

20194307585831

Atoms ; Binding energy ; Carbon nanotubes ; Convergence of numerical methods ; Corrosion ; Electrocatalysis ; Electrocatalysts ; Electrolytic reduction ; Magnetic moments ; Nitrogen ; Oxygen ; Polyelectrolytes ; Proton exchange membrane fuel cells (PEMFC)

Ore Treatment:533.1 ; Magnetism: Basic Concepts and Phenomena:701.2 ; Fuel Cells:702.2 ; Nanotechnology:761 ; Physical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Polymers:815.1.1 ; Numerical Methods:921.6 ; Atomic and Molecular Physics:931.3

MATERIALS SCIENCE

Web of Science

1.Tsinghua Univ, Grad Sch Shenzhen, Shenzhen Geim Graphene Res Ctr, Div Energy & Environm, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
3.Nanyang Technol Univ, Sch Chem & Biomed Engn, Singapore 639798, Singapore

Xia, Dongsheng,Yang, Xin,Xie, Lin,et al. Direct Growth of Carbon Nanotubes Doped with Single Atomic Fe-N-4 Active Sites and Neighboring Graphitic Nitrogen for Efficient and Stable Oxygen Reduction Electrocatalysis[J]. ADVANCED FUNCTIONAL MATERIALS,2019,29(49).

Xia, Dongsheng.,Yang, Xin.,Xie, Lin.,Wei, Yinping.,Jiang, Wulv.,...&Kang, Feiyu.(2019).Direct Growth of Carbon Nanotubes Doped with Single Atomic Fe-N-4 Active Sites and Neighboring Graphitic Nitrogen for Efficient and Stable Oxygen Reduction Electrocatalysis.ADVANCED FUNCTIONAL MATERIALS,29(49).

Xia, Dongsheng,et al."Direct Growth of Carbon Nanotubes Doped with Single Atomic Fe-N-4 Active Sites and Neighboring Graphitic Nitrogen for Efficient and Stable Oxygen Reduction Electrocatalysis".ADVANCED FUNCTIONAL MATERIALS 29.49(2019).