Pyridinic N doped graphene: synthesis, electronic structure, and electrocatalytic property

被引:849
作者
Luo, Zhiqiang [1 ,2 ]
Lim, Sanhua [2 ]
Tian, Zhiqun [2 ]
Shang, Jingzhi [1 ]
Lai, Linfei [1 ,2 ]
MacDonald, Brian [3 ]
Fu, Chao [3 ]
Shen, Zexiang [1 ]
Yu, Ting [1 ,4 ]
Lin, Jianyi [2 ]
机构
[1] Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore
[2] Inst Chem & Engn Sci, Singapore 627833, Singapore
[3] WinTech Nanotechnol Serv Pte Ltd, Singapore 117684, Singapore
[4] Natl Univ Singapore, Dept Phys, Fac Sci, Singapore 117542, Singapore
基金
新加坡国家研究基金会;
关键词
OXYGEN REDUCTION REACTION; CARBON NITRIDE FILMS; X-RAY PHOTOELECTRON; RAMAN-SPECTROSCOPY; O-2; REDUCTION; NITROGEN; GRAPHITE; LAYERS; NANOTUBES; DISORDER;
D O I
10.1039/c1jm10845j
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Different C-N bonding configurations in nitrogen (N) doped carbon materials have different electronic structures. Carbon materials doped with only one kind of C-N bonding configuration are an excellent platform for studying doping effects on the electronic structure and physical/chemical properties. Here we report synthesis of single layer graphene doped with pure pyridinic N by thermal chemical vapour deposition of hydrogen and ethylene on Cu foils in the presence of ammonia. By adjusting the flow rate of ammonia, the atomic ratio of N and C can be modulated from 0 to 16%. The domain like distribution of N incorporated in graphene was revealed by the imaging of Raman spectroscopy and time-of-flight secondary ion mass spectrometry. The ultraviolet photoemission spectroscopy investigation demonstrated that the pyridinic N efficiently changed the valence band structure of graphene, including the raising of density of p states near the Fermi level and the reduction of work function. Such pyridinic N doping in carbon materials was generally considered to be responsible for their oxygen reduction reaction (ORR) activity. The 2e reduction mechanism of ORR on our CN(x) graphene revealed by rotating disk electrode voltammetry indicated that the pyridinic N may not be an effective promoter for ORR activity of carbon materials as previously expected.
引用
收藏
页码:8038 / 8044
页数:7
相关论文
共 43 条
[1]  
BASIUK VA, 2007, CHEM CARBON NANOTUBE, P113
[2]   Structure of nitrogenated carbon films prepared from acetylene and nitrogen mixture in electron cyclotron resonance plasma [J].
Bhattacharyya, S ;
Vallée, C ;
Cardinaud, C ;
Turban, G .
JOURNAL OF APPLIED PHYSICS, 2000, 87 (10) :7524-7532
[3]   PHOTOEMISSION STUDIES OF GRAPHITE HIGH-ENERGY CONDUCTION-BAND AND VALENCE-BAND STATES USING SOFT-X-RAY SYNCHROTRON RADIATION EXCITATION [J].
BIANCONI, A ;
HAGSTROM, SBM ;
BACHRACH, RZ .
PHYSICAL REVIEW B, 1977, 16 (12) :5543-5548
[4]   Rayleigh imaging of graphene and graphene layers [J].
Casiraghi, C. ;
Hartschuh, A. ;
Lidorikis, E. ;
Qian, H. ;
Harutyunyan, H. ;
Gokus, T. ;
Novoselov, K. S. ;
Ferrari, A. C. .
NANO LETTERS, 2007, 7 (09) :2711-2717
[5]   The electronic properties of graphene [J].
Castro Neto, A. H. ;
Guinea, F. ;
Peres, N. M. R. ;
Novoselov, K. S. ;
Geim, A. K. .
REVIEWS OF MODERN PHYSICS, 2009, 81 (01) :109-162
[6]  
Ci L, 2010, NAT MATER, V9, P430, DOI [10.1038/nmat2711, 10.1038/NMAT2711]
[7]   Raman spectroscopy of graphene and graphite: Disorder, electron-phonon coupling, doping and nonadiabatic effects [J].
Ferrari, Andrea C. .
SOLID STATE COMMUNICATIONS, 2007, 143 (1-2) :47-57
[8]   Experimental comparison of N(1s) X-ray photoelectron spectroscopy binding energies of hard and elastic amorphous carbon nitride films with reference organic compounds [J].
Gammon, WJ ;
Kraft, O ;
Reilly, AC ;
Holloway, BC .
CARBON, 2003, 41 (10) :1917-1923
[9]   Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction [J].
Gong, Kuanping ;
Du, Feng ;
Xia, Zhenhai ;
Durstock, Michael ;
Dai, Liming .
SCIENCE, 2009, 323 (5915) :760-764
[10]   Dispersions of surface states on diamond (100) and (111) [J].
Graupner, R ;
Hollering, M ;
Ziegler, A ;
Ristein, J ;
Ley, L ;
Stampfl, A .
PHYSICAL REVIEW B, 1997, 55 (16) :10841-10847