Nitrogen-doped reduced graphene oxide supports for noble metal catalysts with greatly enhanced activity and stability

被引:237
作者
He, Daping [1 ]
Jiang, Yulin [1 ]
Lv, Haifeng [1 ]
Pan, Mu [1 ]
Mu, Shichun [1 ]
机构
[1] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China
基金
中国国家自然科学基金;
关键词
Catalysts; Reduced graphene oxide; Nitrogen-doping; Oxygen reduction reaction; Proton exchange membrane fuel cells; OXYGEN REDUCTION REACTION; CARBON NITRIDE ELECTROCATALYSTS; METHANOL FUEL-CELLS; PLATINUM NANOPARTICLES; NANOTUBES; OXIDATION; NANOSTRUCTURES; GRAPHITE; PEMFCS; ROUTE;
D O I
10.1016/j.apcatb.2012.12.005
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
Pt nanoparticles supported on nitrogen-doped reduced graphene oxide (NRGO) were investigated for use as proton exchange membrane fuel cell catalysts. Artfully, NRGO was synthesized using a lyophilisation-assisted N-doping method, and simultaneous reduction of graphene oxide (GO) was achieved. A nitrogen content as high as 5.06% was obtained with pyridinic-N as the dominant nitrogen species. Pt nanoparticles with an average diameter of 2.5 nm were uniformly loaded on NRGO using impregnation methods. Both cyclic voltammetry and oxygen reduction reaction (ORR) measurements revealed a higher catalytic activity and lower losses of the electrochemically active surface area of this novel Pt/NRGO catalyst in comparison to those of the Pt/GO and conventional Pt/C catalysts. Significantly, the catalytic activity of the Pt/NRGO in ORR showed almost no degradation even after 1000 potential cycles, indicating that our new catalysts have excellent stability. A mechanism for improving the ORR activity and the stability of the Pt/NRGO was tentatively proposed and discussed. (c) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:379 / 388
页数:10
相关论文
共 52 条
[1]   Electrochemical oxidation of aliphatic amines and their attachment to carbon and metal surfaces [J].
Adenier, A ;
Chehimi, MM ;
Gallardo, I ;
Pinson, J ;
Vilà, N .
LANGMUIR, 2004, 20 (19) :8243-8253
[2]   Carbon supports for low-temperature fuel cell catalysts [J].
Antolini, Ermete .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 88 (1-2) :1-24
[3]   Dynamic surface rearrangement and thermal stability of nitrogen functional groups on carbon nanotubes [J].
Arrigo, Rosa ;
Haevecker, Michael ;
Schloegl, Robert ;
Su, Dang Sheng .
CHEMICAL COMMUNICATIONS, 2008, (40) :4891-4893
[4]   Carbon nanotubes - the route toward applications [J].
Baughman, RH ;
Zakhidov, AA ;
de Heer, WA .
SCIENCE, 2002, 297 (5582) :787-792
[5]   Ionic dispersion of Pt over CeO2 by the combustion method:: Structural investigation by XRD, TEM, XPS, and EXAFS [J].
Bera, P ;
Priolkar, KR ;
Gayen, A ;
Sarode, PR ;
Hegde, MS ;
Emura, S ;
Kumashiro, R ;
Jayaram, V ;
Subbanna, GN .
CHEMISTRY OF MATERIALS, 2003, 15 (10) :2049-2060
[6]   Size-selected synthesis of PtRu nano-catalysts: Reaction and size control mechanism [J].
Bock, C ;
Paquet, C ;
Couillard, M ;
Botton, GA ;
MacDougall, BR .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (25) :8028-8037
[7]   Oxidation of CO on a Pt/Al2O3 catalyst:: from the surface elementary steps to light-off tests -: V.: Experimental and kinetic model for light-off tests in excess of O2 [J].
Bourane, A ;
Bianchi, D .
JOURNAL OF CATALYSIS, 2004, 222 (02) :499-510
[8]   Edge-functionalized and substitutionally doped graphene nanoribbons:: Electronic and spin properties [J].
Cervantes-Sodi, F. ;
Csanyi, G. ;
Piscanec, S. ;
Ferrari, A. C. .
PHYSICAL REVIEW B, 2008, 77 (16)
[9]   A Pt-Fe carbon nitride nano-electrocatalyst for polymer electrolyte membrane fuel cells and direct-methanol fuel cells: Synthesis, characterization, and electrochemical studies [J].
Di Noto, Vito ;
Negro, Enrico ;
Gliubizzi, Rocco ;
Lavina, Sandra ;
Pace, Giuseppe ;
Gross, Silvia ;
Maccato, Chiara .
ADVANCED FUNCTIONAL MATERIALS, 2007, 17 (17) :3626-3638
[10]   Preparation, characterization and single-cell performance of a new class of Pd-carbon nitride electrocatalysts for oxygen reduction reaction in PEMFCs [J].
Di Noto, Vito ;
Negro, Enrico ;
Polizzi, Stefano ;
Riello, Pietro ;
Atanassov, Plamen .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2012, 111 :185-199