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Corresponding Author

Lu-hua JIANG(sunshine@dicp.ac.cn);
Gong-quan SUN(gqsun@dicp.ac.cn)

Abstract

The stability of carbon supports is essential for electrocatalysts of fuel cells. Herein, the mesoporous carbon with the high graphitic degree (highly graphitic mesoporous carbon, HGMC) was synthesized by using resorcinol as the carbon precursor, SiO2 as the templates and urea as the reducing agent. The as-prepared HGMC was characterized by XRD, Raman spectroscopy, TEM, N2 adsorption. The stability of HGMC was evaluated by mimicking the start-up/shut-down conditions of fuel cells in a three-electrode system referring to the NREL standard. The obtained HGMC is of moderate surface area (187.4 m2•g-1) and is chemically stable under potentiodynamic cycling as compared to the commercial Vulcan XC-72, while the high graphitic structure is adverse to the mass transport. To overcome the drawback of the HGMC in mass transportation, MWCNTs was introduced as a spacer to construct a 3D multi-scaled support. Compared to the single HGMC supported Pt catalyst and the commercial Pt/C-JM catalyst, the multi-scaled MSGC (the mixture of HGMC and MWCNTs with a mass ratio of 1:1) supported Pt catalyst displayed both enhanced electrochemical stability and significantly improved mass transportation for the oxygen reduction reaction, due to the stability and the multi-scaled structure of the carbon supports.

Graphical Abstract

Keywords

carbon support, platinum, oxygen reduction reaction, fuel cell

Publication Date

2016-04-28

Online Available Date

2016-04-28

Revised Date

2016-04-15

Received Date

2016-01-04

References

[1] Wilson M S, Gottesfeld S. High performance catalyzed membranes of ultra-low pt loadings for polymer electrolyte fuel cells[J]. Journal of The Electrochemical Society, 1992, 139(2): L28-L30.

[2] Wilson M S, Gottesfeld S. Thin-film catalyst layers for polymer electrolyte fuel cell electrodes[J]. Journal of Applied Electrochemistry, 1992, 22(1): 1-7.

[3] Reiser C A, Bregoli L, Patterson T W, et al. A reverse-current decay mechanism for fuel cells[J]. Electrochemical and Solid-State Letters, 2005, 8(6): A273-A276.

[4] Stevens D A, Hicks M T, Haugen G M, et al., Ex situ and in situ stability studies of PEMFC catalysts: Effect of carbon type and humidification on degradation of the carbon[J]. Journal of The Electrochemical Society, 2005, 152(12): A2309-A2315.

[5] Schlögl K, Hanzlik M, Arenz M, Comparative IL-TEM study concerning the degradation of carbon supported pt-based electrocatalysts[J]. Journal of The Electrochemical Society, 2012, 159(6): B677-B682.

[6] Roen L M, Paik C H, Jarvi T D, Electrocatalytic corrosion of carbon support in PEMFC cathodes[J]. Electrochemical and Solid-State Letters, 2004, 7(1): A19-A22.

[7] Meier J C, Galeano C, Katsounaros I, et al., Degradation mechanisms of Pt/C fuel cell catalysts under simulated start-stop conditions[J]. ACS Catalysis, 2012, 2(5): 832-843.

[8] Mayrhofer K J J, Ashton S J, Meier J C, et al. Non-destructive transmission electron microscopy study of catalyst degradation under electrochemical treatment[J]. Journal of Power Sources, 2008, 185(2): 734-739.

[9] Rabis A, Rodriguez P, Schmidt T J. Electrocatalysis for polymer electrolyte fuel cells: Recent achievements and future challenges[J]. ACS Catalysis, 2012, 2(5): 864-890.

[10] Schulenburg H, Schwanitz B, Linse N, et al. 3D imaging of catalyst support corrosion in polymer electrolyte fuel cells[J]. The Journal of Physical Chemistry C, 2011, 115(29): 14236-14243.

[11] Shao Y, Yin G, Gao Y, et al. Durability study of Pt ∕ C and Pt ∕ CNTs catalysts under simulated PEM fuel cell conditions[J]. Journal of The Electrochemical Society, 2006, 153(6): A1093-A1097.

[12] Okamoto M, Fujigaya T, Nakashima N. Design of an assembly of poly(benzimidazole), carbon nanotubes, and Pt nanoparticles for a fuel-cell electrocatalyst with an ideal interfacial nanostructure[J]. Small, 2009, 5(6): 735-740.

[13] Maiyalagan T, Viswanathan B, Varadaraju U V. Nitrogen containing carbon nanotubes as supports for Pt - alternate anodes for fuel cell applications[J]. Electrochemistry Communications, 2005, 7(9): 905-912.

[14] Hasche F, Oezaslan M, Strasser P. Activity, stability and degradation of multi walled carbon nanotube (MWCNT) supported Pt fuel cell electrocatalysts[J]. Physical Chemistry Chemical Physics, 2010, 12(46): 15251-15258.

[15] Hafez I H, Berber M R, Fujigaya T, et al. Enhancement of platinum mass activity on the surface of Polymer-wrapped carbon nanotube-based fuel cell electrocatalysts[J]. Scientific Reports, 2014, 4: 6295.

[16] Fujigaya T, Okamoto M, Nakashima N. Design of an assembly of pyridine-containing polybenzimidazole, carbon nanotubes and Pt nanoparticles for a fuel cell electrocatalyst with a high electrochemically active surface area[J]. Carbon, 2009, 47(14): 3227-3232.

[17] Fujigaya T, Nakashima N. Fuel cell electrocatalyst using polybenzimidazole-modified carbon nanotubes as support materials[J]. Advanced Materials, 2013, 25(12): 1666-1681.

[18] Fujigaya T, Hirata S, Nakashima N. A highly durable fuel cell electrocatalyst based on polybenzimidazole-coated stacked graphene[J]. Journal of Materials Chemistry A, 2014, 2(11): 3888-3893.

[19] Du H Y, Wang C H, Yang C S, et al. A high performance polybenzimidazole-CNT hybrid electrode for high-temperature proton exchange membrane fuel cells[J]. Journal of Materials Chemistry A, 2014, 2(19): 7015-7019.

[20] Zhang L W, Zheng N, Gao A, et al. A robust fuel cell cathode catalyst assembled with nitrogen-doped carbon nanohorn and platinum nanoclusters[J]. Journal of Power Sources, 2012, 220: 449-454.

[21] Yoshitake T, Shimakawa Y, Kuroshima S, et al. Preparation of fine platinum catalyst supported on single-wall carbon nanohorns for fuel cell application[J]. Physica B: Condensed Matter, 2002, 323(1/4): 124-126.

[22] Kou R, Shao Y Y, Wang D H, et al. Enhanced activity and stability of Pt catalysts on functionalized graphene sheets for electrocatalytic oxygen reduction[J]. Electrochemistry Communications, 2009, 11(5): 954-957.

[23] Maruyama J, Sumino K-i, Kawaguchi M, et al. Influence of activated carbon pore structure on oxygen reduction at catalyst layers supported on rotating disk electrodes[J]. Carbon, 2004, 42(15): 3115-3121.

[24] Maruyama J, Abe I. Effective utilization of nanospaces in activated carbon for enhancing catalytic activity in fuel cell electrodes[J]. Journal of The Electrochemical Society, 2004, 151(3): A447-A451.

[25] Qi J, Jiang L H, Wang S L, et al. Synthesis of graphitic mesoporous carbons with high surface areas and their applications in direct methanol fuel cells[J]. Applied Catalysis B: Environmental, 2011, 107(1/2): 95-103.

[26] Zhou Z H, Wang S L, Zhou W L, et al. Novel synthesis of highly active Pt/C cathode electrocatalyst for direct methanol fuel cell[J]. Chemical Communications, 2003, 3: 394-395.

[27] Gloaguen F, Andolfatto F, Durand R, et al. Kinetic study of electrochemical reactions at catalyst-recast ionomer interfaces from thin active layer modelling[J]. Journal of Applied Electrochemistry, 1994, 24(9): 863-869.

[28] Paulus U A, Schmidt T J, Gasteiger H A, et al. Oxygen reduction on a high-surface area Pt/Vulcan carbon catalyst: a thin-film rotating ring-disk electrode study[J]. Journal of Electroanalytical Chemistry, 2001, 495(2): 134-145.

[29] Garsany Y, Baturina O A, Swider-Lyons K E, et al. Experimental methods for quantifying the activity of platinum electrocatalysts for the oxygen reduction reaction[J]. Analytical Chemistry, 2010, 82(15): 6321-6328.

[30] ōya A, Marsh H. Phenomena of catalytic graphitization[J]. Journal of Materials Science, 1982, 17(2): 309-322.

[31] Marsh H, Crawford D, Taylor D W. Catalytic graphitization by iron of isotropic carbon from polyfurfuryl alcohol, 725-1090 K. A high resolution electron microscope study[J]. Carbon, 1983, 21(1): 81-87.

[32] Derbyshire F J, Presland A E B, Trimm D L. Graphite formation by the dissolution-precipitation of carbon in cobalt, nickel and iron[J]. Carbon, 1975, 13(2): 111-113.

[33] Lei Z, Lu L, Zhao X S. The electrocapacitive properties of graphene oxide reduced by urea[J]. Energy & Environmental Science, 2012, 5(4): 6391-6399.

[34] Sevilla M, Sanchís C, Valdés-Solís T, et al. Synthesis of graphitic carbon nanostructures from sawdust and their application as electrocatalyst supports[J]. The Journal of Physical Chemistry C, 2007, 111(27): 9749-9756.

[35] Wu G, Mack N H, Gao W, et al. Nitrogen-doped graphene-rich catalysts derived from heteroatom polymers for oxygen reduction in nonaqueous Lithium-O2 battery cathodes[J]. ACS Nano, 2012, 6(11): 9764-9776.

[36] Tuinstra F, Koenig J L. Raman spectrum of graphite[J]. The Journal of Chemical Physics, 1970, 53(3): 1126-1130.

[37] Mason K S, Neyerlin K C, Kuo M-C, et al. Investigation of a silicotungstic acid functionalized carbon on Pt activity and durability for the oxygen reduction reaction[J]. Journal of The Electrochemical Society, 2012, 159(12): F871-F879.

[38] Riese A, Banham D, Ye S, et al. Accelerated stress testing by rotating disk electrode for carbon corrosion in fuel cell catalyst supports[J]. Journal of The Electrochemical Society, 2015, 162(7): F783-F788.

[39] Tarasevich M R, Bogdanovskaya V A, Zagudaeva N M. Redox reactions of quinones on carbon materials[J]. Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, 1987, 223(1/2): 161-169.

[40] Artyushkova K, Pylypenko S, Dowlapalli M, et al. Structure-to-property relationships in fuel cell catalyst supports: Correlation of surface chemistry and morphology with oxidation resistance of carbon blacks[J]. Journal of Power Sources, 2012, 214: 303-313.

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