A facile method to synthesize supported Pd–Au nanoparticles using graphene oxide as the reductant and their extremely high electrocatalytic activity for the electrooxidation of methanol and ethanol

A facile and environmentally friendly method for preparing Pd–Au/reduced graphene oxide (RGO) hybrids with different Pd/Au ratios has been established. The method uses redox reactions between K2PdCl4, HAuCl4 and GO nanosheets and the subsequent thermal reduction of the material at 200 °C in a vacuum oven. Unlike previous methods for preparing metallic nanoparticles, GO nanosheets were used as the reducing agent, the stabilizing agent and the support for the metallic alloy nanoparticles. The composition and morphology of the Pd–Au/RGO were characterized by X-ray diffraction, thermo-gravimetric analysis, X-ray photoelectron spectroscopy and transmission electron microscopy. The composition of these Pd–Au/RGO catalysts can be adjusted so that the catalysts exhibit high activity for the electrooxidation of methanol and ethanol in alkaline media. Interestingly, Pd–Au/RGO shows better electrocatalytic activity and stability than Pd–RGO for the oxidation of methanol and ethanol. This indicates that these Pd–Au/RGO catalysts should have great potential applications in direct methanol and ethanol fuel cells.

[1]  Jianping Gao,et al.  One pot preparation of reduced graphene oxide (RGO) or Au (Ag) nanoparticle-RGO hybrids using chitosan as a reducing and stabilizing agent and their use in methanol electrooxidation , 2012 .

[2]  Chun‐Sing Lee,et al.  Bimetallic PtPd nanoparticles on Nafion–graphene film as catalyst for ethanol electro-oxidation , 2012 .

[3]  Y. Kuang,et al.  Reduced graphene oxide supported palladium–silver bimetallic nanoparticles for ethanol electro-oxidation in alkaline media , 2012, Journal of Materials Science.

[4]  Zhongyuan Huang,et al.  Preparation of well-dispersed PdAu bimetallic nanoparticles on reduced graphene oxide sheets with excellent electrochemical activity for ethanol oxidation in alkaline media , 2012 .

[5]  Shichao Zhang,et al.  Investigation of methanol electrooxidation on Au/C catalyst in alkaline medium , 2011 .

[6]  Q. Yi,et al.  Electrochemical Activity of Novel Titanium‐Supported Porous Binary Pd‐Ru Particles for Ethanol Oxidation in Alkaline Media , 2011 .

[7]  Jun‐Jie Zhu,et al.  Sonoelectrochemical fabrication of PDDA-RGO-PdPt nanocomposites as electrocatalyst for DAFCs , 2011 .

[8]  Jie Yin,et al.  Facile synthesis of soluble graphene via a green reduction of graphene oxide in tea solution and its biocomposites. , 2011, ACS applied materials & interfaces.

[9]  Shichao Zhang,et al.  Electrocatalytic Performance of Gold Nanoparticles Supported on Activated Carbon for Methanol Oxidation in Alkaline Solution , 2011 .

[10]  Xiao-ru Wang,et al.  Synthesis of "clean" and well-dispersive Pd nanoparticles with excellent electrocatalytic property on graphene oxide. , 2011, Journal of the American Chemical Society.

[11]  Yanchun Zhao,et al.  Enhanced electrocatalytic oxidation of methanol on Pd/polypyrrole-graphene in alkaline medium , 2011 .

[12]  Yan Shi,et al.  Carbon nanotube/raspberry hollow Pd nanosphere hybrids for methanol, ethanol, and formic acid electro-oxidation in alkaline media. , 2010, Journal of colloid and interface science.

[13]  Yanchun Zhao,et al.  MnO2 modified multi-walled carbon nanotubes supported Pd nanoparticles for methanol electro-oxidation in alkaline media , 2010 .

[14]  J. Tour,et al.  Decoration, Migration, and Aggregation of Palladium Nanoparticles on Graphene Sheets , 2010 .

[15]  Chun’an Ma,et al.  Effect of carbon nanofibers microstructure on electrocatalytic activities of Pd electrocatalysts for ethanol oxidation in alkaline medium , 2010 .

[16]  Yanchun Zhao,et al.  Methanol electro-oxidation on Ni@Pd core-shell nanoparticles supported on multi-walled carbon nanotubes in alkaline media , 2010 .

[17]  J. Tascón,et al.  Vitamin C Is an Ideal Substitute for Hydrazine in the Reduction of Graphene Oxide Suspensions , 2010 .

[18]  K. El-Khatib,et al.  Ni-P and Ni-Cu-P modified carbon catalysts for methanol electro-oxidation in KOH solution , 2010 .

[19]  Yuyan Shao,et al.  Facile and controllable electrochemical reduction of graphene oxide and its applications , 2010 .

[20]  Ashutosh Kumar Singh,et al.  Electrocatalytic activities of binary and ternary composite electrodes of Pd, nanocarbon and Ni for electro-oxidation of methanol in alkaline medium , 2009 .

[21]  L. Hong,et al.  Physical and electrochemical characterizations of nanostructured Pd/C and PdNi/C catalysts for methanol oxidation , 2009 .

[22]  Yueming Li,et al.  Preparation and electrochemical performance for methanol oxidation of pt/graphene nanocomposites , 2009 .

[23]  R. Ruoff,et al.  Chemical methods for the production of graphenes. , 2009, Nature nanotechnology.

[24]  Xiaogang Zhang,et al.  Highly dispersed Pd nanoparticles on covalent functional MWNT surfaces for methanol oxidation in alkaline solution , 2009 .

[25]  Ashutosh Kumar Singh,et al.  Electrocatalytic activity of binary and ternary composite films of Pd, MWCNT and Ni, Part II: Methanol electrooxidation in 1 M KOH , 2009 .

[26]  M. S. Hegde,et al.  Controlled Attachment of Ultrafine Platinum Nanoparticles on Functionalized Carbon Nanotubes with High Electrocatalytic Activity for Methanol Oxidation , 2009 .

[27]  T. Maiyalagan.  Synthesis and electro catalytic activity of methanol oxidation on nitrogen containing carbon nanotubes supported Pt electrodes , 2008 .

[28]  Yonglang Guo,et al.  Enhanced activity of PtSn/C anodic electrocatalyst prepared by formic acid reduction for direct ethanol fuel cells , 2008 .

[29]  S. Stankovich,et al.  Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide , 2007 .

[30]  P. Shen,et al.  Methanol and ethanol electrooxidation on Pt and Pd supported on carbon microspheres in alkaline media , 2007 .

[31]  K. Jeng,et al.  Effective preparation of carbon nanotube-supported Pt–Ru electrocatalysts , 2006 .

[32]  S. Stankovich,et al.  Graphene-based composite materials , 2006, Nature.

[33]  J. S. Lee,et al.  Tungsten carbide microspheres as a noble-metal-economic electrocatalyst for methanol oxidation. , 2005, Angewandte Chemie.

[34]  Yuehe Lin,et al.  PtRu/carbon nanotube nanocomposite synthesized in supercritical fluid: a novel electrocatalyst for direct methanol fuel cells. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[35]  J. Datta,et al.  Electrode kinetics of ethanol oxidation on novel CuNi alloy supported catalysts synthesized from PTFE suspension , 2005 .

[36]  Hu-lin Li,et al.  Highly dispersed Ag nanoparticles on functional MWNT surfaces for methanol oxidation in alkaline solution , 2005 .

[37]  G. Kästle,et al.  Oxidation-Resistant Gold-55 Clusters , 2002, Science.

[38]  Sarunya Bangsaruntip,et al.  Spontaneous reduction of metal ions on the sidewalls of carbon nanotubes. , 2002, Journal of the American Chemical Society.

[39]  R. Pattabiraman,et al.  Electrochemical investigations on carbon supported palladium catalysts , 1997 .

[40]  R. Compton,et al.  Magnetically moveable bimetallic (nickel/silver) nanoparticle/carbon nanotube composites for methanol oxidation , 2009 .

[41]  P. Shen,et al.  Alcohol oxidation on nanocrystalline oxide Pd/C promoted electrocatalysts , 2006 .

[42]  C. Ania,et al.  Extension of preparation methods employed with ceramic materials to carbon honeycomb monoliths , 2004 .