Pd-induced Pt(IV) reduction to form Pd@Pt/CNT core@shell catalyst for a more complete oxygen reduction

We describe a facile and controllable process for preparing Pd@Pt/CNT core@shell catalysts for the oxygen reduction reaction (ORR) via Pd-induced Pt(IV) reduction on Pd/CNT. The mass-specific activity for the ORR of the Pd@Pt/CNT catalysts is 7–9 times higher than that of the state-of-the-art Pt/C catalysts, but the yield of H2O2, a harmful species for the stability of catalysts, of the former is only 14.1% of that of the latter. The reason for the enhanced activity and the lower H2O2 yield on the Pd@Pt/CNT catalysts was studied by DFT calculations.

[1]  C. Korzeniewski,et al.  Synthesis of PtCu3 bimetallic nanoparticles as oxygen reduction catalysts via a sonochemical method , 2013 .

[2]  X. Qi,et al.  Experimental and DFT study of thiol-stabilized Pt/CNTs catalysts. , 2012, Physical chemistry chemical physics : PCCP.

[3]  R. Sougrat,et al.  Hollow Au@Pd and Au@Pt core–shell nanoparticles as electrocatalysts for ethanol oxidation reactions , 2012 .

[4]  Yawen Tang,et al.  Platinum–Cobalt alloy networks for methanol oxidation electrocatalysis , 2012 .

[5]  J. Wilcox,et al.  Mechanisms of the Oxygen Reduction Reaction on Defective Graphene-Supported Pt Nanoparticles from First-Principles , 2012 .

[6]  Jennifer Wilcox,et al.  DFT-Based Study on Oxygen Adsorption on Defective Graphene-Supported Pt Nanoparticles , 2011 .

[7]  Lichun Dong,et al.  Enhanced dispersion and durability of Pt nanoparticles on a thiolated CNT support. , 2011, Chemical communications.

[8]  Stanislaus S. Wong,et al.  Enhanced electrocatalytic performance of processed, ultrathin, supported Pd-Pt core-shell nanowire catalysts for the oxygen reduction reaction. , 2011, Journal of the American Chemical Society.

[9]  R. Li,et al.  A highly durable platinum nanocatalyst for proton exchange membrane fuel cells: multiarmed starlike nanowire single crystal. , 2011, Angewandte Chemie.

[10]  Alessandro Troisi,et al.  Electronic Structure of TiO2 Surfaces and Effect of Molecular Adsorbates Using Different DFT Implementations , 2010 .

[11]  Jia X Wang,et al.  Enhancing Oxygen Reduction Reaction Activity via Pd−Au Alloy Sublayer Mediation of Pt Monolayer Electrocatalysts , 2010 .

[12]  M. Engelhard,et al.  Chromium-assisted synthesis of platinum nanocube electrocatalysts. , 2010, Chemical communications.

[13]  J. Kim,et al.  Synthesis of carbon nanotube supported Pd catalysts and evaluation of their catalytic properties for CC bond forming reactions , 2010 .

[14]  Jing Zhuang,et al.  Pd-Pt random alloy nanocubes with tunable compositions and their enhanced electrocatalytic activities. , 2010, Chemical communications.

[15]  Zidong Wei,et al.  Durability study of Pt–Pd/C as PEMFC cathode catalyst , 2010 .

[16]  Xun Wang,et al.  Single-phase aqueous approach toward Pd sub-10 nm nanocubes and Pd-Pt heterostructured ultrathin nanowires. , 2009, Chemical communications.

[17]  Younan Xia,et al.  Pd-Pt Bimetallic Nanodendrites with High Activity for Oxygen Reduction , 2009, Science.

[18]  Jens K. Nørskov,et al.  Combinatorial Density Functional Theory-Based Screening of Surface Alloys for the Oxygen Reduction Reaction , 2009 .

[19]  Younan Xia,et al.  Facile synthesis of highly faceted multioctahedral Pt nanocrystals through controlled overgrowth. , 2008, Nano letters.

[20]  Junliang Zhang,et al.  Bimetallic and Ternary Alloys for Improved Oxygen Reduction Catalysis , 2007 .

[21]  E. Wang,et al.  High-Efficiency and Low-Cost Hybrid Nanomaterial as Enhancing Electrocatalyst: Spongelike Au/Pt Core/Shell Nanomaterial with Hollow Cavity , 2007 .

[22]  Siyu Ye,et al.  Recent advances in activity and durability enhancement of Pt/C catalytic cathode in PEMFC: Part II: Degradation mechanism and durability enhancement of carbon supported platinum catalyst , 2007 .

[23]  Geping Yin,et al.  Understanding and Approaches for the Durability Issues of Pt-Based Catalysts for PEM Fuel Cell , 2007 .

[24]  Geping Yin,et al.  Effect of carbon black support corrosion on the durability of Pt/C catalyst , 2007 .

[25]  C. Yeh,et al.  Poly(vinylpyrrolidone)-modified graphite carbon nanofibers as promising supports for PtRu catalysts in direct methanol fuel cells. , 2007, Journal of the American Chemical Society.

[26]  Yan-hui Xu,et al.  Facile fabrication and electrocatalytic activity of Pt0.9Pd0.1 alloy film catalysts , 2007 .

[27]  Wenzheng Li,et al.  Supportless Pt and PtPd nanotubes as electrocatalysts for oxygen-reduction reactions. , 2007, Angewandte Chemie.

[28]  K. Sasaki,et al.  Stabilization of Platinum Oxygen-Reduction Electrocatalysts Using Gold Clusters , 2007, Science.

[29]  Bongjin Simon Mun,et al.  Trends in electrocatalysis on extended and nanoscale Pt-bimetallic alloy surfaces. , 2007, Nature materials.

[30]  I. Hsing,et al.  The effect of the Pt deposition method and the support on Pt dispersion on carbon nanotubes , 2006 .

[31]  Jens K Nørskov,et al.  Changing the activity of electrocatalysts for oxygen reduction by tuning the surface electronic structure. , 2006, Angewandte Chemie.

[32]  Hong Yang,et al.  Synthesis of porous platinum nanoparticles. , 2006, Small.

[33]  Younan Xia,et al.  Polyol synthesis of platinum nanostructures: control of morphology through the manipulation of reduction kinetics. , 2005, Angewandte Chemie.

[34]  Junliang Zhang,et al.  Controlling the catalytic activity of platinum-monolayer electrocatalysts for oxygen reduction with different substrates. , 2005, Angewandte Chemie.

[35]  H. Gasteiger,et al.  Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs , 2005 .

[36]  Wenzheng Li,et al.  An improved palladium-based DMFCs cathode catalyst. , 2004, Chemical communications.

[37]  William A Goddard,et al.  Agostic interactions and dissociation in the first layer of water on Pt(111). , 2004, Journal of the American Chemical Society.

[38]  Junliang Zhang,et al.  Platinum monolayer electrocatalysts for O2 reduction: Pt monolayer on Pd(111) and on carbon-supported Pd nanoparticles , 2004 .

[39]  C. Brinker,et al.  Controlled synthesis of 2-D and 3-D dendritic platinum nanostructures. , 2004, Journal of the American Chemical Society.

[40]  W. Pompe,et al.  Growth of Platinum Clusters via Addition of Pt(II) Complexes: A First Principles Investigation , 2003 .

[41]  B. Delley Hardness conserving semilocal pseudopotentials , 2002 .

[42]  B. Delley From molecules to solids with the DMol3 approach , 2000 .

[43]  Jihoon Cho,et al.  Particle size and alloying effects of Pt-based alloy catalysts for fuel cell applications , 2000 .

[44]  Jens K. Nørskov,et al.  Theoretical surface science and catalysis—calculations and concepts , 2000 .

[45]  J. Prakash,et al.  Kinetic Investigations of Oxygen Reduction and Evolution Reactions on Lead Ruthenate Catalysts , 1999 .

[46]  Masahiro Watanabe,et al.  Activity and Stability of Ordered and Disordered Co‐Pt Alloys for Phosphoric Acid Fuel Cells , 1994 .

[47]  Sanjeev Mukerjee,et al.  Enhanced electrocatalysis of oxygen reduction on platinum alloys in proton exchange membrane fuel cells , 1993 .

[48]  Wang,et al.  Accurate and simple analytic representation of the electron-gas correlation energy. , 1992, Physical review. B, Condensed matter.

[49]  B. Delley An all‐electron numerical method for solving the local density functional for polyatomic molecules , 1990 .

[50]  E. J. Taylor,et al.  Importance of Interatomic Spacing in Catalytic Reduction of Oxygen in Phosphoric Acid , 1983 .