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Characterization and Theory of Electrocatalysts Based on Scanning Electrochemical Microscopy Screening Methods

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Department of Chemistry and Biochemistry, The University of Texas at Austin, Austin, Texas 78712
Cite this: Langmuir 2006, 22, 25, 10426–10431
Publication Date (Web):September 27, 2006
https://doi.org/10.1021/la061164h
Copyright © 2006 American Chemical Society

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    A strategy for finding new electrocatalysts for the oxygen reduction reaction (ORR) in acidic solutions is outlined and illustrated with results for Pd−Co catalysts. This is based on establishing guidelines for selecting test systems, rapid preparation of arrays, and rapid screening by scanning electrochemical microscopy. Promising candidates are further tested as supported electrocatalysts by larger scale electrochemical methods and in fuel cells, with optimization of the composition and structure. Those that emerge are characterized by a variety of methods, including X-ray diffraction, scanning electron microscopy, and X-ray photoemission spectroscopy. Finally, density functional theory is used for detailed calculations of oxygen adsorption and dissociation on the material and provides better guidelines for further testing.

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     Part of the Electrochemistry special issue.

     Current address:  Facultad de Ingeniería Química, Universidad Nacional del Litoral, Santa Fe, Argentina.

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     To whom correspondence should be addressed.

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    11. Jeffrey Yue, Zheng Du, and Minhua Shao . Mechanisms of Enhanced Electrocatalytic Activity for Oxygen Reduction Reaction on High-Index Platinum n(111)–(111) Surfaces. The Journal of Physical Chemistry Letters 2015, 6 (17) , 3346-3351. https://doi.org/10.1021/acs.jpclett.5b01345
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    13. Stephen E. Fosdick, Sean P. Berglund, C. Buddie Mullins, and Richard M. Crooks . Parallel Screening of Electrocatalyst Candidates Using Bipolar Electrochemistry. Analytical Chemistry 2013, 85 (4) , 2493-2499. https://doi.org/10.1021/ac303581b
    14. Lihui Ou and Shengli Chen . Comparative Study of Oxygen Reduction Reaction Mechanisms on the Pd(111) and Pt(111) Surfaces in Acid Medium by DFT. The Journal of Physical Chemistry C 2013, 117 (3) , 1342-1349. https://doi.org/10.1021/jp309094b
    15. Xiaomei Lin, Liyan Zheng, Gongmin Gao, Yuwu Chi, and Guonan Chen . Electrochemiluminescence Imaging-Based High-Throughput Screening Platform for Electrocatalysts Used in Fuel Cells. Analytical Chemistry 2012, 84 (18) , 7700-7707. https://doi.org/10.1021/ac300875x
    16. Stephen E. Fosdick and Richard M. Crooks . Bipolar Electrodes for Rapid Screening of Electrocatalysts. Journal of the American Chemical Society 2012, 134 (2) , 863-866. https://doi.org/10.1021/ja210354m
    17. Fen Zhang, Vladimir Roznyatovskiy, Fu-Ren F. Fan, Vincent Lynch, Jonathan L. Sessler, and Allen J. Bard . A Method for Rapid Screening of Photosensitizers by Scanning Electrochemical Microscopy (SECM) and the Synthesis and Testing of a Porphyrin Sensitizer. The Journal of Physical Chemistry C 2011, 115 (5) , 2592-2599. https://doi.org/10.1021/jp110482v
    18. Allen J. Bard. Inner-Sphere Heterogeneous Electrode Reactions. Electrocatalysis and Photocatalysis: The Challenge. Journal of the American Chemical Society 2010, 132 (22) , 7559-7567. https://doi.org/10.1021/ja101578m
    19. Sue V. Myers, Anatoly I. Frenkel and Richard M. Crooks . X-ray Absorption Study of PdCu Bimetallic Alloy Nanoparticles Containing an Average of ∼64 Atoms. Chemistry of Materials 2009, 21 (20) , 4824-4829. https://doi.org/10.1021/cm901378x
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    35. Cynthia G. Zoski. Review—Advances in Scanning Electrochemical Microscopy (SECM). Journal of The Electrochemical Society 2016, 163 (4) , H3088-H3100. https://doi.org/10.1149/2.0141604jes
    36. Lihui Ou. Design of Pd-Based Bimetallic Catalysts for ORR: A DFT Calculation Study. Journal of Chemistry 2015, 2015 , 1-11. https://doi.org/10.1155/2015/932616
    37. Andrew J. Wain. Scanning electrochemical microscopy for combinatorial screening applications: A mini-review. Electrochemistry Communications 2014, 46 , 9-12. https://doi.org/10.1016/j.elecom.2014.05.028
    38. Ermete Antolini. Effect of Structural Characteristics of Binary Palladium–Cobalt Fuel Cell Catalysts on the Activity for Oxygen Reduction. ChemPlusChem 2014, 79 (6) , 765-775. https://doi.org/10.1002/cplu.201402034
    39. H. Gharibi, F. Golmohammadi, M. Kheirmand. Palladium/Cobalt Coated on Multi‐Walled Carbon Nanotubes as an Electro‐catalyst for Oxygen Reduction Reaction in Passive Direct Methanol Fuel Cells. Fuel Cells 2013, 13 (6) , 987-1004. https://doi.org/10.1002/fuce.201200220
    40. Kristel Jukk, Nadezda Alexeyeva, Peeter Ritslaid, Jekaterina Kozlova, Väino Sammelselg, Kaido Tammeveski. Electrochemical Reduction of Oxygen on Heat-Treated Pd Nanoparticle/Multi-Walled Carbon Nanotube Composites in Alkaline Solution. Electrocatalysis 2013, 4 (1) , 42-48. https://doi.org/10.1007/s12678-012-0117-y
    41. Hussein Gharibi, Farhad Golmohammadi, Mehdi Kheirmand. Fabrication of MEA based on optimum amount of Co in Pd Co/C alloy nanoparticles as a new cathode for oxygen reduction reaction in passive direct methanol fuel cells. Electrochimica Acta 2013, 89 , 212-221. https://doi.org/10.1016/j.electacta.2012.10.147
    42. Minhua Shao. Palladium-Based Electrocatalysts for Oxygen Reduction Reaction. 2013, 513-531. https://doi.org/10.1007/978-1-4471-4911-8_17
    43. Masahiro Watanabe, Donald A. Tryk, Mitsuru Wakisaka, Hiroshi Yano, Hiroyuki Uchida. Overview of recent developments in oxygen reduction electrocatalysis. Electrochimica Acta 2012, 84 , 187-201. https://doi.org/10.1016/j.electacta.2012.04.035
    44. Wenpeng Li, Fu-Ren F. Fan, Allen J. Bard. The application of scanning electrochemical microscopy to the discovery of Pd–W electrocatalysts for the oxygen reduction reaction that demonstrate high activity, stability, and methanol tolerance. Journal of Solid State Electrochemistry 2012, 16 (7) , 2563-2568. https://doi.org/10.1007/s10008-012-1775-7
    45. Sabine Schimpf, Michael Bron. Catalysis in Low‐Temperature Fuel Cells – An Overview. 2012, 407-438. https://doi.org/10.1002/9783527650248.ch15
    46. Ch. Venkateswara Rao, B. Viswanathan. Microemulsion synthesis and electrocatalytic properties of carbon-supported Pd–Co–Au alloy nanoparticles. Journal of Colloid and Interface Science 2012, 367 (1) , 337-341. https://doi.org/10.1016/j.jcis.2011.10.020
    47. W. Schuhmann, M. Bron. Scanning electrochemical microscopy (SECM) in proton exchange membrane fuel cell research and development. 2012, 399-424. https://doi.org/10.1533/9780857095480.3.399
    48. Yun Cai, Radoslav R. Adzic. Platinum Monolayer Electrocatalysts for the Oxygen Reduction Reaction: Improvements Induced by Surface and Subsurface Modifications of Cores. Advances in Physical Chemistry 2011, 2011 , 1-16. https://doi.org/10.1155/2011/530397
    49. M. Neergat, V. Gunasekar, R. Rahul. Carbon-supported Pd–Fe electrocatalysts for oxygen reduction reaction (ORR) and their methanol tolerance. Journal of Electroanalytical Chemistry 2011, 658 (1-2) , 25-32. https://doi.org/10.1016/j.jelechem.2011.04.016
    50. Minhua Shao. Palladium-based electrocatalysts for hydrogen oxidation and oxygen reduction reactions. Journal of Power Sources 2011, 196 (5) , 2433-2444. https://doi.org/10.1016/j.jpowsour.2010.10.093
    51. Yu-Ching Weng, Cheng-Tse Hsieh. Scanning electrochemical microscopy characterization of bimetallic Pt–M (M=Pd, Ru, Ir) catalysts for hydrogen oxidation. Electrochimica Acta 2011, 56 (5) , 1932-1940. https://doi.org/10.1016/j.electacta.2010.12.029
    52. Tongyu Wang, Baihai Li, Jianhui Yang, Hong Chen, Liang Chen. First principles study of oxygen adsorption and dissociation on the Pd/Au surface alloys. Physical Chemistry Chemical Physics 2011, 13 (15) , 7112. https://doi.org/10.1039/c0cp02007a
    53. S. Venkatachalam, T. Jacob. Density functional theory applied to electrocatalysis. 2010https://doi.org/10.1002/9780470974001.f500008
    54. S. Axnanda, K. D. Cummins, T. He, D. W. Goodman, M. P. Soriaga. Structural, Compositional and Electrochemical Characterization of Pt–Co Oxygen‐Reduction Catalysts. ChemPhysChem 2010, 11 (7) , 1468-1475. https://doi.org/10.1002/cphc.200900924
    55. Ch. Venkateswara Rao, B. Viswanathan. Carbon supported Pd–Co–Mo alloy as an alternative to Pt for oxygen reduction in direct ethanol fuel cells. Electrochimica Acta 2010, 55 (8) , 3002-3007. https://doi.org/10.1016/j.electacta.2009.12.094
    56. John A. Keith, Timo Jacob. Computational Simulations on the Oxygen Reduction Reaction in Electrochemical Systems. 2010, 89-132. https://doi.org/10.1007/978-1-4419-5594-4_3
    57. Stephanus Axnanda, Kyle D. Cummins, D. Wayne Goodman, Manuel P. Soriaga. Characterization of Alloy Electrocatalysts by Combined Low-Energy Ion Scattering Spectroscopy and Electrochemistry. 2010, 1-23. https://doi.org/10.1007/978-1-4419-5594-4_1
    58. Michel Keddam, Nicolas Portail, Dao Trinh, Vincent Vivier. Progress in Scanning Electrochemical Microscopy by Coupling with Electrochemical Impedance and Quartz Crystal Microbalance. ChemPhysChem 2009, 10 (18) , 3175-3182. https://doi.org/10.1002/cphc.200900506
    59. Vladislavs Stonkus, Kristine Edolfa, Ludmila Leite, Janusz W. Sobczak, Ludmila Plyasova, Petya Petrova. Palladium-promoted Co–SiO2 catalysts for 1,4-butanediol cyclization. Applied Catalysis A: General 2009, 362 (1-2) , 147-154. https://doi.org/10.1016/j.apcata.2009.04.033
    60. Ye Xu, Minhua Shao, Manos Mavrikakis, Radoslav R. Adzic. Recent Developments in the Electrocatalysis of the O 2 Reduction Reaction. 2009, 271-315. https://doi.org/10.1002/9780470463772.ch9
    61. Ermete Antolini. Palladium in fuel cell catalysis. Energy & Environmental Science 2009, 2 (9) , 915. https://doi.org/10.1039/b820837a
    62. Cheng-Lan Lin, Carlos M. Sánchez-Sánchez, Allen J. Bard. Methanol Tolerance of Pd–Co Oxygen Reduction Reaction Electrocatalysts Using Scanning Electrochemical Microscopy. Electrochemical and Solid-State Letters 2008, 11 (8) , B136. https://doi.org/10.1149/1.2931020
    63. L. Jiang, L. Colmenares, Z. Jusys, R. J. Behm. Multiple Wall-Jet Flow Cell Setup for Quantitative Parallel Evaluation of Carbon-Supported Electrocatalysts under Fuel Cell Relevant Conditions. Journal of The Electrochemical Society 2008, 155 (9) , B908. https://doi.org/10.1149/1.2946479
    64. J.J. Salvador-Pascual, S. Citalán-Cigarroa, O. Solorza-Feria. Kinetics of oxygen reduction reaction on nanosized Pd electrocatalyst in acid media. Journal of Power Sources 2007, 172 (1) , 229-234. https://doi.org/10.1016/j.jpowsour.2007.05.093
    65. Sabine Szunerits, Sascha E. Pust, Gunther Wittstock. Multidimensional electrochemical imaging in materials science. Analytical and Bioanalytical Chemistry 2007, 389 (4) , 1103-1120. https://doi.org/10.1007/s00216-007-1374-0