Gold dissolution: towards understanding of noble metal corrosion

The electrochemical dissolution of gold is an intricate topic and even though it has been studied for more than 50 years, its understanding remains rather limited. In the current work, we obtain unique information on gold dissolution by using a setup composed of a micro-electrochemical scanning flow cell (SFC) and inductively coupled plasma mass spectrometry (ICP-MS). Thus, comprehensive online gold dissolution profiles during the initial stage of oxidation as a function of the potential, time and pH are presented. A microscopic model explaining the experimental findings is proposed. According to this model, two dissolution mechanisms take place in two different potential regions: at low anodic potentials the dissolution is driven by the place-exchange between metal and adsorbed hydroxyl/oxygen ions, while at higher potentials the oxygen evolution reaction taking place on the surface of gold oxide initiates concomitant gold loss.

[1]  F. Calle‐Vallejo,et al.  Electrochemical water splitting by gold: evidence for an oxide decomposition mechanism , 2013 .

[2]  K. Mayrhofer,et al.  Electrochemical dissolution of gold in acidic medium , 2013 .

[3]  R. Compton,et al.  Surface oxidation of gold nanoparticles supported on a glassy carbon electrode in sulphuric acid medium: contrasts with the behaviour of 'macro' gold. , 2013, Physical chemistry chemical physics : PCCP.

[4]  K. Mayrhofer,et al.  Dissolution of Platinum: Limits for the Deployment of Electrochemical Energy Conversion?** , 2012, Angewandte Chemie.

[5]  K. Mayrhofer,et al.  Time and potential resolved dissolution analysis of rhodium using a microelectrochemical flow cell coupled to an ICP-MS , 2012 .

[6]  Masanobu Chiku,et al.  Simple Preparation of Au Nanoparticles and Their Application to Au Core/Pt Shell Catalysts for Oxygen Reduction Reaction , 2012, Electrocatalysis.

[7]  A. Nishikata,et al.  Channel flow double electrode study on palladium dissolution during potential cycling in sulfuric acid solution , 2012 .

[8]  C. Chung,et al.  Utilization of surface active sites on gold in preparation of highly reactive interfaces for alcohols electrooxidation in alkaline media , 2012 .

[9]  Thomas J. Schmidt,et al.  Electrocatalysis for Polymer Electrolyte Fuel Cells: Recent Achievements and Future Challenges , 2012 .

[10]  A. Kostka,et al.  Degradation Mechanisms of Pt/C Fuel Cell Catalysts under Simulated Start–Stop Conditions , 2012 .

[11]  Yingying Chen,et al.  Heterogeneous Au-Pt nanostructures with enhanced catalytic activity toward oxygen reduction. , 2012, Dalton Transactions.

[12]  Jun Chen,et al.  Metal-air batteries: from oxygen reduction electrochemistry to cathode catalysts. , 2012, Chemical Society reviews.

[13]  Chan-Hwa Chung,et al.  Nanoporous Pt@Au(x)Cu(100-x) by hydrogen evolution assisted electrodeposition of Au(x)Cu(100-x) and galvanic replacement of Cu with Pt: electrocatalytic properties. , 2012, Langmuir : the ACS journal of surfaces and colloids.

[14]  A. Nishikata,et al.  Application of channel flow double electrode to the study on gold dissolution during potential cycling in sulfuric acid solution , 2012 .

[15]  F. Scholz,et al.  The effects of pretreatment of polycrystalline gold with OH• radicals on the electrochemical nucleation and growth of platinum , 2012, Journal of Solid State Electrochemistry.

[16]  A. Nishikata,et al.  Application of channel flow double electrode to the study on platinum dissolution during potential cycling in sulfuric acid solution , 2011 .

[17]  Angel A Topalov,et al.  Development and integration of a LabVIEW-based modular architecture for automated execution of electrochemical catalyst testing. , 2011, The Review of scientific instruments.

[18]  Zhipan Liu,et al.  Mechanism of Oxygen Electro-Reduction on Au-Modified Pt: Minimizing O Coverage and Pt Site Exposure toward Highly Stable and Active Cathode , 2011 .

[19]  C. Chung,et al.  Pt and Pd decorated Au nanowires: Extremely high activity of ethanol oxidation in alkaline media , 2011 .

[20]  A. Shukla,et al.  Durable electrocatalytic-activity of Pt-Au/C cathode in PEMFCs. , 2011, Physical chemistry chemical physics : PCCP.

[21]  Y. Tong,et al.  Electrocatalytic properties of Au@Pt nanoparticles: effects of Pt shell packing density and Au core size. , 2011, Physical chemistry chemical physics : PCCP.

[22]  G. Láng,et al.  RRDE experiments with potential scans at the ring and disk electrodes , 2011 .

[23]  T. Zhao,et al.  Effect of surface composition of Pt-Au alloy cathode catalyst on the performance of direct methanol fuel cells , 2010 .

[24]  Shuo Chen,et al.  Platinum-gold nanoparticles: a highly active bifunctional electrocatalyst for rechargeable lithium-air batteries. , 2010, Journal of the American Chemical Society.

[25]  S. Fletcher,et al.  Selective knockout of gold active sites. , 2010, Angewandte Chemie.

[26]  F. Scholz,et al.  Hydroxyl radicals attack metallic gold. , 2010, Angewandte Chemie.

[27]  M. Bäumer,et al.  Nanoporous Gold Catalysts for Selective Gas-Phase Oxidative Coupling of Methanol at Low Temperature , 2010, Science.

[28]  Fritz Scholz,et al.  Electro analytical methods: guide to experiments and applications. , 2010 .

[29]  Chan-Hwa Chung,et al.  Gold nanowire array electrode for non-enzymatic voltammetric and amperometric glucose detection , 2009 .

[30]  A. Nishikata,et al.  Channel-Flow Double-Electrode Study on the Dissolution and Deposition Potentials of Platinum under Potential Cycles , 2009 .

[31]  A. Skundin,et al.  Boris Vul’fovich (Vladimirovich) Ershler (On occasion of his centenary jubilee) , 2009 .

[32]  Sean James Ashton,et al.  An Electrochemical Cell Configuration Incorporating an Ion Conducting Membrane Separator between Reference and Working Electrode , 2009, International Journal of Electrochemical Science.

[33]  B. Conway,et al.  EQCN study of anodic dissolution and surface oxide film formation at Au in the presence of Cl− or Br− ions: A model process for corrosion studies , 2008 .

[34]  Hui Yang,et al.  Enhanced Durability of Au Cluster Decorated Pt Nanoparticles for the Oxygen Reduction Reaction , 2008 .

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

[36]  H. Tang,et al.  PEM fuel cell cathode carbon corrosion due to the formation of air/fuel boundary at the anode , 2006 .

[37]  L. J. Bregoli,et al.  A Reverse-Current Decay Mechanism for Fuel Cells , 2005 .

[38]  G. Tremiliosi‐Filho,et al.  Growth of surface oxides on gold electrodes under well-defined potential, time and temperature conditions☆ , 2005 .

[39]  Zeitschrift für Elektrochemie, Heft 3/4, 1915 , 2005, Naturwissenschaften.

[40]  Charles T. Campbell,et al.  The Active Site in Nanoparticle Gold Catalysis , 2004, Science.

[41]  M. S. Chen,et al.  The Structure of Catalytically Active Gold on Titania , 2004, Science.

[42]  T. Ohsaka,et al.  Electrocatalysis by nanoparticles: oxygen reduction on gold nanoparticles-electrodeposited platinum electrodes , 2003 .

[43]  B. Conway,et al.  Nanogravimetry study of the initial stages of anodic surface oxide film growth at Au in aqueous HClO4 and H2SO4 by means of EQCN , 2003 .

[44]  D. Kolb Structure studies of metal electrodes by in-situ scanning tunneling microscopy , 2000 .

[45]  K. Uosaki,et al.  An In Situ Electrochemical Quartz Crystal Microbalance Study of the Dissolution Process of a Gold Electrode in Perchloric Acid Solution Containing Chloride Ion , 1998 .

[46]  L. Burke,et al.  Multicomponent hydrous oxide films grown on gold in acid solution , 1998 .

[47]  G. Tremiliosi‐Filho,et al.  Limit to extent of formation of the quasi-two-dimensional oxide state on Au electrodes , 1997 .

[48]  B. Conway,et al.  Electrochemical oxide film formation at noble metals as a surface-chemical process , 1995 .

[49]  V. S. Bagot︠s︡kiĭ Fundamentals of electrochemistry , 1993 .

[50]  B. Conway,et al.  A surface‐electrochemical basis for the direct logarithmic growth law for initial stages of extension of anodic oxide films formed at noble metals , 1990 .

[51]  V. V. Losev,et al.  Relationship between corrosion processes and oxygen evolution on anodes made from noble metals and related metal oxide anodes , 1988 .

[52]  M. Wohlfahrt‐Mehrens,et al.  Oxygen evolution on Ru and RuO2 electrodes studied using isotope labelling and on-line mass spectrometry , 1987 .

[53]  H. Angerstein-Kozlowska,et al.  Elementary steps of electrochemical oxidation of single-crystal planes of Au Part II. A chemical and structural basis of oxidation of the (111) plane , 1987 .

[54]  Hiroshi Sano,et al.  Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C , 1987 .

[55]  H. Angerstein-Kozlowska,et al.  Elementary steps of electrochemical oxidation of single-crystal planes of Au—I. Chemical basis of processes involving geometry of anions and the electrode surfaces , 1986 .

[56]  O. Wolter,et al.  Does the Oxide Layer Take Part in the Oxygen Evolution Reaction on Platinum? A DEMS Study. , 1985 .

[57]  O. Wolter,et al.  Does the oxide layer take part in the oxygen evolution reaction on platinum , 1985 .

[58]  F. R. Foulkes,et al.  A Study of Anodic Dissolution of Gold in Aqueous Alkaline Cyanide , 1978 .

[59]  M. Lohrengel,et al.  Electrochemical properties of anodic gold oxide layers—I: Potentiostatic oxide growth and double layer capacity , 1976 .

[60]  M. Pourbaix Atlas of Electrochemical Equilibria in Aqueous Solutions , 1974 .

[61]  S. Cadle,et al.  Ring-disk electrode study of the anodic behavior of gold in 0.2M sulfuric acid , 1974 .

[62]  Y. Kolotyrkin Use of radioactive indicator and electrochemical methods for determining low corrosion rates , 1973 .

[63]  K. J. Vetter,et al.  Kinetics of layer formation and corrosion processes of passive iron in acid solutions , 1973 .

[64]  Ronald Woods,et al.  A study of the dissolution of platinum, palladium, rhodium and gold electrodes in 1 m sulphuric acid by cyclic voltammetry , 1972 .

[65]  K. J. Vetter,et al.  Stromdichte‐ und pH‐Abhängigkeit des elektrochemischen Auf‐ und Abbaus von Oxydschichten auf Pt, Pd und Au , 1958 .

[66]  N. Cabrera,et al.  Theory of the oxidation of metals , 1949 .

[67]  F. H. Campbell Contributions to the chemistry of gold , 1907 .