Electrochemical aspects of copper atmospheric corrosion in the presence of sodium chloride

Schindelholz, Eric John; Cong, Hongbo; Jove-Colon, Carlos F.; Li, Shengxi; Ohlhausen, James A.; Moffat, Harry K.

doi:10.1016/j.electacta.2018.04.184

Electrochemical aspects of copper atmospheric corrosion in the presence of sodium chloride

Journal Article · Thu Apr 26 00:00:00 EDT 2018 · Electrochimica Acta

DOI:https://doi.org/10.1016/j.electacta.2018.04.184· OSTI ID:1444080

Schindelholz, Eric John ^[1]; Cong, Hongbo ^[2]; Jove-Colon, Carlos F. ^[1]; Li, Shengxi ^[2]; Ohlhausen, James A. ^[1]; Moffat, Harry K. ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
The Univ. of Akron, Akron, OH (United States)

Here, this study describes the evolving state of electrolyte and corrosion processes associated with sodium chloride on copper at the initial stage of corrosion and the critical implications of this behavior on controlling kinetics and damage distributions. Sodium chloride droplets were placed on copper in humid conditions and the resulting electrolyte properties, corrosion products and damage were characterized over time using time-lapse imaging, micro Raman spectroscopy, TOF-SIMS and optical profilometry. Within minutes of NaCl droplet placement, NaOH-rich films resultant from oxygen reduction advanced stepwise from the droplets, leaving behind concentric trenching attack patterns suggestive of moving anode-cathode pairs at the alkaline film front. Corrosion attack under these spreading alkaline films was up to 10x greater than under the original NaCl drops. Furthermore, solid Cu₂Cl(OH)₃ shells formed over the surface of the NaCl drops within hours of exposure. Thermodynamic modeling along with immersed electrochemical experiments in simulated droplet and films electrolytes were used to rationalize this behavior and build a description of the rapidly evolving corroding system.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1444080

Report Number(s):: SAND--2018-4517J; 663928

Journal Information:: Electrochimica Acta, Journal Name: Electrochimica Acta Journal Issue: C Vol. 276; ISSN 0013-4686

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (55)

Corrosion of ancient Chinese bronze money trees studied by Raman microscopy McCann, Lowell I.; Trentelman, K.; Possley, T. Journal of Raman Spectroscopy, Vol. 30, Issue 2 https://doi.org/10.1002/(SICI)1097-4555(199902)30:2<121::AID-JRS355>3.0.CO;2-L	journal	February 1999
Raman investigation of artificial patinas on recent bronze – Part I: climatic chamber exposure Ropret, Polonca; Kosec, Tadeja Journal of Raman Spectroscopy, Vol. 43, Issue 11 https://doi.org/10.1002/jrs.4068	journal	July 2012
Effect of halide ions on passivation and pitting Corrosion of copper in alkaline solutions Allah, A. G. Gad; Abou-Romia, M. M.; Badawy, W. A. Materials and Corrosion/Werkstoffe und Korrosion, Vol. 42, Issue 11 https://doi.org/10.1002/maco.19910421105	journal	November 1991
The molar heat capacity of hydrous copper chloride: atacamite Cu2Cl(OH)3 Bisengalieva, Mira R.; Kiseleva, Irina A.; Melchakova, Lyubov V. The Journal of Chemical Thermodynamics, Vol. 29, Issue 3 https://doi.org/10.1006/jcht.1996.0162	journal	March 1997
Equilibrium constants for the formation of Cu(I) halide complexes Sharma, Virender K.; Millero, Frank J. Journal of Solution Chemistry, Vol. 19, Issue 4 https://doi.org/10.1007/BF00648142	journal	April 1990
The Examination of the Activity Coefficients of Cu(II) Complexes with OH− and Cl− in NaClO4 Using Pitzer Equations: Application to Other Divalent Cations Santana-Casiano, J. M.; González-Dávila, M.; Millero, F. J. Journal of Solution Chemistry, Vol. 37, Issue 6 https://doi.org/10.1007/s10953-008-9274-2	journal	April 2008
Copper patinas formed in the atmosphere—I. Introduction Graedel, T. E.; Nassau, K.; Franey, J. P. Corrosion Science, Vol. 27, Issue 7 https://doi.org/10.1016/0010-938X(87)90047-3	journal	January 1987
Metallographic studies of the copper patina formed in the atmosphere Franey, J. P.; Davis, M. E. Corrosion Science, Vol. 27, Issue 7 https://doi.org/10.1016/0010-938X(87)90048-5	journal	January 1987
Copper patinas formed in the atmosphere—II. A qualitative assessment of mechanisms Graedel, T. E. Corrosion Science, Vol. 27, Issue 7 https://doi.org/10.1016/0010-938X(87)90053-9	journal	January 1987
A study by voltammetry and the photocurrent response method of copper electrode behavior in acidic and alkaline solutions containing chloride ions Modestov, A. D.; Zhou, Guo-Ding; Ge, Hong-Hua Journal of Electroanalytical Chemistry, Vol. 380, Issue 1-2 https://doi.org/10.1016/0022-0728(94)03577-P	journal	January 1995
Use of oxidized copper minerals as environmental indicators Woods, Terri L.; Garrels, Robert M. Applied Geochemistry, Vol. 1, Issue 2 https://doi.org/10.1016/0883-2927(86)90002-8	journal	March 1986
The initiation mechanism of corrosion of zinc by sodium chloride particle deposition Neufeld, A. K.; Cole, I. S.; Bond, A. M. Corrosion Science, Vol. 44, Issue 3 https://doi.org/10.1016/S0010-938X(01)00056-7	journal	March 2002
Electrochemical corrosion of unalloyed copper in chloride media––a critical review Kear, G.; Barker, B. D.; Walsh, F. C. Corrosion Science, Vol. 46, Issue 1 https://doi.org/10.1016/S0010-938X(02)00257-3	journal	January 2004
Prediction of the thermodynamic properties of aqueous metal complexes to 1000°C and 5 kb Sverjensky, D. A.; Shock, E. L.; Helgeson, H. C. Geochimica et Cosmochimica Acta, Vol. 61, Issue 7 https://doi.org/10.1016/S0016-7037(97)00009-4	journal	April 1997
Investigations of copper in aqueous alkaline solutions by cyclic voltammetry Ambrose, J.; Barradas, R. G.; Shoesmith, D. W. Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 47, Issue 1 https://doi.org/10.1016/S0022-0728(73)80344-4	journal	September 1973
Reactions of copper patina compounds—I. Influence of some air pollutants Strandberg, Helena Atmospheric Environment, Vol. 32, Issue 20 https://doi.org/10.1016/S1352-2310(98)00057-0	journal	September 1998
Raman spectroscopy of selected copper minerals of significance in corrosion Frost, R. L. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 59, Issue 6 https://doi.org/10.1016/S1386-1425(02)00315-3	journal	April 2003
Catalogue of 45 reference Raman spectra of minerals concerning research in art history or archaeology, especially on corroded metals and coloured glass Bouchard, M.; Smith, D. C. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 59, Issue 10 https://doi.org/10.1016/S1386-1425(03)00069-6	journal	August 2003
Thermodynamic properties of copper chloride complexes and copper transport in magmatic-hydrothermal solutions Liu, Weihua; McPhail, D. C. Chemical Geology, Vol. 221, Issue 1-2 https://doi.org/10.1016/j.chemgeo.2005.04.009	journal	September 2005
Review of non-reactive and reactive wetting of liquids on surfaces Kumar, Girish; Prabhu, K. Narayan Advances in Colloid and Interface Science, Vol. 133, Issue 2 https://doi.org/10.1016/j.cis.2007.04.009	journal	June 2007
Electrochemical behavior of copper–nickel alloys in acidic chloride solutions Ismail, Khaled M.; Fathi, Ahlam M.; Badawy, Waheed A. Corrosion Science, Vol. 48, Issue 8 https://doi.org/10.1016/j.corsci.2005.07.004	journal	August 2006
Atmospheric corrosion of copper and the colour, structure and composition of natural patinas on copper FitzGerald, K. P.; Nairn, J.; Skennerton, G. Corrosion Science, Vol. 48, Issue 9 https://doi.org/10.1016/j.corsci.2005.09.011	journal	September 2006
In situ observation of formation and spreading of micro-droplets on magnesium and its alloy under cyclic wet–dry conditions Chen, Jian; Wang, Jianqiu; Han, Enhou Corrosion Science, Vol. 49, Issue 3 https://doi.org/10.1016/j.corsci.2006.09.003	journal	March 2007
Corrosion behaviour of copper under chloride-containing thin electrolyte layer Liao, Xiaoning; Cao, Fahe; Zheng, Liyun Corrosion Science, Vol. 53, Issue 10 https://doi.org/10.1016/j.corsci.2011.06.004	journal	October 2011
Study of corrosion behavior of carbon steel under seawater film using the wire beam electrode method Liu, Zaijian; Wang, Wei; Wang, Jia Corrosion Science, Vol. 80 https://doi.org/10.1016/j.corsci.2013.11.012	journal	March 2014
Mechanistic studies of corrosion product flaking on copper and copper-based alloys in marine environments Zhang, Xian; Odnevall Wallinder, Inger; Leygraf, Christofer Corrosion Science, Vol. 85 https://doi.org/10.1016/j.corsci.2014.03.028	journal	August 2014
Formation and growth of micro-droplets during the initial stage of atmospheric corrosion Tsuru, Tooru; Tamiya, Ken-Ichiro; Nishikata, Atsushi Electrochimica Acta, Vol. 49, Issue 17-18 https://doi.org/10.1016/j.electacta.2004.01.032	journal	July 2004
Chloride complexes of copper(I) chloride in aqueous solution Fritz, J. J. The Journal of Physical Chemistry, Vol. 84, Issue 18 https://doi.org/10.1021/j100455a006	journal	September 1980
Viscosities and Densities of Highly Concentrated Aqueous MOH Solutions (M ⁺ = Na ⁺ , K ⁺ , Li ⁺ , Cs ⁺ , (CH ₃ ) ₄ N ⁺ ) at 25.0 °C Sipos, Pal M.; Hefter, Glenn; May, Peter M. Journal of Chemical & Engineering Data, Vol. 45, Issue 4 https://doi.org/10.1021/je000019h	journal	July 2000
Photoelectrochemical Stability of Electrodeposited Cu ₂ O Films Wu, Lingling; Tsui, Lok-kun; Swami, Nathan The Journal of Physical Chemistry C, Vol. 114, Issue 26 https://doi.org/10.1021/jp103437y	journal	June 2010
Hygroscopic Particle Behavior Studied by Interdigitated Array Microelectrode Impedance Sensors Schindelholz, Eric; Tsui, Lok-kun; Kelly, Robert G. The Journal of Physical Chemistry A, Vol. 118, Issue 1 https://doi.org/10.1021/jp4098149	journal	December 2013
Precursor films and corrosion: wetting and hydrodynamic aspects Teschke, O.; Tenan, Mario A. Langmuir, Vol. 4, Issue 1 https://doi.org/10.1021/la00079a043	journal	January 1988
The controlling role of sodium and carbonate on the atmospheric corrosion rate of aluminum Schaller, Rebecca F.; Jove-Colon, Carlos F.; Taylor, Jason M. npj Materials Degradation, Vol. 1, Issue 1 https://doi.org/10.1038/s41529-017-0020-3	journal	November 2017
Precursor film: a key driver to determine wetting behavior in the vicinity of surface heterogeneity Sah, Amit Soft Matter, Vol. 10, Issue 22 https://doi.org/10.1039/C3SM52707G	journal	January 2014
Volumetric Properties of Aqueous Sodium Chloride Solutions Rogers, P. S. Z.; Pitzer, Kenneth S. Journal of Physical and Chemical Reference Data, Vol. 11, Issue 1 https://doi.org/10.1063/1.555660	journal	January 1982
Some Aspects of the Atmospheric Corrosion of Copper in the Presence of Sodium Chloride Strandberg, Helena; Johansson, Lars‐Gunnar Journal of The Electrochemical Society, Vol. 145, Issue 4 https://doi.org/10.1149/1.1838422	journal	April 1998
In Situ Studies of the Effect of CO[sub 2] on the Initial NaCl-Induced Atmospheric Corrosion of Copper Chen, Z. Y.; Persson, D.; Nazarov, A. Journal of The Electrochemical Society, Vol. 152, Issue 9 https://doi.org/10.1149/1.1984448	journal	January 2005
An In Situ Raman Spectroscopy Study of the Anodic Oxidation of Copper in Alkaline Media Mayer, Steven T.; Muller, Rolf H. Journal of The Electrochemical Society, Vol. 139, Issue 2 https://doi.org/10.1149/1.2069234	journal	February 1992
Anodic Polarization Behavior of Copper in Aqueous Chloride/Benzotriazole Solutions Tromans, Desmond; Sun, Ru‐hong Journal of The Electrochemical Society, Vol. 138, Issue 11 https://doi.org/10.1149/1.2085397	journal	November 1991
Effect of Carbon Dioxide on Sodium Chloride-Induced Atmospheric Corrosion of Copper Chen, Z. Y.; Persson, D.; Samie, F. Journal of The Electrochemical Society, Vol. 152, Issue 12 https://doi.org/10.1149/1.2098327	journal	January 2005
In Situ Raman Spectroscopy of Anodic Films Formed on Copper and Silver in Sodium Hydroxide Solution Hamilton, J. C.; Farmer, J. C.; Anderson, R. J. Journal of The Electrochemical Society, Vol. 133, Issue 4 https://doi.org/10.1149/1.2108666	journal	April 1986
Anodic Oxidation of Copper in Alkaline Solutions: I . Nucleation and Growth of Cupric Hydroxide Films Shoesmith, D. W.; Rummery, T. E.; Owen, D. Journal of The Electrochemical Society, Vol. 123, Issue 6 https://doi.org/10.1149/1.2132934	journal	June 1976
On the Electrochemical Behavior and Passivation of Copper and Brass (Cu70∕Zn30) Electrodes in Concentrated Aqueous KOH Solutions Biton, M.; Salitra, G.; Aurbach, D. Journal of The Electrochemical Society, Vol. 153, Issue 12 https://doi.org/10.1149/1.2360735	journal	January 2006
A Mechanism for the Atmospheric Corrosion of Copper Determined by Voltammetry with a Strongly Alkaline Electrolyte Nakayama, Shigeyoshi; Notoya, Takenori; Osakai, Toshiyuki Journal of The Electrochemical Society, Vol. 157, Issue 9 https://doi.org/10.1149/1.3465636	journal	January 2010
Effect of Relative Humidity on Corrosion of Steel under Sea Salt Aerosol Proxies: I. NaCl Schindelholz, E.; Risteen, B. E.; Kelly, R. G. Journal of The Electrochemical Society, Vol. 161, Issue 10 https://doi.org/10.1149/2.0221410jes	journal	January 2014
Effect of Relative Humidity on Corrosion of Steel under Sea Salt Aerosol Proxies: II. MgCl ₂ , Artificial Seawater Schindelholz, E.; Risteen, B. E.; Kelly, R. G. Journal of The Electrochemical Society, Vol. 161, Issue 10 https://doi.org/10.1149/2.0231410jes	journal	January 2014
Atmospheric Corrosion of Cu during Constant Deposition of NaCl Lin, Huang; Frankel, G. S. Journal of The Electrochemical Society, Vol. 160, Issue 8 https://doi.org/10.1149/2.037308jes	journal	January 2013
Bronze Disease: A Review of Some Chemical Problems and the Role of Relative Humidity Scott, David A. Journal of the American Institute for Conservation, Vol. 29, Issue 2 https://doi.org/10.1179/019713690806046064	journal	January 1990
Calculation of the relative metastabilities of proteins using the CHNOSZ software package Dick, Jeffrey M. Geochemical Transactions, Vol. 9, Issue 1 https://doi.org/10.1186/1467-4866-9-10	journal	October 2008
A Spectrophotometric Study of Copper(I) Chloro-Complexes in Aqueous 5M Na(Cl, ClO ₄ ) Solutions Sugasaka, Kazuhiko; Fujii, Ayako Bulletin of the Chemical Society of Japan, Vol. 49, Issue 1 https://doi.org/10.1246/bcsj.49.82	journal	January 1976
Phase relations of some cupric hydroxy minerals Woods, Terri L.; Garrels, Robert M. Economic Geology, Vol. 81, Issue 8 https://doi.org/10.2113/gsecongeo.81.8.1989	journal	December 1986
Corrosion Mechanisms and Products of Copper in Aqueous Solutions at Various pH Values Feng, Y.; Siow, K. -S.; Teo, W. -K. CORROSION, Vol. 53, Issue 5 https://doi.org/10.5006/1.3280482	journal	May 1997
Combined Effects of Gaseous Pollutants and Sodium Chloride Particles on the Atmospheric Corrosion of Copper Chen, Z. Y.; Zakipour, S.; Persson, D. CORROSION, Vol. 61, Issue 11 https://doi.org/10.5006/1.3280618	journal	November 2005
Effect of Sodium Chloride Particles on the Atmospheric Corrosion of Pure Copper Chen, Z. Y.; Zakipour, S.; Persson, D. CORROSION, Vol. 60, Issue 5 https://doi.org/10.5006/1.3299244	journal	May 2004
Electrochemical Behavior of AgCu Alloy in Alkaline Medium in the Presence of Chloride Ions Grekulović, V.; Rajc̆ić-Vujasinović, M. CORROSION, Vol. 68, Issue 2 https://doi.org/10.5006/1.3683225	journal	February 2012

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Electrochemical aspects of copper atmospheric corrosion in the presence of sodium chloride

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