Active/Passive Conditions on Copper Containers under Nuclear Waste Repository Environment
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1 6 th International Workshop on Long-term Prediction of Corrosion Damage in Nuclear Waste Systems, Toronto, Canada, May 9-12, 2016 Active/Passive Conditions on Copper Containers under Nuclear Waste Repository Environment Zack Qin 1, Amy Ai 1, Roshan Deljeet 1, Nasrin Farhangi 1, Jamie Noël 1, Sridhar Ramamurthy 1, David Shoesmith 1, and Fraser King 2 1 Western University, London, Ontario, Canada 2 Integrity Corrosion Consulting Ltd, Nanaimo, British Columbia, Canada 1
2 Outlines Why are we interested in the active/passive conditions on copper containers? How did we invest? The results: active/passive diagrams Future work 2
3 Canadian Deep Geologic Repository for Nuclear Waste Disposal 3
4 Objectives The current Canadian design is a carbon steel container coated with a few millimetres of Cu The near-field environment (bentonite pore water) may be close to the active-passive boundary for Cu corrosion If passive conditions are established, pitting could occur Possible pitting corrosion could penetrate the corrosion allowance (< 3 mm) Crucial to comprehend under what environmental conditions pitting is possible or not possible 4
5 Repository Environment Will Evolve with Time Humid environment Saturated environment pitting corrosion Pitting can only occur during the early period when either environmental and/or radiolytic oxidants are present 5
6 Near-field Environment during Pitting Susceptible Period Even for a fractured granite host rock, it may take 100 years or more for the bentonite to saturate with groundwater. For a low hydraulic conductivity sedimentary site, it may take tens of thousands of years! The period of susceptibility to localised corrosion will be limited to the first few decades following closure of the repository, long before the bentonite equilibrates with the groundwater. Therefore in the near field, the composition of the bentonite pore water rather than that of the groundwater are most relevant. The near-field pore water chemistry will depend on the type of bentonite used, nature of water added to bentonite for compaction, and it will evolve as the bentonite saturates with incoming ground water. Predicted near-field pore water chemistry Temperature ph [Cl - ] (mol/l) [SO 4 2- ] (mol/l) [CO 3 ] tot (mol/l) < 100 C
7 Test electrolytes System [Cl - ] (mol/l) [SO 4 2- ] (mol/l) [CO 3 ] tot (mol/l) unary ~ ~ ~ ~ 0.01 binary ~ ~ ~ ternary ~ ph: from neutral until passivity is induced Temperature: from 25 C to 80 C 7
8 Electrochemical Setup Solution Made up with Type I water Argon purged Working electrode Phosphorous-doped oxygen-free Cu Cu bar without casting/coating Exposed surface area ~10 cm 2 8
9 Electrochemical Procedure 9
10 Cyclic Voltammetry pitting I (ma) 0.05 active I (ma) Cu + 2 Cl - => CuCl e Cu => Cu 2 O passive Cu 2 O => Cu 2+ Cu => Cu E (V vs SCE) E (V vs SCE) For an active system, the current increases exponentially with potential indicating active dissolution as Cu + and exhibits little hysteresis on the reverse scan If passivation occurs the current will peak and decrease due to film formation. A subsequent sudden current increase indicates film breakdown A positive hysteresis on the reverse scan after film breakdown indicates pitting corrosion 10
11 Effect of ph M SO M Cl-, 25 C active passive ph=6.26 ph=9.21 ph=9.95 ph=11.46 I (ma) E (V vs SCE) 11
12 Effect of Temperature M SO = M Cl-, ph=11.46 passive 25 o C 40 o C 60 o C 80 o C I (ma) active E (V vs SCE) 12
13 Active/Passive (A/P) Diagrams Derived from cyclic voltammetry (CV) measurements Define the conditions (in terms of [Cl - ], [SO 4= ], [CO 3 ] tot, ph and T C) under which passivity of Cu is possible (with the possibility of pitting) or is not possible Build a database for a broad set of environmental conditions not limited to the repository conditions Provide a basis for container corrosion models and guidelines regarding the water compositions used when compacting the bentonite, repository saturation time, and container spacing 13
14 Active/Passive Diagram for a Chloride Solution Pourbaix ([Cu(aq)] tot = 10-6 molal and [Cl(aq)] tot = 0.2 molal) 25 C active passive 10 [Cl - ] (mol/l) Pourbaix ([Cu(aq)] tot = 10-6 molal and [Cl(aq)] tot = 1.5 molal) 1E-3 1E ph near-field environment Beverskog, B. et al. (1998), Swedish Nuclear Power Inspectorate, SKI 98:19 14
15 Chloride Solutions 25 C active passive 40 C active passive [Cl - ] (mol/l) [Cl - ] (mol/l) E-3 1E-3 1E ph 60 C active passive 1E ph 80 C active passive [Cl - ] (mol/l) [Cl - ] (mol/l) E ph 1E ph 15
16 Active/Passive Boundaries (Chloride - Sulphate) M SO x M Cl- 25 C [Cl - ] (mol/l) Active Passive 40 C 1E-3 60 C 80 C near-field environment 1E ph 16
17 What We Have Learnt A database of A/P diagrams has been built for Cu corrosion under a wide range of environmental conditions A/P boundaries depend on the type of anion, the anion concentration, the ph, and the temperature While chloride promotes active dissolution, sulphate and carbonate favour the formation of a passive film The higher the ph, the greater the tendency towards passivation, except at very high [Cl - ] where the system remains active at very high ph The increase of temperature reduces the passive region Passivity is only expected in SO 4 2- /HCO 3- /CO 3 2- solutions at extremely low Cl - concentrations 17
18 Specific Potentials Eoc (V/SCE) E corr (V/SCE) 0.01Cl+0.01SO4 ph c OCP.cor I (ma) E rp Time (Sec) E (V vs SCE) E b Corrosion potential E corr achieves a steady state in ~10 minutes Breakdown potential (E b ) and re-passivation potential (E rp ) 18
19 PDF Going Forward Determine the dependence of E corr, E b, and E rp as a function of environmental conditions E b and E rp are distributed parameters, either because of the stochastic nature of film breakdown or because of the variable conditions to which the surface is exposed. The probability distribution functions (pdf s) will be developed for E corr, E b, and E rp at selected conditions where pitting is observable Ecorr Erp Eb Potential (V SCE ) 19 King, F. and Lilja, C. (2014), Swedish Nuclear Fuel and Waste Management Co, TR
20 Amy (Meirong) Ai Acknowledgements Funded by Nuclear Waste Management Organization (NWMO) under the contract DS
21 21
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