Past Abstracts - 1998 part 2

Technical presentations October 1998

1       “High strength cupronickels — past, present and future”, Clive Tuck (Meighs Langley Alloys Division Ltd)

Since the 1930’s, when it was discovered that the addition of aluminium to a solid solution of Cu-Ni produces a strengthening effect through Ni3A1 precipitate formation, a series of high strength engineering alloys based on Cu-Ni-Al have been developed. The initial commercial alloy of this type, HIDURAX SPECIAL, had poor grain size control, but this was improved (together with impact toughness) with the development of HIDURON 191 in the 1960s. At the present time, super high strength cupronickels typical proof stress 730N/mm2) have become established for widespread applications in the offshore oil and gas industry due to their advantages in possessing seawater corrosion resistance and hydrogen embrittlement resistance, together with mechanical properties complying with ASTM A193 Grade B7 carbon steel.

 Principal applications of high strength cupronickels have included high integrity fasteners, high strength connectors and the wide variety of actuator devices, the main properties utilised being strength, corrosion resistance, hydrogen embrittlement resistance, anti-galling behaviour and bio-fouling resistance. In particular, over 250 t of the principal alloy of this type, MARINEL, has been deployed as an engineering alloy in marine environments and it has demonstrated a consistent resistance to hydrogen embrittlement and passivation in hydrogen sulphide media.

 However, evidence has been that if super high strength Cu-Ni-Al alloys are tensioned to levels significantly above the recommended engineering stress regime (i.e. they are abused during installation and service), stress corrosion cracking can result in particular environments if cathodic protection is absent. Slow strain rate testing has suggested that such debilitating environments include aqueous solutions which contain ammonia, organic amines or elevated temperature concentrations of chloride ions. However, recent development of MARINEL has produced the improved alloy, MARLNEL+, which shows marked resistance to stress corrosion and therefore possesses a substantial degree of abuse to tolerance. 

Development work on high strength cupronickels is continuing, and computer-aided (neural network) alloy design methods are being used to further improve the overall mechanical properties of these alloys with a view to enhancing yet further their properties. 

2       Latest developments in the conservation of large ships”, Des Barker (Portsmouth University) 

A review of the conservation programmes being undertaken on the Holland I and Minerva was given. Holland I was the first submarine built for the British Royal Navy and was launched in 1901. Holland I sank in 1913 but was recovered in 1981. Both vessels are undergoing treatment to remove chloride and reduce corrosion rates to avoid further deterioration of the structure. 

3            “Influence of Biomineralisation and Colloids on Marine Biofouling”, Mark Varney (University of Southampton) 

The commercial problems of biofouling are well known and documented. Spores, diatoms and other marine micro-organisms quickly populate underwater surfaces - in the order of days to weeks. Some species have surfaces which appear to offer very effective natural antifouling properties: corals, sponges, macroalgae, for example. Antifouling agents are very much needed against Enteromorpha intestinalis (green alga) and Balanus amphrite (barnacle) which are very common. While a number of very promising molecular agents have been isolated and the search for better ones continues, there is still no fundamental understanding of the various mechanisms underlying (or preceding) biofouling. 

Topics discussed included:

1.        Currently effective agents

2.        Electrochemical Measurement of Biofilming

3.        Colloids

4.        Colloid stabilisation

5.         Biomineralisation

6.        Biomineralisation & colloidal formation 

Biofouling (filming) is only encountered in the field, and cannot be reasonably (or accurately) repeated in the laboratory. Possible control mechanisms to minimise the effects of biofouling centre on understanding the elements of biofilming (on timescales of seconds to minutes). Ca2* binding and colloidal formation seem fundamental, and their involvement in precipitating and stabilising films on underwater surfaces would appear to be plausible. Future control mechanisms would probably centre on the control of colloidal conformation and/or steric effects. There is a clear need for further work in this respect. 

4. “Fundamentals of localised corrosion and SCC of high alloy stainless steels in marine environments”, Roger Newman (UMJST) 

Advances in the understanding and control of stress-corrosion cracking (SCC) often relate to the definition of the local environment, either within a localized corrosion cavity or within a thin liquid layer influenced by evaporative concentration. Several examples of such advances will be given, involving crevice corrosion and its role in SCC initiation, magnesium ions in seawater and their role in creating concentrated environments, and the behaviour of H2S in pits and cracks. Aspects of cathodic hydrogen embrittlement of duplex stainless steels will also be considered. 

Technical presentations July 1998

1.      “Scanning tunnelling microscopy (STM) and marine corrosion”, Peter Farr (Birmingham University)

The superduplex stainless steel studied was Zeron 100. This had a 50:50 austenite ferrite structure with a grain size around 30um and composition (wt%) C 0.24; N 0.21; Cr 24.40; Ni 6.83; Mo 3.70; Mn 0.77; Cu 0.63; Si 0.18; S 0.002; P 0.025; W 0.625. Test surfaces were carefully polished, to minimise the extent of the damage layer, and were cleaned with solvent before electrochemical treatments. 

The electrochemical behaviour of the steel in acidified NaC1 solution (equivalent to activated brines) was established using both potentiodynamic (“dc”) and impedance (“ac”) techniques. In brief, the anodic polarisation curves compared well with those for austenitic (18:8) stainless steel. The breakdown (pitting) potential was far anodic (ca 0.9V SCE). There was evidence of Faradaic activity within the passive region, also for regions of semi-conductor behaviour in the passivating oxide. 

Under electrochemically well-defined breakdown conditions scanning probe microscopy (SPM) showed that 1) even the damage layer on austenite is remarkably stable 2) the earliest attack is at grain boundaries between austenite and ferrite phases 3) the ferrite is much more strongly attacked than austenite, yet does not show pitting until several hundred monolayers have been removed from this surface 4) pitting in deeply etched ferrite is strongly anisotropic, that on austenite is isotropic.  

The results were discussed in the light of current theories of the onset of corrosion on stainless steel and with concern for risks in the engineering application of this superduplex stainless alloy.  

The study was a good vehicle for the assessment of available scanning probe microscopies. These were described briefly (plenty of literature is available for the enthusiast). The techniques are attractive and not prohibitively expensive: but possibilities of imaging artefacts are legion, especially in in situ” electrochemical experiments. Hence most of the images described were produced by atomic force microscopy (a “nanometric” profilametry), the most reliable mode of SPM. The observations were supported by SEM work, at lower magnification.  

2            “Incorporating lessons learned into the corrosion engineering of the BP Bruce Phase II Subsea Development”, Charlie Barraclough (Kvaemer Process)  

Lessons learned from previous problems experienced on other offshore installations were fed into the detailed design of the BP Bruce Platform, Pipeline and Manifold. The through life cost of pipeline operation led to the selection of a CRA lined pipeline and duplex stainless steel manifold. Historical information on riser and pipeline damage led to the use of carrier pipes for both pipelines and risers. The heat-exchangers were channel side seawater in order to prevent the crevice corrosion experienced in some coolers, and the operating temperatures are kept down to prevent pitting which can occur in CRA clad coolers.  

Incidences of hydrogen cracking of duplex stainless steel required all duplex items to be subject to finite element analysis which lead to modifications in design to reduce stresses beyond those normally permitted. In addition no anodes or other such attachments were made to duplex material, and all duplex material was coated with rubber or polyurethane. Crevice corrosion of flanged and hub joints was dealt with by CRA cladding with careful attention to reducing dilution. Valve materials for subsea    use were agreed with vendors at the outset of the project, with particular attention to hard-surfacing. The corrosion of nominally dry gas lines was assessed using factors for relative humidity, and a corrosion allowance allocated for the worst temperature/humidity case and for accidental wet operation. In-deck tanks were reversed so that the stiffeners were on the outside, allowing CRA ‘wall-papering’ inside. Pig-trap door-seal faces were CRA clad to prevent offshore repair costs. The importance of early recognition of problem areas and close liaison with vendors was underlined.

3          “Cathodic protection: Hydrogen pick-up and transport”, Alan Turnbull (National Physical Laboratory)  

The primary cathodic reactions in seawater are reduction of oxygen and reduction of water, the latter resulting in the generation of hydrogen atoms on the metal surface. There is some indication that the presence of oxygen can retard hydrogen atom ingress into the material slightly but this becomes irrelevant with the formation of calcareous scale as access of oxygen to the surface is restricted and the oxygen reduction reaction becomes insignificant. The kinetics of water reduction in seawater and in 3.5%NaC1 at about the same pH are identical for a C-Mn steel but data for other metals are limited. It is noted that the kinetics of water reduction decrease significantly with increasing pH and will hence be low in crevices and cracks (in the absence of dynamic straining) as a consequence of the alkalinity developed. 

The hydrogen atoms produced from cathodic reduction will be absorbed into the metal or recombine as molecular hydrogen which will dissolve in the solution. As the potential is decreased to more negative values the solubility limit of hydrogen in solution will be exceeded and hydrogen gas will form. Under deep sea conditions, hydrostatic pressure will suppress the formation of hydrogen gas and hence the rate of removal of hydrogen. This may encourage increased hydrogen absorption. 

Surface films can have a very significant effect on hydrogen entry. There is no unambiguous study of the effect on hydrogen entry of calcareous scale but for low alloy carbon steels and probably for corrosion resistant alloys (CRAs) it seems unlikely to be marked. In contrast, the oxide films on CRAs cause significant retardation of hydrogen entry. Correspondingly, if the film is ruptured mechanically, hydrogen entry locally can be high relative to adjacent areas. 

In testing for resistance to hydrogen cracking it is important to obtain information about the concentration of hydrogen in the metal and the hydrogen diffusivity. The reliability of such data in the past has not always been ideal but measurement of these parameters by the electrochemical permeation method is now on a more sound basis with the publication of a new standard (BS 7886 1997). Further confirmation of the validity of the technique has been demonstrated by good agreement between measurements of hydrogen content in a duplex stainless steel using both permeation and total extraction methods. 

Values of the diffusion coefficient can range from about 1 .7x10-6 cm2s-1 for a 4360 SOD steel to 2.8x10-11 cm2s-1 for a 22Cr duplex stainless steel at ambient temperatures. This brings up the issue of how long a laboratory test should be to ensure that service behaviour is adequately represented. Corrosion fatigue studies on some low alloy carbon steels cathodically protected in seawater suggest that pre-exposure for a year may be required. There is less certainty about CRAs because of the importance of local hydrogen entry (film-ruptured areas) compared to bulk hydrogen entry. The indications are that test times need not be too long despite the low diffusivity, provided cracking is initiating at the surface. However, further work for different alloys is required. 

The importance of film rupture does point to the need to conduct testing of CRAs under conditions of dynamic strain. Current activity at NPL is focusing on the impact of dynamic straining on hydrogen cracking of duplex stainless steel using plain and notched specimens. 

4 “Cathodic Protection and Hydrogen Embrittlement”, Robin Jacob (Global Corrosion Consultants Ltd) 

Offshore cathodic protection (CP) systems utilising conventional sacrificial anodes, and designed to current recommended practices (DNV, NORSOK), will reach potentials (relative to the Ag/AgCl/seawater reference electrode) between the required level for protection of carbon steels (-800mV) and the anode potential (-lO5OmV). With the formation of calcareous deposits, most will equilibrate at around —95OmV. 

Although satisfactory for normal offshore steels, such an outcome may not be acceptable if materials susceptible to hydrogen embrittlement are required. In recent years cracking, due to a combination of applied CP, inappropriate metallurgical structure and operational stress levels, has been observed in both high strength, and duplex stainless steels. Subsequent laboratory investigation has shown that potentials more negative than ~—-800mV can, under some operating conditions, lease to hydrogen embrittlement. Clearly, where these materials need to be used subsea, a novel approach to CP is required. 

Such an approach can be provided by incorporating voltage limiting devices, such as Schottky barrier rectifiers into the sacrificial anode connections. These ensure that the potential difference between anodes and structure cannot be less than —300mV, leading to protection potentials in the range ~-800 to —75OmV. This does, of course, mean that the generally accepted criterion for protection of any carbon steel in the structure (-800mV) may not be fully achieved, but in practice, corrosion rates even at —75OmV will be acceptably low. Such diode limiting has found application offshore, particularly on mobile jack-ups. An alternative method of achieving the same end, by use of sacrificial alloys developed to have less negative operating potentials than present formulations, appears feasible but has not yet been practically achieved on a significant scale. 

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