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Wang, Yefei (Key Laboratory of Unconventional Oil & Gas Development, China University of Petroleum East China, Ministry of Education, P. R. China, School of Petroleum Engineering, China University of Petroleum East China) | Yang, Zhen (Key Laboratory of Unconventional Oil & Gas Development, China University of Petroleum East China, Ministry of Education, P. R. China, School of Petroleum Engineering, China University of Petroleum East China) | Wang, Renzhuo (Key Laboratory of Unconventional Oil & Gas Development, China University of Petroleum East China, Ministry of Education, P. R. China, School of Petroleum Engineering, China University of Petroleum East China) | Chen, Wuhua (Key Laboratory of Unconventional Oil & Gas Development, China University of Petroleum East China, Ministry of Education, P. R. China, School of Petroleum Engineering, China University of Petroleum East China) | Ding, Mingchen (Key Laboratory of Unconventional Oil & Gas Development, China University of Petroleum East China, Ministry of Education, P. R. China, School of Petroleum Engineering, China University of Petroleum East China) | Zhan, Fengtao (College of Science, China University of Petroleum East China) | Hou, Baofeng (School of Petroleum Engineering, Yangtze University)
A novel indolizine derivative inhibitor for acidization was introduced. It could exhibit effective corrosion inhibition at a much lower concentration without propargyl alcohol and shows economic and environmental advantages. From quinoline, benzyl chloride, and chloroacetic acid, two indolizine derivatives were prepared under certain conditions. These inhibitive indolizine derivatives were both synthesised from benzyl quinoline chloride (BQC), which one of the conventional quaternary ammonium corrosion inhibitors used for acidising. The target compound was purified and instrumental analysis methods including elemental analysis, high-resolution mass spectrometry (HRMS), and NMR were used to characterise the chemical structure. The inhibition performance of the indolizine derivatives in 15 wt.% HCl, 20 wt.% HCl, and mud acid (12%HCl + 3%HF) for N80 steel was investigated by weight loss measurement, electrochemical method (potentiodynamic polarization and EIS), and SEM surface morphology assessment.
When 0.1 wt.% indolizine derivative was added, the inhibition efficiency of N80 steel in 15 wt.% HCl at 90 °C increased to 98.8 % and 99.1 % respectively without the synergistic effect of propargyl alcohol: however, in terms of BQC, even at a dosage of 1.0 wt.%, the inhibition efficiency of N80 steel only reached 83.3 % under the same conditions. The novel derivative could impart an improved corrosion resistance effect. Compared with BQC, there are more active adsorption sites in the derivative and therefore the inhibitor could be better fastened to the steel surface. The firmly adsorbed inhibitors would thereby prevent the metal surface from making contact with H+ ions and finally increase the inhibitory effect. As a high-efficiency corrosion inhibitor, the novel indolizine derivatives may offer a new strategy for corrosion protection in acidising.
The effectiveness of poly (2-acrylamido-2-methylpropane sulfonic acid) (PAMPS) and copolymers with acrylic acid (AA) and acrylamide (AM) magnetic nanogels as protective corrosion of CS in reaction with water by (EIS), (EFM) and tafel polarization method. Polarization method demonstrated that all the polymers are mixed inhibitor type. (EIS) Electrochemical impedance given that the attendance of these investigated polymers declines the double layer capacitance and improvement the charge transfer resistance. The polymers adsorption on surface of steel was follow isotherm Temkin. The morphology of the CS surface was examining by (EDX) energy dispersive X-ray and (SEM) scanning electron microscope. The data obtain showed improvement in efficiencies for inhibition with raising the dose of inhibitor.
CS is the common regularly utilized pipeline materials as a part of petroleum creation. In any case, it is exceptionally inclined to corrosion in environments include sulphur . Corrosion of sulfur has been one of the corrosion sorts in gas/oil manufacture, offering ascend to the pipelines failure and equipment's and utilized in biggest economic reduction and accidents. Likewise, spillage of raw petroleum because of endures consumption of pipelines would actuate fire accident, and natural contamination [2-4]. Explored to comprehend its mechanism, decrease the corrosion rate, additionally create experimental models to survey and foresee the parametric effects and the states-of the-art of internal corrosion of pipelines [5-12]. Theoretical approaches provide means of experimental of these reactions and there are many reports connection with this area . Last papers have study the connection between the efficiency and structure of the inhibitor molecule, but low attention has been paid to the reliance of the protection efficiency on the size and electronic distribution of the protective molecule, Relation between chemical structure and inhibition efficiency was not research, The super paramagnetic Fe3O4 nanoparticles covered with polymers are usually connected to the magnetic cores to ensure a strong magnetic . Attractive nanogels of regular interest are ferromagnetic magnetite (Fe3O4) covered with cross-connected polymer nanogels. The Fe3O4 center has solid attractive characteristic and super paramagnetic conduct, is of generally declines danger to the human body when epitomized in the defensive shell of polymer, which is cross-connected hydrogels polymer. The shell keeps the Fe3O4 center from total oxidation. In this appreciation, the utilizing of nanogels particles as a part of the field of consumption hindrance insurance for steel rather than ordinary natural inhibitors can deliver uniform flimsy film (with no pine opening because of cross-connected polymers) on the surface of CS to coat all surface with no deformities which give focal points over typical natural inhibitors. A few strategies have been produced to get ready attractive miniaturized scale and nanogels, for example, reverse microemulsion polymerization and emulsion polymerization [15-18]. The target of this paper is to calculation the inhibitive effect of these polymers on carbon steel in formation water by various electrochemical methods.
Nanotechnology involves scale, function, and composition that enable macroscopic properties with improved performance and high-value adding for any industry including the coatings industry. The large interest in graphene-based materials and other carbon-based polymorphs and nanomaterials are truly far-reaching. The industrial scale and possibility of applying these nanomaterials to advanced manufacturing and commercial applications have resulted in high throughput synthesis and lower costs. There is primary interest on their electrical and thermal conductivity properties. However, other applications are based on their ability to form very stable colloidal complexes. This talk will focus on the class of graphene (G) and graphene oxide (GO) nanomaterials that have been prepared with high loading in polymer matrices and ultrathin films to result in: anti-corrosion coatings and anti-microbial properties. We describe the preparation of very stable dispersions that can be used for coatings as well as anti-corrosion-superhydrophobic coatings. Interestingly, by preparation of nanoparticles that can be stabilized at dispersions, functional coatings can be prepared which have interesting uses in mitigating corrosion and killing bacteria. Colloidal particles that can be stabilized at liquid-liquid and air-liquid interfaces, functional Janus type nanoparticles can be prepared which have interesting uses in dispersants, rheological modifiers, and smart fluids. An important consideration is their use as anti-corrosion additives and the importance of nanostructuring.
Since the awarding of the Physics Nobel Prize in 2010, graphene, a two-dimensional carbon polymorph nanomaterial has continued to be the subject of much intense research. There has been interest worldwide for both fundamental properties and applications. Other carbon based polymorphs such as carbon nanotubes (CNT)s and fullerene - another Nobel Prize winning discovery followed much earlier are much more commercially available now. Elemental Carbon (C) naturally comes in two basic allotropes, namely graphite and diamond. These are two very different materials based on their chemical orbital hybridization and crystallinity despite being all carbon atoms. But as nanomaterials, they exhibit extraordinary electronic properties and are of primary interest to the materials community.1 There is a lot of interest now in utilizing them for future flexible electronic displays and devices. Graphene a, 2D nanomaterial has unusual electrical and optical properties (Figure 1). It is a single layer of carbon atoms arranged in an aromatic hexagonal lattice resulting in high mobilities and charge carrier generation. This arises of course from the delocalization and hybridization of pi-orbitals in a vast planar network of fused benzene like structures. It is an ideal monolayer coating material due to its impermeability, thermodynamic stability, transparency and flexibility. They exhibit high field effect mobility and can be formed through a number of chemical and physical methods and can be rendered useful in batch compounding. Its potential applications have encompassed a myriad of scientific and engineering disciplines such as high-performance nanocomposites, printed and flexible electronics, supercapacitors, chemical sensors, gas barriers and biomaterials. The latter include applications in gene and drug delivery, cancer treatment, cell growth control, stem cell differentiation, field effect transistor (FET) -based biosensors and as antimicrobial materials.
Aristia, Gabriela (Freie Universität Berlin) | Roth, Christina (Freie Universität Berlin) | Hoa, Le Quynh (BAM - Federal Institute for Materials Research and Testing) | Bäßler, Ralph (BAM - Federal Institute for Materials Research and Testing)
Carbon steel is prone to uniform and pitting corrosion in geothermal brines, whereas high alloyed materials which exhibit excellent corrosion resistance are relatively costly. For these reasons, coating systems become an alternative to protect carbon steel from corrosion in the geothermal environment. In this research, a coating system consisting of polyaniline and silicon dioxide was optimized by investigating differently synthesized polyaniline types in the coating with respect to their protective effect on carbon steel. SEM images of the phosphoric acid and dodecylbenzenesulfonic acid doped polyaniline showed different morphology, which suggested different physical and chemical properties. The geothermal brine found in Indonesia was simulated by an artificial solution with pH 4. Evaluation of the coating system was performed by surface analysis of the exposed specimens and electrochemical tests, i.e. electrochemical impedance spectroscopy (EIS), open circuit potential (OCP), and potentiodynamic polarization at 150 °C with 1 MPa pressure. Visual assessment of exposed specimens with single component addition into coatings showed that coatings underwent degradation, whereas the combination of polyaniline and silicon dioxide showed a better protective behavior.
As one of the renewable energy resources and an alternative to conventional fossil fuel energy, geothermal energy produces low carbon dioxide emission. This aspect in energy production is important because it also contributes to prevent climate change.1,2 Depending on the location and depth of a geothermal well, geothermal brines may contain various ionic species, e.g. chloride and sulphate, various dissolved gases, e.g. CO2, N2, Ar, and they may be present in either liquid dominating phase, vapor dominating phase, or transitional phase.3,4 Geothermal power plant development requires a careful planning, including the evaluation of material performance and durability prior to its construction, because geothermal brine is an aggressive medium which can cause corrosion and scaling on pipelines materials5, for example high alloyed steel, stainless steel, and carbon steel. High alloyed material is expected to have a long lifetime in the operation6-8, however, these are relatively costly materials. The more economical option for such service is by using carbon steel, which is prone to uniform corrosion and pitting corrosion. Protection on the lower resistant material becomes essential to develop alternatives for geothermal application.
A low enthalpy geothermal system consisting of a water production and injection well faced serious injection obstruction problems within two-and-a-half months after start-up. The obstruction was so severe that the operation was suspended and research was done in order to determine the cause. To solve the obstruction problem the system was treated downhole using acid and biocide. During this treatment dangerous amounts of H2S were released. A study was initiated to understand the origin of the H2S and to give options for microbiological treatment and growth prevention. The results showed high amount of bacteria in the obstruction material indicating that microorganisms caused the obstruction. The detected species were typical thermophilic species with optimal growth temperature at 40-60 °C. During the 2,5 month period the casing was unprotected in high corrosive environment and bacteria and iron oxides, iron sulphides (FeS) and iron-copper sulphides (FeCuS2) were identified suspected to have caused the obstruction. The H2S formation was likely caused by a combination of biological FeS and CuFeS2 formation (due to Microbiologically Influenced Corrosion; MIC) and the release of H2S by the addition of acid during cleaning. To prevent this type of issues biocide treatment was applied, however, further investigation showed that microorganisms were still able to grow in the system. Identification of the microorganisms in the production water showed that several MIC related species are already present in the production water. Continuous monitoring and adjustment of kill strategies are essential for safe operation.
A geothermic system in the Netherlands faced serious injection obstruction problems two-and-a-half months after start-up. The obstruction was so severe that the operation was suspended and research was done in order to determine the cause. The conclusion was that the obstruction was caused by a combination of slime forming bacteria and iron and copper oxides/sulphides (possibly formed by bacteria). To solve the obstruction problem the system was treated downhole using acid and biocide. During this treatment dangerous amounts of H2S were released. The hypothesis is that H2S was formed by the activity of (sulphate reducing) bacteria and/or by the chemical reaction during the acid treatment. Due to QHSE (Quality, Health, Safety and Environment) regulations and lack of knowledge about what has happened in this system, there is the need to understand which processes have taken place and what can be expected in the future with regard to obstruction issues, H2S formation and Microbiologically Influenced Corrosion (MIC). To understand the issues better, the microbiology in the injection well was identified and interesting bacterial targets were further used to quantify its activity. To prevent microbiology related issue in the future, biocide was dosed once monthly in the injection well with the aim to prevent microbiological growth. However, after several months the injection pressure started increasing again slowly. Although the injection pressure was well within the production requirements, after more than two years of operation, additional tests were done and further research was performed to understand the reason for this increase in pressure and to get a better understanding and control of risks related to microbiology and MIC threat based on the detected microbiology. This report described the results of this study.
Yang, Zhen (China University of Petroleum) | Wang, Yefei (China University of Petroleum) | Zhan, Fengtao (China University of Petroleum) | Wang, Renzhuo (China University of Petroleum) | Chen, Wuhua (China University of Petroleum) | Ding, Mingchen (China University of Petroleum) | Hou, Baofeng (Yangtze University)
The novel indolizine derivative inhibitor for acidizing shows an effective corrosion inhibition without the synergism of propargyl alcohol. The inhibitive indolizine derivatives were generated from BQC (Benzyl Quinolinium Chloride, a commonly used key compound in acidizing inhibitor) via a moderate 1,3-dipolar cycloaddition mechanism. High Resolution Mass Spectrometry (HRMS) and NMR were used to confirm the detailed chemical structure. The inhibition of two indolizine derivatives in 15 wt.% HCl for N80 steel were studied by weight loss measurement and electrochemical analysis. Without the synergism of propargyl alcohol, the inhibition efficiency of N80 in 15 wt.% HCl at 90°C merely reaches 80.3% even when 1.0 wt.% of BQC was added. However, under the same conditions, when the dosage of two indolizine derivatives is only 0.1 wt.%, the inhibition efficiency significantly grows up to over 99.0 %. The indolizine derivative could display an excellent protection performance at a much lower concentration. Compared with BQC, the active adsorption sites in indolizine derivatives are enhanced and consequently the inhibition is increased. The indolizine derivatives exhibit an enlightening economic advantage and provide an eco-friendly inhibitive material. They might be applied as an important component of new acidizing inhibitor.
Corrosion of metal in acid medium brings not only the waste of resources but also environmental pollution in industrial production and oil field engineering. The use of various corrosion inhibitors is the most convenient and commercial method for reducing the attack of acid onto the raw metal materials.1-2 A variety of organic corrosion inhibitors which contains heteroatoms (N, O, P, S) and/or aromatic unsaturated functional moieties have been developed to retard the corrosion or damage of the metal equipment.3-5
In acidizing engineering, organic acids (such as acetic acid or formic acid) or inorganic acids (e.g. HCl or HCl/HF mixtures) are injected into the near-wellbore at high concentrations and corrosion inhibitors are critical because uninhibited acidizing treatment fluids would induce severe corrosion and damage.6-7 As a result, new effective inhibitors for acidizing are widely researched and always in great demand.8-9 Among the corrosion inhibitors, quaternary heterocyclic ammonium salts, which were usually synthesized by nitrogen-containing heterocyclic bases (pyridine, quinoline or their derivatives) and series of halogenated compounds, have been studied in detail due to their prefect anti-corrosion performance to prevent metal materials from getting corroded in acidizing.10-14 However, these quaternary heterocyclic ammonium salts usually would behavior well via the synergistic effect between the cation moieties of quaternary ammonium and propargyl alcohol, which is a poisonous but indispensable component in commercially available acidizing inhibitors.1,6 With the enhancement of the concept of environmental protection, the research on corrosion inhibitor calls for new type of inhibitors with low toxicity, pollution-free and high efficiency properties. Therefore, many “environmentally friendly” acidizing inhibitors with excellent inhibition performance are explored.15-17
Agarwal, Abhishek (Tata Consultancy Services Limited) | Rathore, Pradeep (Tata Consultancy Services Limited) | Jain, Vinay (Tata Consultancy Services Limited) | Rai, Beena (Tata Consultancy Services Limited)
Quantitative Structure-Activity Relationships (QSAR) based models have been widely used for predicting corrosion inhibition performance of metals. However, one of the major limitations in these studies is that the authors have restricted themselves to use only a single class of molecules having similar molecular structure. In this study, a computational end-to-end framework was developed to investigate the properties of organic corrosion inhibitors which are responsible for inhibition of steel in acidic solution. The framework consists of modules like data preprocessing, descriptor selection and model building. A robust predictive model for multiple class of corrosion inhibitors was developed using advanced machine learning algorithm such as gradient boosting machine (GBM), random forest, support vector machines (SVM) etc. The descriptors were selected using novel integrated ensemble technique. The model based on GBM algorithm was able to predict the corrosion inhibition efficiency of inhibitors with significantly higher accuracy.
Corrosion is one of the major problems in industries which culminates in huge economic losses. In a recent report, NACE International estimated that the global cost due to corrosion annually is around $2.5 trillion.1 One of the most effective methods to combat corrosion in oil and gas industries is the application of corrosion inhibitors.2 The heterocyclic compounds consisting of N, O and S atoms are known to have corrosion inhibition properties.3 The commonly understood mechanism is that they prevent corrosion by formation of a thin film on the metal surface which prevent the access to corrosive substances.4 Toxicity of the inhibitors have become a major issue in their continual usage in industries.5 The regulatory guidelines issued by various agencies such as OSHA (US Occupational Safety and Health Administration) have restricted their usage and thus there is a need to replace these by eco-friendly alternatives.6 Besides, there is also a need to design better, more efficient corrosion inhibitors which perform well even in harsh conditions such as high temperatures, pressure, etc.
Geothermal brine is a complex system containing a wide variety of dissolved salts resulting from the conditions in a geothermal well. These fluids lead to corrosion in pipes and other parts of geothermal system construction and necessitate intense research efforts in finding new suitable materials. Carbon steel is susceptible to corrosion in geothermal brine especially when it is exposed to a high temperature and high-pressure medium, which is considered to be an aggressive environment. An artificial geothermal water, based on a brine composition found in Indonesia, was used to investigate the performance of high alloyed materials. The electrolyte has pH 4 and contains 1,500 mg/l Cl-, 20 mg/l SO42-, 15 mg/l HCO3-, 200 mg/l Ca2+, 250 mg/l K+, and 600 mg/l Na+. In order to protect the bare material in geothermal application, it is necessary to either use high alloyed materials or coatings. In this research, a coating system consisting of polyaniline and silicon dioxide was investigated regarding its behavior to protect carbon steel. In detail, the effect of SiO2 and polyaniline (PANi) addition was evaluated by exposure and electrochemical tests for 7 days, i.e. electrochemical impedance spectroscopy (EiS) and open circuit potential (OCP) at room temperature and 150 °C with 1 MPa pressure.
Geothermal energy is one of the promising renewable energy resources that can be used as an alternative to conventional fossil fuel energy. At the moment, geothermal energy has been widely developed because of its reliability, consistency and lower carbon dioxide emission.1-3 One challenging aspect of geothermal application is the performance and durability of the construction materials under exposure in its severe environment, which commonly causes corrosion and scaling.4-6 Geothermal water is known to be an aggressive medium due to its physicochemical complexity, the operational conditions including high temperature and pressure, and its constituent components containing dissolved salts from different elements.7-9 There are several efforts in finding suitable materials for geothermal applications to avoid operation failure, enhance the lifetime of materials, and obtain a cost effective material, such as material selections,10-13 using high alloyed materials,14-16 or protecting a lower resistant material.17
Corrosion protection is an essential part of material selection in geothermal application, and one of the methods is by using barrier layers or coatings. Coatings have several advantages in comparison with other protective methods, i.e. they are effective, versatile, and have a reasonable cost. However, protective coatings require a proper application, surface preparation and corrosion analysis.18
In this paper, a coating system based on alkyd binder containing polyaniline and silicon dioxide is introduced, using some components that are locally available in Indonesia. Many studies have investigated polyaniline, which is an electroactive polymer, as pigment in coatings to enhance the corrosion resistance.19-21 This study will be carried out in artificial geothermal water with high temperature and high pressure, with the addition of silicon dioxide particles in the coating system to enhance its thermal properties.
Oluwabunmi, Kayode (University of North Texas) | Rizvi, Hussain (University of North Texas) | D'Souza, Nandika (University of North Texas) | Nazrazadani, Seifollah (University of North Texas) | Sanders, Steve (University of North Texas) | Hemmati, Vahid (University of North Texas) | Argade, Gaurav (University of North Texas)
The corrosion properties of PBAT/LDH coating on mild steel substrate was investigated. Tafel tests and electrochemical impedance spectroscopy tests (EIS) was used to analyze the corrosion resistance of the coating on the mild steel substrates. The morphological characteristics of the coatings was done using the scanning vibrating electrode technique (SVET) and environmental scanning electron microscopy (ESEM). Buffered saline solution containing NaCl-0.138 M, KCl-0.0027 M at room temperature and pH of 7.4 was used as electrolyte in the 3 corrosion tests. The tafel results showed that least corrosion current density value of 0.315 (μΑ/cm2) was recorded for 50 % LDH concentration in PBAT. This suggests that 50 % LDH in PBAT was about 98.5 % more corrosion efficient than 1018 bare mild steel and 0.7 % more that the 65 % concentration. The EIS results showed a similar trend. The 65 % LDH concentration showed about 25 % greater impedance to current flow over the 50 % LDH concentration in both the nyquist and bode plots. The SVET results revealed that the greatest corrosion protection of the mild steel substrates was observed with 50 % and 65 % LDH coating. This proved that an increased concentration of LDH in PBAT could potentially improve the corrosion resistance of mild steel when in service in a phosphate buffered saline environment.
Metallic materials used in the biomedical field are susceptible to localized corrosion especially pitting when they come in contact with body fluids and other solutions.1 The phenomenon of corrosion, a natural process that all metallic materials irrespective of the service environment suffer from have been examined using different techniques.2,3 Various forms of protective coatings have been used in the past to mitigate this effect.4 The use of organic coatings has recently gained more attention in the medical field as an environmentally friendly and economical technique for the corrosion protection for metals that come in contact regularly with body fluids. Surface coating of many products have to be carried out not only for aesthetic reasons, but specifically to maintain the integrity of the metallic substrate during their service life.5 Poly (butylene adipate-co-terephthalate) (PBAT) an aliphatic-aromatic biodegradable polyester primarily utilized in packaging industry;6,7 was investigated for its potential medical application.8 The non-cytotoxic behavior of the polymer using different cation exchange montmorillonites as filler at less than 10% by weight showed that through cytotoxicity tests, protein absorption analysis and total blood counts, PBAT composites are valuable in biomedical applications.9,10 Though, low hardness values and inherent non-conducting properties makes it suffers rapid delamination when used as a corrosion resistant coating, it was observed that it possessed the ability to enable platelet mobility which improved its mechanical properties with (less than 6%) of layered clay11,12. Based on this, we hypothesized that, reinforcing PBAT with LDH fillers a type of anion exchanged clays also known as hydrotalcite, with a brucite like structure; having a general formula [MII1-xMIIIx(OH)2x]x+(An”)x/n.mH2O, where Mn represents a divalent metal, Mra a trivalent metal, and An- an anion will help to increase the corrosion resistance of PBAT and give birth to a new set of bioinspired coatings suitable for use in medical implants.
ABSTRACTInhibitors have been used to mitigate corrosion in oil and gas producing assets. The efficiency of inhibitors are affected by several variables with the ability of an inhibitor to transport through the produced fluids onto the metal surface being one of the most important requirements. This can be achieved by formulating inhibitor products with a variety of chemistries that minimize their solubility in oil and are either soluble or dispersible in the brine.The partitioning of inhibitor products between the oil and aqueous phases require a reliable method to evaluate different inhibitor products. An analytical method using fluorescence spectroscopy has been developed as a means to measure inhibitor concentration. This new method offers several advantages over other commonly used techniques, such as dye transfer methods. The method offers a greater degree of accuracy, can be performed in the laboratory or at the well site, and individual analysis can be performed relatively quickly. Further, the performance of such formulations were evaluated under autoclave conditions in order to determine their applicability to existing producing systems.INTRODUCTIONCorrosion in metals is defined as the degradation of the materials' properties due to interactions with their environments1 and it has a significant impact on every stage of the oil and gas industry from production to transportation. In a study conducted from 1999 to 2001 by CC Technologies Laboratories, Inc., with support from the FHWA and NACE the total direct corrosion cost for the oil and gas exploration and production industry in the U.S. was estimated at 1.4 billion. The previous amount included expenses associated with surface pipeline and facilities, downhole tubing and capital expenditures related to corrosion.2 A recent report predicts this figure to be notably higher by 2015 due to the steady increase of direct and indirect costs of corrosion over the years, fueled by inflation and the expansion of oil and gas exploration and production.3