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Revisiting the effects of molybdenum and tungsten alloying on corrosion behavior of nickel-chromium alloys in aqueous corrosion
Minor alloying additions such as molybdenum (Mo) have major effects on the localized corrosion resistance of corrosion resistant alloys containing chromium. However, progress in alloy development is mostly based upon empirical observations, where any mechanistic insights are largely relegated to the latter stages of localized corrosion (i.e., stabilization and propagation) that are more readily accessible experimentally. For instance, it is well understood that Mo and tungsten (W) affect repassivation of local active, as well as widespread transpassive, corrosion sites and Mo surface enrichment during corrosion is well-documented. In this paper, a comprehensive examination of the functions and mechanism by which selected Mo and W operate to improve the passivity and resistance to breakdown during the initial stages of localized corrosion of the most common Ni-based solid solution alloys is presented. Furthermore, it is shown that Mo and W exert considerable influence on many stages of corrosion, including both passivation and film breakdown, re-enforcing old and introducing more recent ideas in this comprehensive review of the current state of corrosion research on Ni-Cr-(Mo + W) alloys.
Atomic faulting drives exceptional toughness in low thermal expansion chromium alloys
Endowing functional properties with mechanical responses in traditional metals has been a frontier topic, akin to transforming base metal into gold. Chromium and its alloys, with their functional deficiencies and limited ductility, serve as typical examples. Herein, we report a Cr96Fe4Ge1.3B1 alloy that unifies low thermal expansion (LTE, αl = 1.79 × 10-6 K-1, 200 − 315 K) with exceptional toughness (240.2 J·cm-3). The enhancement in mechanical responses is primarily attributed to layered Cr2B intermetallic precipitates, which ameliorate interfacial cohesion and simultaneously refine the grain structure. The weakened interlayer interactions within the Cr-B layers facilitate the nucleation and movement of numerous tiny stacking faults in precipitates, efficiently alleviating strain energy and resulting in marked work-hardening ability. Additionally, antiferromagnetic fluctuations in the BCC matrix contribute to the unique LTE behavior. This paves the way for the design of high-performance alloys featuring layered-symmetry precipitates.
Effects of Aluminum and Molybdenum on the Phase Stability of Iron-Chromium Alloys: A First-Principles Study
The interaction between solute atoms is critical to the thermodynamic behavior of Fe-Cr alloys, but the effects of non-dilute Al and Mo on the Fe-Cr phase stability and vacancy formation energy are not clearly understood. In this study, density functional theory, cluster expansion, and Monte Carlo simulation are used to predict the effects of ternary solute elements on the thermodynamic properties in multicomponent Fe-Cr alloys. The machine learning regression approach is applied to train and construct energy models that accurately describe the complex chemical interactions. The computational outcomes include the prediction of the partial ternary phase diagram, mixing enthalpy, and vacancy formation energy for different compositions. The phase boundary calculation predicts a pronounced change of Cr solubility in bcc Fe by the addition of Al and the rejection of Al atoms from a’ precipitates. The mixing enthalpy calculation shows that Mo may also reduce the Cr solubility in bcc Fe. Additionally, the simulations show that non-dilute Cr decreases the vacancy formation energy in bcc Fe, while adding Al results in a less significant effect. Finally, the results demonstrate important applications of using machine learning energy models to study model or commercial alloys with multicomponent solute species and point defects.
A preliminary investigation into the electrodeposition and synthesis of radiopure Copper–Chromium alloys for rare-event physics detector systems
Current investigations into neutrinoless double beta decay and the direct detection of dark matter require increasingly sensitive detector systems that demand ultra-low background materials. These requirements have previously been attained using ultra-radiopure electroformed (EF) copper. However, pure copper possesses high ductility and relatively low strength, which necessitates the need for large amounts of material and extra care during fabrication to help minimize galling and mechanical failure. Furthermore, we investigate an alloying alternative to pure EF copper by examining low wt% copper chrome (Cu–Cr) solid solution alloys, with inquiries into alloy hardness, strength, and radiopurity. Alloyed Cu–Cr layered samples are shown to exhibit significantly increased hardness compared to EF copper, for example showing a 50% increase in exhibited hardness using less than 1% Cr by weight, with limited negative impact to the material’s radiopurity.
Vacancy surface migration mechanisms in dilute nickel-chromium alloys
We investigate the unitary mechanisms related to the surface migration of vacancies in dilute Ni-Cr alloys via first-principle calculations. We survey a complete set of surface and sub-surface migration paths for vacancies near the (100) free surface and calculate the corresponding migration barriers. Our results show that a vacancy migrating towards the free surface will face lower energy barriers to migrate via atomic exchange with a neighboring Cr atom rather than with a Ni atom. Once a vacancy reaches the free surface, it will be trapped there. Our results also reveal that, when a Cr atom sits in the atomic plane just below the free surface, any in-plane vacancy hopping jump that would result in the vacancy sitting on top a subsurface Cr atom is energetically unfavorable. Taken together, these fundamental unitary surface migration mechanisms offer insights into the complex interactions between surface segregation and vacancy migration phenomena in Ni-Cr-based alloys.
Metastable formation and disordering kinetics of body-centered orthorhombic CrNi 2 laths in a Cr-Ni binary alloy
Chromium (Cr) alloys combine low density with high-temperature strength but suffer from brittleness and rapid softening. Body-centered orthorhombic (BCO) CrNi 2 laths have been shown to improve Cr-alloy high-temperature strength retention, yet their thermal stability and transformation behavior remain unclear. CrNi 2 conventionally forms through long-range ordering from a face-centered cubic (FCC) phase. Using multiscale microscopy and neutron diffraction, we show that CrNi 2 instead nucleates from a body-centered cubic (BCC) matrix, in a binary Cr 85 Ni 15 alloy. Despite aging above the equilibrium ordering temperature, CrNi 2 persists for ∼220 h at 760 °C before fully disordering, indicating sluggish transformation kinetics. The formation and decomposition follow differing transformation pathways (BCC → CrNi 2 → FCC), revealing kinetic asymmetry not captured by equilibrium Cr-Ni phase diagrams. In conclusion, these findings redefine the transformation behavior of CrNi 2 , establish its metastable kinetic window, and suggest alloying strategies to stabilize CrNi 2 for precipitation strengthening of high-temperature Cr-alloys.
Crack-Free 30% Chromium-Nickel Alloy Welding Products for Nuclear Service
We report prior research in the development of 30% chromium-nickel alloy nuclear welding wires has resulted in the resolution of primary water stress corrosion cracking (PWSCC) and ductility dip cracking (DDC) as well as improvement in solidification cracking (SC) resistance. The resolution of DDC exhibits some Laves phase, which has a negative effect on SC resistance. In this study, the use of an alternate carbide former, tantalum (Ta), in combination with niobium (Nb) was researched. Three heats of recently designed Filler Metal 52MSS-Ta (i.e., HV1648, HV1673A, and VX131WXW) were melted, fabricated, and systematically studied. DDC and SC were evaluated with thermodynamic modeling using the Scheil solidification simulation model, two types of varestraint tests, and strain-to-fracture (STF) testing. The varestraint and STF test results showed an improved SC resistance with reduced Laves phase and concurrent excellent DDC resistance. Optimized compositions with low Laves phase also exhibited high threshold strain values (TSVs) in the STF test. VX131WXW — which contains 2.81 wt-% Ta, 0.6 wt-% Nb, and 6 wt-% iron (Fe) - exhibited a TSV of 24%. Thermo-Calc computed the Laves phase to be 0.24% for VX131WXW compared to 0.06% in HV1673A. This difference in Laves phase resulted in the lower SC resistance of VX131WXW compared to HV1673A when measured with longitudinal varestraint testing. The maximum crack distance for HV1673A was about 0.6 mm while that of heat VX131WXW was about 1.0 mm. The typical diluted weld deposit made with VX131WXW was also resistant to PWSCC due to the chromium content exceeding 24%. These simultaneous results mark progress toward crack-free welds and provide direction for further optimization of Ta-containing filler metals.
Micromechanical aspects of deformation and failure of advanced Iron-Chromium-Aluminum alloys
Here this work investigates the micromechanical deformation and failure mechanisms of advanced FeCrAl alloys developed for use in nuclear reactors as cladding material. Three different FeCrAl alloys (82-X)Fe-13Cr-5Al-X (X=Nb, TiC, 0 for base alloy) were investigated both in their as-received and welded states. In-situ neutron diffraction with simultaneous digital image correlation was used to determine micromechanical deformation mechanisms not only as a function of elemental composition but also as a condition of state (as-received vs. welded). Ex-situ X-ray computed tomography was used on as-deformed samples to help determine the failure mechanisms and void initiation strains.
A percolation theory for designing corrosion-resistant alloys
Iron-chromium and nickel-chromium binary alloys containing sufficient quantities of chromium serve as the prototypical corrosion-resistant metals owing to the presence of a nanometre-thick protective passive oxide film. Should this film be compromised by a scratch or abrasive wear, it reforms with little accompanying metal dissolution, a key criterion for good passive behaviour. This is a principal reason that stainless steels and other chromium-containing alloys are used in critical applications ranging from biomedical implants to nuclear reactor components. Unravelling the compositional dependence of this electrochemical behaviour is a long-standing unanswered question in corrosion science. Herein, we develop a percolation theory of alloy passivation based on two-dimensional to three-dimensional crossover effects that accounts for selective dissolution and the quantity of metal dissolved during the initial stage of passive film formation. We validate this theory both experimentally and by kinetic Monte Carlo simulation. Our results reveal a path forward for the design of corrosion-resistant metallic alloys.
Ab initio study of phosphorus effect on vacancy-mediated process in nickel alloys – An insight into Ni 2 Cr ordering
The development of long range order in nickel-chromium alloys is of great technological interest but the kinetics and mechanisms of the transformation are poorly understood. The present research utilizes a combined computational and experimental approach to elucidate the mechanism by which phosphorus accelerates the ordering rate of stoichiometric Ni 2 Cr in Ni-Cr alloys. A series of Ni-33%Cr-x%P samples (in atomic percent) were fabricated with phosphorus concentrations, x = <0.005–0.1 at.% and aged between 373 and 470 °C for times up to 3000 h. The first-principles modeling considers fcc Ni with dilute P as a reasonable approximation for the complex Ni-Cr-P alloy system. Calculation results show a pronounced enhancement of vacancy transport by vacancy-solute pair diffusion via consecutive exchange and rotation jumps of vacancies associated with the phosphorus atom. The energy barriers of these two migration paths are at least 0.35 eV lower than that of vacancy-atom exchange in pure Ni solvent. The analytical diffusion model predicts enhanced solvent diffusion by 2 orders of magnitude for 0.1 at.% P at 400–500 °C. The model prediction is in good agreement with the evolution of micro-hardness. We characterize the micro-hardness result by a kinetic ordering model, showing a significant decrease of the activation energy of ordering transformation. These results help gauge the risk of industrial alloys developing long range order which increases strength but degrades ductility and toughness. Specifically, minor alloying additions that bind with excess vacancies and lower the vacancy migration barrier can greatly accelerate hardening via Ni 2 Cr precipitation.
High-temperature oxidation and quenching of chromium-coated zirconium alloy ATF cladding tubes with and w/o pre-damage
Chromium-coated zirconium alloys are one of the promising candidates for accident-tolerant fuel cladding (ATF) tubes for light water reactors (LWRs). In this study, the high temperature oxidation and degradation of two types of Cr coatings (cold spray and physical vapor deposition) with and without pre-damage by scratches were investigated on prototype rod segment samples filled with ZrO 2 pellets and tightly sealed with welded end caps. Isothermal tests at 1100 and 1200 °C were terminated by quenching with water; transient tests were performed up to 1500–1600 °C until complete coating failure. The positive effect of both types of Cr coatings was observed in all tests. Pre-damaged specimens showed only locally increased oxidation of the scratched zone, but no negative effects on the adjacent Cr coating. Finally, the behavior of the two types of coatings is compared and the degradation mechanisms are discussed based on hydrogen release data, extensive metallographic post-test examinations, and the current state of global research.
Hydrogen permeation in iron-chromium-aluminum (FeCrAl) alloys and the effects of microstructure and surface oxide
Iron–chromium–aluminum (FeCrAl) class alloys are candidates for use as cladding for accident-tolerant fuels and moderators. In this context, hydrogen isotope permeation in FeCrAl alloys is an important material property. Here, in the present work, the apparent permeability, effective diffusivity, and apparent solubility of hydrogen in the FeCrAl alloys C26M and Kanthal D (KD) were measured with gas-driven hydrogen permeation. Permeation measurements were conducted at temperatures of 400 to 700 °C and at gas-driven pressures from 1 to 100 kPa. In particular, the effect of grain size on hydrogen transport was studied with KD samples with three different microstructures: nanocrystalline (NC), ultra-fine grained (UFG), and coarse-grained (CG). The UFG and NC specimens had higher apparent activation energies (73.4 kJ mol -1 and 65.2 kJ mol -1 , respectively) for hydrogen permeability than the CG sample (46.9 kJ mol -1 ). An aluminum oxide layer formed on the primary- and secondary-side surfaces of all samples subjected to permeation experiments which demonstrated the propensity of FeCrAl alloys to form these innate oxide permeation barriers.
Microstructural evolution in shear-punch tests: A comparative study of pure Cu and Cu-Cr alloy
Understanding the mechanisms behind microstructural evolution during shear deformation has been a long-standing area of interest. However, establishing a connection between microstructure, mechanical properties, and extent of shear deformation is challenging and requires refined experimental approaches. Shear-punch testing (SPT) provides a controlled method to introduce shear into small volumes of material that later can be subjected to detailed microstructural characterization. In this study, we utilize an SPT device to induce shear deformation to pure copper and a binary copper-chromium alloy. Electron backscatter diffraction and transmission electron microscopy were used to study the mechanisms of plastic deformation after SPT. Our results indicate that shear deformation of pure Cu produces a dense network of intercepting microshear bands upon sustained deformation. Twin boundaries undergo degradation into high angle grain boundaries due to simultaneous deviation from the axis-angle pair condition of 60° misorientation on [111] direction. The presence of 50% volume Cr particles in the soft Cu matrix fundamentally altered the shear deformation mechanism. Preferential deformation of the Cu matrix led to accelerated shear-induced formation of low and high angle grain boundaries, and subsequent grain refinement. Comparatively, no grain refinement occurred in pure Cu at a strain ~10 times larger (ϵ = 4.73) than that of the copper-chromium case (ϵ = 0.42). Overall, our study sheds light on the microstructural evolution during shear deformation and highlights the significant influence of particle reinforcements on the shear deformation mechanisms of metals.
Stainless Steel Corrosion during H-Canyon Resin Digestion
Historically HB-Line has transferred a slurry of used anion exchange resin to the H-Canyon Tank 5.2 where caustic digestion using permanganate was performed prior to transfer to the tank farm. Recent digestions had switched to an acid flowsheet. During recent testing to investigate the hydrogen generation rate (HGR) for the resin acid digestion process, the experimental apparatus fabricated from stainless steel and nickel-chromium alloys was found to have suffered significant localized corrosion which failed a heating rod. This observed corrosion raised concerns about the integrity of Tank 5.2, which is fabricated of 304L stainless steel. An exploratory study was undertaken to better understand the cause of this corrosion as well as during a caustic digestion and to use these data to assess the viability of Tank 5.2 using the current acid digestion flowsheet versus the previous caustic flowsheet.
Vadose and Saturated Zone Flow and Transport Calculations for the Active Trenches of the Low-Level Burial Grounds, Hanford Site, Washington
The purpose of the fate and transport modeling described in this environmental calculation file (ECF) is to evaluate the impacts to groundwater associated with waste disposal operations at Mixed Waste Low-Level Burial Ground (LLBG) Trenches 31 and 34 to satisfy requirements in DOE O 435.1, Radioactive Waste Management. The model integrates the flow and transport in the vadose zone beneath the active trenches with the saturated zone downgradient of the trenches to predict the radionuclide concentration at the point of assessment (POA). DOE M 435.1-1, Radioactive Waste Management Manual, defines the POA as the point of highest projected dose or concentration beyond a 100 m (328 ft) buffer zone surrounding the disposed waste. The modeling is conducted in accordance with the DOE G 435.1, Implementation Guide for Use with DOE M 435.1-1, performance assessment (PA) guidelines. The modeling involves evaluation of the groundwater concentrations and radionuclide arrival times during the 1,000-year compliance and 10,000-year sensitivity-uncertainty periods per DOE O 435.1 and DOE M 435.1. This analysis does not consider radionuclide release during facility operations, only the post-closure impacts of the radionuclides to the environment. The evaluation of potential radiological dose to groundwater receptors caused by releases from a closed facility containing radioactive waste typically includes the following: (1) Release of radionuclides from that facility (2) Transport of those radionuclides through the environment, and (3) Exposure to humans to environmental concentration levels of those radionuclides The fate and transport three-dimensional (3D) model analysis involves the post-closure impacts to the environment of the technetium-99, iodone-129, and uranium (all isotopes in the waste). The residual inventory estimates include several radionuclides, but technetium-99 is typically responsible for almost all of the beta-gamma dose equivalent associated with groundwater (water resources) protection per 40 CFR 141, “National Primary Drinking Water Regulations” (e.g., see the results in WCH-520, Performance Assessment of Environmental Restoration Disposal Facility, Hanford Site, Washington; hereinafter referred to as the ERDF PA), and iodone-129 can also be a significant dose contributor for some waste (e.g., RPP-RPT-59958, Performance Assessment for the Integrated Disposal Facility, Hanford Site, Washington; hereinafter referred to as the IDF PA). Uranium does not typically factor significantly into the impacts to groundwater, even during the 10,000-year sensitivity-uncertainty period, but always remains of interest as a contaminant. This ECF does not address vadose and saturated zone modeling for Trench 94 of the 200 East Area LLBG. Current information confirms the validity of the low corrosion rate of the naval reactor plant carbon steel (HY-80), and the even lower corrosion rate of the nickel-iron-chromium alloy reactor vessel (Inconel Alloy 600) presented in DOE/EIS-0259, Final Environmental Impact Statement on the Disposal of Decommissioned, Defueled Cruiser, Ohio Class, and Los Angeles Class Naval Reactor Plants. Based on these low corrosion rates, the time to breach the reactor vessel to allow release of radionuclides from the activated metal of the reactor vessel internal structure is at least 10,000 years. This time to breach precludes the need to evaluate the vadose and saturated zone transport of contaminants released from the reactor compartment disposal packages in the 200 East Area LLBGs PA (CP-63826, Waste Release Model Package Report for the Active Trenches of the Low-Level Burial Grounds, Hanford Site, Washington).
Fuel performance of chromium-coated zirconium alloy and silicon carbide accident tolerant fuel claddings
The U.S. Department of Energy’s Accident Tolerant Fuel program is focused on extending the time for fuel failure during postulated severe accidents compared to the standard UO2-Zr alloy fuel system. This research investigates the feasibility of two different chromium-coated cladding concepts, one of which is zirconium-alloy based and the other is composite-SiC based. Both claddings had 50µm coatings, deducted from the base layer thicknesses. The claddings were reported on, using the multi- physics fuel performance tool BISON, under steady-state PWR operating conditions as well as two transients: power ramp and a loss-of-coolant accident (LOCA). The chromium-coated claddings showed comparable thermo-mechanical performance to the reference Zircaloy-4 cladding. As chromium is reported to provide an order of magnitude improvement in oxidation resistance, it is expected to be a better alternative in accident scenarios. Simulation results for both concepts call for further experimental investigation as well as modeling of beyond design-basis accidents.
A critical dislocation velocity for serration mechanism transition in a nickel-chromium solid solution alloy
Here, the influence of strain rate across three orders of magnitude (1.70 × 10 –5 /s to 1.43 × 10 –2 /s) along with the effect of the plastic strain accumulation (up to 10%) on the serrated plastic flow were investigated in the nickel-chromium (Ni-Cr) solid solution alloy Nimonic 75 by performing constant-strain-rate tension testing at 600 °C. As the strain rate decreased, the critical strain for the onset of serrations transitioned from normal behavior to inverse behavior. The serrated flow was characterized as Type A+B serration at high strain rate (1.43 × 10 –2 /s). In the intermediate strain-rate regime (1.43 × 10 –3 /s and 1.45 × 10 –4 /s), Type B serrations were observed and followed by a transformation to Type C+B serrations. At the low strain rate (1.70 × 10 –5 /s), the plastic flow immediately displayed Type C serrations, which later evolved into Type C+B serrations. Regardless of the strain rate, plastic strain, or dislocation density, a critical dislocation velocity falling in the range of 1.2 × 10 –6 – 2.2 × 10 –6 m/s was identified to signify the onset of Type C serration, whereby the mobile dislocations break free from the solute cloud for short bursts of deformation. Finally, a novel model by solute rearrangement across dislocation cores was used to understand how the critical dislocation velocity is quantitatively determined by the rate at which solute atoms are able to hop across the glide plane as a partial dislocation core moves through the lattice.