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Cr-rich αʹprecipitation during aging typically leads to hardening and accordingly embrittlement of FeCrAl alloys, which needs to be suppressed. The influence of grain size on αʹprecipitation was studied by aging coarse-grained (CG), ultra-fine grained (UFG), and nanocrystalline (NC) ferritic Kanthal-D [KD; Fe-21Cr-5Al (wt.%) alloy] at 450, 500 and 550 oC for 500h. After aging at 450 and 500 oC, less hardening was observed in the UFG KD than in CG KD. Atom probe tomography indicated a lower number density and larger sized intragranular αʹ in the UFG versus the CG alloy. The smaller grain size and higher defect (vacancy and dislocation) density in the UFG KD facilitated diffusion and accordingly enhanced precipitation kinetics, leading to coarsening of precipitates, as well as saturation of precipitation at lower temperatures, as compared to those in CG KD. No hardening occurred in UFG and CG KD after aging at 550 oC, indicating that the miscibility gap is between 500 and 550 oC. NC KD exhibited softening after aging owing to grain growth. αʹprecipitation occurred in NC KD aged at 450 oC but not at 500 oC, indicating that miscibility gap is between 450 and 500 oC. Thus, the significantly smaller grain size in NC KD decreased the miscibility gap, as compared to that in CG and UFG KD. This is attributed to the absorption of vacancies by migrating grain boundaries during aging, suppressing αʹ nucleation and enhancing Cr solubility. 

Nanostructured steels are expected to have enhanced irradiation tolerance and improved strength. However, they suffer from poor microstructural stability at elevated temperatures. In this study, Fe–21Cr–5Al–0.026C (wt%) Kanthal D (KD) alloy belonging to a class of (FeCrAl) alloys considered for accident‐tolerant fuel cladding in light‐water reactors is nanostructured using two severe plastic deformation techniques of equal‐channel angular pressing (ECAP) and high‐pressure torsion (HPT), and their thermal stability between 500–700 °C is studied and compared. ECAP KD is found to be thermally stable up to 500 °C, whereas HPT KD is unstable at 500 °C. Microstructural characterization reveals that ECAP KD undergoes recovery at 550 °C and recrystallization above 600 °C, while HPT KD shows continuous grain growth after annealing above 500 °C. Enhanced thermal stability of ECAP KD is from significant fraction (>50%) of low‐angle grain boundaries (GBs) (misorientation angle 2–15°) stabilizing the microstructure due to their low mobility. Small grain sizes, a high fraction (>80%) of high‐angle GBs (misorientation angle >15°) and accordingly a large amount of stored GB energy, serve as the driving force for HPT KD to undergo grain growth instead of recrystallization driven by excess stored strain energy.