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Proton-and neutron-irradiated Zircaloy-2 are compared in terms of the nano-scale chemical evolution within second phase particles (SPPs) Zr(Fe,Cr)₂ and Zr₂(Fe,Ni). This is accomplished through ultra-high spatial resolution scanning transmission electron microscopy and the use of energy-dispersive X-ray spectroscopic methods. Fe-depletion is observed from both SPP types after irradiation with both irradiative species, but is heterogeneous in the case of Zr(Fe,Cr)₂, predominantly from the edge region, and homogeneously in the case of Zr₂(Fe,Ni). Further, there is evidence of a delay in the dissolution of the Zr₂(Fe,Ni) SPP with respect to the Zr(Fe,Cr)₂. As such, SPP dissolution results in matrix supersaturation with solute under both irradiative species and proton irradiation is considered well suited to emulate the effects of neutron irradiation in this context. The mechanisms of solute redistribution processes from …