In recent years, high-entropy alloy (HEA) nanoparticles (NPs) have attracted a lot of attention as a new class of nanomaterials in the field of catalysis and energy applications. This attention arises because of their tunable compositions, stability against oxidation and corrosion, high hardness, and exceptional ductility. To enhance the catalytic activity or selectivity of HEA NPs, significant effort is presently put into establishing correlations between composition and property. Therefore, it is essential to synthesize HEA NPs with well-defined sizes, shapes, and compositions. Scientists have demonstrated size control of HEA NPs, but the issue of compositional control, where each metal percentage can be controlled inside the multimetallic HEA NPs, has not been thoroughly addressed. We previously showed that monodisperse core@shell AuCu@PtPdNi NPs generated by colloidal synthesis can be converted into monodisperse HEA AuCuPtPdNi NPs by annealing them at high temperatures. The core@shell NPs were synthesized using random alloy AuCu NPs as seeds for the deposition of PtPdNi shells via seed-mediated co-reduction (SMCR). Now, compositional control of the HEA NPs is further demonstrated by using Au<sub>3</sub>Cu and AuCu<sub>3</sub> as seeds in the SMCR step to create Au or Cu rich HEA NPs, respectively.  In demonstrating the relationship between seed stoichiometry and final NP composition, general principles are established for the predictable synthesis of HEA NPs via NP conversion pathways.

Towards compositional control of monodisperse high-entropy alloy nanoparticles

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