“…Nanostructured metastable ordered intermetallic compounds are difficult to rationally synthesize because the nucleation and growth conditions required to access these phases are not unequivocally known. − Literature reports suggest that the formation of metastable ordered intermetallic nanoparticles can occur only under conditions in which interfacial stabilization by capping agents results in greater stability for the metastable phase relative to equilibrium phases or under conditions in which nucleation rather than solid-state diffusion is rate-limiting. ,,− However, the former case is difficult to predict from first-principles, while the latter often results in materials with poor atomic ordering. ,,, Hence, conventional synthetic methods, such as high-temperature annealing and/or colloidal synthesis, largely exclude the formation of metastable ordered intermetallic compounds under typical reaction conditions. ,− Electrochemical deposition has recently emerged as a flexible technique for the direct preparation of metastable alloys and ordered intermetallic phases, yielding materials which can possess high intrinsic catalytic performance. ,, However, these techniques are limited to the preparation of thin films on flat/nonporous substrates, precluding their implementation in application-relevant contexts that require high surface area, and for designing materials that can harness diffusional transport gradients for enhancing catalytic activity and/or selectivity. , …”