Database-guided thermodynamic-kinetic regulation for PtNi-based intermetallic electrocatalysts

Pt-Ni alloys exhibit outstanding oxygen reduction reaction (ORR) activity, yet achieving structural ordering to enhance stability remains a persistent challenge. Here, we propose a database-guided screening strategy to identify promoter elements (X) that facilitate ordering. By screening the critical disorder-to-order transition temperature ([Formula: see text]), solid solubility ([Formula: see text]), and diffusion pre-exponential factor ([Formula: see text]) of candidate elements from material databases, six sets of L1₀-Pt(NiX) nanoparticles were synthesized. The developed L1₀-PtNiFe catalysts demonstrated a high mass activity (MA) of 4.38 A mg_Pt^-1, retaining 82.1% after 50,000 cycles of accelerated durability testing (ADT) in half-cells, and retaining 79% of its initial MA of 1.1 A mg_Pt^-1 after 30,000 cycles in membrane electrode assembly (MEA). Theoretical calculations reveal that X incorporation broadens the annealing temperature ([Formula: see text]) window by forming Pt(NiX) with higher [Formula: see text] and lowering the kinetic threshold temperature ([Formula: see text]) via enhanced atom mobility. This work establishes a database-guided framework that enables phase transitions previously difficult to access by creating an effective annealing window through coordinated thermodynamic-kinetic regulation, thereby facilitating the formation of ordered PtNi-based intermetallic structures toward durable electrocatalysts.