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

Abstract

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 (TC), solid solubility (Csol), and diffusion pre-exponential factor (D0) 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 mgPt−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 mgPt−1 after 30,000 cycles in membrane electrode assembly (MEA). Theoretical calculations reveal that X incorporation broadens the annealing temperature (Ta) window by forming Pt(NiX) with higher TC and lowering the kinetic threshold temperature (Tkin) 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.