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Dissolution of electrocatalysts during long-term and dynamic operation is achallenging problem in energy conversion and storage devices such as fuel cellsand electrolyzers. To develop stable electrocatalysts, we adopt the designconcept of segregation engineering, which uses solute segregation prone toelectrochemical dissolution at internal defects, i.e., grain boundaries anddislocations. We showcase the feasibility of this approach by stabilizing amodel Pt catalyst with an addition of more noble Au (approximately 5 atomicpercent). We characterized the defects' nanoscale structure and chemistry, andmonitored the electrochemical dissolution of Pt and PtAu alloys by onlineinductively coupled plasma mass spectrometry. Once segregated to defects, Auatoms can stabilize and hence passivate the most vulnerable sites againstelectrochemical dissolution and improve the stability and longevity of the Ptelectrocatalysts by more than an order of magnitude. This opens pathways to usesolute segregation to defects for the development of more stable nanoscaleelectrocatalysts, a concept applicable for a wide range of catalytic systems.

Chemical Partitioning at Crystalline Defects in PtAu as a Pathway to Stabilize Electrocatalysts