Ternary Rare Earth Alloy Pt3-xIrxSc Nanoparticles Modulate Negatively Charged Pt via Charge Transfer To Facilitate pH-Universal Hydrogen Evolution.

Abstract

Rare earth (RE) elements possess electronic configurations that can provide additional pathways for tailoring the electronic structures of active elements through alloying, making it an important area of exploration in electrocatalysis. However, the large negative redox potential between RE and Pt has hindered the development of RE nanoalloys. In this study, a solid-phase synthesis strategy was employed to synthesize ternary Pt3-xIrxSc nanoparticles (NPs). By leveraging the electronegativity difference between Pt (2.28), Ir (2.20), and Sc (1.36), a charge-balance strategy was implemented to stabilize and enhance the catalytic performance of the alloy. The electron transfer from Sc to Pt/Ir results in the latter being negatively charged, and the Ir modifies the electron density of Pt, enabling favorable adsorption of active H species during the hydrogen evolution reaction (HER). Pt2IrSc exhibits enhanced HER activity at all pH values, achieving low overpotentials at 10 mA cm-2 of only 13, 18, and 25 mV in 0.5 M H2SO4, 1 M PBS, and 1 M KOH, respectively. This electrocatalyst also exhibits robust electrocatalytic stability even after 20,000 cycles. This work represents an application of the charge balance strategy to RE nanoalloys, and it is expected to inspire the design and synthesis of highly reactive RE nanoalloys.