Pt-Modified High Entropy\nRare Earth Oxide for Efficient\nHydrogen Evolution\nin pH-Universal Environments

Abstract

The development of efficient and stable catalysts for\nhydrogen\nproduction from electrolytic water in a wide pH range is of great\nsignificance in alleviating the energy crisis. Herein, Pt nanoparticles\n(NPs) anchored on the vacancy of high entropy rare earth oxides (HEREOs)\nwere prepared for the first time for highly efficient hydrogen production\nby water electrolysis. The prepared Pt-(LaCeSmYErGdYb)O showed excellent\nelectrochemical performances, which require only 12, 57, and 77 mV\nto achieve a current density of 100 mA cm^–2 in 0.5\nM H₂SO₄, 1.0 M KOH, and 1.0 M PBS environments,\nrespectively. In addition, Pt-(LaCeSmYErGdYb)O has successfully worked\nat 400 mA cm^–2 @ 60 °C for 100 h in 0.5 M H₂SO₄, presenting the high mass activity of 37.7\nA mg^–1_Pt and turnover frequency (TOF)\nvalue of 38.2 s^–1 @ 12 mV, which is far superior\nto the recently reported hydrogen evolution reaction (HER) catalysts.\nDensity functional theory (DFT) calculations have revealed that the\ninteractions between Pt and HEREO have optimized the electronic structures\nfor electron transfer and the binding strength of intermediates. This\nfurther leads to optimized proton binding and water dissociation,\nsupporting the highly efficient and robust HER performances in different\nenvironments. This work provides a new idea for the design of efficient\nRE-based electrocatalysts.