Pt-Modified High Entropy Rare Earth Oxide for Efficient Hydrogen Evolution in pH-Universal Environments

时间:2024-04-02浏览:11

论文题目:Pt-Modified High Entropy Rare Earth Oxide for Efficient Hydrogen Evolution in pH-Universal Environments

论文作者:Yong Jiang, Zhong Liang, Hao Fu, Ming-Zi Sun, Si-Yuan Wang, Bo-Long Huang*, Ya-Ping Du*

发表期刊:https://doi.org/10.1021/jacs.3c13367

Abstract

The development of efficient and stable catalysts for hydrogen  production from electrolytic water in a wide pH range is of great  significance in alleviating the energy crisis. Herein, Pt nanoparticles  (NPs) anchored on the vacancy of high entropy rare earth oxides (HEREOs)  were prepared for the first time for highly efficient hydrogen  production by water electrolysis. The prepared Pt-(LaCeSmYErGdYb)O  showed excellent electrochemical performances, which require only 12,  57, and 77 mV to achieve a current density of 100 mA cm–2 in 0.5 M H2SO4, 1.0 M KOH, and 1.0 M PBS environments, respectively. In addition, Pt-(LaCeSmYErGdYb)O has successfully worked at 400 mA cm–2 @ 60 °C for 100 h in 0.5 M H2SO4, presenting the high mass activity of 37.7 A mg–1Pt and turnover frequency (TOF) value of 38.2 s–1  @ 12 mV, which is far superior to the recently reported hydrogen  evolution reaction (HER) catalysts. Density functional theory (DFT)  calculations have revealed that the interactions between Pt and HEREO  have optimized the electronic structures for electron transfer and the  binding strength of intermediates. This further leads to  optimized  proton binding and water dissociation, supporting the highly efficient  and robust HER performances in different environments. This work  provides a new idea for the design of efficient RE-based  electrocatalysts.