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Pt-Modified High Entropy Rare Earth Oxide for Efficient Hydrogen Evolution in pH-Universal Environments
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2024-03-22 , DOI: 10.1021/jacs.3c13367
Yong Jiang 1 , Zhong Liang 1 , Hao Fu 1 , Mingzi Sun 2 , Siyuan Wang 1 , Bolong Huang 2, 3 , Yaping Du 1
Affiliation  

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.

中文翻译:

Pt 改性高熵稀土氧化物可在通用 pH 环境中高效析氢

开发高效、稳定的宽pH范围电解水制氢催化剂对于缓解能源危机具有重要意义。在此,首次制备了锚定在高熵稀土氧化物(HEREO)空位上的Pt纳米颗粒(NP),用于通过水电解高效生产氢气。制备的Pt-(LaCeSmYErGdYb)O表现出优异的电化学性能,在0.5 MH 2 SO 4、1.0 M KOH和1.0 M PBS环境中仅需要12、57和77 mV即可实现100 mA cm –2的电流密度, 分别。此外,Pt-(LaCeSmYErGdYb)O已在0.5 MH 2 SO 4中在400 mA cm –2 @ 60 °C下成功工作100小时,呈现出37.7 A mg –1 Pt的高质量活性和周转频率(TOF) 12 mV 时的值为 38.2 s –1,远远优于最近报道的析氢反应 (HER) 催化剂。密度泛函理论(DFT)计算表明,Pt 和 HEREO 之间的相互作用优化了电子转移的电子结构和中间体的结合强度。这进一步优化了质子结合和水解离,支持不同环境下高效、稳健的 HER 性能。这项工作为高效稀土电催化剂的设计提供了新思路。
更新日期:2024-03-22
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