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Enhanced Bifunctional Oxygen Catalysis in Strained LaNiO_3 Perovskites

机译:LaNiO_3钙钛矿中增强的双功能氧催化

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摘要

Strain is known to greatly influence low-temperature oxygen electrocatalysis on noble metal films, leading to significant enhancements in bifunctional activity essential for fuel cells and metal-air batteries. However, its catalytic impact on transition-metal oxide thin films, such as perovskites, is not widely understood. Here, we epitaxially strain the conducting perovskite LaNiO_3 to systematically determine its influence on both the oxygen reduction and oxygen evolution reaction. Uniquely, we found that compressive strain could significantly enhance both reactions, yielding a bifunctional catalyst that surpasses the performance of noble metals such as Pt. We attribute the improved bifunctionality to strain-induced splitting of the e_g orbitals, which can customize orbital asymmetry at the surface. Analogous to strain-induced shifts in the d-band center of noble metals relative to the Fermi level, such splitting can dramatically affect catalytic activity in this perovskite and other potentially more active oxides.
机译:已知应变会极大地影响贵金属膜上的低温氧电催化作用,从而导致燃料电池和金属空气电池必不可少的双功能活性大大提高。然而,其对过渡金属氧化物薄膜如钙钛矿的催化作用尚未广为人知。在这里,我们外延应变导电钙钛矿LaNiO_3,以系统地确定其对氧还原反应和析氧反应的影响。独特地,我们发现压缩应变可以显着增强两个反应,从而产生一种双功能催化剂,其性能超过了贵金属(如Pt)。我们将改善的双功能性归因于应变诱发的e_g轨道分裂,这可以自定义表面的轨道不对称性。类似于应变引起的贵金属d带中心相对于费米能级的位移,这种分裂会极大地影响钙钛矿和其他潜在活性更高的氧化物的催化活性。

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  • 来源
    《Journal of the American Chemical Society》 |2016年第8期|2488-2491|共4页
  • 作者单位

    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States;

    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States;

    Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States;

    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States;

    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States;

    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States;

    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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