Hydrogen absorption in an epitaxial thin film of high-entropy perovskite oxide

Takahiro Ozawa, Kaidong Wang, K. Nishio, R. Shimizu, T. Hitosugi, K. Fukutani
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Abstract

We synthesized an epitaxial film of high-entropy perovskite oxide (HEPO) consisting of three elements (Ca, Sr, Ba) in the A site and 12 elements (Si, Ti, Cr, Mn, Fe, Co, Ni, Ge, Zr, Sn, Ce, Hf) in the B site of ABO3, and investigated hydrogen absorption properties in the HEPO film. The hydrogen depth profile was measured by nuclear reaction analysis via the 1H(15N,αγ)12C reaction, showing the hydrogen absorption in the HEPO film with a maximum atomic concentration of 0.3 in the ABO3 unit. The diffusion coefficient of H in the film was analyzed from the H depth profile, and the activation barrier for diffusion was estimated to be (0.54±0.13) eV. An absorption band was observed at 3290 cm−1 in the infrared absorption spectrum, which corresponds to the O–H stretching vibration. Simultaneous measurements of nuclear reaction and resistance revealed that the HEPO film remained electrically insulating regardless of the hydrogen concentration. We demonstrated that hydrogen is incorporated in HEPO forming OH species while keeping HEPO electrically insulating.
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高熵过氧化物外延薄膜中的氢吸收
我们合成了由 ABO3 的 A 位上的三种元素(Ca、Sr、Ba)和 B 位上的 12 种元素(Si、Ti、Cr、Mn、Fe、Co、Ni、Ge、Zr、Sn、Ce、Hf)组成的高熵过氧化物(HEPO)外延薄膜,并研究了 HEPO 薄膜的氢吸收特性。通过 1H(15N,αγ)12C 反应的核反应分析测量了氢深度剖面,结果显示 HEPO 薄膜中的氢吸收在 ABO3 单元中的最大原子浓度为 0.3。根据氢的深度曲线分析了氢在薄膜中的扩散系数,估计扩散的活化势垒为 (0.54±0.13) eV。在红外吸收光谱中观察到 3290 cm-1 处有一条吸收带,对应于 O-H 伸展振动。同时进行的核反应和电阻测量结果表明,无论氢的浓度如何,HEPO 薄膜都保持电绝缘状态。我们证明了氢在 HEPO 中结合形成 OH 物种,同时保持了 HEPO 的电绝缘性。
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