离子辐照控制金属纳米颗粒溶出的尺寸、组成和分散度,Energy & Environmental Science

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离子辐照控制金属纳米颗粒溶出的尺寸、组成和分散度
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2023-09-25 , DOI: 10.1039/d3ee02448b
Jiayue Wang ₁ , Kevin B. Woller ₁ , Abinash Kumar ₂ , Zhan Zhang ₃ , Hua Zhou ₃ , Iradwikanari Waluyo ₄ , Adrian Hunt ₄ , James M. LeBeau ₂ , Bilge Yildiz _{1,

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Affiliation

纳米工程氧化物在下一代催化剂和微电子学的发展中发挥着前沿作用。最近，氧化物中的金属溶出已成为一种有前途的纳米结构工具，用于制造纳米颗粒装饰的氧化物。然而，控制出溶纳米粒子的尺寸、密度、成分和位置仍然是一个挑战，限制了这些纳米结构可实现的最终性能。在这里，我们将离子辐照作为一个通用平台，通过同时溅射、注入和缺陷生成机制来控制金属纳米颗粒溶出过程中的这些参数。使用薄膜钙钛矿和二元氧化物作为模型系统，我们表明离子束可以通过离子溅射可控地将溶解的纳米粒子的尺寸减小至 2 nm。同时，我们通过离子注入将溶解的纳米颗粒成分从单一金属调整为金属合金。此外，辐照会产生点缺陷和缺陷簇，它们充当金属脱溶的成核位点。通过利用这个过程，我们调整了溶解的纳米粒子的密度和空间分布。最后，我们证明，通过辐射辅助脱溶制备的纳米催化剂比使用传统脱溶方法制备的纳米催化剂对水分解反应表现出优异的催化活性。这些发现凸显了离子辐照在不同材料系统中工程化纳米颗粒溶出的潜力，对电化学和电子应用具有广泛的影响。

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Ion irradiation to control size, composition and dispersion of metal nanoparticle exsolution

Nano-engineered oxides play a frontier role in the development of next-generation catalysts and microelectronics. Recently, metal exsolution from oxides has emerged as a promising nano-structuring tool to fabricate nanoparticle-decorated oxides. However, controlling the size, density, composition, and location of exsolved nanoparticles remains a challenge, limiting the ultimate performance achievable by these nanostructures. Here, we present ion irradiation as a general platform to allow control over these parameters during metal nanoparticle exsolution, by simultaneous sputtering, implantation, and defect generation mechanisms. Using thin-film perovskite and binary oxides as model systems, we showed ion beams can controllably reduce the size of exsolved nanoparticles down to 2 nm through ion sputtering. Meanwhile, we tailored the exsolved nanoparticle composition from unitary metal to metal alloy via ion implantation. Furthermore, irradiation creates point defects and defect clusters, which serve as nucleation sites for metal exsolution. By leveraging this process, we tuned the density and spatial distribution of exsolved nanoparticles. Finally, we demonstrated that nanocatalysts prepared by irradiation-assisted exsolution exhibit superior catalytic activity toward water-splitting reactions than those produced using conventional exsolution methods. These findings highlight the potential of ion irradiation for engineering nanoparticle exsolution in diverse materials systems, with broad implications for electrochemical and electronic applications.

更新日期：2023-09-25

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