Eidgenössische Technische Hochschule Zürich, Rämistrasse 101, 8092, Zurich, Switzerland.
Paul Scherrer Institute, Forschungsstrasse 111, 5232, Villigen, Switzerland.
Angew Chem Int Ed Engl. 2023 Jul 3;62(27):e202301468. doi: 10.1002/anie.202301468. Epub 2023 May 19.
Platinum nanoparticles (NPs) supported by titania exhibit a strong metal-support interaction (SMSI) that can induce overlayer formation and encapsulation of the NP's with a thin layer of support material. This encapsulation modifies the catalyst's properties, such as increasing its chemoselectivity and stabilizing it against sintering. Encapsulation is typically induced during high-temperature reductive activation and can be reversed through oxidative treatments. However, recent findings indicate that the overlayer can be stable in oxygen. Using in situ transmission electron microscopy, we investigated how the overlayer changes with varying conditions. We found that exposure to oxygen below 400 °C caused disorder and removal of the overlayer upon subsequent hydrogen treatment. In contrast, elevating the temperature to 900 °C while maintaining the oxygen atmosphere preserved the overlayer, preventing platinum evaporation when exposed to oxygen. Our findings demonstrate how different treatments can influence the stability of nanoparticles with or without titania overlayers. expanding the concept of SMSI and enabling noble metal catalysts to operate in harsh environments without evaporation associated losses during burn-off cycling.
担载于二氧化钛上的铂纳米粒子(NPs)表现出强烈的金属-载体相互作用(SMSI),这种相互作用可以诱导覆盖层的形成和 NPs 的封装,形成一层薄薄的载体材料。这种封装改变了催化剂的性质,例如增加了它的化学选择性并使其在烧结过程中稳定。封装通常是在高温还原活化过程中诱导的,并可以通过氧化处理来逆转。然而,最近的研究结果表明,覆盖层在氧气中可以稳定。我们使用原位透射电子显微镜研究了覆盖层如何随条件的变化而变化。我们发现,在随后的氢气处理中,暴露在低于 400°C 的氧气中会导致覆盖层的无序和去除。相比之下,将温度升高到 900°C 并保持氧气气氛会保留覆盖层,当暴露于氧气时,防止铂蒸发。我们的研究结果表明,不同的处理方法如何影响具有或不具有二氧化钛覆盖层的纳米粒子的稳定性,扩展了 SMSI 的概念,并使贵金属催化剂能够在苛刻的环境中运行,而不会在燃烧循环过程中因蒸发而损失。