Hojo Hajime, Nakashima Minori, Yoshizaki Satoru, Einaga Hisahiro
Department of Advanced Materials Science and Engineering, Faculty of Engineering Sciences, Kyushu University, 6-1, Kasugakoen, Kasuga, Fukuoka 816-8580, Japan.
Department of Molecular and Material Sciences, Graduate School of Engineering Sciences, Kyushu University, 6-1, Kasugakoen, Kasuga, Fukuoka 816-8580, Japan.
ACS Nano. 2024 Feb 13;18(6):4775-4782. doi: 10.1021/acsnano.3c09092. Epub 2024 Jan 29.
The interaction between a metal and a support, which is known as the metal-support interaction, often plays a determining role in the catalytic properties of supported metal catalysts. Herein, we have developed model Pt/CeO catalysts, which enabled us to investigate the interface atomic and electronic structures between Pt and the {001}, {011}, and {111} planes of CeO using scanning transmission electron microscopy and electron energy-loss spectroscopy. We found that the number of Ce ions around the Pt nanoparticles followed the order {001} > {011} > {111}, which was the opposite order of the generally accepted stability of low index surfaces of CeO. Systematic first-principles calculations revealed that the presence of Pt nanoparticles facilitated the formation of oxygen vacancies and that the appearance of the Pt state was preferred when Pt nanoparticles were in contact with CeO {001} planes due to direct charge transfer from Pt to CeO. These results provide important insights into the nature of the metal-support interaction for a comprehensive understanding of the properties of supported metal catalysts.
金属与载体之间的相互作用,即所谓的金属-载体相互作用,在负载型金属催化剂的催化性能中往往起着决定性作用。在此,我们制备了模型Pt/CeO催化剂,这使我们能够利用扫描透射电子显微镜和电子能量损失谱研究Pt与CeO的{001}、{011}和{111}面之间的界面原子和电子结构。我们发现,Pt纳米颗粒周围Ce离子的数量遵循{001}>{011}>{111}的顺序,这与通常认为的CeO低指数表面稳定性顺序相反。系统的第一性原理计算表明,Pt纳米颗粒的存在促进了氧空位的形成,并且由于Pt向CeO的直接电荷转移,当Pt纳米颗粒与CeO{001}面接触时,Pt态的出现更为有利。这些结果为全面理解负载型金属催化剂的性质提供了关于金属-载体相互作用本质的重要见解。