Zhang Yao, Li Zezhou, Tong Xing, Xie Zhiheng, Huang Siwei, Zhang Yue-E, Ke Hai-Bo, Wang Wei-Hua, Zhou Jihan
Beijing National Laboratory for Molecular Sciences, Center for Integrated Spectroscopy, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
Songshan Lake Materials Laboratory, Dongguan, 523808, China.
Nat Commun. 2024 Sep 2;15(1):7624. doi: 10.1038/s41467-024-52026-w.
Metal-oxide interfaces with poor coherency have specific properties comparing to bulk materials and offer broad applications in heterogeneous catalysis, battery, and electronics. However, current understanding of the three-dimensional (3D) atomic metal-oxide interfaces remains limited because of their inherent structural complexity and the limitations of conventional two-dimensional imaging techniques. Here, we determine the 3D atomic structure of metal-oxide interfaces in zirconium-zirconia nanoparticles using atomic-resolution electron tomography. We quantitatively analyze the atomic concentration and the degree of oxidation, and find the coherency and translational symmetry of the interfaces are broken. Atoms at the interface have low structural ordering, low coordination, and elongated bond length. Moreover, we observe porous structures such as Zr vacancies and nano-pores, and investigate their distribution. Our findings provide a clear 3D atomic picture of metal-oxide interface with direct experimental evidence. We anticipate this work could encourage future studies on fundamental problems of oxides, such as interfacial structures in semiconductor and atomic motion during oxidation process.
与块状材料相比，具有较差相干性的金属-氧化物界面具有特殊性质，并在多相催化、电池和电子学等领域有广泛应用。然而，由于其固有的结构复杂性以及传统二维成像技术的局限性，目前对三维（3D）原子级金属-氧化物界面的理解仍然有限。在此，我们使用原子分辨率电子断层扫描确定了锆-氧化锆纳米颗粒中金属-氧化物界面的3D原子结构。我们定量分析了原子浓度和氧化程度，发现界面的相干性和平移对称性被打破。界面处的原子具有低结构有序性、低配位数和伸长的键长。此外，我们观察到诸如Zr空位和纳米孔等多孔结构，并研究了它们的分布。我们的研究结果提供了具有直接实验证据的金属-氧化物界面清晰3D原子图像。我们预计这项工作可能会鼓励未来对氧化物基本问题的研究，例如半导体中的界面结构和氧化过程中的原子运动。
