Revealing Temperature-Dependent Oxidation Dynamics of Ni Nanoparticles via Ambient Pressure Transmission Electron Microscopy.

Abstract

Understanding the oxidation mechanism of metal nanoparticles under ambient pressure is extremely important to make the best use of them in a variety of applications. Through ambient pressure transmission electron microscopy, we <i>in situ</i> investigated the dynamic oxidation processes of Ni nanoparticles at different temperatures under atmospheric pressure, and a temperature-dependent oxidation behavior was revealed. At a relatively low temperature (e.g., 600 °C), the oxidation of Ni nanoparticles underwent a classic Kirkendall process, accompanied by the formation of oxide shells. In contrast, at a higher temperature (e.g., 800 °C), the oxidation began with a single crystal nucleus at the metal surface and then proceeded along the metal/oxide interface without voids formed during the whole process. Through our experiments and density functional theory calculations, a temperature-dependent oxidation mechanism based on Ni nanoparticles was proposed, which was derived from the discrepancy of gas adsorption and diffusion rates under different temperatures.