Gases that are widely used in research and industry have a significant effect on both the configuration of solid materials and the evolution of reactive systems. Traditional studies on gas–solid interactions have mostly been static and post-mortem and unsatisfactory for elucidating the real active states during the reactions. Recent developments of controlled-atmosphere transmission electron microscopy (TEM) have led to impressive progress towards the simulation of real-world reaction environments, allowing the atomic-scale recording of dynamic events. In this review, on the basis of the in situ research of our group, we outline the principles and features of the controlled-atmosphere TEM techniques and summarize the significant recent progress in the research activities on gas–solid interactions, including nanowire growth, catalysis, and metal failure. Additionally, the challenges and opportunities in the real-time observations on such platform are discussed.

Direct observation of the dissolution behavior of nanomaterials could provide fundamental insight to understanding their anisotropic properties and stability. The dissolution mechanism in solution and vacuum has been well documented. However, the gas-involved dissolution and regrowth have seldom been explored and the mechanisms remain elusive. We report herein, an in situ TEM study of the dissolution and regrowth dynamics of MoO₂ nanowires under oxygen using environmental transmission electron microscopy (ETEM). For the first time, oscillatory dissolution on the nanowire tip is revealed, and, intriguingly, simultaneous layer-by-layer regrowth on the sidewall facets is observed, leading to a shorter and wider nanowire. Combined with first-principles calculations, we found that electron beam irradiation caused oxygen loss in the tip facets, which resulted in changing the preferential growth facets and drove the morphology reshaping.

Nanocrystal coalescence has attracted paramount attention in nanostructure fabrication in the past decades. Tremendous endeavor and progress have been made in understanding its mechanisms, benefiting from the development of transmission electron microscopy. However, many mechanisms still remain unclear, especially for nanocrystals that lack a permanent dipole moment standing on a solid substrate. Here, we report an in situ coalescence of Pt nanocrystals on an amorphous carbon substrate induced by electron-excitation-enhanced van der Waals interactions studied by transmission electron microscopy and first principles calculations. It is found that the electron-beam-induced excitation can significantly enhance the van der Waals interaction between Pt nanocrystals and reduce the binding energy between Pt nanocrystals and the carbon substrate, both of which promote the coalescence. This work extends our understanding of the nanocrystal coalescence observed in a transmission electron microscope and sheds light on a potential pathway toward practical electron-beam-controlled nanofabrication.