“…As a p -type semiconductor, nickel oxide (NiO) has been thoroughly explored as an active material in gas sensing due to its high catalytic activity in many organic compounds’ degradation. , For instance, NiO is an efficient catalyst for the methanol and ethanol oxidation processes, selective acetone hydrogenation, and oxidation of toluene. − Therefore, it is also well suited for the VOC sensing application, as the reduction and oxidation reactions are the fundamental working principles of gas detection in the sensor device. The NiO-based sensing materials have been proven to detect methanol, ethanol, formaldehyde, toluene, and many more. − NiO-based materials can be turned into various dimensionalities from 0D, 1D, 2D, and 3D hierarchical structures to significantly improve the gas sensing performance, as the morphology generally determines the specific surface area and the gas adsorption site. − More recently, researchers have also designed gas sensing materials with highly reactive facets to provide strong surface–adsorbate interactions. , For instance, the {111} surface facet is polar, Ni-terminated, and favorable for the adsorption and sensing of NO x gas, water molecules, and various VOCs. , However, the underlying mechanisms of molecular adsorption–desorption during the gas detection on the {111} surface facet of NiO, although hypothetically proposed in many experimental reports, were poorly investigated in detail by computational and theoretical simulations. This will surely accelerate the rational design of practical high-performance materials, not only for sensors but also for surface-related applications such as catalysis.…”