Abstract
Detection of pollutant gases, such as formaldehyde (HCHO), in our homes and surrounding environment is of high importance for our health and safety. The effect of surface defects and specifically pre-adsorbed oxygen on the gas sensing reaction of HCHO with ZnO nanostructures is largely unknown. Using density functional theory, nonequilibrium Green's function method and ab initio molecular dynamics (AIMD) simulations, we show that the presence of surface oxygen has two key roles in the sensitivity of ZnO towards HCHO: (1) it leads to the presence of charge trap states, which vanish upon the adsorption of HCHO, and (2) it facilitates the dissociative chemisorption of HCHO on the surface. Our ground state and AIMD calculations show that multiple reaction products are produced, which eventually lead to cleaning the surface from the adsorbed species, and hence enhancing the recyclability of the surface. We not only confirm the reaction proposed by experiment, but show that the presence of surface oxygen facilitates other surface reactions as well. Our work provides insights into the gas-surface reaction mechanism of ZnO-nanostructure based gas sensors, not provided before by experiment.