Аннотация:In this work, using a combination of in situ methods, unambiguous correlations were established between the processes occurring on the surface of p-type semiconductor oxide Co3O4 and changes in its electrical conductivity, which form the sensor response towards CO gas. The Co3O4 based sensors showed a significant (by more than two orders of magnitude) increase in sensitivity when detecting CO in the temperature-pulsed mode (a long working phase at close to room temperature and a short-term phase of sensor regeneration at an elevated temperature 300 °C) compared with isothermal heating. The processes of CO oxidation on Co3O4 under sensor operating conditions, as well as its regeneration during annealing at 300 °C, were investigated using a combination of X-ray photoelectron spectroscopy (XPS), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and temperature-programmed desorption with mass spectrometry (TPD-MS). The sensor response of Co3O4 is caused by the CO oxidation with the participation of both chemisorbed and lattice oxygen, which is accompanied by the accumulation of surface carbonates and partial reduction of Co3+ to Co2+ in the near surface layer. Reversible sensor operation requires restoration of the material's initial state, which can be achieved by annealing at elevated temperature in an oxygen-containing atmosphere resulting in the decomposition of surface carbonates and the reoxidation of part of the Co2+ to Co3+ with the recovery of the spinel structure.