The oxidative dehydrogenation of ethyl lactate to ethyl pyruvate, corresponding to the first step of a new process in the industrial production of methionine, has been investigated. Iron and vanadium antimonates were developed as catalysts, and were optimized to reach 87% conversion of ethyl lactate, with 88% selectivity to ethyl pyruvate, at only 275 °C. The catalysts were characterized before and after catalytic testing, and in situ using various techniques, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and XANES spectroscopy. The results show that neither the Sb 3+ /Sb 5+ nor the Fe 2+ /Fe 3+ redox couple were involved in the dehydrogenation of ethyl lactate, or in the catalysts re-oxidation. The active and selective catalytic sites correspond to surface V 5+ species. These species should not be considered as part of the bulk oxide, but as supra-surface species whose surface content is monitored with the bulk composition.