Modification of alumina support with an appropriate amount of magnesia (Mg/Al ¼ 0:1) leads to the stable activity of the supported vanadium-antimony oxide catalyst for the dehydrogenation of ethylbenzene into styrene in the presence of carbon dioxide as oxidant. Correlation between catalytic performance and surface acidity has been found.Catalytic dehydrogenation of ethylbenzene in the presence of carbon dioxide (CO 2 -EBDH) has recently been attempted to explore a new technology for producing styrene selectively because it could provide us with an energy-saving and environmentally friendly process to utilize CO 2 , a greenhouse gas, as a mild oxidant.1-3 Several families of the catalysts, mainly based on supported or mixed oxides of Fe, V, or Cr were found to be active and selective in the CO 2 -EBDH.2-14 However, most of the catalysts have usually shown strong deactivation for this reaction during even a few hours on stream. As a typical example, over Mg-Al-V mixed oxides, the initial styrene yield, 64% after 1 h on stream, decreased to 40% after 7 h. 7 The similar deactivation rate was observed also for VO x /MgO catalyst. 3 We have proposed a very active and selective catalyst, V 0:43 Sb 0:57 O x / Al 2 O 3 (VSb/Al), but its deactivation was also significant mainly owing to coke formation although the deactivation rate was less than other reported catalysts. 12,13 Since the coke precursors are easily formed through the oligomerization of olefins, facilitation of olefins desorption from a catalyst surface could minimize the carbon accumulation. Taking into consideration a basic character of electron-rich olefins including styrene, lower surface acidity of the catalyst appears to induce easier desorption of olefins from the catalyst surface. VO x catalysts loaded on MgAl oxide support exhibited a decreased adsorption and rapid desorption of propylene as compared with those on alumina.14,15 Based on these considerations, an attempt has been made to stabilize the activity of VSb/ Al catalyst in the CO 2 -EBDH by the modification of the alumina support with a basic MgO component.MgO-modified alumina (Mg n Al) supports were obtained by impregnation of an activated alumina with aqueous solutions containing a certain amount of Mg(NO 3 ) 2 . 6H 2 O (Mg n Al; n is an atomic ratio of Mg/Al ¼ 0:1, 0.3, or 0.5) followed by calcination at 670 C. Alumina (Al)-or Mg n Al-supported vanadiumantimony oxide catalysts were prepared by impregnation with the solutions of NH 4 VO 3 and SbCl 3 followed by calcination at 650 C. The loading of the supported V 0:43 Sb 0:57 O x component (20 wt %) was the same for all samples. The catalyst supports and supported catalysts were characterized by BET specific surface area (S BET ) measurements (Micrometrics model ASAP 2400), X-ray diffraction (XRD) (Rigaku D/MAX-3B diffractometer) and the NH 3 -temperature-programmed-desorption method (NH 3 -TPD) (Micrometrics, TPD/TPR 027 Option). The catalytic tests were performed with 1 g of catalyst at 595 C under atmospheric pressure in an isothermal ...