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Reduction of CO2 with hydrogen into CH4 is studied for the first time on carbon‐nanotube‐supported Co and Ni catalysts under supercritical conditions. The extremely high selectivity toward methanation close to 100% is found with a quite good stability of the catalytic activity.

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Reduction of CO2 with hydrogen into CO was studied for the first time on alumina-supported Co and Fe catalysts under supercritical conditions with the goal to produce either CO or CH4 as the target products. The extremely high selectivity towards methanation close to 100% was found for the Co/Al2O3 catalyst, whereas the Fe/Al2O3 system demonstrates a predominance of hydrogenation to CO with noticeable formation of ethane (up to 15%). The space–time yield can be increased by an order of magnitude by using the supercritical conditions as compared to the gas-phase reactions. Differences in the crystallographic phase features of Fe-containing catalysts cause the reverse water gas shift reaction to form carbon monoxide, whereas the reduced iron phases initiate the Fischer–Tropsch reaction to produce a mixture of hydrocarbons. Direct methanation occurs selectively on Co catalysts. No methanol formation was observed on the studied Fe- and Co-containing catalysts.