Composite Co/Al oxide materials were prepared via flame spray pyrolysis and examined as catalysts for the dry reforming of methane. The interaction between the metal (Co) and the support (Al-oxide) was regulated by varying the Co : Al ratio and its influence on catalyst performance studied. The synthesis of materials with a Co content of 30 mol % (Co 3 Al 7 ) promoted the formation of readily reduced and highly-dispersed Co particles. This, in combination with a high relative surface basicity, contributed to Co 3 Al 7 delivering a high and stable activity towards the dry reforming reaction. The formation of bulk Co 3 O 4 particles, which exhibit weak interactions with the support material, in samples with a Co content of 50 (Co 5 Al 5 ) and 70 mol % (Co 7 Al 3 ) caused rapid catalyst deactivation via coking. The findings demonstrate the importance of metalsupport interactions between the Co catalyst and Al-oxide support for the activity and selectivity in the dry reforming of methane. Highly dispersed Co deposits and high support basicity, induced by an ideal FSP Co : Al synthesis ratio, are key to delivering an active and stable catalyst for the dry reforming of methane.[a] Dr.

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