Propane　dehydrogenation　is　one　of　the　most　promising　routes　for　propylene　production　due　to　its　single　reactant,　product　and　high　economic　efficiency.　For　Co-based　catalysts,　the　state　of　Co　species　is　one　of　the　important　factors　affecting　the　performance　of　propane　dehydrogenation.　Here,　we　designed　zeolite　Silicalite-1　(S-1)　with　different　silanol　nests　content　as　support　to　investigate　the　effect　of　silanol　nests　content　to　form　Td-Co(II)　species.　It　is　found　that　the　content　of　silanol　nests　in　the　S-1　supports　have　a　linear　correlation　with　the　formation　of　Td-Co(II)　species　and　corresponding　PDH　catalytic　activity　through　the　study　of　the　catalyst　structure-performance　relationship.　And　the　silanol　nests　of　S-1　could　be　fully　coordinated　with　0.5　wt%　Co　content　over　0.5Co/S-1-1-HTS　in　the　form　of　Td-Co(II)　species　to　maximize　the　Co　atomic　utilization.　Correspondingly,　0.5Co/S-1-1-HTS　shows　the　most　excellent　catalytic　activity　and　stability,　with　C3H6　generation　rate　of　3014　mmol　C3H6　gCo−1　h−1　and　deactivation　rate　of　0.07　h−1　at　550　°C.　©　2024　Elsevier　B.V.