Due　to　their　explicit　structure,　metal-organic　frameworks　(MOFs)　have　been　supposed　to　be　credible　platforms　to　research　the　micro-mechanism　of　heterogeneous　photocatalysis.　In　this　study,　amino-functionalized　MOFs　(MIL-125(Ti)-NH2　(denoted　as　MTi),　UiO-66(Zr)-NH2　(denoted　as　UZr)　and　MIL-68(In)-NH2　(denoted　as　MIn))　with　three　different　metal　centers　were　synthesized　and　applied　for　the　denitrification　of　simulated　fuels　under　visible　light　irradiation,　during　which　pyridine　was　used　as　a　typical　nitrogen-containing　compound.　The　results　showed　that　MTi　had　the　best　activity　among　the　above　three　MOFs,　and　the　denitrogenation　rate　increased　to　80%　after　4　h　of　visible　light　irradiation.　On　the　grounds　of　the　theoretical　calculation　of　pyridine　adsorption　and　actual　activity　experiments,　it　can　be　presumed　that　the　unsaturated　Ti4+　metal　centers　should　be　the　key　active　sites.　Meanwhile,　the　XPS　and　in　situ　infrared　results　verified　that　the　coordinatively　unsaturated　Ti4+　sites　facilitate　the　activation　of　pyridine　molecules　through　the　surface　-NTi-　coordination　species.　The　coordination-photocatalysis　synergism　promotes　the　efficiency　of　photocatalytic　performance　and　the　corresponding　mechanism　is　proposed.　©　2023　The　Royal　Society　of　Chemistry.