A　novel　sp2　carbon-conjugated　covalent　organic　framework　(COF),　PZ-TFPT-COF,　was　designed　for　efficient　sulfur　dioxide　(SO2)　capture,　addressing　the　critical　issue　of　SO2　pollution,　primarily　emitted　from　the　combustion　of　sulfur-rich　fuels.　The　PZ-TFPT-COF　demonstrates　a　remarkable　SO2　adsorption　capacity　of　9.6　mmol/g　at　25　°C　and　1.0　bar,　with　a　superior　SO2/CO2　(0.1/0.9)　Ideal　Adsorbed　Solution　Theory　(IAST)　selectivity　of　36.3.　Structural　characterizations　through　powder　X-ray　diffraction　(PXRD),　N2　adsorption–desorption　isotherms,　scanning　electron　microscopy　(SEM),　and　high-resolution　transmission　electron　microscopy　(HRTEM)　confirm　its　excellent　crystallinity,　uniform　bulk　morphology,　and　abundant,　uniform　nanoporosity.　Additionally,　PZ-TFPT-COF　retains　96.9　%　of　its　initial　capacity　after　8　adsorption–desorption　cycles,　highlighting　its　excellent　recyclability.　The　binding　energy　between　SO2　and　the　pyrazine　nitrogen　sites　was　calculated　to　be　−40.29　kJ/mol,　indicating　their　strong　acid-base　interactions.　These　results　demonstrate　that　PZ-TFPT-COF　is　a　promising　candidate　for　advanced　flue　gas　desulfurization,　offering　significant　potential　for　cleaner　industrial　processes　and　improved　air　quality.　©　2025　Elsevier　B.V.