Organic polymer photocatalysts are a promising materials platform for photosynthesis hydrogen peroxide production from water and oxygen system. However, limited by the controlled structural design and lack of effective active site, the photocatalytic efficiency is unsatisfactory. To address above these issues, we precisely designed and prepared two alkyne-based porous polymers via Sonogashira cross-coupling reaction (POP-DT and POP-DF). Acetylene is served as the oxygen-reducing active site, tuning thiophene or furan ring as the electron donor unit. They exhibited a large specific surface area and rich pore architecture. Under visible light irradiation, the H2O2 generation rate of POP-DT was as high as 2422.2 μmol-g-1-h-1, which was 4.3 times higher than that of POP-DF, represent one of the best performances ever reported polymeric photocatalysts. We found that the combination of acetylene and thiophene resulted in faster charge separation and transfer efficiency, significantly improving the kinetic behaviour of the oxygen reduction reaction. More importantly, combined with In situ diffuse reflectance infrared Fourier transform spectroscopy and theory calculations, we demonstrated that acetylene connected thiophene is more beneficial to electron enrichment of acetylene active site, making it enhanced the adsorption and activation of oxygen, thus boosted photocatalytic efficiency for oxygen reduction reaction. Our work provides a novel strategy for designing advanced polymer photocatalysts for enhanced solar energy conversion efficiency.

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