Polycationic Pp-@g-CN composite was synthesized through an in situ polymerization process of -alkylpyridinium acetylenic alcohol bromide (p-) above the surface of g-CN. The structure of p-0 and the Pp-@g-CN properties were checked by modern technologies. Photocatalytic tests of Pp-@g-CN in water splitting unveiled much better Pp-@g-CN hydrogen evolution activities by comparison with both g-CN and Pp-0. The hydrogen production by Pp-0@g-CN was 1654.5 μmol h g, which is ∼26- and 22-fold greater in relation to what g-CN and Pp-0 produced (62.7 and 75.0 μmol h g, respectively), suggesting strong bilateral and synergistic interactions of g-CN with Pp-0. Although the lengthening methylene chain in the polymers weakened the hydrogen generation ability of Pp-@g-CN, the conjugated double bonds, solubilization, and dispersion of Pp- polycationic surfactants made Pp-@g-CN superior to g-CN in water splitting. Due to the readily available raw materials, a simple way of preparation (starting chemicals to p-0 to Pp-0@g-CN), high photocatalysis efficiency, light irritation stability, recyclable ability, and low toxicity, Pp-0@g-CN is a good candidate for water splitting.
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