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For the first time, bulk-like g-C3N4 was achieved through initiating layer-by-layer assembly, which involves the important process of artificially manipulating protonated and oxygen doped g-C3N4 nanosheets. When acting as a photocatalyst under UV-visible light irradiation, bulk-like g-C3N4 exhibited an excellent photocatalytic H2 production rate of 1538 μmol h-1 g-1, about 8 times higher than that of the bulk g-C3N4 counterpart.We demonstrate a novel method to ionize molecules or molecular clusters by proton transfer at temperatures below
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