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In this work, a new method to extend the light absorption and improve the photocatalytic activity of metal‐organic frameworks (MOFs) with nitrogen‐containing ligand is reported, namely, the protonation of nitrogen. Specifically, a protonated Bi‐based MOF synthesized by a hydrothermal method (Bi‐MMTAA‐H, MMTAA=2‐mercapto‐4‐methyl‐5‐thiazoleacetic acid) displays a wider visible light absorption than...