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A series of MOFs with a 6‐connected spn topology were synthesized (MOF‐808‐(Zr, Hf), PCN‐777‐(Zr, Hf), MOF‐818‐(Zr, Hf)). Through the in situ DRIFTS of NH3 adsorption‐desorption, we found that the activated catalyst mainly contains Lewis acid sites. The effects of different organic ligands on the Lewis acid of the Zr6 cluster were analyzed by XPS and NH3‐TPD, and the relative Lewis acidity of the...