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These results provide the first thermodynamic evidence of structural transitions induced by CO2 sorption in the ZIF-8 framework.Though transition-metal-based materials have emerged as the most promising alternatives to Pt-based electrocatalysts in hydrogen evolution reaction (HER), only a few of them (Fe-, Co-, Ni-, W-, and Mo-based materials) are used as efficient HER electrocatalysts, while others are generally considered as HER-inactive materials with poor activities. Here, a theory-guided experiment is carried out to activate titani