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Achieving highly efficient hydrogen (H 2 ) evolution  via  artificial photosynthesis is a great ambition pursued by scientists in recent decades because H 2  has high specific enthalpy of combustion and benign combustion product. [FeFe]-Hydrogenase ([FeFe]-H 2 ase) mimics have been demonstrated to be promising catalysts for H 2  photoproduction. However, the efficient photocatalytic H 2  generation system, consisting of PAA- g -Fe 2 S 2 , CdSe QDs and H 2 A, suffered from low stability, probably due to the hole accumulation induced photooxidation of CdSe QDs and the subsequent crash of [FeFe]-H 2 ase mimics. In this work, we take advantage of supramolecular interaction for the first time to construct the secondary coordination sphere of electron donors (HA − ) to CdSe QDs. The generated secondary coordination sphere helps realize much faster hole removal with a ~30-fold increase, thus leading to higher stability and activity for H 2  evolution. The unique photocatalytic H 2  evolution system features a great increase of turnover number to 83600, which is the highest one obtained so far for photocatalytic H 2  production by using [FeFe]-H 2 ase mimics as catalysts.

Secondary coordination sphere accelerates hole transfer for enhanced hydrogen photogeneration from [FeFe]-hydrogenase mimic and CdSe QDs in water