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The  oxygen‐evolving  center  (OEC)  in  photosystem  II  (PSII)  of  plants,  algae  and cyanobacteria is a unique natural catalyst that splits water into electrons, protons and dioxygen. The crystallographic studies of PSII have revealed that the OEC is an asymmetric Mn4CaO5‐cluster. The understanding of  the structure‐function  relationship of  this natural Mn4CaO5‐cluster  is  impeded mainly due to the complexity of the protein environment and lack of a rational chemical model as a reference.  Although  it  has  been  a  great  challenge  for  chemists  to  synthesize  the  OEC  in  the laboratory, significant advances have been achieved recently. Different artificial complexes have been  reported,  especially  a  series  of  artificial  Mn4CaO4‐clusters  that  closely  mimic  both  the geometric and electronic structures of the OEC in PSII, which provides a structurally well‐defined chemical model to  investigate the structure‐function relationship of the natural Mn4CaO5‐cluster. The  deep  investigations  on  this  artificial Mn4CaO4‐cluster  could  provide  new  insights  into  the mechanism of the water‐splitting reaction in natural photosynthesis and may help the development of efficient catalysts for the water‐splitting reaction in artificial photosynthesis.

Mimicking the Catalytic Center for the Water-Splitting Reaction in Photosystem II