Use of the mechanistic probe 2-methyl-1-phenylpropan-2-yl hydroperoxide (MPPH) to discriminate between the formation of MnIVMnIV(OH) and MnIVMnVO species

Add time:09/05/2019    Source:sciencedirect.com

High-valent Mn species are key intermediates in the oxygen evolving complex in photosystem II. In some mechanisms, the MnVO moiety is proposed to be a critical species at the final step of oxygen production. This work reports the use of a mechanistic probe 2-methyl-1-phenylpropan-2-yl hydroperoxide (MPPH) to distinguish the formation of MnIVMnIV(OH) and MnIVMnVO species. We demonstrate that a dimeric Mn complex [MnIIIMnIV(2-OH-3,5-diClsalpn)]+ reacts with MPPH, leading to the production of the O–O bond heterolysis product. In this process, the Mn complex transforms into a transient MnIVMnVO species, which undergoes comproportionation rapidly.

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