Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 23, Issue 61, Pages 15370-15376Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201702116
Keywords
hydrogen evolution; organo-functionalization; photocatalysis; polyoxometalate; self-assembly
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Funding
- Deutsche Forschungsgemeinschaft DFG [STR1164/4, INST40-467-1 FUGG]
- DFG Graduate School [GRK1626]
- Ulm University
- EU COST actions [CM1202, CM1203]
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The visible-light-driven hydrogen evolution reaction (HER) by covalent photosensitizer-catalyst dyads is one of the most elegant concepts in supramolecular homogeneous solar energy conversion. The intricacies of catalyst reactivity and photosensitizer-catalyst interactions require a detailed fundamental understanding of the system to rationalize the observed reactivities. Here, we report three dyads based on the covalent imine-bond linkage of an iridium photosensitizer and an organo-functionalized Anderson polyoxometalate anion [MMo6O18{(OCH2)(3)CNH2}(2)](3-) (M=Mn3+, Fe3+, Co3+). Modification of the central metal ion M is used to modulate the HER activity. Detailed theoretical and experimental studies examine the role of the central metal ion M and provide critical understanding of the redox activity and light-driven HER activity of the novel dyads. Thus, the study enables a knowledge-based optimization of HER dyads by chemical modification of the reactive metal oxide components.
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