ABSTRACT Molecular molybdenum sulfides, or thiomolybdates, are well‐established noble‐metal free molecular catalysts for the hydrogen evolution reaction (HER). To‐date, there is a knowledge‐gap regarding the impact of organo‐functionalization on reactivity, stability and heterogenization of this compound class. Here, we report the development of synthetic routes for controlled introduction of organic N‐donor ligands as a first step toward establishing structure‐property‐reactivity relationships in this new compound class. Photophysical studies combined with computational modelling are used to rationalize trends in the observed light‐driven homogeneous HER activity. This work lays the foundation to develop organo‐functionalized thiomolybdate HER catalysts suitable for covalent or supramolecular linkage to photosensitizers and for anchoring on heterogeneous supports, e.g. photocathodes.
Jahn et al. (Sat,) studied this question.
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