MoS2 edges have been identified as the active sites for hydrogen evolution reaction (HER) electrocatalysis. Designing molecular mimics of MoS2 edge sites is an attractive strategy to understand the underlying catalytic mechanism of different edge sites and improve their activities. Herein I will discuss our recent progress in this aspect and their applications in dye-sensitized photocatalytic water reduction. The first example is a dimeric molecular analog [Mo2S12]2-, as the smallest unit possessing both the terminal and bridging disulfide ligands (ref. 1). The second example is a group of compounds with the general formular of MoO(S2)2bpy (ref. 2-3). By varying substitution on the bpy ligand, we demonstrate the induction effect on the S—S ligand, thereby tuning the rate constants for HER and overpotentials. At the end, I will present the use of MoS2 molecular analogs coupled with our design of an organic donor−acceptor dye for dye sensitized photocatalytic water reduction (ref. 4). The dye prevents both dye desorption and semiconductor degradation by mimicking the hydrophobic/hydrophilic properties of lipid bilayer membranes. The protection afforded by this membrane-mimicking dye gives this system excellent stability in extremely acidic (pH 0) conditions. The result is of interest to tandem dye-sensitized photoelectrochemical cells (DSPECs) for total water splitting.

Molecular mimics of MoS2 edges for hydrogen-evolution electrocatalysis

256th National Meeting (2018)

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