[MoO(S2)2L]1-(L = picolinate or pyrimidine-2-carboxylate) Complexes as MoSx-Inspired Electrocatalysts for Hydrogen Production in Aqueous Solution.
Crystalline and amorphous molybdenum sulfide (Mo-S) catalysts are leaders as earth-abundant materials for electrocatalytic hydrogen production. The development of a molecular motif inspired by the Mo-S catalytic materials and their active sites is of interest, as molecular species possess a great degree of tunable electronic properties. Furthermore, these molecular mimics may be important for providing mechanistic insights toward the hydrogen evolution reaction (HER) with Mo-S electrocatalysts. Herein is presented two water-soluble Mo-S complexes based around the [MoO(S2)2L2]1-motif. We present1H NMR spectra that reveal (NEt4)[MoO(S2)2picolinate] (Mo-pic) is stable in a d6-DMSO solution after heating at 100 °C, in air, revealing unprecedented thermal and aerobic stability of the homogeneous electrocatalyst. Both Mo-pic and (NEt4)[MoO(S2)2pyrimidine-2-carboxylate] (Mo-pym) are shown to be homogeneous electrocatalysts for the HER. The TOF of 27-34 s-1and 42-48 s-1for Mo-pic and Mo-pym and onset potentials of 240 mV and 175 mV for Mo-pic and Mo-pym, respectively, reveal these complexes as promising electrocatalysts for the HER.
Department of Chemistry and Biochemistry, The Ohio State University , 100 West 18th Avenue, Columbus, Ohio 43210, United States.
Benjamin R
BR
Garrett
Department of Chemistry and Biochemistry, The Ohio State University , 100 West 18th Avenue, Columbus, Ohio 43210, United States.
Kevin A
KA
Click
Department of Chemistry and Biochemistry, The Ohio State University , 100 West 18th Avenue, Columbus, Ohio 43210, United States.
Christopher B
CB
Durr
Department of Chemistry and Biochemistry, The Ohio State University , 100 West 18th Avenue, Columbus, Ohio 43210, United States.
Christopher M
CM
Hadad
Department of Chemistry and Biochemistry, The Ohio State University , 100 West 18th Avenue, Columbus, Ohio 43210, United States.
Yiying
Y
Wu