期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 41, 页码 13726-13731出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b08652
关键词
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资金
- NSF Chemistry Catalysis Program of the Chemistry Division [CHE-1566106]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1566106] Funding Source: National Science Foundation
Crystalline and amorphous molybderiimi 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(S-2)(2)L-2](1-) motif We present H-1 NMR spectra that reveal (NEt4)[MoO(S-2)(2)picolinate] (Mo-pic) is stable in a d(6)-DMSO Solution after heating at 100 degrees C, in air, revealing unprecedented thermal and aerobic stability of the homogeneous electrocatalyst. Both Mo-pic and (NEt4)[MoO(S-2)(2)pyrimidine-2-carboxylate] (Mo-pym) are shown to be homogeneous electrocatalysts for the HER. The TOF of 27-34 s(-1) and 42-48 s(-1) for 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.
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