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- W2892707754 endingPage "201" @default.
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- W2892707754 abstract "A study of reactions between a distribution of 98MoxSy- clusters ranging from sub-sulfide (x ∼ y) to hypersulfide (y > 2x) is presented, compared with previous studies on homologous MoxOz- clusters, and analyzed with supporting computational studies of the reaction free energy pathways, giving insights into the molecular scale interactions involved in the electro- or photocatalytically driven hydrogen evolution reaction. First, reactions between MoxSy- clusters with water are approximately an order of magnitude slower than reactions between oxides with water, an effect attributed to longer-range repulsion between the cluster anions and water. However, sequential oxidation of the MoxSy- clusters, which generates oxosulfides and H2, is observed for several species. Evidence of oxidation of several hypersulfides with H2 evolution is also observed, indicating that oxidation of S2 groups is also possible. Based on the computational results on several of the bimetallic species, oxidation of the subsulfide Mo2S2− and Mo2S3− clusters is barrierless, while oxidation of the nascent Mo2S2O- cluster formed by oxidation of Mo2S2− is low-barrier. The stoichiometric Mo2S4- + H2O free energy path is predicted to have a modest barrier to the dissociative addition of water, which is consistent with the experimental observation of both oxidation (with H2 production) and water addition reactions. Calculations on the reaction free energy pathways of the oxosulfide species suggest that the formation of two dihydroxide groups, rather than a thiol and hydroxide group, is favored. Oxidation of the oxides is more thermodynamically favored than oxidation of sulfide analogs." @default.
- W2892707754 created "2018-10-05" @default.
- W2892707754 creator A5011183754 @default.
- W2892707754 creator A5020120688 @default.
- W2892707754 creator A5021590110 @default.
- W2892707754 creator A5039602411 @default.
- W2892707754 creator A5086381247 @default.
- W2892707754 date "2018-11-01" @default.
- W2892707754 modified "2023-09-23" @default.
- W2892707754 title "Hydrogen evolution from water reactions with molybdenum sulfide cluster anions" @default.
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