Generation of the triangulo‐Group MOV‐η‐S2 in the “Condensation” of [MoVIO2S2]2 to [MoO2S2(S2)2]2

Rittner, W.; Müller, Achim; Neumann, Axel; Bäther, Wolfgang; Sharma, Ramesh C.

doi:10.1002/anie.197905301

“…This is in line with earlier results on the dimerization of this anion upon acidification [16], which also postulate formation of water rather than H 2 S:…”

Section: Article In Presssupporting

confidence: 89%

Solution preparation of the amorphous molybdenum oxysulfide MoOS2 and its use for catalysis

Genuit

¹

,

Bezverkhyy

²

,

Afanasiev

³

2005

Journal of Solid State Chemistry

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“…The dimeric nanoclusters, [Mo 2 O 2 ( µ -S) 2 (S 2 )(S x )] 2– (where x = 2 or 4), were synthesised by wet-chemical methods in accordance with the original procedures described by Müller et al 16–18 . The syntheses of both compounds are similar and primarily involve exploiting the thiophilicity of molybdenum by exposing an alkaline molybdate solution to sulfurizing conditions (Supplementary Figure 1).…”

Section: Resultsmentioning

confidence: 99%

“…The [Mo 2 O 2 ( µ -S) 2 (S 2 )(S 4 )] 2– cluster was synthesised in accordance with the published procedure by Müller et al 18 . H 2 S gas was bubbled through a suspension of sulphur (8.0 g, 249.5 mmol) in 50 mL 20% NH 3 at room temperature.…”

Section: Methodsmentioning

confidence: 99%

Tuning and mechanistic insights of metal chalcogenide molecular catalysts for the hydrogen-evolution reaction

McAllister

¹

,

Bandeira

²

,

McGlynn

³

et al. 2019

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The production of hydrogen through water splitting using earth-abundant metal catalysts is a promising pathway for converting solar energy into chemical fuels. However, existing approaches for fine stoichiometric control, structural and catalytic modification of materials by appropriate choice of earth abundant elements are either limited or challenging. Here we explore the tuning of redox active immobilised molecular metal-chalcoxide electrocatalysts by controlling the chalcogen or metal stoichiometry and explore critical aspects of the hydrogen evolution reaction (HER). Linear sweep voltammetry (LSV) shows that stoichiometric and structural control leads to the evolution of hydrogen at low overpotential with no catalyst degradation over 1000 cycles. Density functional calculations reveal the effect of the electronic and structural features and confer plausibility to the existence of a unimolecular mechanism in the HER process based on the tested hypotheses. We anticipate these findings to be a starting point for further exploration of molecular catalytic systems.

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“…, were synthesised by wet-chemical methods in accordance with the original procedures described by Müller et al [16][17][18] . The syntheses of both compounds are similar and primarily involve exploiting the thiophilicity of molybdenum by exposing an alkaline molybdate solution to sulfurizing conditions ( Supplementary Figure 1).…”

Section: Synthesis Of the Molecular Catalysts The Dimeric Nanoclustersmentioning

confidence: 99%

Tuning and Mechanistic Insights of Metal Chalcogenide Molecular Catalysts for the Hydrogen-Evolution Reaction

McAllister,

Miras,

Bandeira

et al. 2019

Meet. Abstr.

0

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The production of hydrogen through water splitting using earth-abundant metal catalysts is a promising pathway for converting solar energy into chemical fuels. However, existing approaches for fine stoichiometric control, structural and catalytic modification of materials by appropriate choice of earth abundant elements are either limited or challenging. Here we explore the tuning of redox active immobilised molecular metal-chalcoxide electrocatalysts by controlling the chalcogen or metal stoichiometry and explore critical aspects of the hydrogen evolution reaction (HER). Linear sweep voltammetry (LSV) shows that stoichiometric and structural control leads to the evolution of hydrogen at low overpotential with no catalyst degradation over 1000 cycles. Density functional calculations reveal the effect of the electronic and structural features and confer plausibility to the existence of a unimolecular mechanism in the HER process based on the tested hypotheses. We anticipate these findings to be a starting point for further exploration of molecular catalytic systems.

show abstract

Generation of the triangulo‐Group MO^V‐η‐S₂ in the “Condensation” of [Mo^VIO₂S₂]² to [MoO₂S₂(S₂)₂]²

Abstract: Formation of the η‐disulfidomolybdenum(V) group by a novel intramolecular redox process has been observed on warming aqueous solutions of dithiomolybdate(VI). The structure of the anion in the orange‐red crystals of (1) was determined by X‐ray methods.

Cited by 40 publications

References 5 publications

Solution preparation of the amorphous molybdenum oxysulfide MoOS2 and its use for catalysis

Solution preparation of the amorphous molybdenum oxysulfide MoOS2 and its use for catalysis

Tuning and mechanistic insights of metal chalcogenide molecular catalysts for the hydrogen-evolution reaction

Tuning and Mechanistic Insights of Metal Chalcogenide Molecular Catalysts for the Hydrogen-Evolution Reaction

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