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Palladium N-Heterocyclic Carbene Complexes: Synthesis from Benzimidazolium Salts and Catalytic Activity in Carbon-carbon Bond-forming Reactions
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Mo Insertion into the H2 Bond in MoS- + H2 Reactions
Ankur K Gupta1, Josey E Topolski1, Kathleen A Nickson1
1Department of Chemistry , Indiana University 800 E. Kirkwood Avenue , Bloomington , Indiana 47405 , United States.
The Journal of Physical Chemistry. A
|August 13, 2019
Summary
This study explores hydrogen reactions with molybdenum sulfide clusters. Subsulfides react via H2 insertion, forming dihydride or tetrahydride products, while hypersulfides lose H2S.
Area of Science:
- Inorganic Chemistry
- Materials Science
- Physical Chemistry
Background:
- Molybdenum sulfide clusters are relevant in catalysis and materials science.
- Understanding their reactivity with small molecules like H2 is crucial for developing new applications.
Purpose of the Study:
- To investigate the reaction mechanisms of small molybdenum sulfide clusters (MoS-) with hydrogen (H2).
- To elucidate the role of cluster composition and oxidation states in H2 reactivity.
Main Methods:
- Combined experimental and computational approaches were employed.
- Reactions of H2 with MoS- clusters of varying stoichiometry (subsulfides and hypersulfides) were studied.
Main Results:
- Subsulfide clusters react with H2 via insertion into the H-H bond, forming dihydride products up to Mo oxidation state +4.
- Clusters with a second reducible metal form tetrahydride products through a second H2 insertion.
- Hypersulfides undergo reduction in the presence of H2, with evidence of H2S molecule loss.
Conclusions:
- The reaction pathways of MoS- clusters with H2 are highly dependent on their sulfide content and metal oxidation states.
- Subsulfides exhibit facile H2 activation and insertion, while hypersulfides show reductive behavior.
- The reactivity of sulfides is comparable to analogous oxosulfides, with minor energetic differences.
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