AI Article Synopsis
- The study investigates small cationic tantalum (Ta) clusters and their reactions with methane using ion-trap experiments and theoretical calculations.
- Smaller Ta clusters (1-4 atoms) efficiently dehydrogenate methane and lose hydrogen, while larger clusters (>4 atoms) only adsorb methane without further reaction.
- A unique behavior of the Ta cation allows it to dehydrogenate up to four methane molecules, potentially forming C-C coupled products, with underlying mechanisms involving interactions between different spin states.
Article Abstract
The energetics of small cationic tantalum clusters and their gas-phase adsorption and dehydrogenation reaction pathways with methane are investigated with ion-trap experiments and spin-density-functional-theory calculations. Ta clusters are exposed to methane under multicollision conditions in a cryogenic ring electrode ion-trap. The cluster size affects the reaction efficiency and the number of consecutively dehydrogenated methane molecules. Small clusters ( = 1-4) dehydrogenate CH and concurrently eliminate H, while larger clusters ( > 4) demonstrate only molecular adsorption of methane. Unique behavior is found for the Ta cation, which dehydrogenates consecutively up to four CH molecules and is predicted theoretically to promote formation of a [Ta(CH-CH-CH)(CH)] product, exhibiting C-C coupled groups. Underlying mechanisms, including reaction-enhancing couplings between potential energy surfaces of different spin-multiplicities, are uncovered.
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| http://dx.doi.org/10.1021/acs.jpca.1c02384 | DOI Listing |
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