Journal
ACS CATALYSIS
Volume 9, Issue 6, Pages 5645-5650Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b00721
Keywords
adsorption; host-guest systems; molecular dynamics; agostic interactions; alkene oligomerization; homogeneous catalysis
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Funding
- Research Council of Norway through the OLIGOM project [224980]
- Research Council of Norway through CONFINE project [250795]
- University of Oslo
- European Union's Horizon 2020 research and innovation program [647755 - DYNPOR]
- Research Board of Ghent University (BOF)
- Research Foundation Flanders (FWO)
- FWO [FWO16-PDO-047]
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The active site in ethene oligomerization catalyzed by Ni-zeolites is proposed to be a mobile Ni(II) complex, based on density functional theory-based molecular dynamics (DFT-MD) simulations corroborated by continuous-flow experiments on Ni-SSZ-24 zeolite. The results of the simulations at operating conditions show that ethene molecules reversibly mobilize the active site as they exchange with the zeolite as ligands on Ni during reaction. Microkinetic modeling was conducted on the basis of free-energy profiles derived with DFT-MD for oligomerization on these mobile [(ethene)(2)-Ni-alkyl](+) species. The model reproduces the experimentally observed high selectivity to dimerization and indicates that the mechanism is consistent with the observed second-order rate dependence on ethene pressure.
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