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• W3200501135 abstract "Isolated Ni(II) sites supported on zeolites and other porous materials transform in situ during alkene dimerization to form active Ni(II)-alkyl centers, and their density influences the kinetic orders and mechanisms of deactivation of Ni-Beta zeolites during ethene dimerization (453 K). Ni-Beta containing high Ni site densities shows deactivation rates that are second-order in Ni, consistent with a dual-site deactivation mechanism involving the formation of unreactive Ni-alkyl-Ni intermediates, as confirmed by DFT calculations. Under the same reaction conditions, by contrast, Ni-Beta containing low Ni site densities shows deactivation rates that are first-order in Ni, consistent with a single-site deactivation mechanism reflecting inhibition by strongly bound intermediates derived from heavier alkene oligomers. On Ni-Beta containing low Ni site densities, cofeeding H2 along with ethene results in a higher number of Ni(II)-alkyl intermediates formed at initial reaction times and a concomitant change to deactivation kinetics that become second-order in Ni. These findings reveal the strong influence of the density of active Ni(II)-alkyl centers in porous supports, which depends both on material properties and reaction conditions that generate active centers in situ, on the kinetics and mechanisms of deactivation during alkene oligomerization." @default.
• W3200501135 created "2021-09-27" @default.
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• W3200501135 date "2021-09-13" @default.
• W3200501135 modified "2023-09-23" @default.
• W3200501135 title "Effect of Nickel Active Site Density on the Deactivation of Ni-Beta Zeolite Catalysts during Ethene Dimerization" @default.
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• W3200501135 doi "https://doi.org/10.1021/acsengineeringau.1c00014" @default.
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