Highly Active Heterogeneous Catalyst for Ethylene Dimerization Prepared by Selectively Doping Ni on the Surface of a Zeolitic Imidazolate Framework
Alalouni, Mohammed R.
Liu, L. M.
KAUST DepartmentAdvanced Membranes and Porous Materials Research Center
Physical Science and Engineering (PSE) Division
Advanced Membranes and Porous Materials Center, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia
KAUST Catalysis Center (KCC)
Chemical Science Program
Imaging and Characterization Core Lab
KAUST Grant NumberBAS/1/1372-01
Embargo End Date2022-04-28
Permanent link to this recordhttp://hdl.handle.net/10754/669062
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AbstractThe production of 1-butene by ethylene dimerization is an important chemical industrial process currently implemented using homogeneous catalysts. Here, we describe a highly active heterogeneous catalyst (Ni-ZIF-8) for ethylene dimerization, which consists of isolating Ni-active sites selectively located on the crystal surface of a zeolitic imidazolate framework. Ni-ZIF-8 can be easily prepared by a simple one-pot synthesis method in which site-specific anchoring of Ni is achieved spontaneously because of the incompatibility between the d<sup>8</sup> electronic configuration of Ni<sup>2+</sup> and the three-dimensional framework of ZIF-8. The full exposure and square-planar coordination of the Ni sites accounts for the high catalytic activity of Ni-ZIF-8. It exhibits an average ethylene turnover frequency greater than 1 000 000 h<sup>-1</sup> (1-butene selectivity >85%) at 35 °C and 50 bar, far exceeding the activities of previously reported heterogeneous catalysts and many homogeneous catalysts under similar conditions. Moreover, compared to molecular Ni complexes used as homogeneous catalysts for ethylene dimerization, Ni-ZIF-8 has significantly higher stability and shows constant activity during 4 h of continuous reaction. Isotopic labeling experiments indicate that ethylene dimerization over Ni-ZIF-8 follows the Cossee-Arlman mechanism, and detailed characterizations combined with density functional theory calculations rationalize this observed high activity.
CitationChen, C., Alalouni, M. R., Dong, X., Cao, Z., Cheng, Q., Zheng, L., … Han, Y. (2021). Highly Active Heterogeneous Catalyst for Ethylene Dimerization Prepared by Selectively Doping Ni on the Surface of a Zeolitic Imidazolate Framework. Journal of the American Chemical Society. doi:10.1021/jacs.1c02272
SponsorsThe financial support for this work was provided by Baseline Funds (BAS/1/1372-01-01) to Y.H. from King Abdullah University of Science and Technology (KAUST). M.R.A would like to acknowledge Saudi Aramco Advanced Degree Program. This research used resources of the Core Laboratories of KAUST. The computational simulations were performed on the KAUST supercomputers.
PublisherAmerican Chemical Society (ACS)
Except where otherwise noted, this item's license is described as This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.1c02272.
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