Lulu Song, Long Chen, Junfen Sun, Le Wang*, Mingyuan Li* and Zhengguo Cai*,
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MOF-Supported Diimine Nickel Catalyst for Highly Active and Selective Ethylene Dimerization
Selective oligomerization of ethylene remains one of the most significant industrial processes, but it is still dominated by homogeneous catalysis. Herein, we report the synthesis of a heterogeneous α-diimine nickel catalyst (diimine-Ni@PCN-701) through ligand insertion into the Zr-based MOF (PCN-700) framework, affording single-site nickel active sites that are free of steric encumbrances. Diimine-Ni@PCN-701 achieves significant 1-butene selectivity (up to 97.3%) while keeping a considerable turnover frequency (TOF) of 43,800 h–1. This dimerization behavior stems from the electron density of the nickel center induced by the remotely bound Zr (IV) cluster with a carboxylate group on the diimine ligand, as can be analyzed and verified through atomic charge calculation and DFT calculations.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.