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Synthesis of low-molecular weight and branched polyethylenes ethylene polymerization using 9-(arylimino)-5,6,7,8-tetrahydrocyclohepta-pyridylnickel precatalysts.
Dalton Trans
October 2024
Key Laboratory of Engineering Plastics and Beijing National Laboratory for Molecular Science, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
Targeting pour point depressants of low-molecular weight and branched polyethylenes, a series of 9-[2,4-bis(benzhydryl)-6--phenylimino]-5,6,7,8-tetrahydro-cycloheptapyridine-nickel complexes (Ni1-Ni10) were developed as efficient precatalysts. Upon activation with either EASC or MAO, all nickel complex precatalysts exhibited high activity [up to 8.12 × 10 g PE (mol of Ni) h] with single-site behavior toward ethylene polymerization, producing low-molecular weight and unimodal polyethylenes.
View Article and Find Full Text PDFN, N'-bidentate ligand anchored palladium catalysts on MOFs for efficient Heck reaction.
Nat Commun
August 2024
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing National Laboratory of Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210023, Nanjing, PR China.
Metal-organic frameworks (MOFs), recognized as advanced catalyst carriers due to their adjustable porous, diverse structure and highly exposed active sites, have earned increasing attention for their potential to address the longevity of catalytic centers. In this manuscript, we have devised and synthesized a multifunctional amino-pyridine benzoic acid (APBA) ligand to replace the modulator ligand of the MOF-808 and disperse the palladium catalytic centers atomically on the MOF-APBA. The resulting single-site catalytic system, Pd@MOF-APBA, demonstrates preeminent efficiency and stability, as evidenced by a high average turnover number (95000) and a low metal residue (4.
View Article and Find Full Text PDFHighly Active Immobilized Catalyst for Ethylene Polymerization: Neutral Single Site Y(III) Complex Bearing Bulky Silylallyl Ligand.
Chemistry
October 2024
CPE Lyon, CNRS, UMR 5128, Catalysis, Polymerization, Processes and Materials (CP2M), Université Claude Bernard Lyon 1, 43 Bd du 11 Novembre 1918, 69616, Villeurbanne, France.
Exploring the surface organometallic chemistry on silica of highly electrophilic yttrium complexes is a relatively uncommon endeavor, particularly when focusing on tris-alkyl complexes characterized by Y-C σ-alkyl bonds. A drawback with this class of complexes once grafted on silica, is the frequent occurrence of alkyl transfer by ring opening of siloxane groups, resulting in a mixture of species. Herein, we employed a more stable homoleptic yttrium allyl complex bearing bulky η-1,3-bis(trimethylsilyl)allyl ligand to limit this transfer reaction.
View Article and Find Full Text PDFAlkene Isomerization Using a Heterogeneous Nickel-Hydride Catalyst.
J Am Chem Soc
June 2024
Department of Chemistry and Biochemistry, University of Oregon, Eugene, Oregon 97403, United States.
Transition metal-catalyzed alkene isomerization is an enabling technology used to install an alkene distal to its original site. Due to their well-defined structure, homogeneous catalysts can be fine-tuned to optimize reactivity, stereoselectivity, and positional selectivity, but they often suffer from instability and nonrecyclability. Heterogeneous catalysts are generally highly robust but continue to lack active-site specificity and are challenging to rationally improve through structural modification.
View Article and Find Full Text PDFPd-Mn/NC Dual Single-Atomic Sites with Hollow Mesopores for the Highly Efficient Semihydrogenation of Phenylacetylene.
J Am Chem Soc
January 2024
Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China.
Article Synopsis
- The direct pyrolysis of metal-zeolite imidazolate frameworks has been found to be an effective method for creating single-atom catalysts (M/NC-SACs) that perform well in semihydrogenation reactions, particularly for small molecules like acetylene.
- Despite their effectiveness, M/NC-SACs struggle with larger molecules due to poor reactant adsorption and limited molecular movement.
- A newly designed dual single-atom catalyst (h-Pd-Mn/NC) with hollow mesopores showed dramatically improved activity and selectivity for phenylacetylene, achieving 16 times more efficiency than the traditional Lindlar catalyst, thanks to its unique mesopore structure and the effects of atomically dispersed manganese.
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