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Synthesis And Catalytic Borrowing Hydrogen Reaction Of Ruthenium Complexes With N^N Ligand

Posted on:2020-01-15Degree:MasterType:Thesis
Country:ChinaCandidate:Y Z ZhangFull Text:PDF
GTID:2381330590473652Subject:Chemical Engineering
Abstract/Summary:PDF Full Text Request
Organic ruthenium compounds are important research fields in metal organic chemistry,and metal ruthenium compounds of N^N ligands have been the focus of research in recent years.Most of the metal ruthenium compounds with N^N ligands contain a pyridyl group,because the nitrogen atom of the pyridyl group has a strong coordination ability with the center of the ruthenium atom,and the obtained metal ruthenium compound is relatively stable.Therefore,N^N metal ruthenium compounds having a pyridyl group are widely used in various catalytic reactions,and great progress has been made in related fields.A series of pyridine ligands containing N^N were synthesized and coordinated with the corresponding lanthanum source to obtain a series of metal ruthenium compounds containing N^N ligands.The ring-forming reaction of o-aminobenzyl alcohol and aromatic ketone with the obtained metal ruthenium compound,and the?-alkylation reaction of benzyl alcohol and acetophenone were used as hydrogen borrowing catalytic studies.The main content of this paper includes the following three parts:?1?A hydroxy-substituted rigid bipyridyl ligand 1 and a flexible bidentate pyridine ligand 2-4 substituted with different substituents were synthesized.Using[RuCl2?p-cymene?]2?p-cymene=?-phellandene?as a ruthenium source,N^N coordination with a pyridyl ligand gave the corresponding metal ruthenium compounds 5?6?7 and 8.The structural characteristics of these metal ruthenium compounds containing N^N ligands were discussed and analyzed.?2?A series of metal ruthenium compounds containing N^N ligands were used to catalyze the ring formation reaction of o-aminobenzyl alcohol and acetophenone.The optimum reaction conditions based on the optimum catalyst of compound 7were determined.Substrate expansion of the acetophenone derivative was carried out using the selected compound 7.At the same time,the possible mechanism of the reaction was studied and speculated.?3?A series of metal ruthenium compounds containing N^N ligands were also used to catalyze the?-alkylation reaction of benzyl alcohol and acetophenone.It was confirmed that the compound 7 was the catalyst with the best catalytic effect,and the best catalytic conditions were screened.The benzyl alcohol and acetophenone derivatives containing different substituents were used to expand the substrate,and the catalytic mechanism was speculated.In this dissertation,four unknown compounds and four new organometallic compounds were synthesized.The composition and structure of all the compounds were characterized by 1H NMR?31P NMR?13C NMR?etc.,and the precise structure of compound 6 was determined by X-ray single crystal diffraction.
Keywords/Search Tags:N^N ligand, ruthenium complex, hydrogen reaction, ?-alkylation, ring formation reaction
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