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Title: Immobilization of metal complexes on silane-modified silica surfaces

Abstract

This study aims to investigate the immobilization of the metal complexes RhCl[sub 3], NiCl[sub 2], [Rh(CO)[sub 2]Cl][sub 2], CuCl[sub 2], Sn(CH[sub 3])[sub 2]Cl[sub 2], and Pd(CH[sub 3]COO)[sub 2] on the surface of silica which is modified with silylating agents. It also seeks to investigate the activity of silica supported metal complexes as catalysts in hydrogenation reactions. The modification of the silica surface was accomplished by silylation with (CH[sub 3]O)[sub 3]SiCH[sub 2]CH[sub 2]CH[sub 2]Cl or (CH[sub 3]O)[sub 3]SiCH[sub 2]CH[sub 2]CH[sub 2]NHCH[sub 2]CH[sub 2]NH[sub 2]. The silylalkylchloride-modified silica was further reacted with 2,2'-dipyridylamine or pyrazole to afford N-containing ligands bound to the modified silica support. The silane modified silica, N-functionalized silica surfaces, and the ligand silica transition metal complexes were characterized by DRIFT, [sup 13]C CP/MAS NMR, and [sup 29]Si CP/MAS NMR techniques. The composition of the materials were ascertained using SEM, AAS, and elemental analysis. The modification, functionalization, and immobilization procedures involved in this study were utilized to generate a silica supported Rh(I) catalyst, [Silica-(O)[sub 3]-Si(CH[sub 2])[sub 3]DPA]RhCl. The catalytic activity of this silica supported Rh(I) complex towards cyclohexene hydrogenation was determined in this investigation. Silica bound 2,2'-dipyridylamine and pyrazole are found to immobilize a wide range of metal complexes. Themore » Rh(I) complex of Silica-(O)[sub 3]-Si(CH[sub 2])[sub 3] DPA acts as a catalyst and exhibits high activity towards olefin hydrogenation. Only a slightly reduced activity is observed in the presence of substances such as peroxides that are capable of poisoning catalytic materials.« less

Authors:
Publication Date:
Research Org.:
Ohio Univ., Athens, OH (United States)
OSTI Identifier:
7036549
Alternate Identifier(s):
OSTI ID: 7036549
Resource Type:
Miscellaneous
Resource Relation:
Other Information: Thesis (Ph.D.)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; ALKENES; HYDROGENATION; CATALYSTS; CHEMICAL PREPARATION; COPPER COMPLEXES; CATALYTIC EFFECTS; NICKEL COMPLEXES; PALLADIUM COMPLEXES; RHODIUM COMPLEXES; TIN COMPLEXES; CHEMICAL REACTIONS; COMPLEXES; HYDROCARBONS; ORGANIC COMPOUNDS; SYNTHESIS; TRANSITION ELEMENT COMPLEXES 400201* -- Chemical & Physicochemical Properties; 360601 -- Other Materials-- Preparation & Manufacture

Citation Formats

Giron, O.D.C. Immobilization of metal complexes on silane-modified silica surfaces. United States: N. p., 1993. Web.
Giron, O.D.C. Immobilization of metal complexes on silane-modified silica surfaces. United States.
Giron, O.D.C. Fri . "Immobilization of metal complexes on silane-modified silica surfaces". United States.
@article{osti_7036549,
title = {Immobilization of metal complexes on silane-modified silica surfaces},
author = {Giron, O.D.C.},
abstractNote = {This study aims to investigate the immobilization of the metal complexes RhCl[sub 3], NiCl[sub 2], [Rh(CO)[sub 2]Cl][sub 2], CuCl[sub 2], Sn(CH[sub 3])[sub 2]Cl[sub 2], and Pd(CH[sub 3]COO)[sub 2] on the surface of silica which is modified with silylating agents. It also seeks to investigate the activity of silica supported metal complexes as catalysts in hydrogenation reactions. The modification of the silica surface was accomplished by silylation with (CH[sub 3]O)[sub 3]SiCH[sub 2]CH[sub 2]CH[sub 2]Cl or (CH[sub 3]O)[sub 3]SiCH[sub 2]CH[sub 2]CH[sub 2]NHCH[sub 2]CH[sub 2]NH[sub 2]. The silylalkylchloride-modified silica was further reacted with 2,2'-dipyridylamine or pyrazole to afford N-containing ligands bound to the modified silica support. The silane modified silica, N-functionalized silica surfaces, and the ligand silica transition metal complexes were characterized by DRIFT, [sup 13]C CP/MAS NMR, and [sup 29]Si CP/MAS NMR techniques. The composition of the materials were ascertained using SEM, AAS, and elemental analysis. The modification, functionalization, and immobilization procedures involved in this study were utilized to generate a silica supported Rh(I) catalyst, [Silica-(O)[sub 3]-Si(CH[sub 2])[sub 3]DPA]RhCl. The catalytic activity of this silica supported Rh(I) complex towards cyclohexene hydrogenation was determined in this investigation. Silica bound 2,2'-dipyridylamine and pyrazole are found to immobilize a wide range of metal complexes. The Rh(I) complex of Silica-(O)[sub 3]-Si(CH[sub 2])[sub 3] DPA acts as a catalyst and exhibits high activity towards olefin hydrogenation. Only a slightly reduced activity is observed in the presence of substances such as peroxides that are capable of poisoning catalytic materials.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {1993},
month = {1}
}

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