Immobilized Complexes of Metals with Amino Acid Ligands − A First Step toward the Development of New Biomimetic Catalysts

Luechinger, Marco; Kienhöfer, and Alexander; Pirngruber, Gerhard D.

doi:10.1021/cm052130i

Cited by 33 publications

(28 citation statements)

References 31 publications

(44 reference statements)

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“…The observed increase in regioselectivity, together with the increased activity, could be dependent on the complexation of the Lewis basic substrate onto the Lewis acidic zirconia wall. Pirngruber and coworkers immobilized the histidine and glutamic acid residues on the surface of mesoporous silica supports to construct an Fe(II) complex as a biomimetic catalyst [213]. The biomimetic iron complexes obtained were tested as catalysts for cyclohexane oxidation under mild reaction conditions with hydrogen peroxide as oxidant.…”

Section: Advanced Functions Of Nanohybrids Of Biomolecules and Mesopomentioning

confidence: 99%

Immobilization of Biomolecules on Mesoporous Structured Materials

Vinu

Gokulakrishnan

Mori

et al. 2007

Bio‐inorganic Hybrid Nanomaterials

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Various functional systems have been developed using artificially constructed structures and synthesized compounds, and the nanotechnology based on them has recently received much attention. However, current nanoscale technologies are still highly inferior to those seen in natural systems. The efficiency of the energy conversion that occurs in mitochondrial and photosynthetic systems far exceeds that obtained in artificial systems. A dog can smell and a bat can hear far more sensitively than most artificial sensors. The information processing exhibited by the brain and nervous systems is much more sophisticated than that exhibited by current computers. Nature developed superior nanotechnologies to our own several billion years ago. Therefore, the use of biomaterials for the development of various functional systems can be a very practical approach to reaching several goals in current nanotechnologies.Unfortunately, biomolecules in most cases give their best performance under ambient conditions and are not mechanically and thermally strong enough to be used in harsh conditions. In order to overcome such difficulties, hybridization of biomolecules with supporting materials such as lipid assemblies, polymers and inorganic materials has been proposed to attain both biological functions and mechanical stability . Biomolecules are frequently immobilized on silica supports through a sol-gel process. As advanced silica structures, mesoporous silica molecular sieves and related materials have received much attention as inorganic supports for biomolecules [31][32][33][34][35][36][37][38][39][40]. Mesoporous silica materials are chemically and mechanically stable and resistant to microbial attack. In addition, chemical modification to introduce organic functional groups to the inner silica pore wall is highly possible. Outstanding properties of the mesoporous structure also lie in their high specific surface area and huge specific pore volume, which are definitely advantageous for the efficient accommodation of biomolecules. In addition, the narrow pore size distribution could provide reliable immobilization of biomolecules. According to the j113 Bio-inorganic Hybrid Nanomaterials. Edited

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Section: Advanced Functions Of Nanohybrids Of Biomolecules and Mesopomentioning

confidence: 99%

Immobilization of Biomolecules on Mesoporous Structured Materials

Vinu

Gokulakrishnan

Mori

et al. 2007

Bio‐inorganic Hybrid Nanomaterials

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“…Recently, the immobilization of homogeneous catalysts has attracted increasing interest. [14][15][16][17][18][19] The most widely used support matrices belong to the M41S family of materials, which have very large surface areas ( % 1000 m 2 g…”

Section: Introductionmentioning

confidence: 99%

Mononuclear–Dinuclear Equilibrium of Grafted Copper Complexes Confined in the Nanochannels of MCM‐41 Silica

Zhang

Lam

Albela

et al. 2011

Chemistry A European J

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Following the structural concept of copper-containing proteins in which dinuclear copper centers are connected by hydroxide bridging ligands, a bidentate copper(II) complex has been incorporated into nano-confined MCM-41 silica by a multistep sequential grafting technique. Characterization by a combination of EPR spectroscopy, X-ray photoelectron spectroscopy (XPS), UV/Vis spectroscopy, IR spectroscopy , and solid-state (13)C and (29)Si cross-polarization magic-angle spinning (CP-MAS) NMR suggests that dinuclear Cu complexes are bridged by hydroxide and other counterions (chloride or perchlorate ions), similar to the situation for EPR-undetectable [Cu(II)···Cu(II)] dimer analogues in biological systems. More importantly, a dynamic mononuclear-dinuclear equilibrium between different coordination modes of copper is observed, which strongly depends on the nature of the counterions (Cl(-) or ClO(4)(-)) in the copper precursor and the pore size of the silica matrix (the so-called confinement effect). A proton-transfer mechanism within the hydrogen-bonding network is suggested to explain the dynamic nature of the dinuclear copper complex supported on the MCM-41 silica.

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“…Previously, numerous homogeneous and heterogeneous [2][3][4][5] bioinspired mimics have been synthetised and applied for the oxidation of organic molecules. In these biomimetic catalysts redox-active transition metal ions may be used as the central ion, while amino acids or other molecules, having groups that are able to coordinate to it, as ligands [6].…”

Section: Introductionmentioning

confidence: 99%

Synthesis, structural characterisation, and catalytic activity of Mn(II)–protected amino acid complexes covalently immobilised on chloropropylated silica gel

et al. 2015

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In this work the syntheses, structure, superoxide dismutase (SOD) activity and the catalytic use in the oxidative transformations of cyclohexene of covalently grafted Mn(II)−complexes formed with various C-protected amino acid (L-histidine, L-cysteine and L-cystine) ligands is presented. The structural features of the surface complexes were studied by EPR, X-ray absorption, and mid/far IR spectroscopies. The superoxide dismutase activities of the materials were determined in a biochemical test reaction. The obtained materials were used as catalysts for the oxidation of cyclohexene with peracetic acid in acetone. Covalent grafting and building the complex onto the surface of the chloropropylated silica gel were successful in all cases. It was found that in many instances the structures obtained and the coordinating groups substantially varied upon changing the conditions of the syntheses. All the covalently immobilised Mn(II)-complexes displayed superoxide dismutase activity and could catalyse the oxidation of cyclohexene.

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Immobilized Complexes of Metals with Amino Acid Ligands − A First Step toward the Development of New Biomimetic Catalysts

Cited by 33 publications

References 31 publications

Immobilization of Biomolecules on Mesoporous Structured Materials

Immobilization of Biomolecules on Mesoporous Structured Materials

Mononuclear–Dinuclear Equilibrium of Grafted Copper Complexes Confined in the Nanochannels of MCM‐41 Silica

Synthesis, structural characterisation, and catalytic activity of Mn(II)–protected amino acid complexes covalently immobilised on chloropropylated silica gel

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