8 publications

8 publications

Artificial Metalloenzymes for Enantioselective Catalysis: The Phenomenon of Protein Accelerated Catalysis

Ward, T. R.

J. Organomet. Chem., 2004, 10.1016/j.jorganchem.2004.09.032


Metal: Rh
Host protein: Streptavidin (Sav)
Anchoring strategy: Supramolecular
Optimization: Chemical
Reaction: Hydrogenation
Max TON: ---
ee: 94
PDB: ---
Notes: Reduction of acetamidoacrylic acid. 3.0-fold protein acceleration.

Metal: Rh
Host protein: Avidin (Av)
Anchoring strategy: Supramolecular
Optimization: Chemical
Reaction: Hydrogenation
Max TON: ---
ee: 39
PDB: ---
Notes: Reduction of acetamidoacrylic acid. 12.0-fold protein acceleration.

Artificial Metalloenzymes: (Strept)avidin as Host for Enantioselective Hydrogenation by Achiral Biotinylated Rhodium-Diphosphine Complexes

Ward, T. R.

J. Am. Chem. Soc., 2004, 10.1021/ja0476718


Metal: Rh
Ligand type: Phosphine
Host protein: Streptavidin (Sav)
Anchoring strategy: Supramolecular
Optimization: Chemical & genetic
Reaction: Hydrogenation
Max TON: ---
ee: 94
PDB: ---
Notes: ---

A Site-Selective Dual Anchoring Strategy for Artificial Metalloprotein Design

Lu, Y.

J. Am. Chem. Soc., 2004, 10.1021/ja046908x

Introducing nonnative metal ions or metal-containing prosthetic groups into a protein can dramatically expand the repertoire of its functionalities and thus its range of applications. Particularly challenging is the control of substrate-binding and thus reaction selectivity such as enantioselectivity. To meet this challenge, both non-covalent and single-point attachments of metal complexes have been demonstrated previously. Since the protein template did not evolve to bind artificial metal complexes tightly in a single conformation, efforts to restrict conformational freedom by modifying the metal complexes and/or the protein are required to achieve high enantioselectivity using the above two strategies. Here we report a novel site-selective dual anchoring (two-point covalent attachment) strategy to introduce an achiral manganese salen complex (Mn(salen)), into apo sperm whale myoglobin (Mb) with bioconjugation yield close to 100%. The enantioselective excess increases from 0.3% for non-covalent, to 12.3% for single point, and to 51.3% for dual anchoring attachments. The dual anchoring method has the advantage of restricting the conformational freedom of the metal complex in the protein and can be generally applied to protein incorporation of other metal complexes with minimal structural modification to either the metal complex or the protein.


Metal: Mn
Ligand type: Salen
Host protein: Myoglobin (Mb)
Anchoring strategy: Covalent
Optimization: Genetic
Reaction: Sulfoxidation
Max TON: 3.9
ee: 51
PDB: 1MBO
Notes: Sperm whale myoglobin

De Novo Design of Catalytic Proteins

DeGrado, W. F.

Proc. Natl. Acad. Sci. U. S. A., 2004, 10.1073/pnas.0404387101


Metal: Fe
Ligand type: Amino acid
Host protein: Due Ferro 1
Anchoring strategy: Dative
Optimization: Genetic
Reaction: Alcohol oxidation
Max TON: >100
ee: ---
PDB: ---
Notes: kcat/KM ≈ 1540 M-1*min-1

Hybridization of Modified-Heme Reconstitution and Distal Histidine Mutation to Functionalize Sperm Whale Myoglobin

J. Am. Chem. Soc., 2004, 10.1021/ja038798k


Metal: Fe
Host protein: Myoglobin (Mb)
Anchoring strategy: Reconstitution
Optimization: Genetic
Max TON: ---
ee: ---
PDB: ---
Notes: ---

Metal-Assembled Modular Proteins: Toward Functional Protein Design

Review

Case, M. A.

Acc. Chem. Res., 2004, 10.1021/ar960245+


Notes: ---

New Activities of a Catalytic Antibody with a Peroxidase Activity: Formation of Fe(II)–RNO Complexes and Stereoselective Oxidation of Sulfides

Mahy, J.-P.

Eur. J. Biochem., 2004, 10.1111/j.1432-1033.2004.04032.x


Metal: Fe
Ligand type: Porphyrin
Host protein: Antibody 3A3
Anchoring strategy: Supramolecular
Optimization: ---
Reaction: Sulfoxidation
Max TON: 82
ee: 45
PDB: ---
Notes: ---

Peroxidase Activity of Cationic Metalloporphyrin-Antibody Complexes

Harada, A.

Chem. - Eur. J., 2004, 10.1002/chem.200305692


Metal: Fe
Ligand type: Porphyrin
Host protein: Antibody 12E11G
Anchoring strategy: Antibody
Optimization: ---
Max TON: ---
ee: ---
PDB: ---
Notes: ---