17 publications

17 publications

Addressable DNA–Myoglobin Photocatalysis

Niemeyer, C. M.

Chem. - Asian J., 2009, 10.1002/asia.200900082

A hybrid myoglobin, containing a single‐stranded DNA anchor and a redox‐active ruthenium moiety tethered to the heme center can be used as a photocatalyst. The catalyst can be selectively immobilized on a surface‐bound complementary DNA molecule and thus readily recycled from complex reaction mixtures. This principle may be applied to a range of heme‐dependent enzymes allowing the generation of novel light‐triggered photocatalysts. Photoactivatable myoglobin containing a DNA oligonucleotide as a structural anchor was designed by using the reconstitution of artificial heme moieties containing Ru3+ ions. This semisynthetic DNA–enzyme conjugate was successfully used for the oxidation of peroxidase substrates by using visible light instead of H2O2 for the activation. The DNA anchor was utilized for the immobilization of the enzyme on the surface of magnetic microbeads. Enzyme activity measurements not only indicated undisturbed biofunctionality of the tethered DNA but also enabled magnetic separation‐based enrichment and recycling of the photoactivatable biocatalyst.


Metal: Ru
Ligand type: Bipyridine
Host protein: Myoglobin (Mb)
Anchoring strategy: Supramolecular
Optimization: ---
Reaction: Photooxidation
Max TON: ---
ee: ---
PDB: ---
Notes: Horse heart myoglobin

An Artificial Di-Iron Oxo-Orotein with Phenol Oxidase Activity

DeGrado, W. F.; Lombardi, A.

Nat. Chem. Biol., 2009, 10.1038/nchembio.257

Here we report the de novo design and NMR structure of a four-helical bundle di-iron protein with phenol oxidase activity. The introduction of the cofactor-binding and phenol-binding sites required the incorporation of residues that were detrimental to the free energy of folding of the protein. Sufficient stability was, however, obtained by optimizing the sequence of a loop distant from the active site.


Metal: Fe
Ligand type: Amino acid
Host protein: Due Ferro 1
Anchoring strategy: Dative
Optimization: Genetic
Reaction: Alcohol oxidation
Max TON: >50
ee: ---
PDB: 2KIK
Notes: kcat/KM ≈ 1380 M-1*min-1

Metal: Fe
Ligand type: Amino acid
Host protein: Due Ferro 1
Anchoring strategy: Dative
Optimization: Genetic
Reaction: Amine oxidation
Max TON: ---
ee: ---
PDB: 2KIK
Notes: kcat/KM ≈ 83 M-1*min-1

Artificial Metalloenzymes: Combining the Best Features of Homogeneous and Enzymatic Catalysis

Review

Ward, T. R.

Synlett, 2009, 10.1055/s-0029-1218305


Notes: ---

Artificial Metalloenzymes for Enantioselective Catalysis Based on the Biotin-Avidin Technology

Review

Ward, T. R.

Top. Organomet. Chem., 2009, 10.1007/3418_2008_3


Notes: Book chapter

Artificial Metalloproteins Exploiting Vacant Space: Preparation, Structures, and Functions

Review

Watanabe, Y.

Top. Organomet. Chem., 2009, 10.1007/3418_2008_4


Notes: ---

Design of Functional Metalloproteins

Review

Lu, Y.

Nature, 2009, 10.1038/nature08304


Notes: ---

Directed Evolution of Stereoselective Hybrid Catalysts

Review

Reetz, M. T.

Top. Organomet. Chem., 2009, 10.1007/3418_2008_12


Notes: ---

Incorporation of Biotinylated Manganese-Salen Complexes into Streptavidin: New Artificial Metalloenzymes for Enantioselective Sulfoxidation

Ward, T. R.

J. Organomet. Chem., 2009, 10.1016/j.jorganchem.2008.11.023


Metal: Mn
Ligand type: Oxide; Salen
Host protein: Streptavidin (Sav)
Anchoring strategy: Supramolecular
Optimization: Chemical & genetic
Reaction: Sulfoxidation
Max TON: 28
ee: 13
PDB: ---
Notes: ---

Manganese-Substituted α-Carbonic Anhydrase as an Enantioselective Peroxidase

Review

Kazlauskas, R. J.

Top. Organomet. Chem., 2009, 10.1007/3418_2008_1


Notes: ---

Meso-Unsubstituted Iron Corrole in Hemoproteins: Remarkable Differences in Effects on Peroxidase Activities between Myoglobin and Horseradish Peroxidase

J. Am. Chem. Soc., 2009, 10.1021/ja907428e


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

Metal: Fe
Ligand type: Corrole
Anchoring strategy: Reconstitution
Optimization: ---
Max TON: ---
ee: ---
PDB: ---
Notes: ---

Noncovalent Modulation of pH-Dependent Reactivity of a Mn–Salen Cofactor in Myoglobin with Hydrogen Peroxide

Lu, Y.

Chem. - Eur. J., 2009, 10.1002/chem.200802449


Metal: Mn
Ligand type: Salen
Host protein: Myoglobin (Mb)
Anchoring strategy: Covalent
Optimization: Chemical & genetic
Reaction: Sulfoxidation
Max TON: 4.1
ee: 50
PDB: ---
Notes: Sperm whale myoglobin

Polymerization of Phenylacetylene by Rhodium Complexes within a Discrete Space of apo-Ferritin

Ueno, T.; Watanabe, Y.

J. Am. Chem. Soc., 2009, 10.1021/ja901234j


Metal: Rh
Ligand type: Norbornadiene
Host protein: Ferritin
Anchoring strategy: Dative
Optimization: ---
Max TON: ---
ee: ---
PDB: 2ZUR
Notes: ---

Rational Design of a Structural and Functional Nitric Oxide Reductase

Lu, Y.

Nature, 2009, 10.1038/nature08620


Metal: Fe
Ligand type: Amino acid
Host protein: Myoglobin (Mb)
Anchoring strategy: Dative
Optimization: Genetic
Reaction: NO reduction
Max TON: ~5
ee: ---
PDB: 3K9Z
Notes: Design of a catalytically active non-haem iron-binding site (FeB) in sperm whale myoglobin.

Selective Oxidation of Aromatic Sulfide Catalyzed by an Artificial Metalloenzyme: New Activity of Hemozymes

Mahy, J.-P.

Org. Biomol. Chem., 2009, 10.1039/b907534h


Metal: Fe
Ligand type: Porphyrin
Host protein: Xylanase A (XynA)
Anchoring strategy: Supramolecular
Optimization: ---
Reaction: Sulfoxidation
Max TON: 145
ee: 40
PDB: ---
Notes: ---

Supramolecular Interactions Between Functional Metal Complexes and Proteins

Review

Duhme-Klair, A. K.

Dalton Trans., 2009, 10.1039/b915776j


Notes: ---

The Protein Environment Drives Selectivity for Sulfide Oxidation by an Artificial Metalloenzyme

Cavazza, C.; Ménage, S.

ChemBioChem, 2009, 10.1002/cbic.200800595


Metal: Mn
Ligand type: Salen
Anchoring strategy: Supramolecular
Optimization: Chemical
Reaction: Sulfoxidation
Max TON: 97
ee: ---
PDB: ---
Notes: ---

Various Strategies for Obtaining Artificial Hemoproteins: From "Hemoabzymes" to "Hemozymes"

Mahy, J.-P.

Biochimie, 2009, 10.1016/j.biochi.2009.03.002


Metal: Fe
Ligand type: Porphyrin
Host protein: Xylanase A (XynA)
Anchoring strategy: Supramolecular
Optimization: Chemical
Reaction: Sulfoxidation
Max TON: ---
ee: 36
PDB: ---
Notes: ---