Synthesis of hybrid transition-metalloproteins via thiol-selective covalent anchoring of Rh-phosphine and Ru-phenanthroline complexes.
The preparation of hybrid transition metalloproteins by thiol-selective incorporation of organometallic rhodium- and ruthenium complexes is described. Phosphine ligands and two rhodium-diphosphine complexes bearing a carboxylic acid group were coupled to the cysteine of PYP R52G, yielding a metalloenzyme active in the rhodium catalyzed hydrogenation of dimethyl itaconate. The successful coupling was shown by (31)P NMR spectroscopy and ESI mass spectroscopy. In addition wild-type PYP (PYP WT), PYP R52G and ALBP were successfully modified with a (eta(6)-arene) ruthenium(II) phenanthroline complex via a maleimide linker.
den Heeten
René
R
Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Nieuwe Achtergracht 166, 1018 WV, Amsterdam, The Netherlands.
Muñoz
Bianca K
BK
Popa
Gina
G
Laan
Wouter
W
Kamer
Paul C J
PC
D019943:Amino Acid Substitution; D001426:Bacterial Proteins / Q000737:chemistry* / Q000235:genetics; D002384:Catalysis; D056831:Coordination Complexes / Q000737:chemistry; D006865:Hydrogenation; D009682:Magnetic Resonance Spectroscopy; D008667:Metalloproteins / Q000138:chemical synthesis* / Q000737:chemistry; D009154:Mutation; D010618:Phenanthrolines / Q000737:chemistry*; D010720:Phosphines / Q000737:chemistry*; D020283:Photoreceptors, Microbial / Q000737:chemistry* / Q000235:genetics; D012238:Rhodium / Q000737:chemistry*; D012428:Ruthenium / Q000737:chemistry*; D013386:Succinates / Q000737:chemistry; D013438:Sulfhydryl Compounds / Q000737:chemistry*
D001426:Bacterial Proteins; D056831:Coordination Complexes; D008667:Metalloproteins; D010618:Phenanthrolines; D010720:Phosphines; D020283:Photoreceptors, Microbial; D013386:Succinates; D013438:Sulfhydryl Compounds; C050162:photoactive yellow protein, Bacteria; C518953:dimethyl itaconate; D012428:Ruthenium; D012238:Rhodium; C044646:phosphine