Previous lecture:

•Chemical catalysis-stabilization of transition state

•Acid-base catalysis, Electrophilic catalysis, Covalent catalysis, Metal ion catalysis

•Importance of pKa values

Today: •Carbonic anhydrase •PLP – mediated catalysis Metal ions as Covalent Catalysts- Carbonic anhydrase

- + CO2 + H2O HCO3 +H Metal ion covalent catalysis- Carbonic anhydrase Metal ion covalent catalysis- Carbonic anhydrase

- + CO2 + H2O HCO3 +H

Coenzyme Catalysis

Coenzyme () small organic molecule or (metal ion) essential to the catalytic action of an Common cofactors: FMN FAD flavin dinucleotide NAD+/NADH adenine dinucleotide NADP+ / NADPH nicotinamide adenine dinucleotide PLP pyridoxal 5’-phosphate PMP 5’-phosphate THF tetrahydrofolate CoASH GSH ATP Pyridoxal Phosphate (PLP) Enzymology

•PLP is the modified form of B6 (pyridoxal) •PLP is a coenzyme heavily involved in transformation reactions •Central to its mechanism is the formation of a Schiff base with the enzyme (through a covalent bond with Lys) •Schiff base is formed through the condensation of an amine with a carbonyl group. •Serves to stabilize carbanion intermediates of amino acids Pyridoxal Phosphate (PLP) Enzymology

PLP most commonly involved in or transamination reactions at the α-Carbon of amino acids

HO O H O OH OH HO O P O

N Me O N Me

PLP Pyridoxal Phosphate (PLP) Enzymology Pyridoxal Phosphate (PLP) Enzymology

•PLP-requiring act via the formation of a planar Schiff base between the amino acid to be modified (substrate) and the coenzyme Pyridoxal Phosphate (PLP) Enzymology •PLP-requiring enzymes act via the formation of a planar Schiff base between the amino acid to be modified (substrate) and the coenzyme •That leads to the formation of a resonance-stabilized carbanion with a quinoid structure •The key to catalysis is the electrophilic nitrogen of the ring - draws electrons away from the substrate and stabilizes the carbanion intermediate (electron sink) Aspartate Aminotransferase active site with PLP

Dr. Jack Kirsch-Berkeley

Next Class

Proximity effect Steady state kinetics