Molecular Biochemistry II Amino Acid Catabolism: Carbon Skeletons Copyright © 1999-2007 by Joyce J. Diwan. All rights reserved. Amino Acid Carbon Skeletons Amino acids, when deaminated, yield a-keto acids that, directly or via additional reactions, feed into major metabolic pathways (e.g., Krebs Cycle). Amino acids are grouped into 2 classes, based on whether or not their carbon skeletons can be converted to glucose: glucogenic ketogenic. Carbon skeletons of glucogenic amino acids are degraded to: pyruvate, or a 4-C or 5-C intermediate of Krebs Cycle. These are precursors for gluconeogenesis. Glucogenic amino acids are the major carbon source for gluconeogenesis when glucose levels are low. They can also be catabolized for energy, or converted to glycogen or fatty acids for energy storage. Carbon skeletons of ketogenic amino acids are degraded to: acetyl-CoA, or acetoacetate. Acetyl CoA, & its precursor acetoacetate, cannot yield net production of oxaloacetate, the gluconeogenesis precursor. For every 2-C acetyl residue entering Krebs Cycle, 2 C leave as CO2. Carbon skeletons of ketogenic amino acids can be catabolized for energy in Krebs Cycle, or converted to ketone bodies or fatty acids. They cannot be converted to glucose. CH3 HC COO COO CH2 CH2 CH2 NH3+ COO alanine + C CH3 O COO C CH2 O COO + HC NH3+ COO a-ketoglutarate pyruvate glutamate Aminotransferase (Transaminase) The 3-C a-keto acid pyruvate is produced from alanine, cysteine, glycine, serine, & threonine. Alanine deamination via Transaminase directly yields pyruvate. + H2O NH4 H2O HO CH2 H C COO NH3+ serine H2C C COO O H3C C COO NH3+ aminoacrylate pyruvate Serine Dehydratase Serine is deaminated to pyruvate via Serine Dehydratase. Glycine, which is also product of threonine catabolism, is converted to serine by a reaction involving tetrahydrofolate (to be discussed later). COO COO COO CH2 COO CH2 CH2 CH2 CH2 CH2 HC NH3+ COO + C O COO C O COO + HC NH3+ COO aspartate a-ketoglutarate oxaloacetate glutamate Aminotransferase (Transaminase) The 4-C Krebs Cycle intermediate oxaloacetate is produced from aspartate & asparagine. Aspartate transamination yields oxaloacetate. Aspartate is also converted to fumarate in Urea Cycle. Fumarate is converted to oxaloacetate in Krebs cycle. H2N O H2O NH4+ COO C CH2 HC CH2 NH3+ HC COO asparagine NH3+ COO aspartate Asparaginase Asparagine loses the amino group from its R-group by hydrolysis catalyzed by Asparaginase. This yields aspartate, which can be converted to oxaloacetate, e.g., by transamination. The 4-C Krebs Cycle intermediate succinyl-CoA is produced from isoleucine, valine, & methionine. Propionyl-CoA, an intermediate on these pathways, is also a product of b-oxidation of fatty acids with an odd number of C atoms. The branched chain amino acids initially share in part a common pathway. Branched Chain a-Keto Acid Dehydrogenase (BCKDH) is a multi-subunit complex homologous to Pyruvate Dehydrogenase complex. Genetic deficiency of BCKDH is called Maple Syrup Urine Disease (MSUD). High concentrations of branched chain keto acids in urine give it a characteristic odor. Propionyl-CoA Methylmalonyl-CoA Carboxylase (Biotin) Racemase H HCO 3 H C CH3 C S-CoA O COO H ATP ADP + Pi propionyl-CoA C CH3 C S-CoA O H Methylmalonyl-CoA Mutase (B12) H COO C C H H C S-CoA H COO H C C CoA-S C H O D-methylmalonyl-CoA L-methylmalonyl-CoA H O succinyl-CoA Propionyl-CoA is carboxylated to methylmalonyl-CoA. A racemase yields the L-isomer essential to the subsequent reaction. Methylmalonyl-CoA Mutase catalyzes a molecular rearrangement: the branched C chain of methylmalonyl-CoA is converted to the linear C chain of succinyl-CoA. The carboxyl that is in ester linkage to the thiol of coenzyme A is shifted to an adjacent carbon atom, with opposite shift of a hydrogen atom. SH CH2 b-mercaptoethylamine CH2 NH C O CH2 pantothenate CH2 Recall that coenzyme A is a large molecule. NH C NH2 O HO C H H3C C CH3 O H2C O N N P O O O P N N O CH2 O O H H O H OH H ADP-3'-phosphate Coenzyme A O P O O H Methylmalonyl-CoA Mutase (B12) H COO C C H H C S-CoA O L-methylmalonyl-CoA H COO H C C CoA-S C H H O succinyl-CoA Coenzyme B12, a derivative of vitamin B12 (cobalamin), is the prosthetic group of Methylmalonyl-CoA Mutase. Two views of coenzyme B12 Co dimethylbenzimidazole corrin ring PDB 1REQ A crystal structure of the enzyme-bound coenzyme B12. Coenzyme B12 contains a heme-like corrin ring with a cobalt ion coordinated to 4 ring N atoms. Two views of coenzyme B12 More diagrams in NIH website & U. Bristol website. Co corrin ring Within the active site, the Co atom of coenzyme B12 has 2 axial dimethylbenzimidazole PDB 1REQ ligands: methyl C atom of 5'-deoxyadenosine (not shown). an enzyme histidine N When B12 is free in solution, a ring N of the dimethylbenzimidazole serves as axial ligand to the cobalt. When B12 is enzyme-bound, a His side-chain N substitutes for the dimethylbenzimidazole. Homolytic cleavage of the deoxyadenosyl C-Co bond during catalysis yields a deoxyadenosyl carbon radical, as Co3+ becomes Co2+. Reaction of this with methylmalonyl-CoA generates a radical substrate intermediate and 5'-deoxyadenosine. Following rearrangement of the substrate, the product radical abstracts a H atom from the methyl group of 5'-deoxyadenosine. This yields succinyl-CoA and the 5'-deoxyadenosyl radical, which reacts with coenzyme B12 to reestablish the deoxyadenosyl C-Co bond. Methyl group transfers are also carried out by B12 (cobalamin). Methyl-B12 (methylcobalamin), with a methyl axial ligand substituting for the deoxyadenosyl moiety of coenzyme B12, is an intermediate of such transfers. E.g., B12 is a prosthetic group of the mammalian enzyme that catalyzes methylation of homocysteine to form methionine (to be discussed later). Vitamin B12 is synthesized only by bacteria. Ruminants get B12 from bacteria in their digestive system. Humans obtain B12 from meat or dairy products. Vitamin B12 bound to the protein gastric intrinsic factor is absorbed by cells in the upper part of the human small intestine via receptor-mediated endocytosis. B12 synthesized by bacteria in the large intestine is unavailable. Strict vegetarians eventually become deficient in B12 unless they consume it in pill form. Vitamin B12 is transported in the blood bound to the protein transcobalamin, which is recognized by a receptor that mediates uptake into body cells. SH Two views of coenzyme B12 CH2 corrin ring Co b-mercaptoethylamine CH2 NH C O CH2 pantothenate CH2 NH dimethylbenzimidazole PDB 1REQ Explore via Chime Methylmalonyl-CoA Mutase with its prosthetic group, Coenzyme B12. Desulfo-CoA (without the thiol) is at the active site. C NH2 O HO C H H3C C CH3 O H2C O N N P O O O P N N O CH2 O O H H O H OH H ADP-3'-phosphate O Coenzyme A The deoxyadenosyl moiety is lacking in the crystal. P O O COO COO COO CH2 COO CH2 CH2 CH2 CH2 CH2 HC NH3+ COO + C O COO C O COO + HC NH3+ COO aspartate a-ketoglutarate oxaloacetate glutamate Aminotransferase (Transaminase) The 5-C Krebs Cycle intermediate a-ketoglutarate is produced from arginine, glutamate, glutamine, histidine, & proline. Glutamate deamination via Transaminase directly yields a-ketoglutarate. H2 H2 OOC C C glutamate NH3+ C H COO NAD(P)+ NAD(P)H O H2 H2 OOC C C a-ketoglutarate C COO + NH4+ Glutamate Dehydrogenase Glutamate deamination by Glutamate Dehydrogenase also directly yields a-ketoglutarate. H2 N N H N H Tetrahydrofolate (THF) H HN N H O pteridine H CH2 HN COO O C -aminobenzoate N H C H C C COO H2 H 2 glutamate Histidine is first converted to glutamate. The last step in this pathway involves the cofactor tetrahydrofolate. Tetrahydrofolate (THF), which has a pteridine ring, is a reduced form of the B vitamin folate. Within a cell, THF has an attached chain of several glutamate residues, linked to one another by isopeptide bonds involving the R-group carboxyl. THF exists in various forms, with single-C units, of varying oxidation state, bonded at N5 or N10, or bridging between them. In these diagrams N10 with R is -aminobenzoic acid, linked to a chain of glutamate residues. The cellular pool of THF includes various forms, produced and utilized in different reactions. H2N N H N H H HN N5 H H 10N O Tetrahydrofolate (THF) H2N N CH2 H N R H H H HN N5 H O N5-Methyl-THF CH2 CH3 10N H R H H2N H N N H H HN N5 H O C HN H CH2 10N R H N5-formimino-THF N5-formimino-THF is involved in the pathway for degradation of histidine. Reactions using THF as donor of a single-C unit include synthesis of thymidylate, methionine, f-methionine-tRNA, etc. HC C N CH2 COO NH3+ NH C H In the pathway of histidine degradation, N-formiminoglutamate is converted to glutamate by transfer of the formimino group to THF, yielding N5-formimino-THF. H C histidine NH4+ H2O H2O H C OOC HN CH2 CH2 COO N-formiminoglutamate NH C H THF N 5-formimino-THF OOC H C CH2 NH3+ CH2 COO glutamate H2N N H N H H HN N5 H H O Tetrahydrofolate (THF) CH2 10 N R H Because of the essential roles of THF as acceptor and donor of single carbon units, dietary deficiency of folate, genetic deficiencies in folate metabolism or transport, and the increased catabolism of folate seen in some disease states, result in various metabolic effects leading to increased risk of developmental defects, cardiovascular disease, and cancer. Aromatic Amino Acids Aromatic amino acids phenylalanine & tyrosine are catabolized to fumarate and acetoacetate. Hydroxylation of phenylalanine to form tyrosine involves the reductant tetrahydrobiopterin. Biopterin, like folate, has a pteridine ring. Dihydrobiopterin is reduced to tetrahydrobiopterin by electron transfer from NADH. Thus NADH is secondarily the e donor for conversion of phenylalanine to tyrosine. NH3+ CH2 CH COO phenylalanine Phenylalanine Hydroxylase O2 + tetrahydrobiopterin H2O + dihydrobiopterin NH3+ HO CH2 CH COO tyrosine Overall the reaction is considered a mixed function oxidation, because one O atom of O2 is reduced to water while the other is incorporated into the amino acid product. 7,8-dihydrobiopterin Phenylalanine Hydroxylase includes a non-heme iron atom at its active site. X-ray crystallography has shown the following are ligands to the iron atom: His N, Glu O & water O. (Fe shown in spacefill & ligands in ball & stick). Glu His His PDB 1DMW Phenylalanine Hydroxylase O2, tetrahydrobiopterin, and the iron atom in the ferrous (Fe++) oxidation state participate in the hydroxylation. O2 is thought to react initially with the tetrahydrobiopterin to form a peroxy intermediate. Genetic deficiency of Phenylalanine Hydroxylase leads to the disease phenylketonuria. Transaminase Phenylalanine Phenylpyruvate (Phenylketone) Phenylalanine Deficient in Hydroxylase Phenylketonuria Tyrosine Melanins Phenylalanine & Multiple Reactions phenylpyruvate (the product of Fumarate + Acetoacetate phenylalanine deamination via transaminase) accumulate in blood & urine. Mental retardation results unless treatment begins immediately after birth. Treatment consists of limiting phenylalanine intake to levels barely adequate to support growth. Tyrosine, an essential nutrient for individuals with phenylketonuria, must be supplied in the diet. Transaminase Phenylalanine Phenylpyruvate (Phenylketone) Phenylalanine Deficient in Hydroxylase Phenylketonuria Tyrosine Melanins Multiple Reactions Fumarate + Acetoacetate Tyrosine is a precursor for synthesis of melanins and of epinephrine and norepinephrine. High [phenylalanine] inhibits Tyrosine Hydroxylase, on the pathway for synthesis of the pigment melanin from tyrosine. Individuals with phenylketonuria have light skin & hair color. H3C H3C S H2 C methionine H2 H C C COO NH3+ H2 H2 H C C C + S CH2 NH3+ Adenine O ATP PPi + Pi H H H OH H OH N5-methyl-THF methylated acceptor adenosine H2O H2 H2 H C C C homocysteine S-adenosylmethionine (SAM) acceptor THF HS COO COO H2 H2 H C C C S CH2 NH3+ Adenine O NH3+ H COO H H OH H OH S-adenosylhomocysteine Methionine S-Adenosylmethionine by ATP-dependent reaction. SAM is a methyl group H 3C donor in synthetic reactions. The resulting S-adenosylhomocysteine is hydrolyzed to homocysteine. Homocysteine may be catabolized via a complex pathway to cysteine & succinyl-CoA. adenosine H2O HS C H2 C H2 H C COO + S H C C C H2 H2 CH2 NH3+ Adenine O H COO H H OH H OH S-adenosylmethionine (SAM) acceptor methylated acceptor S CH2 C H2 C H2 homocysteine H COO NH3+ Adenine O NH3+ H C S-adenosylH homocysteine H H OH OH Or methionine may be regenerated from homocysteine by H3C S C H2 methyl transfer from N5-methyl-tetrahydrofolate, methionine via a methyltransferase enzyme that uses B12 as THF prosthetic group. N5-methyl-THF The methyl group is transferred from THF to B12 to homocysteine. Another pathway converts homocysteine to glutathione. HS C H2 C C H2 H2 H C COO NH3+ H C COO NH3+ homocysteine H 3C + S C C H2 H2 CH2 COO NH3+ Adenine O H H C H H OH H OH S-adenosylmethionine (SAM) In various reactions, S-adenosylmethionine (SAM) is a donor of diverse chemical groups including methylene, amino, ribosyl and aminoalkyl groups, and a source of 5'-deoxyadenosyl radicals. But SAM is best known as a methyl group donor. HO H 3C + S C C H2 H2 CH2 OH COO HO CH Adenine H H OH H OH S-adenosylmethionine (SAM) CH2 NH3+ norepinephrine NH3+ O H H C S-adenosylmethionine S-adenosylhomocysteine HO OH HO CH CH2 H N CH3 epinephrine Examples: S-adenosylmethionine as methyl group donor methylation of bases in tRNA methylation of cytosine residues in DNA methylation of norepinephrine epinephrine O O R1 C H2C O O CH H2C C R2 O O P CH3 O CH2 O CH2 + N CH3 CH3 phosphatidylcholine conversion of the glycerophospholipid phosphatidyl ethanolamine phosphatidylcholine via methyl transfer from SAM. Enzymes involved in formation and utilization of S-adenosylmethionine are particularly active in liver. Liver has important roles in synthetic pathways involving methylation reactions, & in regulation of blood methionine. Methyl Group Donors Methyl group donors in synthetic reactions include: methyl-B12 S-adenosylmethionine (SAM) N5-methyl-tetrahydrofolate (N5-methyl-THF) Lysine & Tryptophan The complex pathways for degradation of lysine and tryptophan will not be covered. Check out the OMIM website for an example of an inborn error of metabolism, phenylketonuria, a disease resulting from deficiency of Phenylalanine Hydroxylase.