carbohydrates (mcm chapt 25) glucose: c 6 h 12 o 6 = c 6 (h 2 o) 6 monosaccharides / simple...

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Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = “C 6 (H 2 O) 6 onosaccharides / Simple carbohydrates: an not be hydrolyzed to simpler carbohydrates D-shugars H OH CH 2 OH O H H OH CH 2 OH O H (R )G lyceraldehyde / D -glyceraldehyde H OH H OH CH 2 OH H OH O H R ibose A ldopentose A ldehyde 5 C CH 2 OH O HO H H OH H OH CH 2 OH Fructose K etohexose K etone 6 C

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Monosaccharides - Reactions (McM chapt 25.7) Functional groups: Alchohols, aldehydes/ketones, hemiacetals React like ROH

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Page 1: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Carbohydrates (McM chapt 25)

Glucose: C6H12O6 = “C6(H2O)6”

Monosaccharides / Simple carbohydrates:Can not be hydrolyzed to simpler carbohydrates

D-shugars

H OHCH2OH

OH

H OHCH2OH

OH

(R) Glyceraldehyde / D-glyceraldehyde

H OHH OH

CH2OHH OH

OH

RiboseAldopentose

Aldehyde 5 C

CH2OHO

HO HH OHH OH

CH2OH

FructoseKetohexose

Ketone 6 C

Page 2: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Open and cyclic forms

H OHHO H

H OHH OH

CH2OH

OH

Aldehyde

HO

OH

OH

CH2OH

OHOH O

OHOH

OH

CH2OH

OH

H

Hemiacetal

HO

OH

OH

CH2OH

OHOH

O

OHOH

HOHO

HOH2C

α-D-glucopyrαnose

O

OH

HOHO

HOH2C

OH

β-D-glucopyrαnose

Page 3: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Monosaccharides - Reactions (McM chapt 25.7)Functional groups: Alchohols, aldehydes/ketones, hemiacetals

React like ROH

O

O

OPyridine

H3COCO OCOCH3

O OCOCH3H3COCO

CH3IAg2O

OCH3 OCH3

O OCH3H3CO

OH OH

O OHHO

β-D-riβofurαnose

OH OH

O OHHO

β-D-riβofurαnose

CH3OHαcid

OH OH

O OCH3HO

+

OH OH

O

OCH3

HO

hem iαcetαl αcetαl

Methyl β-D-riβofurαnoside

Glycoside

Page 4: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Glycosides in natureN

N N

NNH2

O

OHHO

HO

Adenine(Vit. B4)

N

N N

NNH2

O

ORHO

OP

O

OOH

P

OO

OHHO

N

OHO

O

NH2

N

N N

NNH2

O

ORHO

OP

O

OOH

P

OO

OHHO

N

OHO

O

NH2

NADH

H H

Nicotinamid adenine dinucleotide

NADR=H

R=Phosphate: NADP+, NADPH

N

N

N

NHH3C

H3C

O

O

H OHOHOHH

H

O P OO

OH

O

OHO O

HO OH

N

N

N

N

NH2

FAD

N

HN

N

NHH3C

H3C

O

ORFADH2

Flavin adenine dinucleotide

DNA / RNA

OHO

OHOHOH

OH

Glucose

OCO2H

OHOOH

OH

UDP-Glucuronate

P P O

HO OH

N

NO

O

RXH

OCO2H

OHOH

OH

XR

More hydrophilic metaboliteof RXH

Metabolism

Page 5: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

O

O

OOH

CO2H

OH

HOOHHOOHO

O

OHNH2

OH

HO

OH

Amfotericin B(Legemiddel mot soppinfeksjon)

O

O

O

HOO

O

NHO

HOHO

O

OO

OH

Erytromycin (Antibiotikum)

CO2H

H

OH

H

O

HO

O

OHCO2H

O

O

CO2HOH

HO

HO

Aglycone

GlycyrrhizinSaponin from liquorice (lakris) rootexpectorants (slimløsende) respir. tract infect.

From microorganisms:

Page 6: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Stereoselectivity in glycoside syntheses

+

HO

OH

OH

CH2OH

OHOH

O

OHOH

HOHO

HOH2C

α-D-glucopyrαnose

Minor

β-D-glucopyrαnose

MαjorH

O

OH

HOHO

HOH2C

O

OH

HOHO

HOH2C

Stereochem icαl info lost

R -OH

AB

O

OOH

HOHO

HOH2C

Alkyl α-D-glucopyrαnoside

Mαjor

O

OH

HOHO

HOH2C

O

Alkyl β-D-glucopyrαnoside

Minor

R

R

O

OH

HOHO

HOH2C

OH

Page 7: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

The anomeric effect

O

O

OO

R

R

No lone-pair repulsjonAxial subst

Lone-pair repulsjonequatorial subst subst

Stereoselective synthesis of β-glycisides - Koenigs Knorr react

OOAc

OAc

AcOAcO

OAcHBr O

BrOAc

AcOAcO

OAc

O

OAcO

AcO

OAc

OH3C

O

O

AcOAcO

OAc

OH3C

R-OH

OO

OAcAcO

AcO

OAc

R

Page 8: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Reduction of carbonyl:

HO O

OH

HO OH

OH

D-glukose

HO OH

OH

HO O

OH

D-glukose

NaBH4 HO OH

OH

HO OH

OH

D-glusitol(sorbitol)

Oxidative reactions:“Reducing shugars”: Easily oxidized (most often aldeh. - acid)

HO O

OH

HO OH

OH

HO OH

OH

HO O

OH

D-glucose

mild oxHO

CO2HOH

OH

HO

OH

HO O

OH

HO O

OH

CH3 no ox. under mild condNot "reducing shugar"

Hemiacetal Aldehyde

Acetal •Tollens•Fehling•Benedict [old diabetes (glucose) test]

Tests (visual results)Not used in synthesis (preparative scale)

Page 9: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Ketoses as “reducing shugars”

CH2OHOHHOHHHHOO

CH2OH

Fructoseketo - tautomer I

Base

CH2OHOHHOHHHHOOH

enol - tautomer

HO

Base

CH2OHOHHOHHHHO

O H

OH

keto - tautomer II

mild ox

CH2OHOHHOHHHHO

O OH

OH

Synthetically useful oxidations

OH

OH

An aldose

Aldehyde

prim alchohol

HNO3

OHO

OHO

Diacid

Br2

H2O, pH 6

OHO

OH

Only aldehyde oxidized

Page 10: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Chain Lengthening and Shortening

OH

An aldose

HCN

CN

H OH1) H2 / cat.2) Hydrol. imine

CH OH

H O

n C-atoms n+1 C atoms

H2N-OH

CH OH

H NOH- H2O

Strong base

Page 11: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Monosaccharides / Simple carbohydrates:Can not be hydrolyzed to simpler carbohydrates

Disaccharides (McM chapt 25.9)

Complex carbohydrates: Disacch., polysacch.Can be hydrol. to monosacch. (cleav. of acetal / hemiacetal)

O

OHHO

HO

OH

O

OHOHHO

O

OH

Maltose

1,4'-α-glycosideGlucose + glucose

1

α 4'

O

OHHO

HO

OHO

OHOHHO

O

OH

Celloβiose

1,4'-β-glycosideGlucose + glucose

4' O

OHHO

OH OHO

OHOHHO

O

OH

Lαctose

1,4'-β-glycosideGαlαctose + glucose

4'

hem iαcetαl αldehyde ; "reducing shugαr"

O

OHHO

HO

OH

O

Sucrose

1,2'-α-glycosideGlucose + fructose

1

α 2'O

OH

HO

OH

OH

No hem iαcetαl fuctionNot "reducing"

Page 12: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Milk intolerance

O

OHHO

OH OHO

OHOHHO

O

OH

Lactose

1,4'-β-glycosideGαlαctose + glucose

4'

Not αβsorβet from intestinesAccum ulαtion - diαrrheα etc

Lαctαse

O

OHHO

OH OHO

OHOHHO

OH

Often m issingαdults

HO

OH

gαlαctαse glucose

norm αl m etαβolism

No isom erisαtion:gαlαctosem iαSevere m ilk intolerαnce (even kids)Mentαl retαrdαtion

Page 13: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Polysaccharides (McM chapt 25.10)

CelluloseLong chains (>1000 monosachh.)H-bond between chainsStructural material - plantsβ-glycoside link., not digested humans

Starch: Amylose and amylopectin

O

OHHOO

OHO

O

OHHO

O

OH

4'O

O

OHHO

OH

O

OHHOO

OH

O

OHHO

O

OH1α 4'

O

OOHHO

O

OH

Amylose ca 20%

O

OHHOO

OH

O

OHHO

O

1α 4'

O

OOHHO

O

OH

O

OHHOO

OH

O

1

α

6'

Brαnches(cα every 25. gluc.)

Amylopectin ca 80%

Energy storage plantsα-glycoside link., digested humans

Glycogen ≈ amylopectin, larger, more branchesEnergy storage animals

Page 14: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Synthesis Di- and Polysaccharides

Building from monosaccharides - Challenges•Regioselectivity•Stereoselectivity•Stability

O

HO

OH OHO

HO

OH OH

OHOH

Galactose Glycal from galComm. avail.

Cl Si

Base O

HO

OH OSi

O-silylationPrim OH

O

N NNN

Prot. as carbonate ester

O

O

OO

Si

O

epoxidationi.e.mCPBA

O

O

OO

Si

O

O

O

O

OOH

O

TBAF

ZnCl2

O

O

OO

Si

O

OH

O

O

O

OO

1,6' β

Page 15: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Other carbohydrates (McM chapt 25.11-12)

OH OH

O OHHO

β-D-riβofurαnose

H OHOHH

H OHOH

H O

OH OH

O

NHO

N

O

NH2

RNA nucleosidei.e . cytidine

riβose

OH

O OHHOH H

OHHH OH

OH

H O

OH

O

NHO

N

O

NH2

DNA nucleosidei.e . deoxycytidine

Deoxyriβose

Page 16: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

O

O

NH3

H

Aminoglycoside antibiotics

O

OH

O

OO

HN

OH

OHHO

NH

H2

N

NH

H2

N

NH

HO

O

NH

HO

HO

Streptomycin

N-Metylglucosamin

L-Streptose

Streptidin

(sykloheksander.)

O

OHO

OHO

O

OH

NH2

NH2

HO

O

HO

NH2

NH2

OH

O

OH

NH2

H2N

Neomycin C

ÿ Basic, water solubile salts phys. pH

ÿ -Glykosides (= acetals) stabile acidic media because of protonated

amino subst.

NH

R'R

O

SOH

HOOH

N

O

R= H, R'=Cl: Klindamycin

R=OH, R'=H: Linkomycin,

Lincomycin antibiotics

Glycoproteins / Glycopeptides

Page 17: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

Neuraminidase InhibitorsEffect on influenza virus A and B(?)Inhib. neuraminidase (enzyme that breaks bonds between HA* in newly HA in formed virus and host cell)Prevents release of virus

HA: Hemaglutinin, (glycoprotein)important for bonding between influenza virus and host

Page 18: Carbohydrates (McM chapt 25) Glucose: C 6 H 12 O 6 = C 6 (H 2 O) 6  Monosaccharides / Simple carbohydrates: Can not be hydrolyzed to simpler carbohydrates

O

CO2H

OGlycopeptide

HO

HN

O

OHHO

HO

NeuraminidaseHO

GlycopeptideO

CO2H

OHHO

HN

O

OHHO

HO

+

Sialic acid≈ SN1

≈ TS‡

ZanamivirRelenza®

OseltamivirTamiflu®

O

CO2H

OGlycopeptide

HO

HN

O

OHHO

HO

Sialic acid

OCO2H

HO

HN

O

OHHO

HO

OH2

O

CO2HHO

HN

O

OHHO

HO

Lead compound Neuramidinase Inhib. (not selective for viral NA)

DANA

First selective drug Carbocyclic drug

CO2HH2N

HN

O

OO

CO2HHO

HN

O

OHHO

HO

O

CO2HHN

HN

O

OHHO

HO

HN NH2