Chapter 19 Carboxylic Acid Derivatives Nucleophilic Acyl Substitution Dr. Wolf's CHM 201 & 202 19-1 Nomenclature of Carboxylic Acid Derivatives Dr. Wolf's CHM 201 & 202 19-2 Acyl Halides O RC X name the acyl group and add the word chloride, fluoride, bromide, or iodide as appropriate acyl chlorides are, by far, the most frequently encountered of the acyl halides Dr. Wolf's CHM 201 & 202 19-3 Acyl Halides O acetyl chloride CH3CCl O H2C CHCH2CCl 3-butenoyl chloride O F Dr. Wolf's CHM 201 & 202 CBr p-fluorobenzoyl bromide 19-4 Acid Anhydrides O O RCOCR' when both acyl groups are the same, name the acid and add the word anhydride when the groups are different, list the names of the corresponding acids in alphabetical order and add the word anhydride Dr. Wolf's CHM 201 & 202 19-5 Acid Anhydrides O O CH3COCCH3 acetic anhydride O O C6H5COCC6H5 benzoic anhydride O O C6H5COC(CH2)5CH3 Dr. Wolf's CHM 201 & 202 benzoic heptanoic anhydride 19-6 Esters O RCOR' name as alkyl alkanoates cite the alkyl group attached to oxygen first (R') name the acyl group second; substitute the suffix -ate for the -ic ending of the corresponding acid Dr. Wolf's CHM 201 & 202 19-7 Esters O CH3COCH2CH3 ethyl acetate O CH3CH2COCH3 methyl propanoate O COCH2CH2Cl Dr. Wolf's CHM 201 & 202 2-chloroethyl benzoate 19-8 Amides having an NH2 group O RCNH2 identify the corresponding carboxylic acid replace the -ic acid or -oic acid ending by -amide. Dr. Wolf's CHM 201 & 202 19-9 Amides having an NH2 group O CH3CNH2 acetamide O (CH3)2CHCH2CNH2 3-methylbutanamide O CNH2 Dr. Wolf's CHM 201 & 202 benzamide 19-10 Amides having substituents on N O RCNHR' O and RCNR'2 name the amide as before precede the name of the amide with the name of the appropriate group or groups precede the names of the groups by the letter N(standing for nitrogen and used as a locant) Dr. Wolf's CHM 201 & 202 19-11 Amides having substituents on N O N-methylacetamide CH3CNHCH3 O CN(CH2CH3)2 N,N-diethylbenzamide O CH3CH2CH2CNCH(CH3)2 CH3 Dr. Wolf's CHM 201 & 202 N-isopropyl-N-methylbutanamide 19-12 Nitriles RC N add the suffix -nitrile to the name of the parent hydrocarbon chain (including the triply bonded carbon of CN) or: replace the -ic acid or -oic acid name of the corresponding carboxylic acid by -onitrile or: name as an alkyl cyanide (functional class name) Dr. Wolf's CHM 201 & 202 19-13 Nitriles CH3C C6H5C N N CH3CHCH3 C Dr. Wolf's CHM 201 & 202 N ethanenitrile or: acetonitrile or: methyl cyanide benzonitrile 2-methylpropanenitrile or: isopropyl cyanide 19-14 Structure of Carboxylic Acid Derivatives Dr. Wolf's CHM 201 & 202 19-15 The key to this chapter is the next slide. It lists the various carboxylic acids in order of decreasing reactivity toward their fundamental reaction type (nucleophilic acyl substitution). The other way to read the list is in order of increasing stabilization of the carbonyl group. Dr. Wolf's CHM 201 & 202 19-16 Most reactive O CH3C O CH3C Cl Least stabilized O OCCH3 O CH3C SCH2CH3 O CH3C Least reactive OCH2CH3 O CH3C Dr. Wolf's CHM 201 & 202 NH2 Most stabilized 19-17 Electron Delocalization and the Carbonyl Group The main structural feature that distinguishes acyl chlorides, anhydrides, thioesters, esters, and amides is the interaction of the substituent with the carbonyl group. It can be represented in resonance terms as: •• – •• O •• •• O •• RC •• X Dr. Wolf's CHM 201 & 202 RC + •• – •• O •• •• X RC + X 19-18 Electron Delocalization and the Carbonyl Group The extent to which the lone pair on X can be delocalized into C=O depends on: 1) the electronegativity of X 2) how well the lone pair orbital of X interacts with the orbital of C=O •• •• – •• – •• O •• •• O •• O •• RC •• X Dr. Wolf's CHM 201 & 202 RC + •• X RC + X 19-19 Orbital overlaps in carboxylic acid derivatives orbital of carbonyl group Dr. Wolf's CHM 201 & 202 19-20 Orbital overlaps in carboxylic acid derivatives lone pair orbital of substituent Dr. Wolf's CHM 201 & 202 19-21 Orbital overlaps in carboxylic acid derivatives electron pair of substituent delocalized into carbonyl orbital Dr. Wolf's CHM 201 & 202 19-22 Acyl Chlorides •• – •• O •• •• O •• R C •• Cl •• •• R C •• Cl + •• acyl chlorides have the least stabilized carbonyl group delocalization of lone pair of Cl into C=O group is not effective because C—Cl bond is too long Dr. Wolf's CHM 201 & 202 19-23 least stabilized C=O O RCCl most stabilized C=O Dr. Wolf's CHM 201 & 202 19-24 Acid Anhydrides •• O •• R C O •• – •• •• O •• C C •• •• O •• R R •• O •• + O C •• R lone pair donation from oxygen stabilizes the carbonyl group of an acid anhydride the other carbonyl group is stabilized in an analogous manner by the lone pair Dr. Wolf's CHM 201 & 202 19-25 least stabilized C=O O RCCl O O RCOCR' most stabilized C=O Dr. Wolf's CHM 201 & 202 19-26 Thioesters – •• •• O •• •• O •• R C •• SR' •• R C + SR' •• Sulfur (like chlorine) is a third-row element. Electron donation to C=O from third-row elements is not very effective. Resonance stabilization of C=O in thioesters is not significant. Dr. Wolf's CHM 201 & 202 19-27 least stabilized C=O O RCCl O O RCOCR' O RCSR' most stabilized C=O Dr. Wolf's CHM 201 & 202 19-28 Esters – •• •• O •• •• O •• R C •• OR' •• R C + OR' •• lone pair donation from oxygen stabilizes the carbonyl group of an ester stabilization greater than comparable stabilization of an anhydride or thioester Dr. Wolf's CHM 201 & 202 19-29 least stabilized C=O O RCCl O O RCOCR' O RCSR' O RCOR' most stabilized C=O Dr. Wolf's CHM 201 & 202 19-30 Amides – •• •• O •• •• O •• R C •• NR'2 R C + NR'2 lone pair donation from nitrogen stabilizes the carbonyl group of an amide N is less electronegative than O; therefore, amides are stabilized more than esters and anhydrides Dr. Wolf's CHM 201 & 202 19-31 Amides – •• •• O •• •• O •• R C •• NR'2 R C + NR'2 amide resonance imparts significant double-bond character to C—N bond activation energy for rotation about C—N bond is 75-85 kJ/mol C—N bond distance is 135 pm in amides versus normal single-bond distance of 147 pm in amines Dr. Wolf's CHM 201 & 202 19-32 least stabilized C=O O RCCl O O RCOCR' O RCSR' O RCOR' O RCNR'2 most stabilized C=O Dr. Wolf's CHM 201 & 202 19-33 Carboxylate ions – •• •• O •• •• O •• R C •• – O •• •• R C O •• •• very efficient electron delocalization and dispersal of negative charge maximum stabilization Dr. Wolf's CHM 201 & 202 19-34 least stabilized C=O O RCCl O O RCOCR' O RCSR' O RCOR' O RCNR'2 O RCO– most stabilized C=O Dr. Wolf's CHM 201 & 202 19-35 Reactivity is related to structure Stabilization Relative rate of hydrolysis RCCl O O very small 1011 RCOCR' small 107 RCOR' O moderate 1.0 RCNR'2 large < 10-2 O O Dr. Wolf's CHM 201 & 202 The more stabilized the carbonyl group, the less reactive it is. 19-36 Nucleophilic Acyl Substitution In general: •• •• O •• R C O •• + X HY R C + HX Y Reaction is feasible when a less stabilized carbonyl is converted to a more stabilized one (more reactive to less reactive). Dr. Wolf's CHM 201 & 202 19-37 most reactive O RCCl O O RCOCR' O RCSR' a carboxylic acid derivative can be converted by nucleophilic acyl substitution to any other type that lies below it in this table Dr. Wolf's CHM 201 & 202 O RCOR' O RCNR'2 O RCO– least reactive 19-38 General Mechanism for Nucleophilic Acyl Substitution Dr. Wolf's CHM 201 & 202 19-39 Nucleophilic Acyl Substitution •• •• O •• R C O •• + X HNu R C + HX Nu Reaction is feasible when a less stabilized carbonyl is converted to a more stabilized one (more reactive to less reactive). Dr. Wolf's CHM 201 & 202 19-40 General Mechanism for Nucleophilic Acyl Substitution involves formation and dissociation of a tetrahedral intermediate •• R C •• OH O •• HNu O •• -HX R C X Nu R C Nu X Both stages can involve several elementary steps. Dr. Wolf's CHM 201 & 202 19-41 General Mechanism for Nucleophilic Acyl Substitution first stage of mechanism (formation of tetrahedral intermediate) is analogous to nucleophilic addition to C=O of aldehydes and ketones •• OH O •• R C HNu R C X Nu X Dr. Wolf's CHM 201 & 202 19-42 General Mechanism for Nucleophilic Acyl Substitution second stage is restoration of C=O by elimination complicating features of each stage involve acid-base chemistry •• R C •• OH O •• HNu O •• -HX R C X Nu R C Nu X Dr. Wolf's CHM 201 & 202 19-43 General Mechanism for Nucleophilic Acyl Substitution Acid-base chemistry in first stage is familiar in that it has to do with acid/base catalysis of nucleophilic addition to C=O. •• R C •• OH O •• HNu O •• -HX R C X Nu R C Nu X Dr. Wolf's CHM 201 & 202 19-44 General Mechanism for Nucleophilic Acyl Substitution Acid-base chemistry in second stage concerns form in which the tetrahedral intermediate exists under the reaction conditions and how it dissociates under those conditions. •• R C •• OH O •• HNu O •• -HX R C X Nu R C Nu X Dr. Wolf's CHM 201 & 202 19-45 The Tetrahedral Intermediate tetrahedral intermediate (TI) •• H O •• R H R O •• •X • C H C •• Nu •• X+ Conjugate acid of tetrahedral intermediate (TI+) Dr. Wolf's CHM 201 & 202 Nu •• R – •• • O •• • C Nu •• •• X Conjugate base of tetrahedral intermediate (TI–) 19-46 Dissociation of TI—H+ B •• H R •• O •• C X + H •• Nu •• +B—H O •• + R Dr. Wolf's CHM 201 & 202 C + •X • H Nu •• 19-47 Dissociation of TI B •• H R •• O •• C X•• •• Nu •• +B—H O •• + R Dr. Wolf's CHM 201 & 202 C + • X •– • • Nu •• 19-48 Dissociation of TI– •• – •• O •• R X•• C •• Nu •• O •• R Dr. Wolf's CHM 201 & 202 C + • X •– • • Nu •• 19-49 Nucleophilic Substitution in Acyl Chlorides Dr. Wolf's CHM 201 & 202 19-50 Preparation of Acyl Chlorides from carboxylic acids and thionyl chloride (Section 12.7) O (CH3)2CHCOH O SOCl2 heat (CH3)2CHCCl + SO2 + HCl (90%) Dr. Wolf's CHM 201 & 202 19-51 Reactions of Acyl Chlorides O RCCl O O RCOCR' O RCOR' O RCNR'2 O RCO– Dr. Wolf's CHM 201 & 202 19-52 Reactions of Acyl Chlorides Acyl chlorides react with carboxylic acids to give acid anhydrides: O O O O RCCl + R'COH RCOCR' + HCl H via: R O O C OCR' Cl Dr. Wolf's CHM 201 & 202 19-53 Example O O CH3(CH2)5CCl + CH3(CH2)5COH pyridine O O CH3(CH2)5COC(CH2)5CH3 (78-83%) Dr. Wolf's CHM 201 & 202 19-54 Reactions of Acyl Chlorides Acyl chlorides react with alcohols to give esters: O O RCCl + R'OH RCOR' + HCl H O via: R C OR' Cl Dr. Wolf's CHM 201 & 202 19-55 Example O O C6H5CCl + (CH3)3COH pyridine C6H5COC(CH3)3 (80%) Dr. Wolf's CHM 201 & 202 19-56 Reactions of Acyl Chlorides Acyl chlorides react with ammonia and amines to give amides: O O RCCl + R'2NH + HO– RCNR'2 + H2O H + Cl– O via: R C NR'2 Cl Dr. Wolf's CHM 201 & 202 19-57 Example O O C6H5CCl + HN NaOH H2O C6H5CN (87-91%) Dr. Wolf's CHM 201 & 202 19-58 Reactions of Acyl Chlorides Acyl chlorides react with water to give carboxylic acids (carboxylate ion in base): O RCCl + H2O O RCCl + 2HO– O RCOH + HCl + Cl– O RCO– + H2O Dr. Wolf's CHM 201 & 202 19-59 Reactions of Acyl Chlorides Acyl chlorides react with water to give carboxylic acids (carboxylate ion in base): O O RCCl + H2O RCOH + HCl H O via: R C OH Cl Dr. Wolf's CHM 201 & 202 19-60 Example O C6H5CH2CCl + H2O Dr. Wolf's CHM 201 & 202 O C6H5CH2COH + HCl 19-61 Reactivity Acyl chlorides undergo nucleophilic substitution much faster than alkyl chlorides. O C6H5CCl Relative rates of hydrolysis (25°C) Dr. Wolf's CHM 201 & 202 1,000 C6H5CH2Cl 1 19-62 Nucleophilic Acyl Substitution in Carboxylic Acid Anhydrides Anhydrides can be prepared from acyl chlorides as described in Table 20.1 Dr. Wolf's CHM 201 & 202 19-63 Some anhydrides are industrial chemicals O O O O CH3COCCH3 O Acetic anhydride Dr. Wolf's CHM 201 & 202 Phthalic anhydride O O O Maleic anhydride 19-64 From dicarboxylic acids Cyclic anhydrides with 5- and 6-membered rings can be prepared by dehydration of dicarboxylic acids O H COH C H C H tetrachloroethane O 130°C COH O Dr. Wolf's CHM 201 & 202 O H + H2 O O (89%) 19-65 Reactions of Anhydrides O O RCOCR' O RCOR' O RCNR'2 O RCO– Dr. Wolf's CHM 201 & 202 19-66 Reactions of Acid Anhydrides Carboxylic acid anhydrides react with alcohols to give esters: O O RCOCR + R'OH O RCOR' O + RCOH normally, symmetrical anhydrides are used (both R groups the same) reaction can be carried out in presence of pyridine (a base) or it can be catalyzed by acids Dr. Wolf's CHM 201 & 202 19-67 Reactions of Acid Anhydrides Carboxylic acid anhydrides react with alcohols to give esters: O O O RCOCR + R'OH RCOR' O + RCOH H O via: R OR' C OCR Dr. Wolf's CHM 201 & 202 O 19-68 Example O O CH3COCCH3 + CH3CHCH2CH3 OH H2SO4 O CH3COCHCH2CH3 (60%) CH3 Dr. Wolf's CHM 201 & 202 19-69 Reactions of Acid Anhydrides Acid anhydrides react with ammonia and amines to give amides: O O O RCOCR RCNR'2 + RCO– + 2R'2NH H + R'2NH2 O via: O R NR'2 C OCR O Dr. Wolf's CHM 201 & 202 19-70 Example O O CH3COCCH3 + H2N CH(CH3)2 O CH3CNH CH(CH3)2 (98%) Dr. Wolf's CHM 201 & 202 19-71 Reactions of Acid Anhydrides Acid anhydrides react with water to give carboxylic acids (carboxylate ion in base): O O RCOCR O + H2O O O RCOCR + 2HO– Dr. Wolf's CHM 201 & 202 2RCOH O 2RCO– + H2O 19-72 Reactions of Acid Anhydrides Acid anhydrides react with water to give carboxylic acids (carboxylate ion in base): O O RCOCR O + H2O 2RCOH H O R OH C OCR O Dr. Wolf's CHM 201 & 202 19-73 Example O O COH O + H2O COH O O Dr. Wolf's CHM 201 & 202 19-74 Sources of Esters Dr. Wolf's CHM 201 & 202 19-75 Esters are very common natural products O CH3COCH2CH2CH(CH3)2 3-methylbutyl acetate also called "isopentyl acetate" and "isoamyl acetate” contributes to characteristic odor of bananas Dr. Wolf's CHM 201 & 202 19-76 Esters of Glycerol O O CH2OCR' RCOCH CH2OCR" O R, R', and R" can be the same or different called "triacylglycerols," "glyceryl triesters," or "triglycerides" fats and oils are mixtures of glyceryl triesters Dr. Wolf's CHM 201 & 202 19-77 Esters of Glycerol O O CH2OC(CH2)16CH3 CH3(CH2)16COCH CH2OC(CH2)16CH3 O Tristearin: found in many animal and vegetable fats Dr. Wolf's CHM 201 & 202 19-78 Cyclic Esters (Lactones) O O CH2(CH2)6CH3 H H (Z)-5-Tetradecen-4-olide (sex pheromone of female Japanese beetle) Dr. Wolf's CHM 201 & 202 19-79 Preparation of Esters Fischer esterification (Chapter 15) from acyl chlorides (Chapters 15 and 19) from carboxylic acid anhydrides (Chapters 15 and 19) Dr. Wolf's CHM 201 & 202 19-80 Physical Properties of Esters Dr. Wolf's CHM 201 & 202 19-81 Boiling Points CH3 CH3CHCH2CH3 O CH3COCH3 boiling point 28°C 57°C OH CH3CHCH2CH3 Dr. Wolf's CHM 201 & 202 99°C Esters have higher boiling points than alkanes because they are more polar. Esters cannot form hydrogen bonds to other ester molecules, so have lower boiling points than alcohols. 19-82 Solubility in Water CH3 Solubility (g/100 g) CH3CHCH2CH3 O ~0 CH3COCH3 33 OH CH3CHCH2CH3 Dr. Wolf's CHM 201 & 202 12.5 Esters can form hydrogen bonds to water, so low molecular weight esters have significant solubility in water. Solubility decreases with increasing number of carbons. 19-83 Reactions of Esters: A Review and a Preview Dr. Wolf's CHM 201 & 202 19-84 Reactions of Esters with Grignard reagents (Chapters 14 & 19) reduction with LiAlH4 (Chapters 15 & 19) with ammonia and amines (Chapter 19) hydrolysis (Chapter 19) Dr. Wolf's CHM 201 & 202 19-85 Acid-Catalyzed Ester Hydrolysis Dr. Wolf's CHM 201 & 202 19-86 Acid-Catalyzed Ester Hydrolysis is the reverse of Fischer esterification O RCOR' + H+ H2O O RCOH + R'OH maximize conversion to ester by removing water maximize ester hydrolysis by having large excess of water equilibrium is closely balanced because carbonyl group of ester and of carboxylic acid are comparably stabilized Dr. Wolf's CHM 201 & 202 19-87 Example O CHCOCH2CH3 + H2O Cl HCl, heat O CHCOH + CH3CH2OH Cl (80-82%) Dr. Wolf's CHM 201 & 202 19-88 Mechanism of Acid-Catalyzed Ester Hydrolysis Is the reverse of the mechanism for acidcatalyzed esterification. Like the mechanism of esterification, it involves two stages: 1) formation of tetrahedral intermediate (3 steps) 2) dissociation of tetrahedral intermediate (3 steps) Dr. Wolf's CHM 201 & 202 19-89 First stage: formation of tetrahedral intermediate O RCOR' + H2O water adds to the carbonyl group of the ester H+ OH RC OH Dr. Wolf's CHM 201 & 202 OR' this stage is analogous to the acidcatalyzed addition of water to a ketone 19-90 Second stage: cleavage of tetrahedral intermediate O + R'OH RCOH H+ OH RC OR' OH Dr. Wolf's CHM 201 & 202 19-91 Mechanism of formation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-92 Step 1 H •• O •• H H RC •O • •• •• +O R' H H •• O •• •• O • • H RC Dr. Wolf's CHM 201 & 202 O •• + R' 19-93 Step 1 •• •• O H RC +O •• •• +O R' H RC •• O •• Dr. Wolf's CHM 201 & 202 carbonyl oxygen is protonated because cation produced is stabilized by electron delocalization (resonance) R' 19-94 Step 2 •• •• OH H + O •• RC •• OR' •• •• +O H H •• O • • RC •• O •• Dr. Wolf's CHM 201 & 202 H R' H 19-95 Step 3 •• •• OH RC H + O •• H H •• OR' •• •• O • • H •• •• OH RC •• OR' •• Dr. Wolf's CHM 201 & 202 H O •• •• + H O •• H H 19-96 Cleavage of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-97 Step 4 •• •• OH RC R' + O •• •• H OH •• •• O • • H H •• •• OH RC R' Dr. Wolf's CHM 201 & 202 O •• •• •• OH H •• H O •• + H 19-98 Step 5 •• •• OH •• RC R' OH + O •• •• H •• •• OH RC + •• OH Dr. Wolf's CHM 201 & 202 •• + •• R' O •• H 19-99 Step 5 •• •• OH RC + •• OH Dr. Wolf's CHM 201 & 202 •• •• + OH RC •• OH •• 19-100 Step 6 H •• O •• RC •• O+ H H •• O H •• •• OH •• H •• +O RC H •• OH •• Dr. Wolf's CHM 201 & 202 19-101 Key Features of Mechanism Activation of carbonyl group by protonation of carbonyl oxygen Nucleophilic addition of water to carbonyl group forms tetrahedral intermediate Elimination of alcohol from tetrahedral intermediate restores carbonyl group Dr. Wolf's CHM 201 & 202 19-102 18O Labeling Studies O COCH2CH3 + H2O Ethyl benzoate, labeled with 18O at the carbonyl oxygen, was subjected to acidcatalyzed hydrolysis. H+ Ethyl benzoate, recovered before the reaction had gone to completion, had lost its 18O label. O This observation is consistent with a tetrahedral intermediate. COCH2CH3 Dr. Wolf's CHM 201 & 202 + H2O 19-103 18O Labeling Studies O COCH2CH3 + H2O H+ OH C H+ OCH2CH3 OH O COCH2CH3 + H2O Dr. Wolf's CHM 201 & 202 19-104 Ester Hydrolysis in Base: Saponification Dr. Wolf's CHM 201 & 202 19-105 Ester Hydrolysis in Aqueous Base O RCOR' O + HO– RCO– + R'OH is called saponification is irreversible, because of strong stabilization of carboxylate ion if carboxylic acid is desired product, saponification is followed by a separate acidification step (simply a pH adjustment) Dr. Wolf's CHM 201 & 202 19-106 Example O CH2OCCH3 CH3 + NaOH water-methanol, heat O CH2OH (95-97%) Dr. Wolf's CHM 201 & 202 + CH3CONa CH3 19-107 Example O H2C CCOCH3 CH3 1. NaOH, H2O, heat 2. H2SO4 O H2C (87%) Dr. Wolf's CHM 201 & 202 CCOH + CH3OH CH3 19-108 Soap-Making Basic hydrolysis of the glyceryl triesters (from fats and oils) gives salts of long-chain carboxylic acids. These salts are O soaps. CH3(CH2)xCOK Dr. Wolf's CHM 201 & 202 O CH2OC(CH2)xCH3 O CH3(CH2)yCOCH CH2OC(CH2)zCH3 O K2CO3, H2O, heat O CH3(CH2)yCOK O CH3(CH2)zCOK 19-109 Which bond is broken when esters are hydrolyzed in base? •• •• •• O •• RCO •• – •• R' + •• OH •• •• O •• •• •– RCO • + R'OH •• •• One possibility is an SN2 attack by hydroxide on the alkyl group of the ester. Carboxylate is the leaving group. Dr. Wolf's CHM 201 & 202 19-110 Which bond is broken when esters are hydrolyzed in base? •• •• •• O RC – •• OR' + •• OH •• •• •• •• O RC – •• OH + •• OR' •• •• •• A second possibility is nucleophilic acyl substitution. Dr. Wolf's CHM 201 & 202 19-111 18O Labeling gives the answer O CH3CH2COCH2CH3 + NaOH O CH3CH2CONa + CH3CH2OH 18O retained in alcohol, not carboxylate; therefore nucleophilic acyl substitution. Dr. Wolf's CHM 201 & 202 19-112 Stereochemistry gives the same answer H O CH3C alcohol has same configuration at chirality center as ester; therefore, nucleophilic acyl substitution C6H5 O C KOH, H2O O CH3COK + HO CH3 H C6H5 C CH3 Dr. Wolf's CHM 201 & 202 not SN2 19-113 Does it proceed via a tetrahedral intermediate? •• •• •• O RC – •• OR' + •• OH •• •• •• •• O RC – •• OH + •• OR' •• •• •• Does nucleophilic acyl substitution proceed in a single step, or is a tetrahedral intermediate involved? Dr. Wolf's CHM 201 & 202 19-114 18O Labeling Studies O COCH2CH3 + H2O Ethyl benzoate, labeled with 18O at the carbonyl oxygen, was subjected to hydrolysis in base. HO– Ethyl benzoate, recovered before the reaction had gone to completion, had lost its 18O label. This observation is consistent with a O tetrahedral intermediate. COCH2CH3 Dr. Wolf's CHM 201 & 202 + H2O 19-115 18O Labeling Studies O COCH2CH3 + H2O HO– OH C HO– OCH2CH3 OH O COCH2CH3 + H2O Dr. Wolf's CHM 201 & 202 19-116 Mechanism of Ester Hydrolysis in Base Involves two stages: 1) formation of tetrahedral intermediate 2) dissociation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-117 First stage: formation of tetrahedral intermediate O RCOR' + H2O HO– OH RC OH Dr. Wolf's CHM 201 & 202 OR' water adds to the carbonyl group of the ester this stage is analogous to the base-catalyzed addition of water to a ketone 19-118 Second stage: cleavage of tetrahedral intermediate O + R'OH RCOH HO– OH RC OR' OH Dr. Wolf's CHM 201 & 202 19-119 Mechanism of formation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-120 Step 1 •• O •• H •• O • • •• – RC • OR' • •• – •• •• O •• RC H O •• •• •• OR' •• Dr. Wolf's CHM 201 & 202 19-121 Step 2 •• •• – •• O • • H •• •• O H O •• H H O •• RC •• •• OR' •• H – •• •• O •• RC H O •• •• •• OR' •• Dr. Wolf's CHM 201 & 202 19-122 Dissociation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-123 Step 3 •• •• – •• O • • H •• •• O H O •• H RC O •• •• •• OR' •• H •• O •• RC •• O •• Dr. Wolf's CHM 201 & 202 H H – •• •• OR' •• 19-124 Step 4 •• O •• RC •• O •• – •• HO– H •• O •• Dr. Wolf's CHM 201 & 202 OR' •• H2O RC •• O •• •• H – •• •• OR' •• 19-125 Key Features of Mechanism Nucleophilic addition of hydroxide ion to carbonyl group in first step Tetrahedral intermediate formed in first stage Hydroxide-induced dissociation of tetrahedral intermediate in second stage Dr. Wolf's CHM 201 & 202 19-126 Reactions of Esters with Ammonia and Amines Dr. Wolf's CHM 201 & 202 19-127 Reactions of Esters O RCOR' O RCNR'2 O RCO– Dr. Wolf's CHM 201 & 202 19-128 Reactions of Esters Esters react with ammonia and amines to give amides: O O RCOR' + R'2NH RCNR'2 + R'OH H O via: R C NR'2 OR' Dr. Wolf's CHM 201 & 202 19-129 Example O H2C CCOCH3 + NH3 CH3 H2O O H2C (75%) Dr. Wolf's CHM 201 & 202 CCNH2 + CH3OH CH3 19-130 Example O FCH2COCH2CH3 + NH2 heat O FCH2CNH + CH3CH2OH (61%) Dr. Wolf's CHM 201 & 202 19-131 Preparation of Tertiary Alcohols From Esters and Grignard Reagents Dr. Wolf's CHM 201 & 202 19-132 Grignard reagents react with esters d– R R' •• d+ OCH •• 3 C MgX O •• •• R' diethyl ether •• R C OCH3 •• ••O •• + MgX •• – but species formed is unstable and dissociates under the reaction conditions to form a ketone Dr. Wolf's CHM 201 & 202 19-133 Grignard reagents react with esters d– R R' •• d+ OCH •• 3 C R' diethyl ether •• R C OCH3 •• ••O •• + MgX •• – MgX O •• •• this ketone then goes on to react with a second mole of the Grignard reagent to give a tertiary alcohol Dr. Wolf's CHM 201 & 202 –CH3OMgX R R' C O •• •• 19-134 Example O 2 CH3MgBr + (CH3)2CHCOCH3 1. diethyl ether 2. H3O+ OH (CH3)2CHCCH3 CH3 (73%) Dr. Wolf's CHM 201 & 202 Two of the groups attached to the tertiary carbon come from the Grignard reagent 19-135 Reactions of Esters with Lithium Aluminum Hydride Dr. Wolf's CHM 201 & 202 19-136 Reduction of Esters Gives Primary Alcohols Lithium aluminum hydride preferred for laboratory reductions Sodium borohydride reduction is too slow to be useful Catalytic hydrogenolysis used in industry but conditions difficult or dangerous to duplicate in the laboratory (special catalyst, high temperature, high pressure Dr. Wolf's CHM 201 & 202 19-137 Example: Reduction of an Ester O COCH2CH3 1. LiAlH4 diethyl ether 2. H2O CH2OH + CH3CH2OH (90%) Dr. Wolf's CHM 201 & 202 19-138 Amides Dr. Wolf's CHM 201 & 202 19-139 Physical Properties of Amides Amides are less reactive toward nucleophilic acyl substitution than other acid derivatives. O C H O O H N H Dr. Wolf's CHM 201 & 202 C H H N H Formamide C H H N H 19-140 Physical Properties of Amides Amides are capable of hydrogen bonding. O H C H N d H d O d H C H d O N H H C H N H Dr. Wolf's CHM 201 & 202 19-141 Physical Properties of Amides Amides are less acidic than carboxylic acids. Nitrogen is less electronegative than oxygen. O CH3CH2NH2 CH3CNH2 pKa (approximate) Dr. Wolf's CHM 201 & 202 36 15 O O O CH3CNCCH3 CH3COH H 10 5 19-142 Preparation of Amides Amides are prepared from amines by acylation with: acyl chlorides anhydrides esters Dr. Wolf's CHM 201 & 202 19-143 Preparation of Amides Amines do not react with carboxylic acids to give amides. The reaction that occurs is proton-transfer (acid-base). O RCOH + R'NH2 O – RCO + + R'NH3 If no heat-sensitive groups are present, the resulting ammonium carboxylate salts can be converted to amides by heating. Dr. Wolf's CHM 201 & 202 19-144 Preparation of Amides Amines do not react with carboxylic acids to give amides. The reaction that occurs is proton-transfer (acid-base). O O RCOH + R'NH2 – RCO + + R'NH3 heat O RCNHR' + H2O Dr. Wolf's CHM 201 & 202 19-145 Example O COH + H2N 225°C O + H2O CNH (80-84%) Dr. Wolf's CHM 201 & 202 19-146 Hydrolysis of Amides Dr. Wolf's CHM 201 & 202 19-147 Hydrolysis of Amides Hydrolysis of amides is irreversible. In acid solution the amine product is protonated to give an ammonium salt. O RCNHR' + H2O + H Dr. Wolf's CHM 201 & 202 O + + RCOH + R'NH3 19-148 Hydrolysis of Amides In basic solution the carboxylic acid product is deprotonated to give a carboxylate ion. O RCNHR' Dr. Wolf's CHM 201 & 202 O – + HO – RCO + R'NH2 19-149 Example: Acid Hydrolysis O O CH3CH2CHCNH2 CH3CH2CHCOH H2O H2SO4 heat + + NH4 HSO4– (88-90%) Dr. Wolf's CHM 201 & 202 19-150 Example: Basic Hydrolysis O NH2 CH3CNH O KOH H2O heat Br CH3COK + Br (95%) Dr. Wolf's CHM 201 & 202 19-151 Mechanism of Acid-Catalyzed Amide Hydrolysis Acid-catalyzed amide hydrolysis proceeds via the customary two stages: 1) formation of tetrahedral intermediate 2) dissociation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-152 First stage: formation of tetrahedral intermediate O RCNH2 + H2O water adds to the carbonyl group of the amide H+ OH RC OH Dr. Wolf's CHM 201 & 202 NH2 this stage is analogous to the acidcatalyzed addition of water to a ketone 19-153 Second stage: cleavage of tetrahedral intermediate O RCOH + + NH4 H+ OH RC NH2 OH Dr. Wolf's CHM 201 & 202 19-154 Mechanism of formation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-155 Step 1 H •• O •• H O •• + H RC • NH2 • •• +O RC H H •• O • • H •• NH2 Dr. Wolf's CHM 201 & 202 19-156 Step 1 •• •• O H RC + NH2 •• +O RC H carbonyl oxygen is protonated because cation produced is stabilized by electron delocalization (resonance) •• NH2 Dr. Wolf's CHM 201 & 202 19-157 Step 2 •• •• OH H + O •• RC •• NH2 •• +O RC •• NH2 Dr. Wolf's CHM 201 & 202 H H H •• O • • H 19-158 Step 3 •• •• OH RC H + O •• H H •• NH2 •• O • • H •• •• OH RC •• NH2 Dr. Wolf's CHM 201 & 202 H O •• •• + H O •• H H 19-159 Cleavage of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-160 Step 4 •• •• OH •• RC H2N H OH + •• •• O • • H H •• •• OH RC H2N •• Dr. Wolf's CHM 201 & 202 H O •• •• H H O •• + H 19-161 Step 5 •• •• OH •• RC H2N OH + •• H •• •• OH RC + •• OH Dr. Wolf's CHM 201 & 202 •• + •• NH3 19-162 Step 6 •• •• OH •• RC H2N OH + •• H + NH 4 •• •• OH RC + •• OH Dr. Wolf's CHM 201 & 202 •• + H3O + •• NH3 19-163 Step 6 •• •• OH RC + •• OH Dr. Wolf's CHM 201 & 202 •• •• + OH RC •• OH •• 19-164 Step 6 H •• O •• RC •• O+ H H •• O H •• •• OH •• H •• +O RC H •• OH •• Dr. Wolf's CHM 201 & 202 19-165 Mechanism of Amide Hydrolysis in Base Involves two stages: 1) formation of tetrahedral intermediate 2) dissociation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-166 First stage: formation of tetrahedral intermediate O RCNH2 + H2O HO– OH RC OH Dr. Wolf's CHM 201 & 202 NH2 water adds to the carbonyl group of the amide this stage is analogous to the base-catalyzed addition of water to a ketone 19-167 Second stage: cleavage of tetrahedral intermediate O – RCO + NH3 HO– OH RC NH2 OH Dr. Wolf's CHM 201 & 202 19-168 Mechanism of formation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-169 Step 1 •• O •• H •• O • • •• – RC • NH2 • – •• •• O •• RC H O •• •• •• NH2 Dr. Wolf's CHM 201 & 202 19-170 Step 2 •• •• – •• O • • H •• •• O H O •• H H O •• RC •• •• NH2 H – •• •• O •• RC H O •• •• •• NH2 Dr. Wolf's CHM 201 & 202 19-171 Dissociation of tetrahedral intermediate Dr. Wolf's CHM 201 & 202 19-172 Step 3 •• •• OH •• RC H2N H OH + •• •• O • •• • – H •• •• OH RC H2N •• Dr. Wolf's CHM 201 & 202 H O •• •• H H O •• •• 19-173 Step 4 •• O •• H •• – •• O • • H •• •• O H RC OH •• H3N + H •• O •• RC •• O •• Dr. Wolf's CHM 201 & 202 •• H •• NH3 19-174 Step 5 •• O •• RC •• O •• – •• HO– •• O •• RC •• O •• Dr. Wolf's CHM 201 & 202 H •• NH3 19-175 Lactams Dr. Wolf's CHM 201 & 202 19-176 Lactams Lactams are cyclic amides. Some are industrial chemicals, others occur naturally. d N O -Caprolactam*: used to prepare a type of nylon H *Caproic acid is the common name for hexanoic acid. Dr. Wolf's CHM 201 & 202 19-177 Lactams Lactams are cyclic amides. Some are industrial chemicals, others occur naturally. O C6H5CH2CNH N O S CH3 CH3 CO2H Penicillin G: a -lactam antibiotic Dr. Wolf's CHM 201 & 202 19-178 Preparation of Nitriles Dr. Wolf's CHM 201 & 202 19-179 Preparation of Nitriles Nitriles are prepared by: nucleophilic substitution by cyanide on alkyl halides cyanohydrin formation dehydration of amides Dr. Wolf's CHM 201 & 202 19-180 Example KCN CH3(CH2)8CH2Cl ethanolwater CH3(CH2)8CH2C N (95%) SN2 Dr. Wolf's CHM 201 & 202 19-181 Example O OH KCN CH3CH2CCH2CH3 H+ CH3CH2CCH2CH3 C N (75%) Dr. Wolf's CHM 201 & 202 19-182 Preparation of Nitriles By dehydration of amides uses the reagent P4O10 (often written as P2O5) O P4O10 (CH3)2CHCNH2 200°C (CH3)2CHC N (69-86%) Dr. Wolf's CHM 201 & 202 19-183 Hydrolysis of Nitriles Dr. Wolf's CHM 201 & 202 19-184 Hydrolysis of Nitriles O RCN + 2H2O + H + + RCOH + NH4 Hydrolysis of nitriles resembles the hydrolysis of amides. The reaction is irreversible. Ammonia is produced and is protonated to ammonium ion in acid solution. Dr. Wolf's CHM 201 & 202 19-185 Hydrolysis of Nitriles O RCN – + H2O + HO – RCO + NH3 In basic solution the carboxylic acid product is deprotonated to give a carboxylate ion. Dr. Wolf's CHM 201 & 202 19-186 Example: Acid Hydrolysis O CH2CN CH2COH H2O H2SO4 heat NO2 NO2 (92-95%) Dr. Wolf's CHM 201 & 202 19-187 Example: Basic Hydrolysis O CH3(CH2)9CN 1. KOH, H2O, heat 2. H+ CH3(CH2)9COH (80%) Dr. Wolf's CHM 201 & 202 19-188 Mechanism of Hydrolysis of Nitriles O RC N H2O RCNH2 O H2O RCOH Hydrolysis of nitriles proceeds via the corresponding amide. We already know the mechanism of amide hydrolysis. Therefore, all we need to do is to see how amides are formed from nitriles under the conditions of hydrolysis. Dr. Wolf's CHM 201 & 202 19-189 Mechanism of Hydrolysis of Nitriles OH RC N H2O RC O NH RCNH2 The mechanism of amide formation is analogous to that of conversion of alkynes to ketones. It begins with the addition of water across the carbon-nitrogen triple bond. The product of this addition is the nitrogen analog of an enol. It is transformed to an amide under the reaction conditions. Dr. Wolf's CHM 201 & 202 19-190 Step 1 H H – •• O • • •• RC •• O •• N •• RC •• N •• – Dr. Wolf's CHM 201 & 202 19-191 Step 2 H •• O •• RC H •• N •• H – O •• H O •• •• •• RC •• N Dr. Wolf's CHM 201 & 202 H H •• O •• – •• 19-192 Step 3 H •• O •• H H •• O •• – •• •• • O• H RC – •• N H O •• •• •• RC •• N Dr. Wolf's CHM 201 & 202 H 19-193 Step 4 •• • O• •• • O• RC RC •• N H H – •• •• O •• H Dr. Wolf's CHM 201 & 202 – •• N H •• H •• O •• H 19-194 Addition of Grignard Reagents to Nitriles Dr. Wolf's CHM 201 & 202 19-195 Addition of Grignard Reagents to Nitriles NMgX RC N R'MgX RCR' NH H2O RCR' diethyl ether Grignard reagents add to carbon-nitrogen triple bonds in the same way that they add to carbonoxygen double bonds. The product of the reaction is an imine. Dr. Wolf's CHM 201 & 202 19-196 Addition of Grignard Reagents to Nitriles NMgX RC N R'MgX diethyl ether RCR' NH H2O RCR' H3O+ Imines are readily hydrolyzed to ketones. O Therefore, the reaction of Grignard reagents with nitriles can be used as a RCR' synthesis of ketones. Dr. Wolf's CHM 201 & 202 19-197 Example C N + CH3MgI F3C 1. diethyl ether 2. H3O+, heat O CCH3 Dr. Wolf's CHM 201 & 202 F3C (79%) 19-198 Spectroscopic Analysis of Carboxylic Acid Derivatives Dr. Wolf's CHM 201 & 202 19-199 Infrared Spectroscopy C=O stretching frequency depends on whether the compound is an acyl chloride, anhydride, ester, or amide. C=O stretching frequency O O O CH3CCl CH3COCCH3 1822 cm-1 1748 and 1815 cm-1 Dr. Wolf's CHM 201 & 202 O O CH3COCH3 CH3CNH2 1736 cm-1 1694 cm-1 19-200 Infrared Spectroscopy Anhydrides have two peaks due to C=O stretching. One results from symmetrical stretching of the C=O unit, the other from an antisymmetrical stretch. C=O stretching frequency O O CH3COCCH3 1748 and 1815 cm-1 Dr. Wolf's CHM 201 & 202 19-201 Infrared Spectroscopy Nitriles are readily identified by absorption due to carbon-nitrogen triple bond stretching in the 22102260 cm-1 region. Dr. Wolf's CHM 201 & 202 19-202 1H NMR 1H NMR readily distinguishes between isomeric esters of the type: O RCOR' O and R'COR O O C H Dr. Wolf's CHM 201 & 202 is less shielded than C C H 19-203 1H NMR For example: O CH3COCH2CH3 O and CH3CH2COCH3 Both have a triplet-quartet pattern for an ethyl group and a methyl singlet. They can be identified, however, on the basis of chemical shifts. Dr. Wolf's CHM 201 & 202 19-204 O O Figure 20.9 CH3CH2COCH3 CH3COCH2CH3 5.0 4.0 3.0 Dr. Wolf's CHM 201 & 202 2.0 1.0 0 5.0 Chemical shift (d, ppm) 4.0 3.0 2.0 1.0 0 19-205 13C NMR Carbonyl carbon is at low field (d 160-180 ppm), but not as deshielded as the carbonyl carbon of an aldehyde or ketone (d 190-215 ppm). The carbon of a CN group appears near d 120 ppm. Dr. Wolf's CHM 201 & 202 19-206 UV-VIS n* absorption: max O O O CH3CCl CH3COCCH3 235 nm 225 nm Dr. Wolf's CHM 201 & 202 O O CH3COCH3 CH3CNH2 207 nm 214 nm 19-207 Mass Spectrometry Most carboxylic acid derivatives give a prominent peak for an acylium ion derived by the fragmentation shown. •• O •• RCX •• Dr. Wolf's CHM 201 & 202 •+ O •• RCX •• RC + O •• + • X •• 19-208 Mass Spectrometry Amides, however, cleave in the direction that gives a nitrogen-stabilized cation. •• O •• RCNR'2 •• Dr. Wolf's CHM 201 & 202 •+ O •• RCNR'2 •• •• R • + •• O C + NR'2 19-209 End of Chapter 19 Dr. Wolf's CHM 201 & 202 19-210