CHAPTER 14
ORGANOMETALLIC COMPOUNDS
O
rganometallic compounds are compounds that have a carbon–metal bond; they
lie at the place where organic and inorganic chemistry meet. You are already
familiar with at least one organometallic compound, sodium acetylide
(NaCPCH), which has an ionic bond between carbon and sodium. But just because a
compound contains both a metal and carbon isn’t enough to classify it as organometal-
lic. Like sodium acetylide, sodium methoxide (NaOCH
3
) is an ionic compound. Unlike
sodium acetylide, however, the negative charge in sodium methoxide resides on oxygen,
not carbon.
The properties of organometallic compounds are much different from those of the
other classes we have studied to this point. Most important, many organometallic com-
pounds are powerful sources of nucleophilic carbon, something that makes them espe-
cially valuable to the synthetic organic chemist. For example, the preparation of alkynes
by the reaction of sodium acetylide with alkyl halides (Section 9.6) depends on the pres-
ence of a negatively charged, nucleophilic carbon in acetylide ion.
Synthetic procedures that use organometallic reagents are among the most impor-
tant methods for carbon–carbon bond formation in organic chemistry. In this chapter you
will learn how to prepare organic derivatives of lithium, magnesium, copper, and zinc and
see how their novel properties can be used in organic synthesis. We will also finish the
story of polyethylene and polypropylene begun in Chapter 6 and continued in Chapter 7
to see the unique way that organometallic compounds catalyze alkene polymerization.
Sodium acetylide
(has a carbon-to-metal bond)
Na
H11001
CPCH
H11002
Sodium methoxide
(does not have a carbon-to-metal bond)
Na
H11001
OCH
3
H11002
546
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14.1 ORGANOMETALLIC NOMENCLATURE
Organometallic compounds are named as substituted derivatives of metals. The metal is
the base name, and the attached alkyl groups are identified by the appropriate prefix.
When the metal bears a substituent other than carbon, the substituent is treated as if it
were an anion and named separately.
PROBLEM 14.1 Both of the following organometallic reagents will be encoun-
tered later in this chapter. Suggest a suitable name for each.
(a) (CH
3
)
3
CLi (b)
SAMPLE SOLUTION (a) The metal lithium provides the base name for (CH
3
)
3
CLi.
The alkyl group to which lithium is bonded is tert-butyl, and so the name of this
organometallic compound is tert-butylithium. An alternative, equally correct name
is 1,1-dimethylethyllithium.
An exception to this type of nomenclature is NaCPCH, which is normally referred to
as sodium acetylide. Both sodium acetylide and ethynylsodium are acceptable IUPAC names.
14.2 CARBON–METAL BONDS IN ORGANOMETALLIC COMPOUNDS
With an electronegativity of 2.5 (Table 14.1), carbon is neither strongly electropositive
nor strongly electronegative. When carbon is bonded to an element more electronegative
than itself, such as oxygen or chlorine, the electron distribution in the bond is polarized
H
MgCl
CH
3
MgI
Methylmagnesium iodide
(CH
3
CH
2
)
2
AlCl
Diethylaluminum chloride
Li
H
Cyclopropyllithium
CH
2
CHNa
Vinylsodium
(CH
3
CH
2
)
2
Mg
Diethylmagnesium
14.2 Carbon–Metal Bonds in Organometallic Compounds 547
TABLE 14.1 Electronegativities of Some Representative Elements
Element
F
O
Cl
N
C
H
Cu
Zn
Al
Mg
Li
Na
K
4.0
3.5
3.0
3.0
2.5
2.1
1.9
1.6
1.5
1.2
1.0
0.9
0.8
Electronegativity
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so that carbon is slightly positive and the more electronegative atom is slightly negative.
Conversely, when carbon is bonded to a less electronegative element, such as a metal,
the electrons in the bond are more strongly attracted toward carbon.
Figure 14.1 uses electrostatic potential maps to show how different the electron distri-
bution is between methyl fluoride (CH
3
F) and methyllithium (CH
3
Li).
An anion that contains a negatively charged carbon is referred to as a carbanion.
Covalently bonded organometallic compounds are said to have carbanionic character.
As the metal becomes more electropositive, the ionic character of the carbon–metal bond
becomes more pronounced. Organosodium and organopotassium compounds have ionic
carbon–metal bonds; organolithium and organomagnesium compounds tend to have
covalent, but rather polar, carbon–metal bonds with significant carbanionic character. It
is the carbanionic character of such compounds that is responsible for their usefulness
as synthetic reagents.
C M
H9254H11002 H9254H11001
M is less electronegative
than carbon
C X
H9254H11001 H9254H11002
X is more electronegative
than carbon
548 CHAPTER FOURTEEN Organometallic Compounds
(a) Methyl fluoride
(b) Methyllithium
FIGURE 14.1 Electro-
static potential maps of
(a) methyl fluoride and of
(b) methyllithium. The elec-
tron distribution is reversed
in the two compounds. Car-
bon is electron-poor (blue) in
methyl fluoride, but electron-
rich (red) in methyllithium.
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14.3 PREPARATION OF ORGANOLITHIUM COMPOUNDS
Before we describe the applications of organometallic reagents to organic synthesis, let
us examine their preparation. Organolithium compounds and other Group I organometal-
lic compounds are prepared by the reaction of an alkyl halide with the appropriate metal.
The alkyl halide can be primary, secondary, or tertiary. Alkyl iodides are the most reac-
tive, followed by bromides, then chlorides. Fluorides are relatively unreactive.
Unlike elimination and nucleophilic substitution reactions, formation of organo-
lithium compounds does not require that the halogen be bonded to sp
3
-hybridized carbon.
Compounds such as vinyl halides and aryl halides, in which the halogen is bonded to sp
2
-
hybridized carbon, react in the same way as alkyl halides, but at somewhat slower rates.
Organolithium compounds are sometimes prepared in hydrocarbon solvents such
as pentane and hexane, but normally diethyl ether is used. It is especially important that
the solvent be anhydrous. Even trace amounts of water or alcohols react with lithium to
form insoluble lithium hydroxide or lithium alkoxides that coat the surface of the metal
and prevent it from reacting with the alkyl halide. Furthermore, organolithium reagents
are strong bases and react rapidly with even weak proton sources to form hydrocarbons.
We shall discuss this property of organolithium reagents in Section 14.5.
PROBLEM 14.2 Write an equation showing the formation of each of the fol-
lowing from the appropriate bromide:
(a) Isopropenyllithium (b) sec-Butyllithium
SAMPLE SOLUTION (a) In the preparation of organolithium compounds from
organic halides, lithium becomes bonded to the carbon that bore the halogen.
Therefore, isopropenyllithium must arise from isopropenyl bromide.
Reaction with an alkyl halide takes place at the metal surface. In the first step, an
electron is transferred from the metal to the alkyl halide.
H11001H11001Li
H11001
Lithium cationLithium
Li
Alkyl halide
RX
Anion radical
[R ]
H11002
X
H11001CH
2
?CCH
3
W
Br
Isopropenyl bromide
2Li
Lithium
H11001
W
Li
CH
2
?CCH
3
Isopropenyllithium
LiBr
Lithium bromide
diethyl
ether
diethyl ether
35°C
Br
Bromobenzene
H11001 2Li
Lithium
Li
Phenyllithium
(95–99%)
H11001 LiBr
Lithium
bromide
H11001H11001RX
Alkyl
halide
2M
Group I
metal
M
H11001
X
H11002
Metal
halide
RM
Group I
organometallic
compound
H11001H11001(CH
3
)
3
CCl
tert-Butyl chloride
2Li
Lithium
LiCl
Lithium
chloride
(CH
3
)
3
CLi
tert-Butyllithium
(75%)
diethyl ether
H1100230°C
14.3 Preparation of Organolithium Compounds 549
The reaction of an alkyl
halide with lithium was cited
earlier (Section 2.16) as an
example of an oxidation–
reduction. Group I metals are
powerful reducing agents.
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Having gained one electron, the alkyl halide is now negatively charged and has an odd
number of electrons. It is an anion radical. The extra electron occupies an antibonding
orbital. This anion radical fragments to an alkyl radical and a halide anion.
Following fragmentation, the alkyl radical rapidly combines with a lithium atom to form
the organometallic compound.
14.4 PREPARATION OF ORGANOMAGNESIUM COMPOUNDS:
GRIGNARD REAGENTS
The most important organometallic reagents in organic chemistry are organomagnesium
compounds. They are called Grignard reagents after the French chemist Victor
Grignard. Grignard developed efficient methods for the preparation of organic deriva-
tives of magnesium and demonstrated their application in the synthesis of alcohols. For
these achievements he was a corecipient of the 1912 Nobel Prize in chemistry.
Grignard reagents are prepared from organic halides by reaction with magnesium,
a Group II metal.
(R may be methyl or primary, secondary, or tertiary alkyl; it may also be a cycloalkyl,
alkenyl, or aryl group.)
Anhydrous diethyl ether is the customary solvent used when preparing organo-
magnesium compounds. Sometimes the reaction does not begin readily, but once started,
it is exothermic and maintains the temperature of the reaction mixture at the boiling point
of diethyl ether (35°C).
The order of halide reactivity is I H11022 Br H11022 Cl H11022 F, and alkyl halides are more reac-
tive than aryl and vinyl halides. Indeed, aryl and vinyl chlorides do not form Grignard
reagents in diethyl ether. When more vigorous reaction conditions are required, tetrahy-
drofuran (THF) is used as the solvent.
Mg
THF, 60°C
Vinyl chloride
CH
2
CHCl
Vinylmagnesium chloride (92%)
CH
2
CHMgCl
diethyl ether
35°C
Cl
H
Cyclohexyl chloride
H11001 Mg
Magnesium
H
MgCl
Cyclohexylmagnesium chloride (96%)
diethyl ether
35°C
Br
Bromobenzene
H11001 Mg
Magnesium
MgBr
Phenylmagnesium bromide (95%)
H11001
Organic halide
RX
Magnesium
Mg
Organomagnesium halide
RMgX
H11001
Alkyl radical
R
Lithium
Li
Alkyllithium
RLi
H11001
Alkyl radical
R
Halide anion
X
H11002
Anion radical
[R ]
H11002
X
550 CHAPTER FOURTEEN Organometallic Compounds
Grignard shared the prize
with Paul Sabatier, who, as
was mentioned in Chapter 6,
showed that finely divided
nickel could be used to cat-
alyze the hydrogenation of
alkenes.
Recall the structure of
tetrahydrofuran from Sec-
tion 3.15:
O
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PROBLEM 14.3 Write the structure of the Grignard reagent formed from each
of the following compounds on reaction with magnesium in diethyl ether:
(a) p-Bromofluorobenzene (c) Iodocyclobutane
(b) Allyl chloride (d) 1-Bromocyclohexene
SAMPLE SOLUTION (a) Of the two halogen substituents on the aromatic ring,
bromine reacts much faster than fluorine with magnesium. Therefore, fluorine is
left intact on the ring, while the carbon–bromine bond is converted to a car-
bon–magnesium bond.
The formation of a Grignard reagent is analogous to that of organolithium reagents
except that each magnesium atom can participate in two separate one-electron transfer steps:
Organolithium and organomagnesium compounds find their chief use in the prepara-
tion of alcohols by reaction with aldehydes and ketones. Before discussing these reactions,
let us first examine the reactions of these organometallic compounds with proton donors.
14.5 ORGANOLITHIUM AND ORGANOMAGNESIUM COMPOUNDS
AS BR?NSTED BASES
Organolithium and organomagnesium compounds are stable species when prepared in
suitable solvents such as diethyl ether. They are strongly basic, however, and react
instantly with proton donors even as weakly acidic as water and alcohols. A proton is
transferred from the hydroxyl group to the negatively polarized carbon of the
organometallic compound to form a hydrocarbon.
H
H9254H11001
H9254H11002
ORH11032
H9254H11001
M
H9254H11002
R
RHH11001 RH11032OM
H11001
H11002
CH
3
CH
2
CH
2
CH
2
Li
Butyllithium
H11001 H
2
O
Water
CH
3
CH
2
CH
2
CH
3
Butane (100%)
H11001 LiOH
Lithium hydroxide
MgBr
Phenylmagnesium
bromide
H11001 CH
3
OH
Methanol Benzene
(100%)
H11001 CH
3
OMgBr
Methoxymagnesium
bromide
H11001H11001
Magnesium
Mg Mg
H11001
Alkyl halide
RX
Anion radical
[R ]
H11002
X
H11001
Alkyl
radical
R
Halide
ion
X
H11002
Anion radical
[R ]
H11002
X
Alkylmagnesium halide
Mg
H11001
XR
H11002Mg
H11001
H11001BrF
p-Bromofluorobenzene
Mg
Magnesium
diethyl
ether
MgBrF
p-Fluorophenylmagnesium
bromide
14.5 Organolithium and Organomagnesium Compounds as Br?nsted Bases 551
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Because of their basicity organolithium compounds and Grignard reagents can-
not be prepared or used in the presence of any material that bears a hydroxyl group.
Nor are these reagents compatible with ±NH or ±SH groups, which can also con-
vert an organolithium or organomagnesium compound to a hydrocarbon by proton
transfer.
The carbon–metal bonds of organolithium and organomagnesium compounds have
appreciable carbanionic character. Carbanions rank among the strongest bases that we’ll
see in this text. Their conjugate acids are hydrocarbons—very weak acids indeed. The
equilibrium constants K
a
for ionization of hydrocarbons are much smaller than the K
a
’s
for water and alcohols.
Table 14.2 presents some approximate data for the acid strengths of representative hydro-
carbons.
Acidity increases in progressing from the top of Table 14.2 to the bottom. An acid
will transfer a proton to the conjugate base of any acid above it in the table. Organo-
lithium compounds and Grignard reagents act like carbanions and will abstract a proton
from any substance more acidic than a hydrocarbon. Thus, N±H groups and terminal
alkynes (RCPC±H) are converted to their conjugate bases by proton transfer to
organolithium and organomagnesium compounds.
H11001C H
Hydrocarbon
(very weak acid)
Proton
H
H11001 H11002
C
Carbanion
(very strong base)
552 CHAPTER FOURTEEN Organometallic Compounds
TABLE 14.2
Approximate Acidities of Some Hydrocarbons and Reference
Materials
Compound
2-Methylpropane
Ethane
Methane
Ethylene
Benzene
Ammonia
Acetylene
Ethanol
Water
10
H1100271
10
H1100262
10
H1100260
10
H1100245
10
H1100243
10
H1100236
10
H1100226
10
H1100216
1.8 H11003 10
H1100216
K
a
71
62
60
45
43
36
26
16
15.7
pK
a
Formula*
(CH
3
)
3
C±H
CH
3
CH
2
±H
CH
3
±H
CH
2
?CH±H
H
2
N±H
HCPC±H
CH
3
CH
2
O±H
HO±H
H
H
H
H
H
H
Conjugate base
H11002
H
H
H
H
H
(CH
3
)
3
C
H11002
H
3
C
H11002
HCPC
H11002
H
2
N
H11002
CH
3
CH
2
O
H11002
HO
H11002
CH
3
CH
2
H11002
CH
2
?CH
H11002
*The acidic proton in each compound is shaded in red.
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PROBLEM 14.4 Butyllithium is commercially available and is frequently used by
organic chemists as a strong base. Show how you could use butyllithium to pre-
pare solutions containing
(a) Lithium diethylamide, (CH
3
CH
2
)
2
NLi
(b) Lithium 1-hexanolate, CH
3
(CH
2
)
4
CH
2
OLi
(c) Lithium benzenethiolate, C
6
H
5
SLi
SAMPLE SOLUTION When butyllithium is used as a base, it abstracts a proton,
in this case a proton attached to nitrogen. The source of lithium diethylamide
must be diethylamine.
Although diethylamine is not specifically listed in Table 14.2, its strength as an
acid (K
a
H11015 10
H1100236
) is, as might be expected, similar to that of ammonia.
It is sometimes necessary in a synthesis to reduce an alkyl halide to a hydrocar-
bon. In such cases converting the halide to a Grignard reagent and then adding water or
an alcohol as a proton source is a satisfactory procedure. Adding D
2
O to a Grignard
reagent is a commonly used method for introducing deuterium into a molecule at a spe-
cific location.
14.6 SYNTHESIS OF ALCOHOLS USING GRIGNARD REAGENTS
The main synthetic application of Grignard reagents is their reaction with certain car-
bonyl-containing compounds to produce alcohols. Carbon–carbon bond formation is
rapid and exothermic when a Grignard reagent reacts with an aldehyde or ketone.
A carbonyl group is quite polar, and its carbon atom is electrophilic. Grignard reagents
are nucleophilic and add to carbonyl groups, forming a new carbon–carbon bond. This
normally
written as
COMgX
R
C
R
H11001
MgX
O
H11002
MgXR
C O
H9254H11001
H9254H11001H9254H11002
H9254H11002
Mg
THF
D
2
O
1-Bromopropene
CH
3
CH CHBr
Propenylmagnesium bromide
CH
3
CH CHMgBr
1-Deuteriopropene (70%)
CH
3
CH CHD
H11001(CH
3
CH
2
)
2
NH
Diethylamine
(stronger acid)
CH
3
CH
2
CH
2
CH
2
Li
Butyllithium
(stronger base)
H11001(CH
3
CH
2
)
2
NLi
Lithium
diethylamide
(weaker base)
CH
3
CH
2
CH
2
CH
3
Butane
(weaker acid)
CH
3
Li
Methyllithium
(stronger base)
H11001 NH
3
Ammonia
(stronger acid:
K
a
H11005 10
H1100236
)
CH
4
Methane
(weaker acid:
K
a
H33360 10
H1100260
)
H11001 LiNH
2
Lithium amide
(weaker base)
CH
3
CH
2
MgBr
Ethylmagnesium
bromide
(stronger base)
H11001 HCPCH
Acetylene
(stronger acid:
K
a
H33360 10
H1100226
)
CH
3
CH
3
Ethane
(weaker acid:
K
a
H33360 10
H1100262
)
H11001 HCPCMgBr
Ethynylmagnesium
bromide
(weaker base)
14.6 Synthesis of Alcohols Using Grignard Reagents 553
Deuterium is the mass 2 iso-
tope of hydrogen. Deute-
rium oxide (D
2
O) is some-
times called “heavy water.”
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addition step leads to an alkoxymagnesium halide, which in the second stage of the syn-
thesis is converted to an alcohol by adding aqueous acid.
The type of alcohol produced depends on the carbonyl compound. Substituents pres-
ent on the carbonyl group of an aldehyde or ketone stay there—they become substituents
on the carbon that bears the hydroxyl group in the product. Thus as shown in Table 14.3,
formaldehyde reacts with Grignard reagents to yield primary alcohols, aldehydes yield
secondary alcohols, and ketones yield tertiary alcohols.
PROBLEM 14.5 Write the structure of the product of the reaction of propyl-
magnesium bromide with each of the following. Assume that the reactions are
worked up by the addition of dilute aqueous acid.
(a) (c)
(b) (d)
SAMPLE SOLUTION (a) Grignard reagents react with formaldehyde to give pri-
mary alcohols having one more carbon atom than the alkyl halide from which the
Grignard reagent was prepared. The product is 1-butanol.
An ability to form carbon–carbon bonds is fundamental to organic synthesis. The
addition of Grignard reagents to aldehydes and ketones is one of the most frequently
used reactions in synthetic organic chemistry. Not only does it permit the extension of
carbon chains, but since the product is an alcohol, a wide variety of subsequent func-
tional group transformations is possible.
14.7 SYNTHESIS OF ALCOHOLS USING ORGANOLITHIUM
REAGENTS
Organolithium reagents react with carbonyl groups in the same way that Grignard
reagents do. In their reactions with aldehydes and ketones, organolithium reagents are
somewhat more reactive than Grignard reagents.
diethyl
ether H
3
O
H11001
CH
3
CH
2
CH
2
MgBr
C
H
H
O
Propylmagnesium bromide
H11001 formaldehyde
CH
3
CH
2
CH
2
H
H
C OMgBr
CH
3
CH
2
CH
2
CH
2
OH
1-Butanol
2-Butanone, CH
3
CCH
2
CH
3
O
Benzaldehyde, C
6
H
5
CH
O
Cyclohexanone, O
Formaldehyde, HCH
O
H11001H11001H11001H11001H
3
O
H11001
Hydronium
ion
H
2
O
Water
Mg
2H11001
Magnesium
ion
X
H11002
Halide
ion
Alkoxymagnesium
halide
COMgXR
Alcohol
COHR
554 CHAPTER FOURTEEN Organometallic Compounds
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14.7 Synthesis of Alcohols Using Organolithium Reagents 555
TABLE 14.3 Reactions of Grignard Reagents with Aldehydes and Ketones
Reaction
Reaction with formaldehyde
Grignard reagents react with formal-
dehyde (CH
2
?O) to give primary
alcohols having one more carbon
than the Grignard reagent.
Reaction with aldehydes Grignard
reagents react with aldehydes
(RCH?O) to give secondary alcohols.
Reaction with ketones Grignard
reagents react with ketones (RCRH11032)
to give tertiary alcohols.
O
X
General equation and specific example
RMgX
Grignard
reagent
H11001
Formaldehyde
HCH
O
diethyl
ether H
3
O
H11001
OMgX
H
RC
H
Primary
alkoxymagnesium
halide
OH
H
RC
H
Primary
alcohol
RMgX
Grignard
reagent
H11001
Aldehyde
RH11032CH
O
diethyl
ether H
3
O
H11001
OMgX
H
RC
RH11032
Secondary
alkoxymagnesium
halide
OH
H
RC
RH11032
Secondary
alcohol
RMgX
Grignard
reagent
H11001
Ketone
RH11032CRH11033
O
diethyl
ether H
3
O
H11001
OMgXRC
RH11032
RH11033
Tertiary
alkoxymagnesium
halide
OHRC
RH11032
RH11033
Tertiary
alcohol
MgCl
Cyclohexylmagnesium
chloride
CH
2
OH
Cyclohexylmethanol
(64–69%)
H11001
Formaldehyde
HCH
O
1. diethyl ether
2. H
3
O
H11001
H11001CH
3
(CH
2
)
4
CH
2
MgBr
Hexylmagnesium
bromide
Ethanal
(acetaldehyde)
CH
3
CH
O
2-Octanol (84%)
CH
3
(CH
2
)
4
CH
2
CHCH
3
OH
1. diethyl ether
2. H
3
O
H11001
CH
3
MgCl
Methylmagnesium
chloride
O
Cyclopentanone
H11001
1-Methylcyclopentanol
(62%)
H
3
COH
1. diethyl ether
2. H
3
O
H11001
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14.8 SYNTHESIS OF ACETYLENIC ALCOHOLS
The first organometallic compounds we encountered were compounds of the type
RCPCNa obtained by treatment of terminal alkynes with sodium amide in liquid
ammonia (Section 9.6):
These compounds are sources of the nucleophilic anion RCPC
:
H11002
, and their reaction
with primary alkyl halides provides an effective synthesis of alkynes (Section 9.6). The
nucleophilicity of acetylide anions is also evident in their reactions with aldehydes and
ketones, which are entirely analogous to those of Grignard and organolithium reagents.
Acetylenic Grignard reagents of the type RCPCMgBr are prepared, not from an
acetylenic halide, but by an acid–base reaction in which a Grignard reagent abstracts a
proton from a terminal alkyne.
H11001 CH
3
CH
2
MgBr
Ethylmagnesium
bromide
H11001 CH
3
CH
3
Ethane
diethyl ether
CH
3
(CH
2
)
3
CCH
1-Hexyne
CH
3
(CH
2
)
3
C CMgBr
1-Hexynylmagnesium
bromide
HC CNa
Sodium acetylide
H11001
O
Cyclohexanone
1. NH
3
2. H
3
O
H11001
1-Ethynylcyclohexanol
(65–75%)
CHO CH
H11001 RH11032CRH11033
O
Aldehyde
or ketone
H
3
O
H11001
NH
3
RC CNa
Sodium
alkynide
Sodium salt of an
alkynyl alcohol
C ONa
RH11033
RH11032
RC C
Alkynyl
alcohol
CCOH
RH11033
RH11032
RC
NaNH
2
Sodium
amide
H11001RCPCH
Terminal
alkyne
NH
3
Ammonia
H11001RCPCNa
Sodium
alkynide
NH
3
H1100233°C
RLi
Alkyllithium
compound
H11001 C O
Aldehyde
or ketone
R C OLi
Lithium alkoxide
H
3
O
H11001
R C OH
Alcohol
CH
2
CHLi
Vinyllithium
H11001 CH
O
Benzaldehyde
CHCH
OH
CH
2
1-Phenyl-2-propen-1-ol (76%)
1. diethyl ether
2. H
3
O
H11001
556 CHAPTER FOURTEEN Organometallic Compounds
In this particular example,
the product can be variously
described as a secondary al-
cohol, a benzylic alcohol,
and an allylic alcohol. Can
you identify the structural
reason for each classifica-
tion?
These reactions are normally
carried out in liquid ammo-
nia because that is the sol-
vent in which the sodium salt
of the alkyne is prepared.
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PROBLEM 14.6 Write the equation for the reaction of 1-hexyne with ethyl-
magnesium bromide as if it involved ethyl anion instead of
CH
3
CH
2
MgBr and use curved arrows to represent the flow of electrons.
14.9 RETROSYNTHETIC ANALYSIS
In our earlier discussions of synthesis, we stressed the value of reasoning backward from
the target molecule to suitable starting materials. A name for this process is retrosyn-
thetic analysis. Organic chemists have employed this approach for many years, but the
term was invented and a formal statement of its principles was set forth only relatively
recently by E. J. Corey at Harvard University. Beginning in the 1960s, Corey began stud-
ies aimed at making the strategy of organic synthesis sufficiently systematic so that the
power of electronic computers could be applied to assist synthetic planning.
A symbol used to indicate a retrosynthetic step is an open arrow written from prod-
uct to suitable precursors or fragments of those precursors.
Often the precursor is not defined completely, but rather its chemical nature is empha-
sized by writing it as a species to which it is equivalent for synthetic purposes. Thus, a
Grignard reagent or an organolithium reagent might be considered synthetically equiva-
lent to a carbanion:
Figure 14.2 illustrates how retrosynthetic analysis can guide you in planning the
synthesis of alcohols by identifying suitable Grignard reagent and carbonyl-containing
precursors. In the first step, locate the carbon of the target alcohol that bears the hydroxyl
group, remembering that this carbon originated in the C?O group. Next, as shown in
Figure 14.2, step 2, mentally disconnect a bond between that carbon and one of its
attached groups (other than hydrogen). The attached group is the group that is to be trans-
ferred from the Grignard reagent. Once you recognize these two structural fragments,
the carbonyl partner and the carbanion that attacks it (Figure 14.2, step 3), you can read-
ily determine the synthetic mode wherein a Grignard reagent is used as the synthetic
equivalent of a carbanion (Figure 14.2, step 4).
Primary alcohols, by this analysis, are seen to be the products of Grignard addi-
tion to formaldehyde:
Disconnect this bond
RC
H
H
OH R
H11002
O
H
H
C
RMgX or RLi is synthetically equivalent to R
H11002
Target molecule precursors
(CH
3
CH
2
H11002
)
CH
3
(CH
2
)
3
C CMgBr
1-Hexynylmagnesium
bromide
CH
3
(CH
2
)
3
C CCH
2
OH
2-Heptyn-1-ol (82%)
H11001 HCH
O
Formaldehyde
1. diethyl ether
2. H
3
O
H11001
14.9 Retrosynthetic Analysis 557
Corey was honored with the
1990 Nobel Prize for his
achievements in synthetic or-
ganic chemistry.
Problem 14.6 at the end of
the preceding section intro-
duced this idea with the sug-
gestion that ethylmagnesium
bromide be represented as
ethyl anion.
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Secondary alcohols may be prepared by two different combinations of Grignard
reagent and aldehyde:
R
H11002
H
RH11032
OC R C
H
RH11032
OH RH11032
H11002
H
R
OC
Disconnect R±C Disconnect RH11032±C
558 CHAPTER FOURTEEN Organometallic Compounds
Step 1: Locate the hydroxyl-bearing carbon.
Step 2: Disconnect one of the organic substituents attached to the carbon that
bears the hydroxyl group.
Step 3: Steps 1 and 2 reveal the carbonyl-containing substrate and the
carbanionic fragment.
Step 4: Since a Grignard reagent may be considered as synthetically equivalent to
a carbanion, this suggests the synthesis shown.
RMgBr
This carbon must have been part of the C?O
group in the starting material
X
C
Y
O
R
H11002
H11001 C O
X
Y
1. diethyl
ether
2. H
3
O
H11001
R
X
C
Y
OH
R
XYC
OH
Disconnect this bondR
XYC
OH
R
XYC
OH
FIGURE 14.2 A retrosynthetic analysis of alcohol preparation by way of the addition of a
Grignard reagent to an aldehyde or ketone.
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Three combinations of Grignard reagent and ketone give rise to tertiary alcohols:
Usually, there is little to choose among the various routes leading to a particular
target alcohol. For example, all three of the following combinations have been used to
prepare the tertiary alcohol 2-phenyl-2-butanol:
PROBLEM 14.7 Suggest two ways in which each of the following alcohols might
be prepared by using a Grignard reagent:
(a)
(b)
SAMPLE SOLUTION (a) Since 2-hexanol is a secondary alcohol, we consider the
reaction of a Grignard reagent with an aldehyde. Disconnection of bonds to the
hydroxyl-bearing carbon generates two pairs of structural fragments:
2-Phenyl-2-propanol, C
6
H
5
C(CH
3
)
2
OH
2-Hexanol, CH
3
CHCH
2
CH
2
CH
2
CH
3
OH
CH
3
MgI
Methylmagnesium
iodide
H11001 CCH
2
CH
3
O
1-Phenyl-1-propanone
CH
3
CCH
2
CH
3
OH
2-Phenyl-2-butanol
1. diethyl ether
2. H
3
O
H11001
CH
3
CH
2
MgBr
Ethylmagnesium
bromide
H11001 CCH
3
O
Acetophenone
CH
3
CCH
2
CH
3
OH
2-Phenyl-2-butanol
1. diethyl ether
2. H
3
O
H11001
MgBr
Phenylmagnesium
bromide
H11001 CH
3
CCH
2
CH
3
O
2-Butanone
CH
3
CCH
2
CH
3
OH
2-Phenyl-2-butanol
1. diethyl ether
2. H
3
O
H11001
R
H11002
RH11033
RH11032
OC RC
RH11032
RH11033
OH RH11032
H11002
RH11033
R
OC
Disconnect R±C Disconnect RH11032±C
Disconnect RH11033±C
RH11033
H11002
RH11032
R
OC
14.9 Retrosynthetic Analysis 559
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Therefore, one route involves the addition of a methyl Grignard reagent to a five-
carbon aldehyde:
The other requires addition of a butylmagnesium halide to a two-carbon alde-
hyde:
All that has been said in this section applies with equal force to the use of organo-
lithium reagents in the synthesis of alcohols. Grignard reagents are one source of nucleo-
philic carbon; organolithium reagents are another. Both have substantial carbanionic
character in their carbon–metal bonds and undergo the same kind of reaction with alde-
hydes and ketones.
14.10 PREPARATION OF TERTIARY ALCOHOLS FROM ESTERS AND
GRIGNARD REAGENTS
Tertiary alcohols can be prepared by a variation of the Grignard synthesis that employs
an ester as the carbonyl component. Methyl and ethyl esters are readily available and
are the types most often used. Two moles of a Grignard reagent are required per mole
of ester; the first mole reacts with the ester, converting it to a ketone.
The ketone is not isolated, but reacts rapidly with the Grignard reagent to give, after
adding aqueous acid, a tertiary alcohol. Ketones are more reactive than esters toward
Grignard reagents, and so it is not normally possible to interrupt the reaction at the ketone
stage even if only one equivalent of the Grignard reagent is used.
RMgX
Grignard
reagent
H11001 RH11032COCH
3
O
Methyl
ester
diethyl ether
RH11032C OCH
3
O
R
MgX
RH11032CR
O
Ketone
H11001 CH
3
OMgX
Methoxymagnesium
halide
CH
3
CH
2
CH
2
CH
2
MgBr
Butylmagnesium
bromide
H11001
Acetaldehyde
CH
3
CH
O
1. diethyl ether
2. H
3
O
H11001
CH
3
CH
2
CH
2
CH
2
CHCH
3
OH
2-Hexanol
CH
3
MgI
Methylmagnesium
iodide
H11001
Pentanal
CH
3
CH
2
CH
2
CH
2
CH
O
1. diethyl ether
2. H
3
O
H11001
CH
3
CH
2
CH
2
CH
2
CHCH
3
OH
2-Hexanol
and
CH
3
CHCH
2
CH
2
CH
2
CH
3
OH
CH
3
CHCH
2
CH
2
CH
2
CH
3
OH
H11002
CH
2
CH
2
CH
2
CH
3
HCCH
2
CH
2
CH
2
CH
3
O
H11002
CH
3
CH
3
CH
O
560 CHAPTER FOURTEEN Organometallic Compounds
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Two of the groups bonded to the hydroxyl-bearing carbon of the alcohol are the same
because they are derived from the Grignard reagent. For example,
PROBLEM 14.8 What combination of ester and Grignard reagent could you use
to prepare each of the following tertiary alcohols?
(a) (b)
SAMPLE SOLUTION (a) To apply the principles of retrosynthetic analysis to this
case, we disconnect both ethyl groups from the tertiary carbon and identify them
as arising from the Grignard reagent. The phenyl group originates in an ester of
the type C
6
H
5
CO
2
R (a benzoate ester).
An appropriate synthesis would be
14.11 ALKANE SYNTHESIS USING ORGANOCOPPER REAGENTS
Organometallic compounds of copper have been known for a long time, but their ver-
satility as reagents in synthetic organic chemistry has only recently been recognized. The
most useful organocopper reagents are the lithium dialkylcuprates, which result when a
copper(I) halide reacts with two equivalents of an alkyllithium in diethyl ether or tetrahy-
drofuran.
H11001H110012RLi
Alkyllithium
CuX
Cu(I) halide
(X H11005 Cl, Br, I)
LiX
Lithium
halide
R
2
CuLi
Lithium
dialkylcuprate
diethyl ether
or THF
2CH
3
CH
2
MgBr
Ethylmagnesium
bromide
H11001
Methyl
benzoate
C
6
H
5
COCH
3
O
1. diethyl ether
2. H
3
O
H11001
C
6
H
5
C(CH
2
CH
3
)
2
OH
3-Phenyl-3-pentanol
C
6
H
5
C(CH
2
CH
3
)
2
OH
C
6
H
5
COR
O
H11001 2CH
3
CH
2
MgX
(C
6
H
5
)
2
C
OH
C
6
H
5
C(CH
2
CH
3
)
2
OH
2CH
3
MgBr
Methylmagnesium
bromide
CH
3
OH
Methanol
H11001H11001(CH
3
)
2
CHCCH
3
OH
CH
3
2,3-Dimethyl-
2-butanol (73%)
(CH
3
)
2
CHCOCH
3
O
Methyl
2-methylpropanoate
1. diethyl ether
2. H
3
O
H11001
RMgX
Grignard
reagent
H11001 RH11032CR
OH
R
Tertiary
alcohol
RH11032CR
O
Ketone
1. diethyl ether
2. H
3
O
H11001
14.11 Alkane Synthesis Using Organocopper Reagents 561
Copper(I) salts are also
known as cuprous salts.
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In the first stage of the preparation, one molar equivalent of alkyllithium displaces halide
from copper to give an alkylcopper(I) species:
The second molar equivalent of the alkyllithium adds to the alkylcopper to give a neg-
atively charged dialkyl-substituted derivative of copper(I) called a dialkylcuprate anion.
It is formed as its lithium salt, a lithium dialkylcuprate.
Lithium dialkylcuprates react with alkyl halides to produce alkanes by carbon–car-
bon bond formation between the alkyl group of the alkyl halide and the alkyl group of
the dialkylcuprate:
Primary alkyl halides, especially iodides, are the best substrates. Elimination becomes a
problem with secondary and tertiary alkyl halides:
Lithium diarylcuprates are prepared in the same way as lithium dialkylcuprates and
undergo comparable reactions with primary alkyl halides:
The most frequently used organocuprates are those in which the alkyl group is pri-
mary. Steric hindrance makes organocuprates that bear secondary and tertiary alkyl
groups less reactive, and they tend to decompose before they react with the alkyl halide.
The reaction of cuprate reagents with alkyl halides follows the usual S
N
2 order: CH
3
H11022
primary H11022 secondary H11022 tertiary, and I H11022 Br H11022 Cl H11022 F. p-Toluenesulfonate esters are
suitable substrates and are somewhat more reactive than halides. Because the alkyl halide
and dialkylcuprate reagent should both be primary in order to produce satisfactory yields
of coupled products, the reaction is limited to the formation of RCH
2
±CH
2
RH11032 and
RCH
2
±CH
3
bonds in alkanes.
A key step in the reaction mechanism appears to be nucleophilic attack on the
alkyl halide by the negatively charged copper atom, but the details of the mechanism
are not well understood. Indeed, there is probably more than one mechanism by which
H11001(C
6
H
5
)
2
CuLi
Lithium
diphenylcuprate
ICH
2
(CH
2
)
6
CH
3
1-Iodooctane
C
6
H
5
CH
2
(CH
2
)
6
CH
3
1-Phenyloctane (99%)
diethyl ether
H11001(CH
3
)
2
CuLi
Lithium
dimethylcuprate
CH
3
(CH
2
)
8
CH
2
I
1-Iododecane
CH
3
(CH
2
)
8
CH
2
CH
3
Undecane (90%)
ether
0°C
R
2
CuLi
Lithium
dialkylcuprate
RRH11032
Alkane
RH11032X
Alkyl halide
RCu
Alkylcopper
LiX
Lithium
halide
H11001 H11001H11001
Li R
Alkyllithium
[R Cu R]Li
H11001
H11002
Lithium dialkylcuprate
(soluble in ether and in THF)
Cu R
Alkylcopper
H11001
RLi
Cu I
LiI
Lithium iodide
H11001RCu
Alkylcopper
562 CHAPTER FOURTEEN Organometallic Compounds
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cuprates react with organic halogen compounds. Vinyl halides and aryl halides
are known to be very unreactive toward nucleophilic attack, yet react with lithium
dialkylcuprates:
PROBLEM 14.9 Suggest a combination of organic halide and cuprate reagent
appropriate for the preparation of each of the following compounds:
(a) 2-Methylbutane
(b) 1,3,3-Trimethylcyclopentene
SAMPLE SOLUTION (a) First inspect the target molecule to see which bonds are
capable of being formed by reaction of an alkyl halide and a cuprate, bearing in
mind that neither the alkyl halide nor the alkyl group of the lithium dialkylcuprate
should be secondary or tertiary.
There are two combinations, both acceptable, that give the CH
3
±CH
2
bond:
14.12 AN ORGANOZINC REAGENT FOR CYCLOPROPANE SYNTHESIS
Zinc reacts with alkyl halides in a manner similar to that of magnesium.
Organozinc reagents are not nearly as reactive toward aldehydes and ketones as Grignard
reagents and organolithium compounds but are intermediates in certain reactions of
alkyl halides.
An organozinc compound that occupies a special niche in organic synthesis is
iodomethylzinc iodide (ICH
2
ZnI), prepared by the reaction of zinc–copper couple
[Zn(Cu), zinc that has had its surface activated with a little copper] with diiodomethane
in ether.
H11001RX
Alkyl halide
Zn
Zinc Alkylzinc halide
RZnX
ether
(CH
3
)
2
CuLi
Lithium
dimethylcuprate
H11001
1-Bromo-
2-methylpropane
BrCH
2
CH(CH
3
)
2
CH
3
CH
2
CH(CH
3
)
2
2-Methylbutane
CH
3
I
Iodomethane
H11001
Lithium diisobutylcuprate
LiCu[CH
2
CH(CH
3
)
2
]
2
CH
3
CH
2
CH(CH
3
)
2
2-Methylbutane
A bond between a
methyl group and a
methylene group can
be formed.
None of the bonds to the
methine group can be
formed efficiently.
CH
3
CH
2
CH
3
CH CH
3
14.12 An Organozinc Reagent for Cyclopropane Synthesis 563
diethyl ether
(CH
3
CH
2
CH
2
CH
2
)
2
CuLi
Lithium dibutylcuprate
H11001 Br
1-Bromocyclohexene
CH
2
CH
2
CH
2
CH
3
1-Butylcyclohexene (80%)
diethyl ether
(CH
3
CH
2
CH
2
CH
2
)
2
CuLi
Lithium dibutylcuprate
I
Iodobenzene
CH
2
CH
2
CH
2
CH
3
Butylbenzene (75%)
H11001
Victor Grignard was led to
study organomagnesium
compounds because of ear-
lier work he performed with
organic derivatives of zinc.
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What makes iodomethylzinc iodide such a useful reagent is that it reacts with alkenes
to give cyclopropanes.
This reaction is called the Simmons–Smith reaction and is one of the few methods avail-
able for the synthesis of cyclopropanes. Mechanistically, the Simmons–Smith reaction
seems to proceed by a single-step cycloaddition of a methylene (CH
2
) unit from
iodomethylzinc iodide to the alkene:
PROBLEM 14.10 What alkenes would you choose as starting materials in order
to prepare each of the following cyclopropane derivatives by reaction with
iodomethylzinc iodide?
(a) (b)
SAMPLE SOLUTION (a) In a cyclopropane synthesis using the Simmons–Smith
reagent, you should remember that a CH
2
unit is transferred. Therefore, retro-
synthetically disconnect the bonds to a CH
2
group of a three-membered ring to
identify the starting alkene.
The complete synthesis is:
Methylene transfer from iodomethylzinc iodide is stereospecific. Substituents that
were cis in the alkene remain cis in the cyclopropane.
CH
3
1-Methylcycloheptene
CH
3
1-Methylbicyclo[5.1.0]octane (55%)
CH
2
I
2
, Zn(Cu)
diethyl ether
[CH
2
]
CH
2
CH
3
CH
3
H11001
CH
3
ZnI
2
ICH
2
ZnI
C C
C
CH
2
C
I ZnI
Transition state for methylene transfer
C
CH
2
C H11001
CH
2
CH
3
CH
2
CH
3
C
2-Methyl-1-butene
CH
2
CH
3
CH
3
1-Ethyl-1-methylcyclopropane (79%)
CH
2
I
2
, Zn(Cu)
diethyl ether
H11001ICH
2
I
Diiodomethane
Zn
Zinc Iodomethylzinc iodide
ICH
2
ZnI
diethyl ether
Cu
564 CHAPTER FOURTEEN Organometallic Compounds
Iodomethylzinc iodide is
known as the Simmons–
Smith reagent, after Howard
E. Simmons and Ronald D.
Smith of Du Pont, who first
described its use in the
preparation of cyclo-
propanes.
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Yields in Simmons–Smith reactions are sometimes low. Nevertheless, since it often
provides the only feasible route to a particular cyclopropane derivative, it is a valuable
addition to the organic chemist’s store of synthetic methods.
14.13 CARBENES AND CARBENOIDS
Iodomethylzinc iodide is often referred to as a carbenoid, meaning that it resembles a
carbene in its chemical reactions. Carbenes are neutral molecules in which one of the
carbon atoms has six valence electrons. Such carbons are divalent; they are directly
bonded to only two other atoms and have no multiple bonds. Iodomethylzinc iodide
reacts as if it were a source of the carbene .
It is clear that free
:
CH
2
is not involved in the Simmons–Smith reaction, but there
is substantial evidence to indicate that carbenes are formed as intermediates in certain
other reactions that convert alkenes to cyclopropanes. The most studied examples of these
reactions involve dichlorocarbene and dibromocarbene.
Carbenes are too reactive to be isolated and stored, but have been trapped in frozen argon
for spectroscopic study at very low temperatures.
Dihalocarbenes are formed when trihalomethanes are treated with a strong base,
such as potassium tert-butoxide. The trihalomethyl anion produced on proton abstraction
dissociates to a dihalocarbene and a halide anion:
When generated in the presence of an alkene, dihalocarbenes undergo cycloaddition to
the double bond to give dihalocyclopropanes:
Br
3
CH
Tribromomethane
H11001 OC(CH
3
)
3
H11002
tert-Butoxide
ion
Br
3
C
H11002
Tribromomethide
ion
H11001 H OC(CH
3
)
3
tert-Butyl
alcohol
C
Br
Br
Br
H11002
Tribromomethide ion
Br
Br
C
Dibromocarbene
H11001 Br
H11002
Bromide ion
C
Cl Cl
Dichlorocarbene
C
Br Br
Dibromocarbene
H±C±H
CH
2
I
2
Zn(Cu)
ether
CH
2
CH
3
HH
CH
3
CH
2
CC
(Z)-3-Hexene
CH
3
CH
2
H
CH
2
CH
3
H
cis-1,2-Diethylcyclopropane (34%)
CH
2
I
2
Zn(Cu)
ether
CH
2
CH
3
H
H
CH
3
CH
2
CC
(E)-3-Hexene
CH
3
CH
2
HCH
2
CH
3
H
trans-1,2-Diethylcyclopropane (15%)
14.13 Carbenes and Carbenoids 565
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The reaction of dihalocarbenes with alkenes is stereospecific, and syn addition is
observed.
PROBLEM 14.11 The syn stereochemistry of dibromocarbene cycloaddition was
demonstrated in experiments using cis- and trans-2-butene. Give the structure of
the product obtained from addition of dibromocarbene to each alkene.
The process in which a dihalocarbene is formed from a trihalomethane corresponds
to an elimination in which a proton and a halide are lost from the same carbon. It is an
H9251-elimination proceeding via the organometallic intermediate K
H11001
[
:
CX
3
]
H11002
.
14.14 TRANSITION-METAL ORGANOMETALLIC COMPOUNDS
A large number of organometallic compounds are based on transition metals. Examples
include organic derivatives of iron, nickel, chromium, platinum, and rhodium. Many
important industrial processes are catalyzed by transition metals or their complexes.
Before we look at these processes, a few words about the structures of transition-metal
complexes are in order.
A transition-metal complex consists of a transition-metal atom or ion bearing
attached groups called ligands. Essentially, anything attached to a metal is a ligand. A
ligand can be an element (O
2
, N
2
), a compound (NO), or an ion (CN
H11002
); it can be inor-
ganic as in the examples just cited or it can be an organic ligand. Ligands differ in the
number of electrons that they share with the transition metal to which they are attached.
Carbon monoxide is a frequently encountered ligand in transition-metal complexes and
contributes two electrons; it is best thought of in terms of the Lewis structure
in which carbon is the reactive site. An example of a carbonyl complex of a transition
metal is nickel carbonyl, a very toxic substance, which was first prepared over a hun-
dred years ago and is an intermediate in the purification of nickel. It forms spontaneously
when carbon monoxide is passed over elemental nickel.
Many transition-metal complexes, including Ni(CO)
4
, obey what is called the 18-
electron rule, which is to transition-metal complexes as the octet rule is to main-group
elements. It states that for transition-metal complexes, the number of ligands that can be
attached to a metal will be such that the sum of the electrons brought by the ligands
plus the valence electrons of the metal equals 18. With an atomic number of 28, nickel
has the electron configuration [Ar]4s
2
3d
8
(10 valence electrons). The 18-electron rule is
satisfied by adding to these 10 the 8 electrons from four carbon monoxide ligands. A
useful point to remember about the 18-electron rule when we discuss some reactions of
transition-metal complexes is that if the number is less than 18, the metal is considered
coordinatively unsaturated and can accept additional ligands.
PROBLEM 14.12 Like nickel, iron reacts with carbon monoxide to form a com-
pound having the formula M(CO)
n
that obeys the 18-electron rule. What is the
value of n in the formula Fe(CO)
n
?
H11001Ni
Nickel
4CO
Carbon monoxide
Ni(CO)
4
Nickel carbonyl
CPO
H11002H11001
Cyclohexene
H11001 CHBr
3
Tribromomethane
KOC(CH
3
)
3
(CH
3
)
3
COH
Br
Br
7,7-Dibromobicyclo[4.1.0]heptane (75%)
566 CHAPTER FOURTEEN Organometallic Compounds
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14.15 Ziegler–Natta Catalysis of Alkene Polymerization 567
Not all ligands use just two electrons to bond to transition metals. Chromium has
the electron configuration [Ar]4s
2
3d
4
(6 valence electrons) and needs 12 more to satisfy
the 18-electron rule. In the compound (benzene)tricarbonylchromium, 6 of these 12 are
the H9266 electrons of the benzene ring; the remaining 6 are from the three carbonyl ligands.
Ferrocene has an even more interesting structure. A central iron is H9266-bonded to two
cyclopentadienyl ligands in what is aptly described as a sandwich. It, too, obeys the 18-
electron rule. Each cyclopentadienyl ligand contributes 5 electrons for a total of 10 and
iron, with an electron configuration of [Ar]4s
2
3d
6
contributes 8. Alternatively, ferrocene
can be viewed as being derived from Fe
2H11001
(6 valence electrons) and two aromatic
cyclopentadienide rings (6 electrons each). Indeed, ferrocene was first prepared by adding
iron(II) chloride to cyclopentadienylsodium. Instead of the expected H9268-bonded species
shown in the equation, ferrocene was formed.
After ferrocene, a large number of related molecules have been prepared—even
some in which uranium is the metal. There is now an entire subset of transition-metal
organometallic complexes known as metallocenes based on cyclopentadienide ligands.
These compounds are not only structurally interesting, but many of them have useful
applications as catalysts for industrial processes.
Naturally occurring compounds with carbon–metal bonds are very rare. The best
example of such an organometallic compound is coenzyme B
12
, which has a
carbon–cobalt H9268 bond (Figure 14.3). Pernicious anemia results from a coenzyme B
12
deficiency and can be treated by adding sources of cobalt to the diet. One source of
cobalt is vitamin B
12
, a compound structurally related to, but not identical with, coen-
zyme B
12
.
14.15 ZIEGLER–NATTA CATALYSIS OF ALKENE POLYMERIZATION
In Section 6.21 we listed three main methods for polymerizing alkenes: cationic, free-
radical, and coordination polymerization. In Section 7.15 we extended our knowledge of
polymers to their stereochemical aspects by noting that although free-radical polymer-
ization of propene gives atactic polypropylene, coordination polymerization produces a
stereoregular polymer with superior physical properties. Because the catalysts responsi-
ble for coordination polymerization are organometallic compounds, we are now in a posi-
tion to examine coordination polymerization in more detail, especially with respect to
how the catalyst works.
2
H11002
Na
H11001
Cyclopentadienylsodium
H11001 FeCl
2
Iron(II)
chloride
H
Fe
H
(Not formed)
H11001 2NaCl
(Benzene)tricarbonylchromium
HH
HH
HH
Cr
CO
COOC
Fe
Ferrocene
Cyclopentadienylsodium is
ionic. Its anion is the cyclo-
pentadienide ion, which con-
tains six H9266 electrons.
The first page of this
chapter displayed an electrosta-
tic potential map of ferrocene.
You may wish to view a molecu-
lar model of it on Learning By
Modeling.
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568 CHAPTER FOURTEEN Organometallic Compounds
AN ORGANOMETALLIC COMPOUND THAT OCCURS NATURALLY: COENZYME B
12
P
ernicious anemia is a disease characterized, as
are all anemias, by a deficiency of red blood
cells. Unlike ordinary anemia, pernicious anemia
does not respond to treatment with sources of iron,
and before effective treatments were developed, was
often fatal. Injection of liver extracts was one such
treatment, and in 1948 chemists succeeded in isolat-
ing the “antipernicious anemia factor” from beef
liver as a red crystalline compound, which they called
vitamin B
12
. This compound had the formula
C
63
H
88
CoN
14
O
14
P. Its complexity precluded structure
determination by classical degradation techniques,
and spectroscopic methods were too primitive to be
of much help. The structure was solved by Dorothy
Crowfoot Hodgkin of Oxford University in 1955 using
X-ray diffraction techniques and is shown in Figure
14.3a. Structure determination by X-ray crystallogra-
phy can be superficially considered as taking a photo-
graph of a molecule with X-rays. It is a demanding
task and earned Hodgkin the 1964 Nobel Prize in
chemistry. Modern structural studies by X-ray crystal-
lography use computers to collect and analyze the
diffraction data and take only a fraction of the time
required years ago to solve the vitamin B
12
structure.
The structure of vitamin B
12
is interesting in
that it contains a central cobalt atom that is sur-
rounded by six atoms in an octahedral geometry. One
substituent, the cyano (±CN) group, is what is
known as an “artifact.” It appears to be introduced
into the molecule during the isolation process and
leads to the synonym cyanocobalamin for vitamin
B
12
. This material is used to treat pernicious anemia,
but this is not the form in which it exerts its activity.
The biologically active material is called coenzyme
B
12
and differs from vitamin B
12
in the substituent at-
tached to cobalt (Figure 14.3b). Coenzyme B
12
is the
only known naturally occurring substance that has a
carbon–metal bond. Moreover, coenzyme B
12
was
discovered before any compound containing an alkyl
group H9268-bonded to cobalt had ever been isolated in
the laboratory!
N
N
N
N
O
O
O
P
O
H11002
HO
O
O
HN
O
O
O
H
2
N
H
2
N
H
2
N
HOCH
2
H
3
C
O
CH
3
CH
3
N
N
N
O
O
N
R
Co
H11001 (a)
O N
N
H
2
N
CH
2
OHHO
(b) R H11005
R H11005H11002C
P
N
CH
3
CH
3
CH
3
CH
3
CH
3
NH
2
H
3
C
NH
2
NH
2
CH
3
CH
3
FIGURE 14.3 The structures of (a) vitamin B
12
and (b) coenzyme B
12
.
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In the early 1950s, Karl Ziegler, then at the Max Planck Institute for Coal Research
in Germany, was studying the use of aluminum compounds as catalysts for the oligomer-
ization of ethylene.
Ziegler found that adding certain metals or their compounds to the reaction mixture led
to the formation of ethylene oligomers with 6–18 carbons, but others promoted the for-
mation of very long carbon chains giving polyethylene. Both were major discoveries.
The 6–18 carbon ethylene oligomers constitute a class of industrial organic chemicals
known as linear H9251 olefins that are produced at a rate of 10
9
pounds/year in the United
States. The Ziegler route to polyethylene is even more important because it occurs at
modest temperatures and pressures and gives high-density polyethylene, which has prop-
erties superior to the low-density material formed by free-radical polymerization
described in Section 6.21.
A typical Ziegler catalyst is a combination of titanium tetrachloride (TiCl
4
) and
diethylaluminum chloride [(CH
3
CH
2
)
2
AlCl], but other combinations such as
TiCl
3
/(CH
3
CH
2
)
3
Al also work as do catalysts based on metallocenes. Although still in
question, a plausible mechanism for the polymerization of ethylene in the presence of
such catalysts has been offered and is outlined in Figure 14.4.
Al(CH
2
CH
3
)
3
Ethylene
nH
2
C CH
2
Ethylene oligomers
CH
3
CH
2
(CH
2
CH
2
)
nH110022
CH CH
2
14.15 Ziegler–Natta Catalysis of Alkene Polymerization 569
Step 1: A titanium halide and an ethylaluminum compound combine to place an ethyl group on titanium, giving
the active catalyst. Titanium has one or more vacant coordination sites, shown here as an empty orbital.
Step 2: Ethylene reacts with the active form of the catalyst. The π orbital of ethylene with its two electrons
overlaps with the vacant titanium orbital to bind ethylene as a ligand to titanium.
Step 3: The flow of electrons from ethylene to titanium increases the electron density at titanium and weakens
the TiQCH
2
CH
3
bond. The ethyl group migrates from titanium to one of the carbons of ethylene.
Step 4: The catalyst now has a butyl ligand on titanium instead of an ethyl group. Repeating steps 2 and 3
converts the butyl group to a hexyl group, then an octyl group, and so on. After thousands of repetitions,
polyethylene is formed.
CH
3
CH
2
Cl
n
Ti
W
H11001 H
2
C?CH
2
X
CH
2
CH
2
CH
3
CH
2
W
CH
2
Cl
n
Ti±CH
2
CH
3
CH
2
Cl
n
Ti
W
CH
3
CH
2
Cl
n
Ti
W
X
CH
2
CH
2
CH
3
CH
2
Cl
n
Ti
W
FIGURE 14.4 A proposed mechanism for the polymerization of ethylene in the presence of a Ziegler–Natta catalyst.
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Ziegler had a working relationship with the Italian chemical company Montecatini,
for which Giulio Natta of the Milan Polytechnic Institute was a consultant. When Natta
used Ziegler’s catalyst to polymerize propene, he discovered that the catalyst was not
only effective but that it gave mainly isotactic polypropylene. (Recall from Section 7.15
that free-radical polymerization of propene gives atactic polypropylene.) Isotactic
polypropylene has a higher melting point than the atactic form and can be drawn into
fibers or molded into hard, durable materials. Before coordination polymerization was
discovered by Ziegler and applied to propene by Natta, there was no polypropylene indus-
try. Now, more than 10
10
pounds of it are prepared each year in the United States. Ziegler
and Natta shared the 1963 Nobel Prize in chemistry: Ziegler for discovering novel cat-
alytic systems for alkene polymerization and Natta for stereoregular polymerization.
14.16 SUMMARY
Section 14.1 Organometallic compounds contain a carbon–metal bond. They are
named as alkyl (or aryl) derivatives of metals.
Section 14.2 Carbon is more electronegative than metals and carbon–metal bonds are
polarized so that carbon bears a partial to complete negative charge and
the metal bears a partial to complete positive charge.
Section 14.3 See Table 14.4
Section 14.4 See Table 14.4
Section 14.5 Organolithium compounds and Grignard reagents are strong bases and
react instantly with compounds that have ±OH groups.
These organometallic compounds cannot therefore be formed or used in
solvents such as water and ethanol. The most commonly employed sol-
vents are diethyl ether and tetrahydrofuran.
Section 14.6 See Tables 14.3 and 14.5
Section 14.7 See Table 14.5
Section 14.8 See Table 14.5
Section 14.9 When planning the synthesis of a compound using an organometallic
reagent, or indeed any synthesis, the best approach is to reason backward
from the product. This method is called retrosynthetic analysis. Retro-
synthetic analysis of 1-methylcyclohexanol suggests it can be prepared
by the reaction of methylmagnesium bromide and cyclohexanone.
RHRM H11001H11001
H11002
ORH11032M
H11001
HORH11032
HC Na
H11001
C
H11002
Sodium acetylide has an
ionic bond between carbon
and sodium.
H9254H11002
C Li
H9254H11001
H
H
H
Methyllithium has a polar
covalent carbon–lithium
bond.
Butyllithium
CH
3
CH
2
CH
2
CH
2
Li
Phenylmagnesium bromide
C
6
H
5
MgBr
570 CHAPTER FOURTEEN Organometallic Compounds
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Section 14.10 See Table 14.5
Section 14.11 See Tables 14.4 and 14.5
Section 14.12 See Tables 14.4 and 14.5
Section 14.13 Carbenes are species that contain a divalent carbon; that is, a carbon with
only two bonds. One of the characteristic reactions of carbenes is with
alkenes to give cyclopropane derivatives.
KOC(CH
3
)
3
(CH
3
)
3
COH
H11001
Cl
CH
3
CH
3
Cl
1,1-Dichloro-2,2-dimethylcyclopropane
(65%)
2-Methylpropene
CH
3
CH
3
H
2
C C CHCl
3
CH
3
MgBr
Methylmagnesium
bromide
H11001O
Cyclohexanone1-Methylcyclohexanol
CH
3
OH
14.16 Summary 571
TABLE 14.4 Preparation of Organometallic Reagents Used in Synthesis
Type of organometallic reagent
(section) and comments
Organolithium reagents (Section 14.3) Lithi-
um metal reacts with organic halides to pro-
duce organolithium compounds. The organic
halide may be alkyl, alkenyl, or aryl. Iodides
react most and fluorides least readily; bro-
mides are used most often. Suitable solvents
include hexane, diethyl ether, and tetrahy-
drofuran.
Lithium dialkylcuprates (Section 14.11) These
reagents contain a negatively charged cop-
per atom and are formed by the reaction of
a copper(I) salt with two equivalents of an
organolithium reagent.
Iodomethylzinc iodide (Section 14.12) This is
the Simmons–Smith reagent. It is prepared
by the reaction of zinc (usually in the pres-
ence of copper) with diiodomethane.
Grignard reagents (Section 14.4) Grignard
reagents are prepared in a manner similar to
that used for organolithium compounds.
Diethyl ether and tetrahydrofuran are appro-
priate solvents.
General equation for preparation
and specific example
H11001
Magnesium
Mg RMgX
Alkylmagnesium halide
(Grignard reagent)
RX
Alkyl
halide
H11001
Copper(I)
halide
CuX2RLi
Alkyllithium
H11001
Lithium
halide
LiXR
2
CuLi
Lithium
dialkylcuprate
CH
3
CH
2
CH
2
Br
Propyl bromide
CH
3
CH
2
CH
2
Li
Propyllithium (78%)
Li
diethyl ether
Lithium
2Li H11001
Lithium
halide
LiX
Alkyl
halide
RX
Alkyllithium
RLiH11001
2CH
3
Li
Methyllithium
CuI
Copper(I)
iodide
H11001 (CH
3
)
2
CuLi
Lithium
dimethylcuprate
LiI
Lithium
iodide
H11001
diethyl ether
C
6
H
5
CH
2
Cl
Benzyl chloride
C
6
H
5
CH
2
MgCl
Benzylmagnesium chloride (93%)
Mg
diethyl ether
H11001CH
2
I
2
Diiodomethane
ICH
2
ZnI
Iodomethylzinc
iodide
Zn
Zinc
diethyl ether
Cu
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Certain organometallic compounds resemble carbenes in their reactions
and are referred to as carbenoids. Iodomethylzinc iodide (Section 14.12)
is an example.
Section 14.14 Transition-metal complexes that contain one or more organic ligands
offer a rich variety of structural types and reactivity. Organic ligands can
be bonded to a metal by a H9268 bond or through its H9266 system. Metallocenes
are transition-metal complexes in which one or more of the ligands is a
572 CHAPTER FOURTEEN Organometallic Compounds
TABLE 14.5 Carbon–Carbon Bond-Forming Reactions of Organometallic Reagents
Reaction (section) and comments
Alcohol synthesis via the reaction of
Grignard reagents with carbonyl com-
pounds (Section 14.6) This is one of the
most useful reactions in synthetic organ-
ic chemistry. Grignard reagents react
with formaldehyde to yield primary alco-
hols, with aldehydes to give secondary
alcohols, and with ketones to form terti-
ary alcohols.
Synthesis of alcohols using organolithi-
um reagents (Section 14.7) Organolithi-
um reagents react with aldehydes and
ketones in a manner similar to that of
Grignard reagents to produce alcohols.
Reaction of Grignard reagents with
esters (Section 14.10) Tertiary alcohols in
which two of the substituents on the
hydroxyl carbon are the same may be
prepared by the reaction of an ester
with two equivalents of a Grignard
reagent.
(Continued)
General equation and specific example
Aldehyde
or ketone
RH11032CRH11033
O
X
Grignard
reagent
RMgX
Alcohol
RCOH
W
W
RH11032
RH11033
H11001
1. diethyl ether
2. H
3
O
H11001
Ester
RH11032CORH11033
O
X
Grignard
reagent
2RMgX
Tertiary
alcohol
RCOH
W
W
RH11032
R
H11001
1. diethyl ether
2. H
3
O
H11001
Aldehyde
or ketone
RH11032CRH11033
O
X
Alkyllithium
RLi
Alcohol
RCOH
W
W
RH11032
RH11033
H11001
1. diethyl ether
2. H
3
O
H11001
Butanal
CH
3
CH
2
CH
2
CH
O
X
Methylmagnesium
iodide
CH
3
MgI
2-Pentanol (82%)
CH
3
CH
2
CH
2
CHCH
3
W
OH
H11001
1. diethyl ether
2. H
3
O
H11001
Ethyl benzoate
C
6
H
5
COCH
2
CH
3
O
X
Phenylmagnesium
bromide
2C
6
H
5
MgBr
Triphenylmethanol
(89–93%)
(C
6
H
5
)
3
COHH11001
1. diethyl ether
2. H
3
O
H11001
3,3-Dimethyl-
2-butanone
CH
3
CC(CH
3
)
3
O
X
H11001
1. diethyl ether
2. H
3
O
H11001
Li
Cyclopropyllithium
CC(CH
3
)
3
W
W
OH
CH
3
2-Cyclopropyl-
3,3-dimethyl-
2-butanol (71%)
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cyclopentadienyl ring. Ferrocene was the first metallocene synthesized;
its structure is shown on the opening page of this chapter.
Section 14.15 Coordination polymerization of ethylene and propene has the biggest eco-
nomic impact of any organic chemical process. Ziegler–Natta polymer-
ization is carried out in the presence of catalysts derived from transition
metals such as titanium. H9266-Bonded and H9268-bonded organometallic com-
pounds are intermediates in coordination polymerization.
Problems
14.13 Write structural formulas for each of the following compounds. Specify which compounds
qualify as organometallic compounds.
(a) Cyclopentyllithium (d) Lithium divinylcuprate
(b) Ethoxymagnesium chloride (e) Sodium carbonate
(c) 2-Phenylethylmagnesium iodide (f) Benzylpotassium
Problems 573
TABLE 14.5 Carbon–Carbon Bond-Forming Reactions of Organometallic Reagents (Continued)
Reaction (section) and comments
Synthesis of acetylenic alcohols (Section
14.8) Sodium acetylide and acetylenic
Grignard reagents react with aldehydes
and ketones to give alcohols of the type
CPC±COH.
The Simmons-Smith reaction (Section
14.12) Methylene transfer from iodo-
methylzinc iodide converts alkenes to
cyclopropanes. The reaction is a stereo-
specific syn addition of a CH
2
group to
the double bond.
Preparation of alkanes using lithium di-
alkylcuprates (Section 14.11) Two alkyl
groups may be coupled together to form
an alkane by the reaction of an alkyl hal-
ide with a lithium dialkylcuprate. Both
alkyl groups must be primary (or meth-
yl). Aryl and vinyl halides may be used in
place of alkyl halides.
General equation and specific example
Aldehyde
or ketone
RCRH11032
O
X
Sodium
acetylide
NaCPCH
Alcohol
HCPCCRH11032
W
W
OH
R
H11001
1. NH
3
, H1100233°C
2. H
3
O
H11001
2-Butanone
CH
3
CCH
2
CH
3
O
X
Sodium
acetylide
NaCPCH H11001
1. NH
3
, H1100233°C
2. H
3
O
H11001
3-Methyl-1-pentyn-3-ol
(72%)
HCPCCCH
2
CH
3
W
W
OH
CH
3
H11001 RH11032CH
2
X RCH
2
RH11032
Alkane
R
2
CuLi
Lithium
dialkylcuprate
Primary
alkyl halide
(CH
3
)
2
CuLi
Lithium
dimethylcuprate
C
6
H
5
CH
2
Cl
Benzyl
chloride
H11001 C
6
H
5
CH
2
CH
3
Ethylbenzene (80%)
diethyl ether
Iodomethylzinc
iodide
ICH
2
ZnI
Alkene
R
2
C?CR
2
H11001
Zinc
iodide
ZnI
2
H11001
diethyl ether
R
RR
R
Cyclopropane
derivative
CH
2
I
2
, Zn(Cu)
diethyl ether
Bicyclo[3.1.0]hexane
(53%)
Cyclopentene
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14.14 Dibal is an informal name given to the organometallic compound [(CH
3
)
2
CHCH
2
]
2
AlH,
used as a reducing agent in certain reactions. Can you figure out the systematic name from which
“dibal” is derived?
14.15 Suggest appropriate methods for preparing each of the following compounds from the start-
ing material of your choice.
(a) CH
3
CH
2
CH
2
CH
2
CH
2
MgI (c) CH
3
CH
2
CH
2
CH
2
CH
2
Li
(b) CH
3
CH
2
CPCMgI (d) (CH
3
CH
2
CH
2
CH
2
CH
2
)
2
CuLi
14.16 Which compound in each of the following pairs would you expect to have the more polar
carbon–metal bond? Compare the models on Learning By Modeling with respect to the charge on
the carbon bonded to the metal.
(a) CH
3
CH
2
Li or (CH
3
CH
2
)
3
Al (c) CH
3
CH
2
MgBr or HCPCMgBr
(b) (CH
3
)
2
Zn or (CH
3
)
2
Mg
14.17 Write the structure of the principal organic product of each of the following reactions:
(a) 1-Bromopropane with lithium in diethyl ether
(b) 1-Bromopropane with magnesium in diethyl ether
(c) 2-Iodopropane with lithium in diethyl ether
(d) 2-Iodopropane with magnesium in diethyl ether
(e) Product of part (a) with copper(I) iodide
(f) Product of part (e) with 1-bromobutane
(g) Product of part (e) with iodobenzene
(h) Product of part (b) with D
2
O and DCl
(i) Product of part (c) with D
2
O and DCl
(j) Product of part (a) with formaldehyde in ether, followed by dilute acid
(k) Product of part (b) with benzaldehyde in ether, followed by dilute acid
(l) Product of part (c) with cycloheptanone in ether, followed by dilute acid
(m) Product of part (d) with in ether, followed by dilute acid
(n) Product of part (b) with (2 mol) in ether, followed by dilute acid
(o) 1-Octene with diiodomethane and zinc–copper couple in ether
(p) (E)-2-Decene with diiodomethane and zinc–copper couple in ether
(q) (Z )-3-Decene with diiodomethane and zinc–copper couple in ether
(r) 1-Pentene with tribromomethane and potassium tert-butoxide in tert-butyl alcohol
14.18 Using 1-bromobutane and any necessary organic or inorganic reagents, suggest efficient syn-
theses of each of the following alcohols:
(a) 1-Pentanol (d) 3-Methyl-3-heptanol
(b) 2-Hexanol (e) 1-Butylcyclobutanol
(c) 1-Phenyl-1-pentanol
14.19 Using bromobenzene and any necessary organic or inorganic reagents, suggest efficient syn-
theses of each of the following:
(a) Benzyl alcohol (b) 1-Phenyl-1-hexanol
C
6
H
5
COCH
3
O
X
CH
3
CCH
2
CH
3
O
X
574 CHAPTER FOURTEEN Organometallic Compounds
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(c) Bromodiphenylmethane (e) 1-Phenylcyclooctanol
(d) 4-Phenyl-4-heptanol (f) trans-2-Phenylcyclooctanol
14.20 Analyze the following structures so as to determine all the practical combinations of Grig-
nard reagent and carbonyl compound that will give rise to each:
(a) (d) 6-Methyl-5-hepten-2-ol
(b) (e)
(c) (CH
3
)
3
CCH
2
OH
14.21 A number of drugs are prepared by reactions of the type described in this chapter. Indicate
what you believe would be a reasonable last step in the synthesis of each of the following:
(a)
(b)
(c)
14.22 Predict the principal organic product of each of the following reactions:
(a)
(b)
(c)
(d)
CH
2
I
2
Zn(Cu)
diethyl ether
CH
2
CH CH
2
1. Mg, THF
2.
HCH
O
X
3. H
3
O
H11001
Br
1. diethyl ether
2. H
3
O
H11001
O
H11001 CH
3
CH
2
Li
C
O
H11001 NaC CH
1. liquid ammonia
2. H
3
O
H11001
CH
3
O
CH
3
OH
CCH
Mestranol, an estrogenic
component of oral
contraceptive drugs
(C
6
H
5
)
2
CCH
OH
CH
3
N Diphepanol, an antitussive (cough suppressant)
CH
3
CH
2
CC
CH
3
OH
CH Meparfynol, a mild hypnotic or sleep-inducing agent
OH
CH OCH
3
OH
CH
3
CH
2
CHCH
2
CH(CH
3
)
2
OH
Problems 575
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(e)
(f)
(g)
14.23 Addition of phenylmagnesium bromide to 4-tert-butylcyclohexanone gives two isomeric ter-
tiary alcohols as products. Both alcohols yield the same alkene when subjected to acid-catalyzed
dehydration. Suggest reasonable structures for these two alcohols.
14.24 (a) Unlike other esters, which react with Grignard reagents to give tertiary alcohols, ethyl
formate yields a different class of alcohols on treatment with Grignard
reagents. What kind of alcohol is formed in this case and why?
(b) Diethyl carbonate reacts with excess Grignard reagent to yield
alcohols of a particular type. What is the structural feature that characterizes alcohols
prepared in this way?
14.25 Reaction of lithium diphenylcuprate with optically active 2-bromobutane yields 2-phenylbu-
tane, with high net inversion of configuration. When the 2-bromobutane used has the stereostruc-
ture shown, will the 2-phenylbutane formed have the R or the S configuration?
14.26 Suggest reasonable structures for compounds A, B, and C in the following reactions:
Compound C is more stable than compound A. OTs stands for toluenesulfonate.
LiCu(CH
3
)
2
(CH
3
)
3
C
OTs
compound A
(C
11
H
22
)
H11001 compound B
(C
10
H
18
)
LiCu(CH
3
)
2
(CH
3
)
3
C
OTs
compound B H11001 compound C
(C
11
H
22
)
CH
3
CH
2
CH
3
C
Br
H
(CH
3
CH
2
OCOCH
2
CH
3
)
O
X
(HCOCH
2
CH
3
)
O
X
O C(CH
3
)
3
4-tert-Butylcyclohexanone
H11001 LiCu(CH
2
CH
2
CH
2
CH
3
)
2
CH
3
O
CH
2
OS
O
O
CH
3
O
I
LiCu(CH
3
)
2
H11001
CH
2
I
2
Zn(Cu)
ether
CH
2
H
H CH
3
CC
576 CHAPTER FOURTEEN Organometallic Compounds
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14.27 The following conversion has been reported in the chemical literature. It was carried out in
two steps, the first of which involved formation of a p-toluenesulfonate ester. Indicate the reagents
for this step, and show how you could convert the p-toluenesulfonate to the desired product.
14.28 Sometimes the strongly basic properties of Grignard reagents can be turned to synthetic
advantage. A chemist needed samples of butane specifically labeled with deuterium, the mass 2
isotope of hydrogen, as shown:
(a) CH
3
CH
2
CH
2
CH
2
D (b) CH
3
CHDCH
2
CH
3
Suggest methods for the preparation of each of these using heavy water (D
2
O) as the source of
deuterium, butanols of your choice, and any necessary organic or inorganic reagents.
14.29 Diphenylmethane is significantly more acidic than benzene, and triphenylmethane is more
acidic than either. Identify the most acidic proton in each compound, and suggest a reason for the
trend in acidity.
14.30 The 18-electron rule is a general, but not universal, guide for assessing whether a certain
transition-metal complex is stable or not. Both of the following are stable compounds, but only
one obeys the 18-electron rule. Which one?
14.31 One of the main uses of the “linear H9251-olefins” prepared by oligomerization of ethylene is
in the preparation of linear low-density polyethylene. Linear low-density polyethylene is a copoly-
mer produced when ethylene is polymerized in the presence of a “linear H9251-olefin” such as
1-decene [CH
2
?CH(CH
2
)
7
CH
3
]. 1-Decene replaces ethylene at random points in the growing
polymer chain. Can you deduce how the structure of linear low-density polyethylene differs from
a linear chain of CH
2
units?
14.32 Make a molecular model of 7,7-dimethylbicyclo[2.2.1]heptan-2-one. Two diastereomeric
alcohols may be formed when it reacts with methylmagnesium bromide. Which one is formed in
greater amounts?
7,7-Dimethylbicyclo[2.2.1]heptan-2-one
CH
3
H
3
C
O
HH
HH
Fe
CO
COOC
Ti
Cl
Cl
C
6
H
6
Benzene
K
a
H11015 10
H1100245
(C
6
H
5
)
2
CH
2
Diphenylmethane
K
a
H11015 10
H1100234
(C
6
H
5
)
3
CH
Triphenylmethane
K
a
H11015 10
H1100232
O OH O
two steps
Problems 577
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14.33 Make molecular models of the product of addition of dichlorocarbene to:
(a) trans-2-Butene
(b) cis-2-Butene
Which product is achiral? Which one is formed as a racemic mixture?
14.34 Examine the molecular model of ferrocene on Learning By Modeling. Does ferrocene have
a dipole moment? Would you expect the cyclopentadienyl rings of ferrocene to be more reactive
toward nucleophiles or electrophiles? Where is the region of highest electrostatic potential?
14.35 Inspect the electrostatic potential surface of the benzyl anion structure given on Learning
By Modeling. What is the hybridization state of the benzylic carbon? Does the region of highest
electrostatic potential lie in the plane of the molecule or perpendicular to it? Which ring carbons
bear the greatest share of negative charge?
578 CHAPTER FOURTEEN Organometallic Compounds
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