Front Matter

(Tina Sui) #1
In the above-mentioned examples, the regioselective removal of fatty acids was

achieved using hydrolysis reactions, but alcoholysis reactions may be used for the

same purpose. For example, in the synthesis of lysophospholipids, alcoholysis in

pure alcohol (ethanol or other short-chain alcohols) was carried out usingRhizomu-

cor mieheilipase as catalyst (Sarney et al., 1994). The reaction was regioselective for

thesn-1 position, and a conversion of more than 98 % was achieved. In order to

prepare the other regioisomer, 1-acyl-lysophosphatidylcholine, acyl migration

was induced by ammonia vapors (Sarney et al., 1994) (Figure 6).

14.5 Esterification reactions for the incorporation


of fatty acids into lipids


14.5.1 Lipase-catalyzed esterification

Esterification of glycerophosphate

Glycerophosphate constitutes a basic building block for glycerophospholipids. For

the synthesis of the natural isomers, puresn-3-glycerophosphate should be used as

substrate unless the enzymatic reactions are stereoselective enough to involve only

the natural enantiomer. When an enantiomerically pure product is not needed, ra-

cemic glycerophosphate may be used as starting material.

Glycerophosphate is a highly polar compound, and the reaction to couple it en-

zymatically to hydrophobic fatty acids is not straightforward. The reaction was first

reported using Lipozyme in a solvent-free system with free fatty acid as acyl donor.

The monoacylation product, lysophosphatidic acid (LPA), was obtained in moderate

yield (32 %) and small amounts of the diacylation product, phosphatidic acid, were

also formed (Han and Rhee, 1995). The yield of LPA (containing caproic acid) was

increased to 45 % when the water activity of the solvent-free reaction mixture was

maintained at 0.18 by the introduction of a suitable salt hydrate pair in the headspace

of the reactor (Han and Rhee, 1998).

The use of fatty acid vinyl esters as acyl donors has proven quite favorable in the

acylation of glycerophosphate usingRhizopus arrhizuslipase as catalyst (Virto et al.,

1999). Vinyl esters are frequently used in transesterification reactions to make them

virtually irreversible. The vinyl alcohol formed as reaction product spontaneously

tautomerizes to acetaldehyde, thereby shifting the equilibrium position; hence it is

possible to achieve very high conversions. Vinyl laurate which was used for acyla-

14.5 Esterification reactions for the incorporation of fatty acids into lipids 297

Figure 6. Lipase-catalyzed alcoholysis of phosphatidylcholine. The lipase produces the 2-acyl-lyso-
phosphatidylcholine. In order to obtain the other regioisomer, 1-acyl-lysophosphatidylcholine, acyl mi-
gration was induced by ammonia vapor. (From Sarney et al., 1994.)

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