Carica papaya Latex Lipase: sn-3 Stereoselectivity
or Short-Chain Selectivity? Model Chiral
Triglycerides Are Removing the Ambiguity
P. Villeneuve, M. Pina, D. Montet and J. Graille*
CIRAD-CP, Laboratoire de Lipotechnie, F34032 Montpellier Cedex, France
ABSTRACT: Short-chain fatty acids are usually located at po-
sition sn-3 in natural triglycerides, particulary in dairy fats. As a
result, it is extremely difficult to differentiate between sn-3 stere-
ospecificity and short-chain typoselectivity in many lipases and
acyltransferases that perform in this way. This ambiguity can be
removed through successive use of a chiral triglyceride with a
short fatty acid in position sn-1 and of its racemic in controlled
hydrolysis reactions. After checking that the proposed method
effectively confirmed the type of activity of control biocatalysts
(Candida cylindracea nonspecific lipase and Mucor miehei 1-3
regiospecific lipase), we confirmed that Carica papaya latex has
a strict sn-3 stereospecificity.
JAOCS 72, 7.53-755 (1995).
KEY WORDS: Carica papaya latex, chiral triglyceride, enzy-
matic hydrolysis, racemic triglyceride, stereospecificity, typose-
lectivity.
Lipases (E.C 3.1.1.3) play a predominant role in the digestion
mechanism of humans and animals (1). Therefore, there is a
considerable amount of literature on the hydrolysis of acyl-
glycerols by these enzymes (2-4). A distinction can be made
between three kinds of lipases: nonspecific; stereoselective,
preferentially hydrolyzing one of the triglyceride positions;
and typoselective lipases, which preferentially hydrolyze
given fatty acids, irrespective of their positions.
There is probably no enzyme that is specific to a single
fatty acid; usually, a marked preference for a category of fatty
acids, such as short-chain fatty acids from C 4 to Cl0, is ob-
served. In dairy fats (5) and in the great majority of natural
fats and oils, short-chain fatty acids are distributed in posi-
tion sn-3. Studying sn-3 specificity is therefore intricate be-
cause it becomes difficult to make a distinction between
short-chain fatty acid typoselectivity and sn-3 stereoselectiv-
ity. We recently proposed a procedure (6) for synthesis of chi-
ral triglycerides with a short-chain fatty acid in position sn-1
and their corresponding racemics.
Such molecules remove ambiguity. This article concerns
the hydrolytic performance of Carica papaya latex, an acyl-
transferase obtained from a plant extract known for its prefer-
*To whomcorrespondence should be addressedat CIDAD-CP, Laboratoire
de Lipotechnie, BP5035,F34032Montpellier Cedex,France.
ence for short chains in dairy fat bioconversion operations.
But, is it really short-chain fatty acid typoselective or sn-3
stereospecific? The approach taken in this work provides the
answer.
EXPERIMENTAL PROCEDURES
Triglycerides. The synthesis and stereochemical anaIysis of
triglycerides were described recently (6).
Enzymes. The Cariea papaya latex was a purified extract
(Sigma, Saint Priest, France), and the granular material was
ground up before use. The lipozyme IM (Novo Nordisk,
Copenhagen, Denmark) was the lipase from Mucor miehei,
fixed on an ion exchange resin. The Candida cylindracea li-
pase (Sigma) was a preparation that contained lactose.
Hydrolysis. Seventy mg of triglycerides was added to 2.3
mL of 0.2M Tris HC1 buffer (pH 8); then 10 mg of enzyme
preparation was added and shaken at 40°C for a time, t, in an
ultraturax (IKA-Werk, Paris, France) at 10,000 rpm to obtain
a hydrolysis rate of about 10% (t = 2 rain for Carica papaya,
t = 30 s for Candida cylindracea and for Lipozyme IM).
The hydrolysis was stopped by the addition of 1.5 mL of
saline acid solution (0.1M H2SO 4, 2.5M NaC1). The fat was
extracted three times with 3 mL of ether/heptane solution
(75:25, vol/vol). The lipolysis products were then separated
by thin-layer chromatography, and the sample was applied
with an automatic applicator (Camag Linomat III; Camag,
Ltd., Muttenz, Switzerland) to a preparative plate (Kieselgel
60, 0.25 Mesh; Merck, Darmstadt, Germany). Development
was carried out in a hexane/ether/acetic acid mixture
(50:50:1, vol/vol/vol).
The diglycerides and free fatty acids bands were located
by transparency and transformed into isopropyl esters.
Measurement of the degree of lipolysis. The degree of
lipolysis was obtained by KOH titration of the free acids in
the reaction medium from a 1-mL sample taken from the 9
mL of ether/heptane extract (75:25, vol/vol).
Derivation into isopropyl esters (7). The total amount of
diglycerides and free fatty acids recovered were dissolved in
a hexane/isopropanol mixture (3:2, vol/vol). Then, 400 ~tL of
6M H2SO 4 and l mL isopropanol were added. The tube was
hermetically sealed, shaken, and placed in the oven for 1 h at
100°C. The tube was then cooled in an ice bath, and 5 mL dis-
Copyright © 1995 by AOCS Press 753 IAOCS, Vol. 72, no. 6 (1995)