Citation: Venturi, V.; Lerin, L.A.;
Presini, F.; Giovannini, P.P.; Catani,
M.; Buratti, A.; Marchetti, N.; Dilliraj,
L.N.; Aprile, S. Enzymatic Synthesis
of Ascorbic Acid-Ketone Body
Hybrids. Catalysts 2023, 13, 691.
https://doi.org/10.3390/
catal13040691
Academic Editors: Yan Zhang and
Raushan Kumar Singh
Received: 16 March 2023
Revised: 28 March 2023
Accepted: 31 March 2023
Published: 1 April 2023
Copyright: © 2023 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
catalysts
Article
Enzymatic Synthesis of Ascorbic Acid-Ketone Body Hybrids
Valentina Venturi
1
, Lindomar Alberto Lerin
2
, Francesco Presini
2
, Pier Paolo Giovannini
2,
* , Martina Catani
2
,
Alessandro Buratti
2
, Nicola Marchetti
2
, Latha Nagamani Dilliraj
2
and Simona Aprile
2
1
Department of Environmental and Prevention Sciences, University of Ferrara, Via Luigi Borsari, 46, 44121
Ferrara, Italy; valentina.venturi@unife.it
2
Department of Chemistry, Pharmaceutical and Agricultural Sciences, University of Ferrara, Via Luigi Borsari,
46, 44121 Ferrara, Italy; lindomaralberto.lerin@unife.it (L.A.L.); francesco.presini@unife.it (F.P.);
martina.catani@unife.it (M.C.); alessandro.buratti@unife.it (A.B.); nicola.marchetti@unife.it (N.M.);
latha7481@yahoo.com (L.N.D.); simona.aprile@unife.it (S.A.)
* Correspondence: pierpaolo.giovannini@unife.it; Tel.: +39-053-297-4532
Abstract: Molecular hybrids obtained by connecting two or more bioactive molecules through a
metabolizable linker are used as multi-target drugs for the therapy of multifactorial diseases. Ascorbic
acid, as well as the ketone bodies acetoacetate and (R)-3-hydroxybutyrate, are bioactive molecules
that have common fields of application in the treatment and prevention of neurodegenerative diseases
and cardiac injuries as well. In spite of this, the preparation of ascorbic acid ketone body hybrids
is uncovered by the literature. Herein, we report the lipase-catalyzed condensation of methyl
acetoacetate with ascorbic acid, which affords the 6-O-acetoacetyl ascorbic acid in quantitative yield.
The same approach, employing the methyl (R)-3-hydroxybutyrate in place of the methyl acetoacetate,
allows the preparation of the 6-O-(R)-3-hydroxybutyryl ascorbic acid in 57% yield. A better result
(90% overall yield) is achieved through the lipase-catalyzed coupling of ascorbic acid with methyl
(R)-3-O-methoxymethyl-3-hydroxybutyrate followed by the cleavage of the MOM protecting group.
The two novel products are fully characterized and additional information on the antioxidant activity
of the new products is also given.
Keywords: molecular hybrids; ascorbyl esters; lipase; biocatalysis; antioxidant activity
1. Introduction
Humans have exploited for millennia the properties of plant-derived foods and bever-
ages to preserve their health, and the knowledge growth in various scientific fields has led
to the identification of the substances responsible for the protective or curative effects. More
recently, thanks to in vitro as well as in vivo experiments, the mechanisms by which many
plant-derived bioactive compounds produce health benefits have been discovered [1,2].
It is worth noting that a number of bioactive compounds are employed in the treatment
or prevention of multifactorial diseases, namely illnesses with complex etiopathology due
to the involvement of multiple organ systems and tissues [3]. The treatment of such dis-
eases moved from the traditional single-drug therapy toward multidrug approaches that
include the administration of drug cocktails or multicomponent drugs obtained by the
co-formulation of more than one active ingredient [4]. An alternative emerging strategy
is the design of multi-target drugs that integrate multiple pharmacophores into a single
drug molecule in order to simultaneously act at multiple sites of relevance to a disease [5,6].
Multi-target drugs can be prepared by connecting two or more drugs through a stable or
metabolizable linker or by merging the haptophoric moieties of different drugs. The two
strategies afford hybrid and chimeric drugs, respectively [3], although this specification is
not strictly followed in the literature and the term molecular hybrid is often used to indi-
cate multi-target drugs achieved through both connection strategies [3,7]. Many bioactive
natural products have been employed as a starting scaffold in multi-target drug discovery
Catalysts 2023, 13, 691. https://doi.org/10.3390/catal13040691 https://www.mdpi.com/journal/catalysts