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Thus, when injected into anopheline mosquitoes previously infected with a variety of Plasmodium spe-cies, the antimicrobial peptides disrupted sporogonic Keywords antimicrobial peptide;

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Multifunctional host defense peptides: antiparasitic

activities

Amram Mor

Department of Biotechnology & Food Engineering, Technion – Israel Institute of Technology, Haifa, Israel

Introduction

Human parasites are responsible for millions of deaths

around the world every year Malaria, for instance, is

endemic in over 100 Third World countries, with an

estimated 400 million clinical cases correlating with

1–3 million deaths annually, and over 3 billion

inhabit-ants of tropical regions are considered to be at risk [1]

Of particular concern is the causative agent of human

malaria, Plasmodium falciparum, a large number of

strains of which are drug resistant, in particular to

chloroquine [2] Reports of field strains of P

falcipa-rum demonstrating in vitro resistance to artemisinins –

recently introduced antimalarial drugs – are also

alarming [3] Similarly, leishmaniases are important

causes of morbidity and mortality in humans and

ani-mals on four continents, and are extremely difficult to

treat [4] There is thus a clear need for new therapeutic agents against these and related parasites A multitude

of preliminary studies suggest that host defense pep-tides (HDPs) represent a promising route towards developing new, efficient antiparasitic therapies [5] Magainins and cecropins were among the very first examples of animal HDPs reported to display antipar-asitic activities, some 20 years ago [6], and synthetic hybrids of cecropin and melittin have exhibited enhanced potency [7] These notorious antimicrobial peptides are known to function as part of an inducible immune response against a number of microbial infec-tions Thus, when injected into anopheline mosquitoes previously infected with a variety of Plasmodium spe-cies, the antimicrobial peptides disrupted sporogonic

Keywords

antimicrobial peptide; chemical mimicry;

drug design; drug resistance; infectious

disease; Leishmaniasis; malaria; membrane

active compound; oligo-acyl-lysyl;

peptide-mimetic

Correspondence

A Mor, Laboratory of Antimicrobial Peptides

Investigation (LAPI), Department of

Biotechnology & Food Engineering,

Technion – Israel Institute of Technology,

Haifa, Israel

Fax: +972 4 829 3399

Tel: +972 4 829 3340

E-mail: amor@tx.technion.ac.il

(Received 28 April 2009, revised 12 August

2009, accepted 12 August 2009)

doi:10.1111/j.1742-4658.2009.07358.x

Whereas significant knowledge is accumulating on the antibacterial and antifungal properties of host defense peptides (HDPs) and their synthetic mimics, much less is known of their activities against parasites A variety

of in vitro and in vivo antiparasitic assays suggest that these notorious anti-microbial compounds could represent a powerful tool for the development

of novel drugs to fight parasites in the vertebrate host or to complement current therapeutic strategies, albeit the fact that HDPs essentially act by nonspecific mechanisms casts serious doubt on their ability to exert suffi-cient selectivity to be considered ideal candidates for drug development This minireview summarizes recent efforts to assess the antiparasitic prop-erties of HDPs and their synthetic derivatives, focusing on two of the most used models – Plasmodium and Leishmania species – for antiparasitic assays against the different development stages

Abbreviations

APP, antilipopolysaccharide factor; HDP, host defense peptide; Hst5, histatin-5; OAK, oligo-acyl-lysyl.

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development by aborting the normal development of

oocysts As the vector cannot transmit the parasite to

another host, this suggested the possibility of

induc-ing effective transmission-blockinduc-ing immunity in the

mosquito vector by transgeneic expression of genes

coding for magainins, cecropins or similarly acting

parasiticidal peptides in the mosquito genome [6]

Since then, antiparasitic activities have been reported

for numerous additional antimicrobial peptides and

their synthetic derivatives Representative antiparasitic

peptides (APPs) are listed in Table 1, and reports from

the past decade are briefly outlined below

APPs

Among the structurally constrained peptides, defensins are by far the most investigated family of HDPs, and numerous members have been reported to exert a vari-ety of antiparasitic activities For instance, the classic antifungal defensin, drosomycin, was shown to signifi-cantly inhibit the development of Plasmodium berghei ookinetes at micromolar concentrations [8] Scorpine,

a 75-mer peptide from scorpion venom Pandinus impe-rator whose structure resembles a hybrid between defensin and cecropin, was reported to inhibit both the

Table 1 List of representative natural and synthetic antiparasitic peptides MIC and IC50: minimal concentrations inducing 100% and 50% inhibition of parasite growth, respectively MLC and LC 50 : minimal concentrations inducing 100% and 50% lysis of the parasite, respectively.

Antiparasitic effect (l M ) Reference

Tetrahymena pyriformis MIC = 8.1 Acanthamoeba castellani MIC = 0.9

Leishmania pifanoi LC50= 14.4

SSGHCSPSLKCWCEGC

a Acyl-lysyl oligomers where: l, dodecanoyl; L, aminododecanoyl; K, lysyl Underlined letter designates amino acids in the D -configuration.

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ookinete and gamete developmental stages of

Plasmo-dium berghei with ED50 values of 0.7 and 10 lm,

respectively [9] There are newer reports of transgenic

scorpine producing 98% mortality in the sexual

stages of P berghei at 15 lm and a 100% reduction in

P falciparum parasitemia at 5 lm [10] Various

defen-sins also have leishmanicidal properties, possibly by

inducing apoptosis [11] The fact that substantially

higher leishmanicidal activity was observed against

mutant strains of Leishmania major in which

leishman-olysin, a surface metalloprotease, was knocked out

suggests that virulence factors such as leishmanolysin

might prevent antimicrobial peptide-mediated

apop-totic killing Longicin, another member of the defensin

family, from the tick Haemaphysalis longicornis,

exhib-ited antiparasitic activity in vitro and in vivo against

the erythrocyte stage of Babesia, the merozoites, by

preventing or retarding their proliferation The fact

that longicin exerted a hemoparasiticidal effect without

demonstrable toxicity against mammalian host cells

suggests its usefulness as a model for the development

of chemotherapeutic compounds against tick-borne

disease organisms [12] A recent report studied clinical

isolates from three microsporidia species, using spore

germination and enterocyte-like cell infection assays

to determine the effect of a panel of antimicrobial

peptides: lactoferrin, lysozyme, human b-defensin-2,

human a-defensin-5, and human a-defensin-1 The

antimicrobial peptides have been reported to efficiently

inhibit spore germination and⁄ or cell infection of one

or a number of isolates, either alone or upon

combina-tion with lysozyme, suggesting that intestinal

anti-microbial peptides contribute to the prevention of

infection by luminal microsporidia spores [13]

The linear 27-residue synthetic derivative of the

porcine protein NK-lysin, NK-2, was found to exert

selective activity against P falciparum [14] Infected

human erythrocytes were rapidly permeabilized by

NK2 at 5–10 lm, which reduced the viability of the

intracellular parasite, whereas noninfected cells were

hardly affected This selectivity was ascribed to loss

of plasma membrane asymmetry and concomitant

exposure of phosphatidylserine upon infection NK-2

was also reported to kill the intracellular parasite

Try-panosoma cruzi, the causative agent of Chagas disease,

leaving the host cell unharmed [15]

Angiotensin II and a related peptide, vanicere-5,

were studied in culture and in mosquitos for their

effects on the development of Plasmodium gallinaceum

sporozoites When injected into the insect thoraxes,

these peptides reduced infection intensities in the

mos-quito salivary glands by 88% and 76%, respectively

Although the mechanism of action is not fully

under-stood, the authors proposed that these peptides selec-tively disrupt the cell membrane of P gallinaceum, and showed additionally that preincubation of sporozoites

in vitro with vanicere-5 reduced the infectivity of the parasites with regard to their vertebrate host [16] Bombinin H4 is a native antimicrobial peptide of animal origin with a single l-amino acid to d-amino acid isomerization in position 2, which improves its biostability Bombinin H4 was reported to affect the viability of both insect and mammalian forms of Leish-mania by rapidly perturbing their plasma membranes

at micromolar concentrations The mode of action involved rapid (within minutes) depolarization and loss

of integrity of the plasma membrane, associated with rapid bioenergetic collapse [17]

The 13-residue-long temporins show leishmanicidal activity while maintaining biological functions in serum Their lethal mechanism is believed to involve plasma membrane disruption, on the basis of the observations that the peptides induce rapid collapse of the plasma membrane potential, influx of exogenic molecules, and reduced intracellular ATP levels [18] Buforin activity against Cryptosporidium parvum was strongly dependent on the parasite life cycle: the oocyst was barely affected after 3 h of incubation with

10 lm buforin, whereas the sporozoite’s viability decreased by almost 100% The authors speculate that the sporozoites are susceptible because their cytoplas-mic membrane is somewhat structurally similar to the bacterial cytoplasmic membrane [19] This group also showed that the moderate activity of buforin can be enhanced upon combination with azithromycin or minocycline, > 90% parasite reduction being observed

at the highest concentration tested [20]

A recent study investigated the antiparasitic activi-ties of different antimicrobial peptides isolated from aquatic animals These included penaeidin-3 from the shrimp Litopenaeus vannamei, the antilipopolysaccha-ride factor (ALF) from Penaeus monodon, clavanin A from the ascidean Styela clava, an analog of magainin (MSI-94) from the frog Xenopus laevis, tachyplesin I from the limulid Tachypleus tridentatus, and mytilin A from the mussel Mytilus edulis These antimicrobial peptides were selected because of their previously dem-onstrated potent effects against bacteria, yeasts, and filamentous fungi The antiparasitic activity was eval-uated against the promastigote form of Leishmania braziliensis as well as against the epimastigote and trypomastigote forms of Trypanosoma cruzi Tachylep-sin was found to be the most potent peptide in killing both L braziliensis and T cruzi, and was therefore suggested to be the most suitable candidate for further investigation as a therapeutic agent [21] A

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tachylep-sin-related peptide called gomesin was tested against

asexual, sexual and presporogonic forms of P

falcipa-rum and P berghei parasites When added to culture

of P berghei mature gametocytes, gomesin inhibited

the exflagellation of male gametes and the formation

of ookinetes In vivo, the peptide reduced the number

of oocysts of both Plasmodium species in

Anophe-les stephensimosquitoes [22]

Attacin is an immune effector peptide that has been

shown to inhibit the growth of Gram-negative

bacte-ria In Glossina morsitans morsitans, which serves as

the sole vector of African trypanosomes, attacin was

implicated in trypanosome resistance and in

maintain-ing parasite numbers at homeostatic levels in infected

individuals [23]

Studies of the histidine-rich antimicrobial peptide

LAH4 resulted in several active derivatives [24] The

most selective APP was a 26 amino acid analog,

D-HALO-rev, which showed high potency (IC50 of

0.1 lm) against the human malarial parasite P

falci-parum, and concentrations toxic against erythrocytes

and fibroblasts at least two orders of magnitude

higher than those needed for its antiplasmodial

activ-ity The mechanism of the antiplasmodial activity is

unclear; however, important differences in the

mem-brane composition of Plasmodium spp versus the

host cells are predicted to enhance the activity of

designed antiplasmodial peptides (for a recent review

see [25]) By contrast, another histidine-rich APP,

human histatin-5 (Hst5), seems to target

mitochon-drial ATP synthesis [26] In the human parasitic

pro-tozoan Leishmania, mitochondrial ATP production is

crucial, as the organism lacks the bioenergetic switch

between glycolysis and oxidative phosphorylation

described in some yeasts Hst5 displays activity

against both stages of the parasite life cycle,

prom-astigotes and amprom-astigotes (LC50 values of 7.3 lm and

14.4 lm, respectively) Hst5 was proposed to induce a

lethal effect by causing limited and temporary

dam-age to the plasma membrane of the parasites, as

assessed by electron microscopy, membrane

depolar-ization, and uncontrolled entrance of a vital dye

Fol-lowing this initial interaction, Hst5 translocates into

the cytoplasm of Leishmania in a nonstereospecific,

receptor-independent manner, accumulates in the

mitochondrion, and produces bioenergetic collapse of

the parasite by decreasing the synthesis of

mitochon-drial ATP

Tyrothricin, a complex mixture of antibiotic peptides

produced by Bacillus brevis, was reported in 1944 to

have antimalarial activity rivaling that of quinine in

chickens infected with P gallinaceum More than

60 years later, the major components of tyrothricin,

cyclic decapeptides collectively known as the tyroci-dines, were isolated and tested against P falciparum Although the tyrocidines differ from each other by conservative amino acid substitutions in only three positions, their parasite inhibitory concentrations spanned three orders of magnitude (IC50 of the most potent compounds ranged between 0.6 and 360 nm) For comparison, gramicidin S, a structurally analogous antibiotic peptide tested under the same conditions, was not as active (IC50 of 1.3 lm) but exerted anti-parasitic activity by rapid lysis of infected erythro-cytes Like those of previously described antimicrobial peptides, tyrocidine activities correlated strictly with increased apparent hydrophobicity and reduced total side chain surface area due to the presence of ornithine and phenylalanine in key positions Unlike antiplasmo-dial activity, however, mammalian cell toxicities of the respective peptides were considerably less variable, ranging only from 2.6 to 28 lm [27]

Various native members of the frog-derived derm-aseptin family exhibit potent antiparasitic properties against both Leishmania [28] and P falciparum [29] Synthetic derivatives of dermaseptin S4, such as the 28-mer K4K20-S4 or its short analog K4S4(1–13), dis-played enhanced activity towards human erythrocytes infected with P falciparum, killing the parasite through lysis of the host cells [30] Both derivatives were more efficient in inhibiting parasite growth at the mature trophozoite stage than at the younger ring stage This fact supports the view that the antiplasmodial effect is essentially derived from lysing the host cell membrane; that is, because the host cell membrane evolves with parasite maturation, trophozoites are expected to be more sensitive than rings, as observed [30] Various conjugation derivatives of K4S4(1–13) were assayed with the aim of avoiding lysis of host cells These derivatives have established that increased hydropho-bicity at the N-terminus invariably results in an ampli-fied antiplasmodial effect, irrespective of the linearity

or bulkiness of the additive However, increased hydrophobicity was also generally associated with increased hemolysis and lack of discrimination between infected and noninfected erythrocytes [31] By contrast, aminoacyl counterparts were generally more selective [32] Thus, as compared with the parent peptide, the aminoheptanoylated version displayed both increased antiparasitic efficiency and reduced hemolysis, includ-ing against infected cells Presumably, by selectively dissipating the parasite plasma membrane potential and causing depletion of intraparasite potassium, this derivative exerted more than 50% growth inhibition at peptide concentrations that did not cause detectable hemolysis Hence, unlike the parent peptide, the

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aminoheptanoylated derivative was not stage-selective,

being equally inhibitory for both the ring and

tropho-zoite stages Additional new members of the

derma-septin family also act as APPs, displaying potent

activity against Leshmania (e.g dermaseptins O1 and

H3) and against T cruzi (e.g dermaseptins D11 and

D12) [25,38,39]

Chemical mimicry of APPs

In addition to the naturally occurring APPs and their

de novo designed synthetic derivatives, recent studies

suggest that potent antiparasitic properties can be

generated from HDP-mimetic compounds designed to

mimic the structure and⁄ or function of the native

peptides [33,34] The potential therapeutic use of

anti-parasitic HDPs is likely to be significantly limited by

several major obstacles pertaining to less than ideal

properties, including relative toxicity and

bioavail-ability issues as well as a relatively high production

cost By reproducing the critical biophysical

character-istics of HDPs, peptidomimetics might better address

these issues while endowing resistance to degradation

enzymes

Recently developed HDP mimetics, termed

oligo-acyl-lysyls (OAKs), were based on a linear sequence of

alternating aminoacyl chains and cationic amino acids

so as to mimic the prototypical sequence of linear

HDPs Like potent HDPs, OAKs can display rapid,

nonhemolytic, broad-spectrum microbicidal properties

both in vitro and in vivo Various OAK sequences were

shown to inhibit the growth of different plasmodial

strains (IC50 range 0.08–0.14 lm) Further

investiga-tions performed with a representative OAK revealed

that the ring and trophozoite stages of the parasite

developmental cycle were equally sensitive to this

com-pound, unlike the case with the parent dermaseptin

peptides A shortcoming of the OAK was the need for

long incubation times in order for it to exert its full

effect [35] Nevertheless, certain OAKs displayed

highly selective antiparasitic activity, the ratio of LC50

(hemolysis) to IC50 (parasite growth inhibition) being

> 10 000 for the most selective OAK, composed of

only three acyl-lysyl subunits (Table 1) These results

indicated that the OAK did not exert its antimalarial

action by lysis of infected erythrocytes, as was the case

with the parent dermaseptins, and pointed to the

potential of the OAK system to generate simple, highly

selective and low-cost compounds that might be useful

in fighting malaria Note that, although the OAKs

rep-resent, so far, the only HDP mimetic system able to

generate antiparasitic compounds, it is anticipated that

future studies of various existing and⁄ or new future

mimic strategies will reveal interesting antiparasitic properties Because of their chemical robustness, such compounds are likely to overcome various drawbacks

of conventional antimicrobial peptides, including sus-ceptibility to proteases, and might therefore be both useful investigation tools and new, promising candi-dates for therapeutic developments

Possible mechanisms for APPs

Attempts to understand the mechanism(s) underlying the observed antiplasmodial activity suggest that the activities of distinct APPs obey many of the rules governing their ability to disrupt bacterial membranes (discussed extensively elsewhere in this issue) This type

of interaction appears to be acutely influenced by the respective charges and amphipathies of the reactants

In fact, a comparison between the peptides’ ability to inhibit the growth of malaria parasites and that of bacteria demonstrates a remarkable parallelism in the way that each modification affects both activities, as assessed with numerous substitution⁄ truncation deriv-atives [28–31] Additional support for this view is provided by the results obtained with experiments on kinetics and the dissipation of the membrane potential,

as well as from the fact that activity is rapid and is independent of a chiral center [32] Therefore, a variety

of experimental evidence suggests that the mode of antiplasmodial activity of some antimicrobial peptides might be based on selective membrane disruption, despite the fact that the parasite’s membrane is well hidden within its host cell As shown in Fig 1, it is speculated that, owing to differences in membrane composition [25,40], APPs have a higher affinity for the membranes of infected erythrocytes than for those

of normal erythrocytes (hence the often observed greater extent of hemolysis of infected cells), but must have a still higher affinity for the parasite’s membrane The observed labeling of intracellular parasites in non-lysed, infected erythrocytes (i.e under nonhemolytic conditions) supports this view (Fig 1), although the apparent differential distribution of rhodaminated peptides may also be due to an experimental artefact: the fluorescence may be collisionally quenched by hemoglobin, which is present only in the host cell com-partment Nevertheless, colocalization evidence exists (although unpublished) suggesting that, in macro-phage-infected amastigotes, the antileishmanial activity also might proceed by direct interaction of dermasep-tin with the intracellular parasite (Fig 2) Thus, when dermaseptin, for instance, binds the membrane of a hosting erythrocyte, the peptide is somehow able to transfer to the parasitic membrane in an affinity-driven

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Fig 1 Proposed model for APP interaction with infected erythrocytes The left panel shows phase-contrast and fluorescence confocal microscope images providing evidence for the direct interaction of the rhodamine-labeled dermaseptin derivative, aminohexyl-K4-S4(1–13), with unfixed intraerythrocyte P falciparum trophozoites The right panel is a cartoon illustration of two hypothetical modes of action The upper drawing shows the initial adhesion of the lipophilic APP (blue) to the erythrocyte membrane Subsequently, hemolytic APPs can assemble to disrupt that membrane (right drawing) The resulting hemoglobin leakage will lead to parasite starvation Nonhemolytic APPs (left drawing) can undergo an affinity-driven transfer (through lateral diffusion?) from the erythrocyte to the parasite membranes The lower drawings represent potential APP fates once they have reached the parasite’s membrane: (1) superficial carpet-like interactions can modify the membrane properties (e.g charge and fluidity of lipids and protein components) and interfere with their proper normal functions [40]; (2) APP internalization and interruption of vital biological processes (e.g DNA functions) [34]; (3) APPs can also disrupt the parasite’s plasma membrane (similarly to the hemolytic process) as evidenced by the APP’s ability to dissipate the parasite plasma membrane potential and cause depletion of intraparasite potassium under nonhemolytic conditions [32].

Fig 2 Proposed model for APP interactions with infected macrophages The left panel shows the experimental colocalization of APP and parasites in a human macrophage infected with L major amastigotes, as visualized by fluorescence confocal microscopy: (A) rhodaminated dermaseptin applied to unfixed cells; (B) fluoresceinated antiparasite antibody applied after cell fixation; (C) merged image of (A) and (B); (D) phase-contrast image of the infected macrophage shown in (A), (B) and (C) The right panel is a cartoon illustration of two hypothetical routes leading to the colocalization of dermaseptin and parasite in an infected macrophage In the upper drawings, the cartoon shows that cationic APPs could reach the cytoplasm by diffusion, exploiting the negative-inside transmembrane potential or via vesicle-like internalization followed by fusion with the parasitophorous vacuole The subsequent events that might follow are described in the lower drawings of Fig 1.

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manner and to exert a membrane-lytic activity upon

the pathogen Namely, such a ‘transfer’ could

physi-cally occur through the new permeability pathways

that are induced by the parasite in the membrane of

the host erythrocyte As the parasite is completely

engulfed within a parasitophorous vacuole membrane,

solutes which leave or enter the parasite must therefore

traverse three membranes: that of the host erythrocyte,

the parasitophorous vacuole membrane, and the

para-site membrane Experimental evidence for the ability

of APPs to gain access to the parasite in

malaria-infected cells, obtained using confocal microscopy

analysis of labeled dermaseptins, is shown in Fig 1

[32] The data showed that, in infected cells, the

labeled peptide crossed the erythrocyte plasma

mem-brane and concentrated in internal compartments,

although it is presently unclear what was the peptide’s

ultimate target, e.g the parasite membrane, the

mito-chondrion, or nucleic acids Antimicrobial peptides are

known to target each and⁄ or all of the above [34]

Conclusions

Although the mechanism of action of most

antimicro-bial peptides is far from being fully understood, the

vast majority are now believed to act by one or even a

combination of different nonspecific mechanisms that

can target not only the cell membrane integrity but

also extracellular and intracellular processes (reviewed

by Pierre Nicolas in [41]; this issue) Such a multitarget

mode of action is in good agreement with the observed

large spectrum of sensitive microorganisms, and

signifi-cantly reduces the likelihood of emergence of efficient

resistance mechanisms Thus, even though the

antipar-asitic properties have not been investigated thoroughly,

as yet, an increasing number of convincing studies

seem to support the view that the antiparasitic activity

of antimicrobial peptides also emanates from

interac-tions with multiple targets Most remarkably, however,

at least a few peptides exhibit very high potency (IC50

values in the nanomolar range) and a selectivity factor

of several orders of magnitude These selective

com-pounds appear to be endowed with the formidable

ability to cross a number of membrane systems before

specifically disrupting a target(s) in the intracellular

parasite Although differences in membrane

composi-tion are likely to contribute to this selectivity, the

molecular basis for these observations remains largely

ill-understood Nonetheless, these studies strongly

sug-gest that the physicochemical attributes resulting from

the molecular structure of antimicrobial peptides can

be useful in engineering selective and efficient

antipara-sitic therapeutic drugs

Acknowledgement

This research was supported by the Israel Science Foundation (grant 283⁄ 08)

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