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Conformational changes of Newcastle disease virus envelopeglycoproteins triggered by gangliosides Laura Ferreira, Enrique Villar and Isabel Mun˜oz-Barroso Departamento de Bioquı´mica y B

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Conformational changes of Newcastle disease virus envelope

glycoproteins triggered by gangliosides

Laura Ferreira, Enrique Villar and Isabel Mun˜oz-Barroso

Departamento de Bioquı´mica y Biologı´a Molecular, Universidad de Salamanca, Spain

We have investigated the conformational changes of

New-castle disease virus (NDV) glycoproteins in response to

receptor binding, using

1,1-bis(4-anilino)naphthalene-5,5-disulfonic acid (bis-ANS) as a hydrophobicity-sensitive

probe Temperature- and pH-dependent conformational

changes were detected in the presence of free bovine

gan-gliosides The fluorescence of bis-ANS was maximal at

pH 5 The binding of bis-ANS to NDV was not affected

by chemicals that denature the fusion glycoprotein, such as

reducing agents, nor by the presence of neuraminidase

inhibitors such as N-acetyl neuramicic acid Gangliosides

partially inhibited fusion and hemadsorption, but not neuraminidase hemagglutinin-neuraminidase glycoprotein (HN) activity A conformational intermediate of HN, trig-gered by the presence of gangliosides acting as receptor mimics, was detected Our results indicate that, upon binding

to free gangliosides, HN undergoes a certain conformational change that does not affect the fusion glycoprotein Keywords: NDV; bis-ANS; conformational intermediates; paramyxovirus receptors; gangliosides

Newcastle disease virus (NDV) is an avian enveloped

virus belonging to the family of Paramyxoviridae, genus

Avulavirus The membrane contains two transmembrane

glycoproteins, hemagglutin-neuraminidase (HN) and the

fusion (F) protein [1] HN binds to sialic acid-containing

receptors at the cell surface through its hemagglutinating

activity (receptor-binding activity) and it also displays

neuraminidase or sialidase activity (receptor-destroying

activity), which probably prevents the aggregation of the

viral progeny In addition, a third activity (the so-called

fusion promotion activity) has been proposed for the HN

protein [2–4] The F protein is directly responsible for the

fusion between the viral envelope and the target

mem-brane For paramyxoviruses, the fusion mechanism has

been proposed to occur at neutral pH; nevertheless, we

have previously shown that the fusion of NDV with

cultured cells is enhanced at acidic pH [5] The F protein

is produced as a single inactive polypeptide, Fo, which,

once cleaved by a cellular protease (reviewed in [6]),

becomes the active F1-F2 form, with two peptides linked

by a disulfide bond [7] To date, three domains of the F1 polypeptide have been suggested to be involved in the fusion mechanism of NDV These are the N-terminal fusion peptide [8] and two heptad repeat (HR) regions of the ectodomain, one (HR1) located adjacent to the fusion peptide, and the other (HR2) at the C-terminal adjacent to the transmembrane domain [9–11] Once activated, the F protein is thought to undergo a series of conformational changes that result in exposure of the fusion peptide and interaction of the HR1 and HR2 domains A six-helix bundle has emerged as the fusion core structure of many viral fusion proteins, the N-terminal HR forming the inner core, surrounded by antiparallel C-terminal helices along the grooves located between the helices of the central HR coiled-coil The formation of this structure is believed to pull the viral and cell membranes into close proximity for merging The complete mechanism of NDV-induced membrane fusion remains unknown As with many other paramyxo-viruses, NDV needs type-specific HN–F interactions that must be present in the same bilayer to induce fusion (reviewed in [12]) It has been proposed that the interaction

of HN with the cellular receptor induces conformational changes in the HN protein that activates the F protein [12], although the nature of such changes is obscure

In the present study we analyzed the possible conform-ational changes ocurring in NDV envelope glycoproteins when interacting with free gangliosides as receptor mimics These changes were revealed through use of the fluorescent probe 1,1-bis(4-anilino)naphthalene-5,5-disulfonic acid (bis-ANS), which is nonfluorescent in aqueous solution but increases its quantum yield when bound to hydrophobic groups [13,14] We observed that bis-ANS fluorescence was maximal at 37C and at acidic pH As reduction of the disulfide bond of the F protein did not affect bis-ANS

Correspondence to I Mun˜oz-Barroso and E Villar, Departamento

de Bioquı´mica y Biologı´a Molecular, Universidad de Salamanca,

Edificio Departamental Laboratory 108, Plaza Doctores

de la Reina s/n, 37007 Salamanca, Spain.

Fax: + 34 923 294579, Tel.: + 34 923 294465,

E-mail: imunbar@usal.es and evillar@usal.es

Abbreviations: bis-ANS, 1,1-bis(4-anilino)naphthalene-5,5-disulfonic

acid; DMEM, Dulbecco’s modified Eagle’s medium; F protein,

fusion glycoprotein; FDQ, fluorescence dequenching; HA,

influenza hemagglutinin; Had, hemadsorption; HN,

hemagglutinin-neuraminidase glycoprotein; HR, heptad repeat; KNP, 120 m M KCl,

30 m M NaCl, 10 m M sodium phosphate pH 7.4; NDV, Newcastle

disease virus; NeuAc, N-acetylneuraminic acid; p.f.u., plaque

formation units; R 18 , octadecylrhodamine B chloride.

(Received 7 November 2003, accepted 9 December 2003)

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fluorescence, we suggest that the binding of NDV to free

gangliosides results in the formation of a conformational

intermediate of HN

Materials and methods

Materials

Bis-ANS and octadecyl rhodamine B chloride (R18) were

from Molecular Probes Inc (Junction City, OR, USA)

Bovine brain gangliosides, disialoganglioside GD1a,

lacto-cerebrosides, dithiothreitol, 2-mercaptoethanol,

N-acetyl-neuraminic acid and Triton X-100 were all from SIGMA

(St Louis, MO, USA) Cell culture media were from BIO

Whittaker (Walkersvile, Maryland, USA) Fresh blood from

healthy donors (with their consent) was obtained from the

Blood Bank of the University Hospital in Salamanca (Spain)

Cells and viruses

NDV Clone 30 was grown and purified essentially as

described elsewhere [15] COS-7, HeLa and Vero cells were

obtained from the American Type Culture Collection and

were maintained in Dulbecco’s Modified Eagle Medium

(DMEM) supplemented with L-glutamine (580 mgÆL)1),

penicillin/streptomycin (100 UÆmL)1/100 lgÆmL)1), and

heat-inactivated fetal bovine serum at 10% (v/v) for

COS-7 and HeLa cells and at 5% (v/v) for Vero cells

For the fusion experiments, COS-7 cells grown in

monolayers were detached with trypsin/EDTA Trypsin

was inactivated by the addition of DMEM The cells were

washed twice with 15mM Hepes buffer (130 mM NaCl,

5 mM KCl, 2 mM CaCl2, 1 mM MgCl2, 10 mM glucose),

pH 7.4, and resuspended at 2.5· 106 cells in 200 lL of

Hepes buffer, pH 7.4

Ganglioside-induced conformational changes

Bis-ANS was added to 20 lg of NDV at 3 lM in Hepes

buffer (final volume, 2 mL) under constant stirring in the

fluorimeter cuvette Then, different concentrations of

gan-gliosides were added, and the fluorescence progress curve

was recorded for 2 min on a Hitachi F-4010

spectrofluo-rimeter (excitation, 395nm; emission, 500 nm; slit widths

5and 10 nm for excitation and emission, respectively) The

background fluorescence resulting from gangliosides was

calculated

To analyse the bis-ANS data, the relative fluorescence

(Irel) was calculated according to [16]:

IrelðtÞ¼ ðIðtÞ INDVþbis-ANSÞ=ðImaxBGIbis-ANSÞ ð1Þ

where I(t)is the fluorescence intensity at any given time,

INDV + bis-ANSis the fluorescence intensity of bis-ANS in the

presence of the virus, ImaxBGis the final fluorescence intensity

of bis-ANS in the presence of gangliosides, and Ibis-ANSis the

fluorescence intensity of bis-ANS in aqueous solution

R18fusion assays

Dequenching fusion assays were accomplished as described

previously [5] Briefly, purified NDV was labeled with the

fluorescent probe octadecylrhodamine (R18) and after mixing with the target cells, the progress curve of R18 fluorescence was spectrofluorimetrically monitored Neuraminidase assays

Neuraminidase activity was determined by a fluorimetric procedure using 2¢-(4-methylumbelliferyl)a-D -N-acetyl-neuraminic acid as substrate [17]

Hemadsorption assays The hemadsorption (Had) activity of HN protein was determined according to [18] with modifications HeLa cells were plated in 24-well plate 12 h before infection Then, the cell monolayers were infected with NDV at 1 multiplicity of infection At 24 h postinfection, the cells were washed twice with NaCl/Pi(10 mMKH2PO4, 15 0 mMNaCl, pH 7.2) and incubated for 30 min at 4C with 2% of human erythro-cytes After washing twice with NaCl/Pi, adsorbed erythro-cytes were lysed in 50 mMNH4Cl for 5min at 4C The lysates were clarified by centrifugation and Had activity was quantified by measuring the absorbance at 540 nm and subtracting the background absorbance obtained with uninfected cells To analyse the effect of gangliosides on Had activity, the cells were incubated in the presence of different concentrations of gangliosides for 10 min at 37C before the addition of red blood cells

Results and discussion

It has been shown previously that the exposure of hydro-phobic regions of viral proteins as a consequence of conformational changes can be analyzed by means of the hydrophobic-sensitive probe bis-ANS [14,16,19] This water-soluble fluorophore undergoes a strong increase in its quantum yield upon binding to hydrophobic sites [16] and has been used to study protein structural changes [14,16,19,20] The exposure of hydrophobic segments of NDV envelope proteins triggered by gangliosides was tested

by measuring binding to bis-ANS Initially, the effect of increasing concentrations of NDV or gangliosides on bis-ANS fluorescence was studied For these experiments, at zero time the virus was added to 37C-prewarmed Hepes buffer at pH 7.4 in the fluorimeter cuvette, followed by the addition of 3 lM of bis-ANS The fluorescence emitted, taken as INDV+bisANS, became stablilized after a few seconds Then, gangliosides were added and the progress curve of the fluorescence emission at 500 nm was recorded for 2 min To process the data, Irelwas calculated according

to Eqn (1) INDV+bis-ANSwas subtracted from the intensity

of fluorescence observed at any given time and this was related to the term ImaxBG–Ibis-ANS, i.e the maximal fluorescence of gangliosides in the absence of virus (ImaxBG) after subtracting the fluorescence emission of the probe in buffer (Ibis-ANS) Figure 1 shows the dose–response curves

of bis-ANS fluorescence in the presence of different concentrations of NDV As can be seen, after 20 lg of NDV the fluorescence reached a plateau, suggesting saturation Similarly, different concentrations of bovine brain gangliosides or of the disialoganglioside GD1a

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(5–30 lg) were added to 20 lg of NDV in the presence of

bis-ANS (Fig 2), and it was found that 10 lg of bovine

brain gangliosides and 5 lg of GD1a were sufficient to

observe saturation under the conditions of the experiment

The observed saturation of the extent of bis-ANS

fluores-cence (Figs 1 and 2) may indicate that the conformational

change undergone by NDV glycoproteins in the presence of

gangliosides is limited (see below)

To assess the specific effect of gangliosides, 20 lg of NDV

was preincubated in the presence of 10 lg of bovine

gangliosides at 37C for 10 min Then, an additional

10 lg was added and no increase in bis-ANS fluorescence

was detected above background (Table 1) We interpret

these results as pointing to the irreversibility of the

conformational change triggered by gangliosides In

addi-tion, neutral glycolipids such as lactocerebrosides did not

lead to an increase in the fluorescence of bis-ANS (Table 1)

The temperature-dependence of bis-ANS fluorescence at

neutral pH in the presence of NDV and gangliosides was

analyzed (Fig 3) The fluorescence of bis-ANS in the

Fig 1 Effect of NDV concentration on bis-ANS fluorescence At zero time, 3 l M bis-ANS was added to 37 C prewarmed buffer containing different concentrations of NDV, after which 25 lg of bovine gangliosides was added Fluorescence was recorded continuously over 2 min at excitation and emission wavelengths of 395and 500 nm, respectively The relative fluorescence, I rel , is shown (see Materials and methods) (A) Kinetics of bis-ANS fluorescence at different NDV concentrations from a representative experiment (B) Relative fluorescence of bis-ANS, I rel , at

90 s of reaction at the desired NDV concentration Data taken from different experiments similar to that shown in (A) Data are means ± SE of at least three independent experiments.

Fig 2 Effect of ganglioside concentrations on bis-ANS fluorescence At zero time, 3 l M bis-ANS was added to 37 C prewarmed buffer containing

20 lg of NDV, after which different concentrations of bovine brain gangliosides or GD1a were added Fluorescence was recorded continuously for

2 min at excitation and emission wavelengths of 395and 500 nm, respectively The relative fluorescence, I rel , is shown (see Materials and methods) (A) Kinetics of ANS fluorescence at different ganglioside concentrations from a representative experiment (B) Relative fluorescence of bis-ANS, I rel , at 90 s of reaction at the desired ganglioside concentration; (d), bovine brain gangliosides; (m), GD1a Data taken from different experiments similar to that shown in (A) Data are means ± SE of at least two independent experiments.

Table 1 Effect of preincubation of NDV with different agents on the fluorescence of bis-ANS NDV (20 lg) was incubated in the presence of

10 lg of bovine brain gangliosides, 10 m M NeuAc or 50 m M NeuAc for 10 min at 37 C Then, 3 l M bis-ANS was added to prewarmed buffer at 37 C containing 20 lg of treated virus, after which 10 lg of bovine gangliosides or 10 m M NeuAc were added for triggering the conformational change Fluorescence was recorded continuously over

2 min at excitation and emission wavelengths of 395and 5 00 nm, respectively I rel at 90 min of reaction are shown (see Materials and methods).

Preincubation

Trigger of the conformational change I rel

– Bovine gangliosides (10 lg) 6.98 – NeuAc (10 m M ) 15.45 – Lactocerebrosides (10 lg) 0.85 Bovine gangliosides (10 lg) Bovine gangliosides (10 lg) 0.6 Bovine gangliosides (10 lg) NeuAc (10 m M ) 12.71 NeuAc (10 m M ) Bovine gangliosides (10 lg) 8.31 NeuAc (50 m M ) NeuAc (10 m M ) 1.97

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presence of NDV but in the absence of gangliosides

[INDV+bisANSfrom Eqn (1)], was independent of

tempera-ture (data not shown) No increase in fluorescence was

observed at 4C, whereas it increased gradually at 15and

25C, showing a sharper increase after 30 C These data

are comparable to those of the temperature-dependence of

NDV fusion with cultured cells reported by us previously

[5] In both cases, we failed to detect an increase in

fluorescence at 4C Nevertheless, it has been established

that the HN protein of paramixoviruses can bind to the

sialoglycosides of the cell surface at 4C [21], suggesting

that NDV may interact with gangliosides at this

tempera-ture However, this binding seems to be insufficient to

trigger any conformational change in NDV glycoproteins

detectable with the bis-ANS technique

The pH-dependence of the fluorescence of bis-ANS in the

presence of NDV and gangliosides was also analyzed

(Fig 4) At zero time, NDV was added to 37C-prewarmed

buffer at the desired pH, followed by the addition of 3 lM

bis-ANS and then gangliosides; next Irelwas calculated as

described above Figure 4A shows the kinetics of bis-ANS

fluorescence in the presence of NDV and gangliosides at different pH values; Fig 4B depicts the final extent of bis-ANS fluorescence after 90 s of virus–ganglioside contact The extent of bis-ANS fluorescence at the different

pH values assayed occurred in the following order:

pH 5 > pH 5.5 > pH 6.5 > pH 7 It has been reported that the increase in fluorescence at low pH can be partly explained in terms of the protonation of negatively charged groups, which facilitates the binding of bis-ANS [14] In this sense, we detected a slight increase in the fluorescence of bis-ANS in the presence of NDV upon lowering the pH [INDV+bis-ANSin Eqn (1)], but these figures were subtracted from the fluorescence intensity emitted in the presence of gangliosides (Eqn 1) In Fig 4B, a sharp increase in fluorescence intensity at pH < 6.5can be seen The fluorescence intensity observed at pH 5was about twice the value seen at pH 7.4 This difference is smaller than that reported for viruses that show a pH-dependent entry mechanism, since for influenza virus Korte and Herrman (1994) [14] have reported that bis-ANS fluorescence is five times higher at acidic than at neutral pH Our data on the

Fig 4 pH-dependence of the bis-ANS fluorescence At zero time, 3 l M bis-ANS was added to 37 C prewarmed buffer at the desired pH containing

20 lg of NDV, after which 15 lg of bovine gangliosides was added Fluorescence was recorded continuously over 2 min at excitation and emission wavelengths of 395and 500 nm, respectively The relative fluorescence, I rel , is shown (see Materials and methods) (A) Kinetics of bis-ANS fluorescence at different pHs from a representative experiment (B) Relative fluorescence of bis-ANS, I rel , at 90 s of reaction at different pHs Data are means ± SE of two independent experiments.

Fig 3 Temperature-dependence of bis-ANS fluorescence At zero time, 3 l M bis-ANS was added to buffer prewarmed to the desired temperature containing 25 lg of NDV, after which 10 lg of bovine gangliosides was added Fluorescence was recorded continuously over 2 min at excitation and emission wavelengths of 395and 500 nm, respectively The relative fluorescence, I rel , is shown (see Materials and methods) (A) Kinetics of bis-ANS fluorescence at different temperatures from a representative experiment (B) Relative fluorescence of bis-bis-ANS, I rel , at 90 s of reaction at the desired temperature Data are means ± SE of two independent experiments.

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pH-dependence of bis-ANS fluorescence indicate that the

conformation of NDV proteins triggered at acidic pH

exposes a higher number of hydrophobic

fluorophore-binding sites It is interesting to note the similarities between

the pH-dependence of NDV fusion activity reported

previously by us [5] and that of bis-ANS fluorescence,

pointing to the maximal extent of both fusion and bis-ANS

fluorescence at pH 5.0 We have previously hypothesized [5]

that NDV might use the endocytic pathway as a secondary

mechanism of entry If the conformational change

under-gone by HN protein after receptor binding (see below) is

activated at acidic pH, as well as NDV fusion activity, the

present data confirm our hypothesis concerning the acidic

pH enhancement of NDV entry Moreover, the

pH-dependence of viral entry seems debatable In this sense,

Mothes et al [22] have reported that the entry of the avian

leukosis virus, a retrovirus, into the host cell depends on a

low pH step that acts after receptor binding For these

authors, partial conformational changes in env protein in

the presence of soluble receptors may be due to receptor

priming rather than complete activation Additionally, it

has been recently reported [23] that the SER paramyxovirus

shows a low-pH-dependent fusion activity

We performed a series of experiments to elucidate

whether the binding of bis-ANS to hydrophobic sites of

NDV glycoproteins was located in F and/or HN protein

First, NDV was incubated in the presence of 10 mM

2-mercaptoethanol or 2 mM dithiothreitol (agents that

reduce the disulfide bonds of the F protein) for 30 min at

37C before the addition of bis-ANS and gangliosides As

deduced by PAGE analysis (data not shown), treatment of

viruses with 2-mercaptoethanol led to the loss of F0protein

In another series of experiments, viruses were incubated in

the presence of 50 mM of N-acetylneuraminic sialic acid

(NeuAc) for 30 min at 37C This compound is both a

product and an inhibitor of the neuraminidase activity of

the HN protein through binding to its active site [17]

Neither treatment affected the emission of bis-ANS

fluor-escence with respect to the control (NDV without

treat-ment) when gangliosides were added to treated viruses in the

bis-ANS assay (Table 1 and data not shown) To test the

possibility that bis-ANS might bind nonspecifically to

2-mercaptoethanol-treated-virus, we performed the

follow-ing experiment Twenty micrograms of virus, both treated

and nontreated with the reducing agent, were preincubated

in the presence of 10 lg of bovine gangliosides for 10 min at

37C Then, a further 10 lg of gangliosides was added

in the bis-ANS assay In both cases, no increase in bis-ANS

fluorescence was detected above the background level,

unlike the findings on treated virus not preincubated in the

presence of gangliosides (data not shown) We therefore

assume that the fluorescence of bis-ANS of reduced virus in

the presence of gangliosides would not be due to the

nonspecific binding of the probe to

2-mercaptoethanol-treated-NDV Because viruses treated with these reducing

agents are fusion-deficient (data not shown), this seems to

indicate that the newly exposed hydrophobic binding sites

are not located within the F protein On the other hand, the

increase in bis-ANS fluorescence did not vary after

pre-incubation with NeuAc, suggesting that the binding of

gangliosides, the putative agents of the conformational

change, did not compete with the neuraminidase inhibitor

NeuAc To test this hypothesis, we performed a direct binding assay between the sialic acid NeuAc and NDV using the bis-ANS technique Our data indicate that, similarly to gangliosides, NeuAc leads to an increase in the fluorescence of bis-ANS in the presence of NDV (Table 1) We performed a series of experiments to analyze the relationship between ganglioside and NeuAc binding sites NDV was incubated in the presence of 10 lg of bovine brain gangliosides or 10 mMNeuAc for 10 min at 37C Then, 3 lM bis-ANS was added to prewarmed buffer at

37C containing 20 lg of treated virus, after which an additional 10 lg of bovine gangliosides or 10 mMNeuAc were added to trigger the conformational change Our results revealed that preincubation of NDV in the presence

of NeuAc did not abolish the increase in fluorescence when gangliosides were added, but it did abolish it when additional NeuAc was added By contrast, preincubation

of NDV in the presence of gangliosides did not abolish the increase in fluorescence when NeuAc was added, but it did

so when additional gangliosides were added (Table 1) Our conclusion is that the binding sites for NeuAc do not compete with the binding sites for gangliosides

As mentioned above, we detected the exposure of hydro-phobic binding sites of NDV proteins as measured by the increase in bis-ANS emission intensity (Figs 1–4), triggered

by gangliosides We assume that the new hydrophobic binding sites must belong to the envelope glycoproteins of NDV as the fluorophore shows a pronounced affinity for the hydrophobic sites of proteins in comparison with its affinity for lipids ([14] and references therein) The next step was to investigate whether the presence of gangliosides might exert some effect on NDV envelope glycoprotein activities First, the fusion of NDV with COS-7 cells was analyzed by assaying the dequenching of the R18incorporated into the viral membrane (see Materials and methods) For this, 20 lg

of R18-labeled NDV was incubated in the presence of 25 lg

of bovine gangliosides for 10 min at 37C Then, 2.5 · 106 COS-7 cells were added and the dequenching of R18 fluorescence was recorded for 30 min Data from a typical experiment are depicted in Fig 5 As can be seen, fusion was not abolished although it was partially inhibited, showing an inhibition of the extent of fusion of about 27% as compared with controls at 30 min of virus–cell contact This reduction was slightly lower if gangliosides were added to the virus–cell mixture (at time zero) without preincubation (20% as compared with control) As we observed that the denatur-ation of F protein by the cleavage of disulfide bonds did not exert any effect on bis-ANS fluorescence (data not shown),

we assume that the partial inhibition of fusion exerted by gangliosides could be an indirect effect on fusion due to a certain inhibition of the virus binding to cells in the presence

of gangliosides As discussed below, gangliosides would bind

to HN, lowering its interaction with COS-7 cell receptors and subsequently fusion of the virus with the cells In addition, the ability of the gangliosides to inhibit HN hemadsorption activity was analyzed NDV-infected HeLa cells were incubated in the presence of different concentrations of gangliosides for 1 h at 37C before the addition of red blood cells As shown in Fig 6, the data indicated that the inhibition of the Had activity of NDV HN protein exerted

by bovine brain gangliosides was dose-dependent Taken together, these results strongly suggest a specific interaction

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of the viral proteins with gangliosides, which would act as

receptor mimics In this sense, free gangliosides might

compete with the actual receptors of the cell surface,

inhibiting viral glycoproteins activities (Figs 5and 6) Other

simple molecules have previously been used to trigger

conformational changes on viral receptors as soluble CD4

that induces certain conformational changes upon binding

to envelope glycoproteins of HIV and SIV [20,24]

Viral HN glycoprotein has three different biological activities, sialidase or neuraminidase, hemagglutinating or receptor-binding, and fusion promotion Although there is a considerable body of evidence both in favour of and against the topological separation of the neuraminidase and recep-tor-binding site ([18] and references therein), the crystal structure of NDV HN protein [25] supports the notion of a single site Recently, on the basis of their crystallographic data on the HN protein of NDV, Crennell et al [25] have proposed the existence of a single sialic acid recognition site switchable between both activities: the binding site or catalytic site As summarized above, here we assayed (a) the effect of neuraminidase inhibitors on bis-ANS fluorescence and (b) the effect of gangliosides on neuraminidase and hemagglutinating activities The extent of bis-ANS fluores-cence triggered by gangliosides was not affected by the neuraminidase inhibitor NeuAc (Table 1) Moreover, the presence of gangliosides did not exert any effect on the neuraminidase activity of HN protein (data not shown), although they did inhibit Had in a dose-dependent manner (Fig 6) In addition, gangliosides and NeuAc did not compete for their binding sites in the bis-ANS assay (Table 1) Taken together, these data suggest that ganglio-sides bind to the receptor-binding site of HN protein and that this binding is not altered by the presence of neuraminidase inhibitors Therefore, the data presented here together with those from our previous work [19,26] fail

to account for the topological coincidence of both sites, although they do not allow us to propose their separation

In current models of membrane fusion induced by viral proteins, exposure of the fusion peptide that triggers membrane merging is a consequence of the conformational change of the F protein that involves the two heptad repeat regions (revised in [12]) The nature of these interactions and changes is not completely understood, although it has been established that for viruses that fuse with the target membrane through a pH-independent mechanism, such as most paramixoviruses and retroviruses, the conformational change of the F protein must be triggered after receptor binding Upon comparing the 3D structure of HN, both alone and in a complex with the neuraminidase substrate 2-deoxy-2,3-dehydro-N-acetylneuraminic acid, Takimoto

et al [27] suggested that receptor binding induces a structural change in the hydrophobic surface of the HN protein that disrupts physical HN–F interactions, triggering the activation of F protein to initiate membrane fusion Despite this, our results indicate that the binding alone of simple molecules is insufficient to induce strong HN conformational changes that would in turn affect the

F protein In other words, the conformational changes induced by free receptor mimic molecules are only partial

As we have shown here, NDV glycoproteins undergo conformational changes in the presence of gangliosides, as indicated by the exposure of new hydrophobic binding sites for the bis-ANS probe Our data strongly support the idea that binding to these receptor mimics induces a conform-ational change in HN protein Our observation that inactivation of the F protein did not affect the extent of bis-ANS fluorescence suggests that the fusion protein does not undergo any conformational change in the presence

of gangliosides Therefore, functional HN–F interactions

in vivo, i.e interactions that drive fusion, may need a more

Fig 5 Effect of bovine gangliosides on NDV fusion with COS-7 cells.

R 18 -labeled NDV (20 lg) was incubated in the presence of 25 lg of

bovine gangliosides for 10 min at 37 C Then, 2.5 · 10 5 COS-7 cells

were added and the sample was incubated at 37 C for 30 min under

continuous stirring Fusion was monitored continuously, as described

in Materials and methods, by measuring the dequenching of R 18 (d)

Control; (m) virus and gangliosides with preincubation; (j) virus and

gangliosides without preincubation.

Fig 6 Dose–response effect of ganglioside inhibition of hemadsorption.

HeLa cells were infected with NDV at 1 multiplicity of infection At

24 h postinfection, the cells were incubated in the presence of different

concentrations of gangliosides for 10 min at 37 C and then incubated

for 30 min at 4 C with 2% of human erythrocytes The rate of

hemadsorption in comparison with controls was calculated by

meas-uring the absorbance at 540 nm of the erythrocytes bound to

NDV-infected cells after lysing in 50 m M NH 4 Cl Data are means ± SE of

two independent experiments.

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complex environment than the presence alone of a putative

receptor, in this case gangliosides In addition, the

con-formational change undergone by the HN protein after

binding to gangliosides can be completed in the presence of

the correct target, i.e the cell membrane The binding of

viruses to the host cell surface is a more complex

phenom-enon than a mere bimolecular interaction between a viral

protein and a cellular receptor In this sense, viral binding

may occur through multiple interactions among several

viral and cellular molecules, accompanied by

conforma-tional changes in viral proteins Therefore, a major task

would be to study the conformational changes of NDV

proteins in the presence of cells Nevertheless, the high

extent of bis-ANS binding to hydrophobic sites of the cell

surface did not allow us to use this assay with intact cells as

targets (data not shown)

The existence of conformational intermediates for viral

proteins such as influenza HA [16], vesicular stomatitis

virus fusion protein [19,28] or HIV envelope glycoproteins

[20] has been reported Additionally, the binding of

bis-ANS to different viral glycoproteins [14,16,19,20] has been

correlated with the fusion activation of the proteins

Nevertheless, here we observed a conformational

inter-mediate of the HN protein prior to membrane merging,

confirming that changes leading to fusion might be slow

in the virus upon binding to the target membrane [16]

The newly exposed hydrophobic sequence of the HN

protein triggered by gangliosides is not clear We suggest

several possibilities: (a) the HR stalk region, which has

been proposed to be responsible for HN–F interactions

[29]; (b) the interfaces of HN dimers, which presumably

dissociate after ganglioside binding [27]; or (c) sequential

conformational changes in HN protein, as proposed for

other viral proteins [16]

In summary, here we have demonstrated that

ganglio-sides bind to NDV, inducing the exposure of hydrophobic

binding sites for bis-ANS We propose that the binding site

for gangliosides would be the receptor-binding site of HN

protein, triggering the conformational change detected here

Our results indicate that the bis-ANS assay would also be

useful for studying conformational changes in viral proteins

that do not require an acidic pH to start fusion and that

simple molecules such as gangliosides can be used as

receptor mimics for triggering these changes

Acknowledgements

This work was partially supported by the Spanish Fondo de

Investigaciones Sanitarias, FIS (PI021848) and Junta de Castilla y

Leo´n (SA 064/02) grants to E V.; L F is a predoctoral fellowship

supported by the Ministerio de Ciencia y Tecnologı´a, Spain (Grant

DGES PM97-0160) We thank Drs E Dı´ez Espada and J A.

Rodrı´guez from Intervet Laboratories (Salamanca, Spain) for

providing the lentogenic Clone 30 strain of NDV Thanks are

also due to N Skinner for language corrections and proofreading

the manuscript.

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