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N-Terminal segment of potato virus X coat protein subunitsis glycosylated and mediates formation of a bound water shell on the virion surface Lyudmila A.. Orekhovich Institute of Biomedi

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N-Terminal segment of potato virus X coat protein subunits

is glycosylated and mediates formation of a bound water

shell on the virion surface

Lyudmila A Baratova1, Nataliya V Fedorova1, Eugenie N Dobrov1, Elena V Lukashina1,

Andrey N Kharlanov2, Vitaly V Nasonov3, Marina V Serebryakova4, Stanislav V Kozlovsky1,

Olga V Zayakina1and Nina P Rodionova1

1

A N Belozersky Institute of Physico-Chemical Biology, Moscow State University, Russia;2Department of Chemistry, Moscow State University, Russia;3M M Shemyakin and Yu A Ovchinnikov Institute of Bioorganic Chemistry, Russian Academy of Sciences, Moscow, Russia;4V N Orekhovich Institute of Biomedical Chemistry, Russian Academy of Medical Sciences, Moscow, Russia

The primary structures of N-terminal 19-mer peptides,

released by limited trypsin treatment of coat protein (CP)

subunits in intact virions of three potato virus X (PVX)

isolates, were analyzed Two wild-type PVX strains, Russian

(Ru) and British (UK3), were used and also the ST mutant of

UK3 in which all 12 serine and threonine residues in the CP

N-terminal segment were replaced by glycine or alanine

With the help of direct carbohydrate analysis and MS, it was

found that the acetylated N-terminal peptides of both

wild-type strains are glycosylated by a single monosaccharide

residue (galactose or fucose) at NAcSer in the first position

of the CP sequence, whereas the acetylated N-terminal

seg-ment of the ST mutant CP is unglycosylated Fourier

transform infrared spectra in the 1000–4000 cm)1 region

were measured for films of the intact and in situ

trypsin-degraded PVX preparations at low and high humidity

These spectra revealed the presence of a broad-band in the

region of valent vibrations of OH bonds (3100–3700 cm)1), which can be represented by superposition of three bands corresponding to tightly bound, weakly bound, and free OH groups On calculating difference (wet minus dry) spectra,

it was found that the intact wild-type PVX virions are characterized by high water-absorbing capacity and the ability to order a large number of water molecules on the virus particle This effect was much weaker for the ST mutant and completely absent in the trypsin-treated PVX

It is proposed that the surface-located and glycosylated N-terminal CP segments of intact PVX virions induce the formation of a columnar-type shell from bound water molecules around the virions, which probably play a major role in maintaining the virion surface structure

Keywords: bound water; coat protein; Fourier transform infrared spectroscopy; glycosylation; potato virus X

Potato virus X (PVX) is the type member of the potexvirus

group of filamentous plant viruses [1] Its coat protein (CP)

was extensively studied and it has been shown that the CP

participation in the PVX infection cycle is not limited to its

role in virion formation The PVX CP has been shown to be

involved in processes of genomic RNA accumulation and

infection transport in plants [2–4] It is also responsible for

induction of the Rxresistance system in potato plants [5,6],

and has been recently shown to play a major part in

regulation of virion translational activity at different stages

of the infection process [7–10] These (and many others)

studies demonstrate the importance of potexvirus CP at all

stages of virus–plant interactions Thus, the question arises

which features of the CP structure determine the different kinds of its activity

It is well known that, on SDS/PAGE, intact PVX CP displays anomalously slow electrophoretic mobility This mobility corresponds for different PVX strains to molecular masses of 27–29 kDa, instead of 25 kDa as determined from the primary structure [11,12] In 1994 Tozzini et al [13] found that PVX CP contains O-linked carbohydrates It was the first report on the presence of glycosyl residues in coat proteins of plant viruses However, the exact nature of the glycosyl residues, their location in the PVX CP sequence, and their functional importance remain unknown Thus, a more detailed analysis is needed, all the more so, as it is now generally accepted that glycosylation can induce significant alterations in biopolymer structure and flexibility [14] High-resolution X-ray (fiber) diffraction data for potex-viruses are not available and only one, more or less detailed, model of PVX CP structure in the virion (based on tritium planigraphy and secondary-structure prediction data) has been suggested [15]

The N-terminal region of potexvirus CP is surface-located [15,16], highly sensitive to the action of plant sap proteases [12], and can be easily removed by mild trypsin treatment without disruption of the virion structure [17] To

Correspondence to L A Baratova, Department of Chromatography,

A.N Belozersky Institute of Physico-Chemical Biology, Moscow

State University, Moscow 119992, Russia Fax: + 7095 9393181,

Tel.: + 7095 9395408, E-mail: baratova@belozersky.msu.ru

Abbreviations: CP, coat protein; CPY, carboxypeptidase Y;

FTIR, Fourier transform infrared; PVX, potato virus X.

(Received 24 January 2004, revised 15 May 2004,

accepted 3 June 2004)

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elucidate the role of the PVX CP N-terminal region in

determining the physicochemical properties of the virion

surface, preservation of the virion integrity, and the

anomalous electrophoretic mobility, we used a special

PVX CP mutant In this mutant (designated ST) all serine

and threonine residues (potential glycosylation sites) in the

N-terminal segment are substituted by glycine or alanine

residues [7]

The aim of this work was to determine the presence and

nature of carbohydrate residues in the peptides removed by

a limited trypsin hydrolysis from the intact PVX virions of

two wild-type strains (Russian and British) and the ST

mutant The N-terminal amino-acid sequences of these

three PVX isolate CPs are shown in Fig 1 [7,18,19] It is

widely known that many polyoxy molecules (including

proteins) exist in water solution in a hydrated state, and the

presence of carbohydrate residues may greatly increase the

bound water content [20] To estimate bound water content

in the intact and trypsin-treated PVX virions, we used

Fourier transform infrared (FTIR) spectroscopy A possible

role for the surface-located and glycosylated PVX CP

N-terminal segment in preserving the structural and

func-tional integrity of the PVX virions is discussed

Materials and methods

Reagents and chemicals

Trypsin treated with 1-chloro-4-phenyl-3-L

-toluene-p-sulfo-namidobutan-2-one (TPCK-trypsin) was obtained from

Sigma Trifluoroacetic acid was from Perkin-Elmer

Aceto-nitrile was from Criochrom (St Petersburg, Russia)

Rea-gents for preparing gels were from Bio-Rad Laboratories

Water was obtained using a Milli-Q System (Millipore) All

other chemicals were analytical grade

For carbohydrate analysis, only freshly prepared reagents

thrice-distilled in quartz glassware water were used

Meth-anol was additionally purified by distillation over

magnes-ium methylate, and ethanol by distillation over calcmagnes-ium

oxide Pyridine was distilled twice over sodium hydroxide

and once over barium oxide HCl and trifluoroacetic acid

were additionally purified by distillation in borosilicate

glassware

Virus preparations

The Russian (Ru) and British (UK3) strains of PVX were

purified from systemically infected leaves of Nicotiana

benthamiana and Datura stramonium as described

previ-ously [9] The ST mutant of the UK3 strain with the

wild-type N-terminal sequence, SAPASTTQPIGSTTSTTTKT,

changed to AAPAGGAQPIGAGGAAGAKA was obtained

as described by Kozlovsky et al [7]

Limited tryptic digestion of the virus preparations Limited tryptic digestion of PVX virions (500 lg virus preparation in 0.5–1 mL 0.025MTris/HCl buffer, pH 8.0) was carried out at an enzyme/substrate ratio of 1 : 500 (w/w) for 2 h at 37C in 0.2MTris/HCl buffer, pH 8.0 In the case of the ST mutant, the tryptic digestion was carried out at an enzyme/substrate ratio of 1 : 2000 (w/w) Then the virus particles were pelleted by high-speed centrifugation

(50.2Ti rotor, Beckman L5-50; 105 000 g, 4C, 1.5 h), and pellets and peptide-containing supernatants were used for further analysis

SDS/PAGE SDS/PAGE (8–20% gels) was carried out essentially as described by Laemmli [21] The protein bands were visual-ized by staining with Coomassie Brilliant Blue (G-250)

HPLC equipment and conditions HPLC analyses were performed on a narrow-bore column (Milichrom A-02; EnviroChrom LC, Chromatography Institute ECONOVA, Novosibirsk, Russia; 75· 2 mm) packed with 5-lm particles of Nucleosil C18, pore size 120 A˚ (Macherey-Nagel, Duren, Germany) Separations were performed at 25C; a dual wavelength (214 nm and

280 nm) detector was used The elution gradient profile was as follows The elution solvents were A (0.1% trifluoroacetic acid in water, pH 2.2) and B (acetonitrile with 0.1% trifluoroacetic acid) The linear gradient was 0–60% B in 60 min and then 60–80% B in 10 min; the flow rate was 80 lLÆmin)1 Fractions were collected for subse-quent analysis using a Gilson 201 fraction collector Peptide yields were 30–50% The conditions used allowed separ-ation of all full-size PVX CP tryptic peptides

Identification of carbohydrates in tryptic peptides The method for determining the monosaccharide compo-sition of glycoconjugates (glycopeptides and glycoproteins) involved derivatization of the monosaccharides, released on acid hydrolysis, into N-(4-methylcoumarin-7-yl)glycamines (AMC-sugars) and their subsequent analysis by reverse-phase (RP) HPLC with fluorimetric detection [22] The authentic AMC-sugars were prepared by reductive N-alkylation of 7-amino-4-methylcoumarin with the fol-lowing monosaccharides in the presence of NaCNBH3:

D-Glc, D-Gal, D-Man, L-Fuc, D-GlcNAc, D-GalNAc,

D-ManNAc

HPLC analyses were performed on a Du Pont 8800 chromatograph equipped with fluorescence detector Columns with Ultrasphere ODS (Beckman; 250· 4.6 mm internal diameter) were used AMC-sugars were separated

at 25C using 17.5% ethanol in water with 0.1% trifluoro-acetic acid, pH 2.5–2.6 The flow rate was 0.75 mLÆmin)1

Carboxypeptidase Y (CPY) hydrolysis of N-terminal PVX CP tryptic peptide

For CPY hydrolysis, peptide-containing solutions were dried to eliminate trifluoroacetic acid and dissolved in water Fig 1 N-Terminal amino-acid sequences of the coat proteins of Russian

(Ru) and British (UK3) PVX strains and the ST mutant of UK3 PVX.

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to a concentration of  0.1 mgÆmL)1 CPY (Sigma) was

added to this solution to an enzyme/peptide ratio of 1 : 5

(w/w) Hydrolysis was carried out at 22C To obtain

MALDI mass spectra, 0.5-lL samples were removed at

different times from the hydrolysis start

Mass spectrometry

Mass spectra were obtained using a MALDI-TOF mass

spectrometer (Reflex III model; Bruker Analytic GmbH,

Bremen, Germany) with 337 nm UV laser A study sample

solution (0.5 lL) was mixed with an equal volume of

2,5-dihydroxybenzoic acid (Aldrich; 10 mgÆmL)1in 20%

acetonitrile in water with 0.1% trifluoroacetic acid), and the

mixture was dried in the air

Mass spectra of material from HPLC fractions and CPY

hydrolysates of NAcSAPAS-peptide were obtained in

reflectron mode with positive ion detection (mass peak

accuracy 0.015%) Mass spectra of CPY hydrolysates of the

N-terminal PVX CP tryptic peptide and its C-terminal

fragment were obtained in reflectron mode with negative ion

detection (peak accuracy 0.02%)

FTIR spectroscopy

IR spectra were acquired with a FTIR spectrometer

Equinox 55/S (Bruker Analytic GmbH, Bremen, Germany)

in the wavenumber range 1000–4000 cm)1 To obtain thin

films, 10 lL of the virus suspensions ( 6 mgÆmL)1) in

20 mMTris/HCl buffer, pH 7.8, were applied to BaF2plates

and dried in a vacuum desiccator (at 0.13 Pa) over P2O5at

20C, with visual control of the film homogeneity To

create 100% humidity, distilled water was placed at the

bottom of the desiccator

Analytical methods

Tryptic peptides were hydrolyzed as described by Tsugita &

Scheffler [23], and amino-acid analysis was carried out on a

Hitachi-835 analyzer (Tokyo, Japan) in the standard mode

for protein hydrolysate analysis with cation-exchange

separation and ninhydrin postcolumn derivatization The

short N-terminal amino-acid sequences of the tryptic

peptides were determined by Edman degradation on the

automated Procise cLC Protein Sequencing System (model

491; PE Applied Biosystems) Phenylthiohydantoin

deriva-tives of amino acids were identified with the PTH Analyzer

(model 120A; PE Applied Biosystems)

Results

Electrophoretic analysis of wild-type and mutant PVX CP

On SDS/PAGE of PVX preparations, it was found that

the intact wild-type and ST mutant CPs differ in their

electrophoretic mobility, and this difference disappears after

mild trypsin treatment resulting in removal of the

N-terminal CP peptide (Fig 2) This indicates that the

anomalous PVX CP electrophoretic mobility is determined

by the N-terminal segment

The relatively large difference in electrophoretic

mobili-ties between the intact wild-type and ST mutant CPs can

hardly be explained by minor differences in molecular mass and may be due to the absence of certain post-translational modifications in the mutant protein (see below)

HPLC analysis of the PVX CP peptides released

on limited trypsin hydrolysis After the trypsin treatment, PVX virions were pelleted by high-speed centrifugation, and the peptide-containing sup-ernatants were subjected to RP-HPLC The surface location

of the N-terminal CP peptide in PVX virions [15,16] suggests that the peptides released from the PVX virions on mild trypsin hydrolysis correspond to the N-terminal regions of the PVX CP subunits As can be seen in Fig 3, the supernatant from the ST mutant contains one major peptide fraction and the supernatants from the UK3 and Ru strains contain two [The differences in peak mobilities for the UK3 and Ru peptides are probably due to differences

in their amino-acid sequences: the former has proline and isoleucine at positions 9 and 10, respectively, and the latter has alanine and threonine (Fig 1).] The elution of the ST mutant peptide at higher acetonitrile concentrations than the UK3 peptide may be due to the substitution of 11 serine and threonine residues with glycine and alanine, which would increase the peptide hydrophobicity The minor amounts of other peptides observed in the chromatographic profiles in Fig 3 were not analysed further

Determination of primary structure of trypsin-cleaved peptides

The HPLC-purified peptide fractions were used for amino-acid analysis, microsequencing and MALDI MS The only peptide released on mild trypsinolysis of the ST mutant (Fig 3C) was the acetylated N-terminal peptide with a molecular mass of 1535 Da (Table 1), corresponding exactly to the calculated mass of the first 19 amino acids

of the ST mutant CP with an acetyl group The trypsin-cleaved peptides of the wild-type (Ru and UK3) PVX strains each gave two peaks (1 and 2) on RP-HPLC (Fig 3A,B) For both viruses, the amino-acid compositions

of the material in the two peaks were identical and coincided with that predicted for the corresponding N-terminal (19 residues) sequence (Fig 1) Microsequencing results were negative for all four peaks, confirming that material in all

Fig 2 Analysis of wild-type (UK3) PVX and ST mutant preparations

by SDS/PAGE (8–20% gels) Lanes 1 and 2, UK3 PVX; lanes 3 and 4,

ST mutant; lanes 1 and 3, CPs from intact virions; lanes 2 and 4, CPs from trypsin-treated virions.

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the peaks was N-blocked, in accordance with our previous results [15] Possible reasons for the differences in chroma-tographic mobility of peak 1 and peak 2 material were revealed by MS (Table 1) The molecular masses for both

Ru and UK3 peptides turned out to be significantly higher than expected In peak 1 (of both strains) this difference was

162 Da, corresponding exactly to the addition of a hexose residue In peak 2 (again for both viruses), a more complex picture was observed Some material had the same mass as

in peak 1, but there was also material with a molecular mass that differed from that expected by 146 Da (Table 1) This may correspond to the addition of a deoxyhexose residue

No peaks corresponding to more than a singly glycosylated peptide (i.e for instance, 2041 + 162 or 2041 + 146 in the case of the UK3 strain peak 1) were detected in the mass spectrograms These results forced us to turn to direct carbohydrate analysis

Chromatographic analysis of the PVX CP N-terminal peptide carbohydrates

Direct determination of carbohydrates in the PVX CP N-terminal peptides involved acid hydrolysis, derivatization

of released monosaccharides to AMC-sugars, and identifi-cation of derivatives by RP-HPLC with fluorescence detection [22] This analysis revealed (for both Ru and UK3 strains) the presence of a galactose residue (the additional 162 Da) in the material of peak 1 (Fig 3A,B) and both galactose and fucose (the additional 146 Da) residues in peak 2 (the data for the Ru strain are shown in Fig 4) These results correlated closely with the results of

MS (Table 1) No carbohydrates were found in the CP N-terminal peptide of the ST mutant, also in accordance with the MS

Thus, from the results of both MS and direct carbo-hydrate determination it follows that the surface-located N-terminal CP segments of the two wild-type PVX strains studied are glycosylated and contain a sugar residue (galactose or fucose) O-linked to serine or threonine residues, which are absent from the N-terminal CP peptide

of the ST mutant

The presence of galactose in both peak 1 and peak 2 may

be explained by the glycoconjugate stereochemistry It is known that carbohydrate diastereomers differ in their physicochemical properties, and therefore they may have

Fig 3 RP-HPLC separation of PVX CP preparations after mild

trypsin hydrolysis of intact virions (A) Russian strain (Ru); (B) British

strain (UK3); (C) ST mutant.

Table 1 Results of MS analysis of trypsin-cleaved PVX CP N-terminal fragments.

PVX strain

Peptide fraction number (Fig 3)

Peptide molecular mass (Da)

Observed Calculated Difference

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different chromatographic mobility on highly selective

sorbents

The question arises: are all CP subunits in the PVX

virions N-terminally glycosylated? On one hand, we

found no other major peaks on HPLC other than peaks

1 and 2 (Fig 3A,B), which indicates that the vast

majority of the 1300 CP molecules in the PVX virion

are glycosylated On the other, on mass spectrograms of

tryptic hydrolysates of the isolated full-size UK3 and Ru

CPs some material with molecular masses corresponding

to unglycosylated peptides (1879 and 1841 Da,

respect-ively) could be seen (data not shown) This may mean

that PVX virions contain a proportion (not more than

10%) of CP molecules that are not N-terminally

glycosy-lated, assuming that it is not the result of partial peptide

deglycosylation in the course of MS We did not observe

any peaks corresponding to deacetylated PVX CP

N-terminal peptides

Identification of glycosylation site(s) in the PVX CP N-terminal segment

To locate glycosylation site(s) in the N-terminal segment of PVX CP, we obtained spectra of MS fragmentation of material from chromatographic peaks 1 and 2, prepared by mild trypsin treatment of UK3 PVX virions (Fig 3) Standard MS fragmentation methods should lead to formation of ions of the peptide C-terminal fragments, because the dominant protonation site (Lys19) is located at the C-terminus In MALDI postsource decay spectra [24],

we observed only masses corresponding to ions of C-terminal fragments (y-ions) of our peptide without carbohydrate residues On the basis of these results, it may be suggested that the glycosylation site is located on the N-terminal serine of the peptide However, it is well known that, on MALDI fragmentation, intensive deglycosyla-tion takes place [25], making unequivocal conclusions

Fig 4 RP-HPLC analysis of carbohydrate content of the Ru strain CP N-terminal peptide Monosaccharides were analyzed as AMC derivatives (A) Analysis of a blank sample (eluate fraction between peaks in chromatographic profile shown in Fig 3) (B) Analysis of a standard mixture containing Glc, Gal, Man, Fuc, GlcNAc, GalNAc, ManNAc (C) Analysis of peak 1 (Fig 3A) (D) Analysis of peak 2 (Fig 3A).

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impossible MS sequencing using electrospray ionization

also resulted in deglycosylation

Therefore we decided to obtain a series of MALDI

spectra of PVX CP N-terminal tryptic peptides shortened

from the C-terminus by CPY hydrolysis [26] For these

experiments, we modified the procedure for preparing the

N-terminal PVX CP segment: time, temperature and

trypsin/protein ratio were kept the same, but the PVX

virion (and enzyme) concentration was increased about

fivefold On HPLC of the peptide-containing sample, three

major peaks were eluted before peaks 1 and 2 (Fig 5A)

Previously, we sometimes obtained similar

chromato-graphic profiles but did not analyze them further supposing

that they resulted from overhydrolysis However, this time

we performed MALDI MS analysis of all five peaks eluted

at the beginning of the chromatogram (peaks 1*, 2*, 3*, 1 and 2 in Fig 5A)

For peaks 1 and 2, molecular masses of 2025 and

2041 Da were obtained as before (Table 1) The molecular mass of peak 3* was 1424 Da, corresponding to the unglycosylated C-terminal part of the PVX CP N-terminal tryptic peptide (Thr6–Lys19; Fig 1) Figure 5B shows a combined MALDI mass spectrum of peptides from peaks 3*, 1 and 2 after partial CPY hydrolysis The observed mass values of fragments produced by sequential removal of the C-terminal residues (up to Ile10) from the initial tryptic peptide confirm the localization of a carbohydrate residue

in the nonfragmented N-terminal part of the analyzed CP peptide Moreover, the mass spectrum of peak 3* material treated with CPY confirmed our suggestion about its

Fig 5 Stages of glycosylation site identification (A) Initial part of RP-HPLC profile of PVX preparation after modification of the trypsin treatment procedure (see text) (B) Combined MALDI mass spectrum of material from peaks 3*, 1 and 2 after partial CPY hydrolysis (C) MALDI mass spectra of peak 2* material before (upper part) and after (lower part) CPY treatment (642 Da, sodium salt of deoxyhexose-containing peptide;

658 Da, potassium salt of the same peptide and/or sodium salt of hexose-containing peptide; 674 Da, potassium salt of hexose-containing peptide; additional peaks in lower spectrum correspond to salts from CPY solution).

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primary structure Thus, carbohydrate residues could be

linked only to Ser1 or Ser5 of our peptide N-terminal

pentameric part NAcSAPAS-

Peaks 1* and 2* were shown to contain only these

modified N-terminal pentapeptides: in peak 1*, hexose was

linked to the peptide, and in peak 2* (just as in peak 2) either

hexose or deoxyhexose With the help of CPY hydrolysis,

we managed to unambiguously localize the glycosylation

site in the PVX CP N-terminal segment In Fig 5C,

MALDI mass spectra of peak 2* material before and after

CPY treatment are shown (upper and lower parts,

respect-ively) Mass values in the upper part correspond to ions of

sodium and potassium salts of the glycosylated peptide

NAcSAPAS After CPY treatment, the unglycosylated

C-terminal serine was released (lower part of Fig 5C),

confirming our suggestion that a hexose or deoxyhexose

residue is linked to the acetylated N-terminal serine residue

(NAcSer1) of the PVX CP

As far as we know, this type of glycosylation has not

previously been observed in plant virus proteins

FTIR spectroscopy of wild-type and mutant virus

preparations

Figure 6 shows FTIR spectra in the 1000–4000 cm)1region

for films of the intact and trypsin-treated Ru PVX and the

intact ST mutant preparations To compare the

water-absorbing capacity of the different PVX variants, we

measured their FTIR spectra in dry films and after

saturation of the film with water at 100% relative humidity Infrared band assignments were taken from Parker’s book [27] In the FTIR spectra, peaks corresponding to valent CH-bond vibrations ( 2900 cm)1), valent C¼O bond vibrations (amide I,  1650 cm)1), deformational amide group vibrations (amide II, 1550 cm)1, and amide III,

 1300 cm)1) can be seen (Fig 6) A broad-band in the 3100–3700 cm)1 region corresponds to superposition of several absorption peaks Here a complex band of valent water OH-bond vibrations is overlapped with peaks of valent OH-bond and NH-bond vibrations of PVX CP Thus, to estimate the state of water molecules in the virus preparations, we calculated FTIR difference spectra (the samples at 100% humidity minus dry samples)

The broad 3100–3700 cm)1band in the difference spectra (Fig 7) can be represented by superposition of three bands corresponding to absorption of OH bonds in tightly bound

OH groups (the band at 3240 cm)1), in weakly bound

OH groups ( 3440 cm)1) and in free OH groups of absorbed water molecules ( 3600 cm)1) [27] From the data in Fig 7, it can be seen that the intact wild-type PVX differs from the other virus preparations by a greatly increased water-absorbing capacity What is even more important, on saturation of the wild-type PVX film with water, an intense 3240 cm)1 band was observed in the difference spectrum, supporting the ordering of a large number of water molecules on the virus particle This effect was much weaker for the ST mutant and completely absent

in the case of the trypsin-treated PVX

Fig 6 FTIR absorbance spectra of the intact and trypsin-treated Ru PVX and of the intact ST mutant preparations in the 1000–4000 cm-1region, for dry films and after saturation of the film with water at 100% relative humidity.

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The role of CP glycosylation in plant virus life cycles

remains unclear, although data on the effects of

glycosyla-tion on the conformaglycosyla-tion and dynamics of O-linked

glycoproteins are accumulating [28–30]

First, we were interested in the presence of glycosyl

modification(s) in the trypsin-cleaved PVX CP N-terminal

segment Structural analysis of the peptides cleaved from the

wild-type protein revealed the presence of two

monosac-charides, galactose and fucose, alternatively linked to

NAcSer in the first position of the CP sequence

It was also shown that almost all PVX CP subunits in the

wild-type PVX virion contain sugar residues in their

N-terminal peptides Small amounts of unglycosylated CP

in the virus samples may originate from the virion ends,

where the subunit conformation may be unsuitable for

glycosylation

What is the importance of this CP N-terminal

glycosy-lation for PVX virion structure and function? According to

our model [15], the PVX CP N-terminal segment is located

on the virion surface and forms a super-secondary structure,

a three-stranded b-sheet We presume that removal of this

structure leads to drastic changes in the physicochemical

properties of the PVX virion surface

It is widely known that water in close proximity to the

protein surface is fundamental to protein folding, stability,

recognition and activity, and thus understanding protein

hydration is crucial in unraveling protein functions [31]

Virus particles with their unique highly regular morphology

may be especially interesting in this respect Different types

of macromolecule structures are known to have different

types of hydration shell: columnar or sheet-like Cylindrical structures (which helical viruses have) usually induce the columnar type of hydration [20]

The results of our comparative FTIR spectroscopy study

of the intact wild-type and ST mutant PVX virions and the trypsin-treated wild-type virus particles suggest the pres-ence of a large number of ordered water molecules (water shell) around intact wild-type virions Thus, a PVX virion may be considered as an electric cable with several layers of insulation The virus RNA is packed into the ordered helical protein shell The surface-located CP subunit N-terminal segments with their fixed super-secondary structure of three b-strands and glycosyl residues linked

to the N-terminal serines form the next ordered layer of the cable structure The surface layer of the cable is formed by

a shell consisting of ordered water molecules NMR and ESR data show [32] that two water molecules are usually bound per sugar ring, i.e about 2600 molecules per PVX virion

Besides the presence of sugar residues, the wild-type PVX

CP N-terminal segment is also characterized by exception-ally high content of hydroxyl-containing amino acids (11 serine and threonine residues in the 19-residue sequence) This, as well as the predicted existence of a three-stranded b structure in this segment [15], may facilitate tightly bound water shell formation Moreover the presence

of deep grooves on the surface of helical PVX particles was recently demonstrated by fiber X-ray diffraction analysis [33], and, as shown by Falconi et al [31], water hydration sites are mainly located around protein cavities and clefts Raman optical activity spectra also indicate a high degree of hydration in PVX virions [34]

Fig 7 FTIR difference (‘wet’ minus ‘dry’) spectra of the intact and trypsin-treated Ru PVX and the intact ST mutant preparations in the 2500–

4000 cm)1region.

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The PVX virions without N-terminal CP peptide do not

simply lose the surface layer of water molecules; this loss

would lead to drastic changes in physicochemical properties

of the virion surface We propose that the absence of the

outer ordered water layer explains the greater sensitivity to

trypsin of the ST mutant virions compared with the

wild-type PVX particles [7]

Other data [2,17] support our suggestion of critical

changes in PVX virions on cleavage (or changing) of the CP

N-terminal peptide In their 1972 electron microscopy

study, Tremaine & Agrawal [17] observed unusual twisting

of trypsin-treated PVX particles In 1992 Chapman et al [2]

reported that a PVX CP deletion mutant, devoid of 19

N-terminal amino-acid residues, produces virions with

abnormal morphology

We suggest that the presence of an ordered water

column around PVX virions, by itself and/or through

formation of a water-mediated net of hydrogen bonds

between (or inside) CP subunits, strongly affects the

structure and properties of the externally located regions

of the virus protein coat However, it cannot be excluded

that the structure of internally located parts of the virion

protein subunits and the structure of the virion itself are

affected by changes in the state of the virion water shell

and this state may be altered by changes in glycosylation,

phosphorylation and other types of modification of the

externally located virus CP regions In this way the

structure of a whole virion may be changed by a signal

molecule binding to the virion surface Recent observations

[7–10] that the ST mutant intravirus RNA, in contrast with

that of the wild-type PVX, is accessible to ribosomes in the

intact virions and can be effectively translated in cell-free

systems may be an example of such a structural transition

We plan to continue to study structural alterations in the

PVX CP subunits in virions induced by N-terminal

segment modification or cleavage

Acknowledgements

We thank Professor J G Atabekov for valuable discussions The work

was partially supported by Russian Foundation for Basic Research

(grants 02-04-48651 and 03-04-48833).

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