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Identification of different isoforms of eEF1A in the nuclear fractionof human T-lymphoblastic cancer cell line specifically binding to aptameric cytotoxic GT oligomers Barbara Dapas1, Gi

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Identification of different isoforms of eEF1A in the nuclear fraction

of human T-lymphoblastic cancer cell line specifically binding

to aptameric cytotoxic GT oligomers

Barbara Dapas1, Gianluca Tell2, Andrea Scaloni3, Alex Pines2, Lino Ferrara3, Franco Quadrifoglio1

and Bruna Scaggiante1

1

Department of Biomedical Sciences and Technologies, University of Udine, Italy;2Department of Biochemistry, Biophysics and Macromolecular Chemistry, University of Trieste, Italy;3Proteomics and Mass Spectrometry Laboratory, ISPAAM,

National Research Council, Naples, Italy

GT oligomers, showing a dose-dependent cytotoxic effect on

a variety of human cancer cell lines, but not on normal

human lymphocytes, recognize and form complexes with

nuclear proteins.By working with human T-lymphoblastic

CCRF-CEM cells and by using MS and SouthWestern

blotting, we identified eukaryotic elongation factor 1 alpha

(eEF1A) as the main nuclear protein that specifically

recognizes these oligonucleotides.Western blotting and

supershift assays confirmed the nature of this protein and

its involvement in forming a cytotoxicity-related complex

(CRC).On the contrary, normal human lymphocytes did

not show nuclear proteins able to produce CRC in a

SouthWestern blot.Comparative bidimensional PAGE and

Western-blotting analysis for eEF1A revealed the presence

of a specific cluster of spots, focusing at more basic pH, in nuclear extracts of cancer cells but absent in those of normal lymphocytes.Moreover, a bidimensional PAGE South-Western blot demonstrated that cytotoxic GT oligomers selectively recognized the more basic eEF1A isoform expressed only in cancer cells.These results suggest the involvement of eEF1A, associated with the nuclear-enriched fraction, in the growth and maintenance of tumour cells, possibly modulated by post-translational processing of the polypeptide chain

Keywords: aptameric oligonucleotides; eEF1A; proteomics; CCRF-CEM cells; cytotoxicity

Oligonucleotides, widely used as agents to specifically

inhibit gene expression by antisense [1] or antigene [2]

strategies, often display unexpected effects by interacting

with cellular proteins.In fact, they are able to bind to either

membrane or intracellular proteins, probably by their

polyanionic nature and/or by nonspecific or specific

sequence-related mechanisms [3].In the last decade,

oligo-nucleotides have progressively gained aptameric function,

specifically recognizing proteins as natural or non-natural

ligands [4].Constitutive proteins that bind to

single-stranded DNA oligomers are widely recognized to be

involved in important mechanisms associated with DNA

replication, repair and recombination [5–7].Furthermore,

many reports evidenced that modulation of gene expression

[8,9], and stimulation or inhibition of cellular replication

[10,11], are influenced by single-stranded DNA sequences

specifically interacting with cellular proteins

Oligonucleotides composed exclusively of G and T bases have previously been shown to exert a specific, selective and dose-dependent effect of cell growth inhibition on a variety

of human cancer cell lines [12].The cytotoxic effect of these

GT oligomers was shown to be highly related to their ability

to form complexes with nuclear proteins, as measured by

UV cross-linking assays [12–15].However, the nature of these nuclear proteins behaving as single-stranded DNA-binding proteins has not yet been identified [12–15].A protein isolated from fibroblasts with such an activity has been already described [16], but it was able to tightly bind either GA or GT oligomers.On the contrary, the nuclear proteins binding to our GT oligomers did not specifically recognize GA sequences [12].More recently, it has been shown that GT oligonucleotides, capable of forming G-quartet structures, exerted a cytotoxic effect on human cancer cell lines.By UV cross-linking assay, these oligomers have been reported to interact with nucleolin, forming a main complex of >100 kDa molecular mass [17].This complex was not formed when GT oligomers unable to form a G-quartet structure were used [17,18].The oligonu-cleotide under our investigation (a 27-mer; see the Materials and methods, below) did not present appreciable G-quartet structures, as deduced by gel electrophoresis and circular dichroism analysis [14]; on the contrary, it was able to form

a cytotoxic-related complex (CRC), with an apparent molecular mass of 45 ± 7 kDa, with nuclear proteins of different tumour cell lines [12–15].Thus, the characteriza-tion of these nuclear species seemed particularly interesting,

Correspondence to B.Scaggiante, Department of Biomedical Sciences

and Technologies, University of Udine, p.le Kolbe 4, 33100 Udine,

Italy.Fax: + 39 432 494301; Tel.: + 39 432 494311;

E-mail: bscaggiante@makek.dstb.uniud.it

Abbreviations: CRC, cytotoxicity-related complex; CRS, control

rabbit total serum; eEF1A, eukaryotic elongation factor 1 alpha;

Egr1, early growth response protein 1; IPG, immobilized pH gradient;

PSD, postsource decay; TBP, TATA-binding protein.

(Received 7 March 2003, revised 27 May 2003, accepted 10 June 2003)

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either for using to elucidate new potential molecular targets

in tumour biology or to highlight the mechanism of action

of our cytotoxic GT oligonucleotides

In this article, we report the identification of eukaryotic

elongation factor 1 alpha (eEF1A) as a nuclear component

of the CRC in T-lymphoblastic CCRF-CEM cancer cells

In these cells, we found a striking relationship between the

growth-inhibition effect exerted by cytotoxic GT oligomers

and their selective binding to nuclear eEF1A.In fact, in

normal human lymphocytes no appreciable binding of GT

oligomer to nuclear eEF1A was shown and, accordingly,

these cells were not sensitive to its cytotoxic action.A

possible role for nuclear eEF1A in tumour cell growth or

maintenance is suggested by the selective identification of

more basic isoforms of eEF1A in cancer cells, but not in

normal lymphocytes

Materials and methods

Oligonucleotides

Oligonucleotides were purchased from MWG Biotech

(Ebersberg, Germany) as HPLC pure species and their

purity was confirmed by electrophoresis on an 18%

polyacrylamide/7Murea gel.For cell cultures,

oligonucleo-tides were resuspended in water and sterilized by

centri-fugation on a spin-X tube provided with a 0.22-lM filter

(Costar, Cambridge, MA, USA).The GT oligomer

sequence was: 5¢-TGT TTG TTT GTT TGT TTG TTT

GTT TGT-3¢; and the control CT sequence was: 5¢-TCT

TTC TTT CTT TCT TTC TTT CTT TCT-3¢.The

oligomers were 5¢ end-labelled by [c-32P]ATP with T4

polynucleotide kinase (MBI, Fermentas, MGMBH, St

Leon-Rot, Germany)

Cell culture and cytotoxic assay

The T-lymphoblastic leukaemic cell line (CCRF-CEM) and

normal human lymphocytes, obtained from peripheral

blood by separation on Ficoll–Isopaque (Gibco BRL, Life

Technologies, Milan, Italy), were cultured in RPMI-1640

supplemented with 10% fetal calf serum (FCS), 2 mM

L-glutamine, 100 UÆmL)1penicillin and 100 lgÆmL)1

strep-tomycin (Euroclone, Celbio, Devon, UK)

CCRF-CEM cells in exponential growth phase, and

lymphocytes, were seeded at 104cells in 100 lL of complete

medium containing 10% fetal clone serum (Euroclone,

Celbio) in a 96-well microtiter plate.The oligonucleotides

were added directly to the medium 4 h after seeding.After

24 h of incubation, 100 lL of fresh medium was added

The cellular growth was evaluated 72 h after addition

of oligonucleotides by assessing the incorporation of

0.5 mgÆmL)1 of

3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl-tetrazolium bromide (Sigma Chemical Co., St Louis, MO,

USA) into viable cells [19].The percentage of viable cells in

the treated samples was estimated, taking, as 100% cellular

viability, that of the internal-control nontreated cells

Preparation of total nuclear extracts

Total nuclear extracts were obtained from 2· 107cells by

using a minor modification of the Dignam’s method, as

previously described [12].The protein content was deter-mined by the Bradford method [19] using BSA as standard EMSA, UV crosslinking and supershift assays

In the EMSA, 1 ng of [c-32P]ATP-labelled oligonucleotide was incubated with 2 lg of total nuclear or cytoplasmic extracts supplemented with protease inhibitors (2 lgÆmL)1 apoprotinin, 1 lgÆmL)1 pepstatin, 1 mM dithiothreitol) (Sigma Chemical Co.) in 20 mM Hepes, 0.42M NaCl, 1.5 mM MgCl2, 0 2 mM EDTA, 25% glycerol, pH 7.0, containing nonspecific competitors [1 lg of salmon-sperm DNA or 1 lg of poly(dIdC)] (Pharmacia, Uppsala, Sweden) and the indicated amounts of unlabelled specific CT oligomer competitor.When indicated, the protein excised from the Coomassie-stained gel was recovered in 50 mM Tris/HCl, pH 8.0, containing 0.1% SDS, 0.1 mgÆmL)1 BSA, 0.2 mM EDTA, 2.5% glycerol After two steps of freeze/thawing, followed by precipitation with cold acetone, the protein was rinsed with methanol, denatured with 8M urea and then renatured by overnight incubation in a fixed volume of 50 mM Tris/HCl, pH 7.6, 100 mMKCl, 5 mM dithiothreitol, 0.1 mM phenylmethanesulfonyl fluoride.It was not possible to quantify the amount of recovered protein owing to the presence of a high molar excess of BSA remaining in the buffer.Therefore, a fixed aliquot of the protein was incubated with the indicated probes, as previously described.After 25 min of incubation at room temperature, the samples were loaded onto a native 7% polyacrylamide gel in 20 mM Tris/borate/0.5 mM EDTA buffer (TBE) and electrophoresed at 10 V cm)1, at a temperature of 4C

In the supershift gel-mobility assay, samples of total nuclear extracts were diluted 1 : 5 (v/v) in water and 0.5 lg

of protein was incubated for 2.5 h at room temperature with the indicated amounts of specific rabbit polyclonal anti-eEF1A serum or with corresponding amounts of control total serum obtained from unimmunized rabbits.Then,

2 ng of specific [c-32P]-labelled GT oligonucleotide was added to 30 lL of 20 mM Tris/HCl buffer, pH 7.5, containing 75 mM KCl, 5 mM dithiotreitol, 6 lg BSA, 0.1% Tween 20, 0.025 mMEscherichia coliDNA, and 15% glycerol.After 30 min of incubation at room temperature, the samples were loaded onto a 7% native polyacrylamide gel in 20 mMTBE buffer and electrophoresed for 90 min

at 10 V cm)1, at 15C.The gel was then dried and auto-radiographed

In the UV cross-linking assay, the samples were incuba-ted at room temperature, as described above for the EMSA assay, and then irradiated at 302 nm for 10 min using a transilluminator (Bio-Rad Laboratories).The samples were denatured by adding Laemmli sample buffer and boiled before electrophoresis through a 12% SDS polyacrylamide gel, according to the procedure of Laemmli [20]

Electroblotting Nuclear proteins separated by SDS/PAGE were electro-phoretically transferred onto a 0.22-lm nitrocellulose membrane (Schleicher & Schuell, Keene, NH, USA) in

50 mM Tris, 40 mM glycine, 0.4% SDS, 20% methanol buffer using a transblot semidry apparatus system

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(Amersham Pharmacia Biotech).The membrane was

stained with Ponceau S (Sigma Chemical Co.) and destained

with deionized water

SouthWestern blotting analysis

Fifty micrograms of total nuclear protein was separated by

SDS/PAGE (29 : 1, acrylamide/bisacrylamide) (8% gel)

Proteins were transferred to nitrocellulose and then

dena-tured and slowly renadena-tured by washing for 30 min at room

temperature consecutively with 6-, 4-, 3-, 2- and 1M

guanidine hydrochloride solution in water.The membrane

was incubated overnight on a rocking shaker, at 4C, in

50 mMHepes, pH 7.2, containing 0.1MKCl, 1 mMMgCl2,

5 mM dithiothreitol, 1 mM EDTA and 10% glycerol

Membranes derived from bidimensional PAGE blotting

were processed without the denaturation/renaturation

pro-cedure.Membranes were blocked by washing with the same

buffer, containing 5% nonfat dried milk and 5 mM

dithiothreitol, for 1 h.Protein–DNA interaction was

per-formed overnight, at 4C, with 10 pmol of [c-32P]-labelled

oligonucleotide.Membranes were then washed between two

and four times for 10 min at room temperature, until the

background radioactivity started to decline, and were then

exposed to autoradiography

Expression of recombinant eEF1A

Full-length eEF1A cDNA was cloned into pET11a (kindly

provided by Dr George M.C.Janssen, University of Leiden)

at the Nde1/BamH1 site for bacterial

expression.Recom-binant eEF1A protein was obtained from overexpression in

E coli [21].Briefly, E coli BL21 cell culture (2 mL),

transformed with pET11a–eEF1A, was grown overnight

at 37C in LB (Luria–Bertani) medium supplemented with

50 lgÆmL)1ampicillin.Fresh and prewarmed (37C) LB

medium was inoculated with the overnight culture to an

absorbance (A) value of 0.05–0.1 The culture was grown

until the A reached a value of 0.5–0.7, then isopropyl

thio-b-D-galactoside was added to a final concentration of 1 mM

Expression of eEF1A protein was induced by culturing the

cells for additional 3 h at 37C.Cells were harvested by

centrifugation (10 000 g, 10 min, 4C), resuspended in

10 mL of lysis buffer (20 mMTris/HCl, 5 mMdithiothreitol,

250 mMNaCl, 1 mMEDTA, 0.25% Tween-20, 0.3 lgÆlL)1

lysozyme) per gram of bacterial pellet and disrupted by

sonication.The lysate was centrifuged (10 000 g, 20 min,

4C) and the recombinant eEF1A protein collected in the

supernatant as a soluble protein

Western blotting analysis

The blotted membrane was blocked with 3% nonfat dried

milk in PBS (NaCl/Pi) and incubated with eEF1A

mono-clonal antibody (mAb) (1 lg/mL) (Upstate Biotechnology,

Lake Placid, NY, USA) in NaCl/Pi, overnight, at 4C with

constant rocking.Then, it was washed twice with deionized

water and incubated for 1.5 h with an anti-mouse

IgG-conjugated horseradish peroxidase secondary antibody

(Promega, Madison, WI, USA).After washing once with

NaCl/Picontaining 0.05% Tween-20 and four times with

deionized water, the nitrocellulose blot was developed using

enhanced chemiluminescence detection (Pierce, Rockford,

IL, USA) according to the manufacturer’s protocols, and then exposed to X-ray film

The same filter was stripped by a 10-min incubation in

4M guanidine hydrochloride, rinsed with 10 volumes of NaCl/Pi, blocked with 5% nonfat dried milk and then probed with b-actin antibody (VWR International Onco-gene) for 1 h, at room temperature, followed by incubation for 1 h with a goat anti-mouse IgM-conjugated horseradish peroxidase secondary antibody (Sigma Chemical Co.) The blot was developed by using the chemiluminescence detec-tion kit.Band intensities were evaluated by scanning with

a Gel Doc2000 phosphoimager densitometer equipped with a multianalyst PC software analysis system (Bio-Rad Laboratories)

To test the nuclear enrichment, the presence of two nuclear transcription factors – the early growth response protein 1 (Egr1) and the TATA-binding protein (TBP) – was confirmed by probing with specific rabbit antibodies (Santa Cruz) on the cytoplasmic and nuclear extracts.The membrane was incubated with the antibodies for 1 h at room temperature.After three washes with NaCl/Pi containing 0.1% Tween-20, the membrane was incubated with anti-rabbit IgG–horseradish peroxidase conjugate (Sigma Chemical Co.) for 60 min at room temperature The filter was then washed several times with NaCl/Pi containing 0.1% Tween-20, and the blot was developed using the enhanced chemiluminescence procedure (Amer-sham Pharmacia Biotech)

MS analysis Bands from SDS/PAGE were excised from the gel, tritu-rated and washed with water.Proteins were in-gel reduced, S-alkylated and digested with trypsin, as previously des-cribed [22].Digest aliquots were removed and used directly

or subjected to a desalting/concentration step on lZip-TipC18 (Millipore Corp., Bedford, MA, USA) before analysis by MALDI-MS.Peptide mixtures were loaded onto the MALDI target, using the dried droplet technique and a-cyano-4-hydroxycinnamic as matrix, and analysed by using a Voyager-DE PRO mass spectrometer (Applied Biosystems, Framingham, MA, USA).Internal-mass calib-ration was performed with peptides deriving from trypsin autoproteolysis.The mass spectra were acquired in either reflectron or linear mode with delayed extraction.Post-source decay (PSD) fragment ion spectra were acquired for intense signals after isolation of the appropriate precursor

by using timed ion selection.Fragment ions were refocused onto the detector by stepping the voltage applied to the reflectron in the following ratios: 1.000 (precursor ion segment), 0.960, 0.750, 0.563, 0.422, 0.316, 0.237, 0.178, 0.133, 0.100, 0.075, 0.056 and 0.042 (fragment segments) Individual segments were superimposed by using theDATA EXPLORER4.0 software (Applied Biosystems) All precursor ion segments were acquired at low laser power (variable attenuator¼ 1950), for less than 200 laser pulses, to avoid saturating the detector.The laser power was increased to

200 units for all the remaining segments of the PSD acquisitions.Typically, 300 laser pulses were acquired for each fragment-ion segment.The PSD data were acquired with an Acquiris digitizer at a digitization rate of 500 MHz

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PROTEINPROSPECTOR and PROWL software packages were

used to identify spots unambiguously from independent

nonredundant sequence databases [23,24].Candidates from

peptide-matching analysis were further evaluated by

com-parison with their calculated mass and pI using the

experimental values obtained from bidimensional PAGE

Bidimensional gel analysis

Proteins of total nuclear extract (30 lg) were precipitated at

)20 C with four volumes of acetone, washed with cold

methanol, and dried.Pellets were dissolved in 120 lL of

rehydration buffer (Amersham Pharmacia Biotech)

con-taining 8M urea, 2% CHAPS, 0.5% immobilized pH

gradient (IPG) buffer (pH 6–11), 65 mMdithiothreitol and

0.01% Bromophenol Blue, and used immediately in

bidi-mensional PAGE experiments.IEF was performed on 7-cm

IPG strips (range: pH 6–11) by using the IPGphor

Isoelec-tric Focusing System (Amersham Pharmacia Biotech).The

second dimension was performed on a 12% SDS/PAGE

system after equilibrating the strips for 10 min in SDS

Equilibration buffer containing 50 mMTris/HCl (pH 8.8),

6M urea, 30% glycerol, 2% SDS, 2% dithiothreitol and

2.5% iodoacetamide Gels were then used for Western or

SouthWestern blot analysis, as described above.As internal

normalizer, the presence of the nuclear protein, Ran-GTP,

was detected by Western blot on the same filters used to

analyse eEF1A protein, by using a specific mAb (BD

Pharmingen, CA, USA)

Results

Identification of eEF1A as a nuclear protein specifically

related to the cytotoxicity of GT oligomer in cancer cells

In order to identify the nuclear proteins that specifically

recognize cytotoxic GT oligomers, a 27-mer GT sequence

was used [12].This oligomer forms a specific CRC with an

apparent molecular weight of 45 ± 7 kDa [12–15].The

T-lymphoblastic CCRF-CEM cancer cell line was chosen

for this investigation as it was previously used to

demonstrate the specific cytotoxic action of the GT

oligomers [12–15].Figure 1A shows that in SouthWestern

blots, the labelled GT oligomer bound (in a specific

manner) two main proteins, named P1 and P2, compared

with the binding of a labelled nontoxic CT oligomer, used

as a control.The latter showed a weak interaction with P1

and P2 proteins, whereas it preferentially bound to a

nuclear protein with a mass of 70 kDa (marked by an

asterisk), recognized to the same extent also by the GT

sequence.Binding of the GT oligomer was not a result of

DNA interaction with the more abundant components of

the nuclear extract, as revealed by Ponceau staining of the

immobilized proteins.In fact, many other bands, equally

or more intense than those recognized by the GT

oligomer, were also detected (data not shown).To test

for nuclear enrichment, nuclear and cytoplasmic extracts

were blotted and assayed for the nuclear proteins Egr1

and TBP.The results displayed in Fig.1B clearly indicate

that the proteins Egr1 and TBP were detected only in the

nuclear fraction.This demonstrated that nuclear extracts

are effectively enriched in nuclear proteins.Moreover,

b-actin, used as a loading control, occurred at a higher level in the cytoplasmic fraction, similar to the cellular distribution of the protein

P1 migrated with an apparent molecular mass similar to that previously reported for the CRC (45 ± 7 kDa) [12]

In contrast, P2 showed a higher apparent molecular mass P1 and P2 were excised from a Coomassie-stained gel, alkylated and digested.MALDI-MS analysis of the P1 digest yielded a series of peptide-mass values that were used for nonredundant sequence database searching (Fig.2A)

Fig 1 SouthWestern blot analysis of GT oligomer binding to nuclear proteins and immunoblot of the subcellular fractions (A) SouthWestern blot on the nuclear extract.Fifty micrograms of total nuclear extract derived from CCRF-CEM cells was separated by SDS/PAGE (8% gel) and then transferred, by semidry blotting, onto a nitrocellulose filter.The proteins were denatured and renatured as described in the Materials and methods.One half of the filter was tested for protein– DNA interactions with a c 32 P-labelled GT probe (GT) and the other half with a c32P-labelled CT oligomer (CT) as a control, at 4 C (each probe counted 650 000 c.p.m.) After incubation overnight, the filters were rinsed and then exposed to Omat XAR Kodak film.(B) Immu-noblotting of subcellular fractions.Twenty micrograms of cytoplasmic (lane 1) or nuclear extract (lane 2) fractions of CCRF-CEM cells was separated by SDS/PAGE (8% gel).After blotting onto nitrocellulose membrane, the filter was probed with the nuclear-specific antibodies anti-TBP or anti-Egr1, as described in the Materials and methods.As a loading control, the presence of b-actin protein was also confirmed by using specific antibody, as described in the Materials and methods.

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The comparison of this peptide-mass fingerprint with the

theoretical ones, calculated by an in silico digestion of all

human sequences occurring in the databases, identified P1

as eEF1A.Furthermore, PSD experiments performed on

selected peptide precursor ions (i.e m/z 1405.4 and 1780.9)

generated internal sequence tags that unambiguously

con-firmed the nature of this protein (data not shown)

Moreover, the spectrum reported in the figure showed the

occurrence of a series of signals that were not interpreted

simply on the basis of the eEF1A sequence, but according to

the post-translational modifications already described

for this protein [25].It demonstrated the occurrence of

Ne-dimethyllysine (Lys55, Lys165) and Ne-trimethyllysine

(Lys79, Lys318) in the eEF1A sample purified from

T-lymphoblastic CCRF-CEM cancer cells.No data on

the modification status of Lys36 (methylation), Glu301 and

Glu374 (glyceryl-phosphoryl-ethanolamine addition) were

inferred.MS analysis allowed a 50% coverage of the entire

eEF1A sequence.All signals occurring in the spectrum were

assigned to this protein, thus ruling out the possibility that

other polypeptide species comigrated in SDS/PAGE with

eEF1A

Moreover, the possibility that P1 was the oncogenic N-terminal truncated form of eEF1A protein, already known as PTI-1 [26,27], seemed unlikely on the basis of the signals occurring in the spectrum reported in Fig.2A.In fact, at least eight signals matched perfectly with those expected for eEF1A (MH+at m/z 1492.9, 2501.8, 2516.9, 2997.6, 3023.6, 3151.9, 3980.3 and 4108.5) and demonstra-ted the absence of seven of the eight amino acid substitu-tions described for PTI-1 (Ala65Met, Glu66Gln, Arg67Ser, Lys100Gln, Arg247Gly, Ala281Gly and Arg423Cys, respectively).Moreover, clear MH+signals, corresponding

to the N-terminal region of eEF1A, were present; this region

is totally deleted in PTI-1.Similar considerations were taken into account to exclude the possibility that P1 corresponded

to isoforms of eEF1A other than eEF1A1, already described

Similarly, peptide-mass fingerprint analysis by

MALDI-MS identified P2 as nucleolin (data not shown).Different authors have already reported this protein as being able to specifically generate a 100-kDa complex with GT oligomers that form a G-quartet structure, thus exerting a cytotoxic effect on human cancer cell lines [10,17].PSD experiments performed on selected precursor ions (i.e m/z 2201.3 and 1649.7) allowed internal sequence tags to be obtained, definitively demonstrating the nature of this species (Fig.2B)

The identity of P1 was also assayed by Western-blotting experiments with a mAb for eEF1A.As illustrated in Fig.3A, the protein excised from the Coomassie-stained gel was recognized by the specific eEF1A antibody (Fig.3A, lane 3).As controls, recombinant eEF1A protein (Fig.3A, lane 1) and a sample obtained from total nuclear extracts (Fig 3A, lane 2) were tested

The EMSA with the protein eluted from the P1 band excised from the Coomassie-stained gel of CCRF-CEM cell nuclear extracts showed that this protein selectively recog-nized the GT oligomer with respect to control CT sequence, similarly to results obtained with the total nuclear extracts [12–15].It is noteworthy that all the EMSA and UV cross-linking assays were performed using a buffer containing 25% glycerol to preserve the activity of eEF1A.As illustrated in Fig.3B, the eEF1A recovered from the P1-excised band showed a stronger interaction when incubated with the labelled GT oligomer (Fig.3B, lane 1) than when incubated with the labelled control CT oligomer (Fig.3B, lane 7).Moreover, the presence of a fivefold molar excess of CT-unlabelled competitor (Fig.3B, lane 5), did not completely displace the GT oligonucleotide from the protein interaction.On the contrary, only a fivefold molar excess of GT-unlabelled oligonucleotide competitor removed all the labelled CT control oligomer from the complex (Fig.3B, lane 8)

To explore the possibility that eEF1A was the protein component present in the CRC [12], supershift assays were performed under native conditions.The results shown in Fig.4 demonstrate that a rabbit polyclonal antibody recognizing eEF1A elicited a specific supershift (marked

by an arrow; Fig.4, lanes 4 and 5) from the complex.No supershift resulted from incubation of the nuclear protein extract with the same amounts of a total rabbit preimmune serum, which displayed only nonspecific competition (Fig.4, lanes 6 and 7).The slight reduction in DNA-binding

Fig 2 MALDI-MS analysis of P1 and P2 proteins (A) MALDI-MS

analysis of component P1 following digestion with trypsin.The mass

values reported in the spectrum represent average values.Numbers in

parentheses indicate amino acid residues in the eEF1A sequence.

Possible methylation sites are shown and assigned based on the

observed mass values, eEF1A sequence and previously published

results [25].Peptides originating from trypsin autoproteolysis are

indi-cated as open circles.(B) Postsource decay (PSD)-MALDI fragment

ion mass spectrum of the P2 tryptic peptide, GLSEDTTEETLK

ESFDGSVR, with MH + at m/z 2201.3 (average value) The mass

values reported in the spectrum are indicated as monoisotopic values.

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activity shown in the presence of control rabbit total serum

(CRS) could be caused by nonspecific sequestration of

eEF1A by serum proteins

More interestingly, as illustrated in Fig.5A, with respect

to the protein of the nuclear extracts, the soluble eEF1A

recovered from the cytoplamic fraction did not bind to a GT

oligomer in SouthWestern blotting.Although comparable

quantities of the protein were loaded onto the gel, as evidenced by Western blotting, in the cytoplasmic extract, only the nucleolin band was evident.Similarly to this and to the previous results [12], in the UV cross-linking assay the specific CRC displayed by the nuclear extract was not present in the cytoplasmic sample (Fig.5B) On the contrary, the cytoplasmic extract showed a band of about

28 kDa, previously demonstrated to bind to GT in a nonspecific manner [12]

Characterization of eEF1A in normal and cancer cells

In order to compare the binding properties of the nuclear eEF1A in normal cells compared with those in cancer CCRF-CEM cells, human lymphocytes were isolated from the peripheral blood of normal donors.These cells were not sensitive to the cytotoxic effect of GT oligomers

Fig 3 P1 Western blotting analysis and affinity measurements for GT

oligomer (A) Western blotting analysis.Protein samples were

separ-ated by SDS/PAGE (12% gel) and then transferred onto a

nitrocel-lulose filter and incubated with mAb for eEF1A, as described in the

Materials and methods.Lane 1, bacterial recombinant eEF1A protein

(R eEF1A); lane 2, eEF1A protein from total nuclear extracts (NE

eEF1A); lane 3, P1 band excised from an SDS/PAGE gel (P1).(B) P1

affinity for GT oligomer.P1 protein, excised from an SDS/PAGE gel

loaded with 50 lg of total nuclear extract, was renatured as described

in the Materials and methods.Five microlitres of sample was then

incubated with 2 ng of [c-32P]-labelled GT probe (GT) in buffer

(200 m M Tris/HCl, pH 7.5, containing 750 m M KCl, 10 m M

dithio-threitol, 50 lgÆmL)1BSA) in the absence (lane 1) or in the presence of

10 ng (lane 2), 20 ng (lane 3), 50 ng (lane 4), 100 ng (lane 5) or 200 ng

(lane 6) of nonlabelled CT oligomer.An identical aliquot was

incu-bated with 2 ng of c 32 P-labelled CT probe (CT) in the absence (lane 7)

or in the presence of 10 ng (lane 8), 20 ng (lane 9), 50 ng (lane 10),

100 ng (lane 11) or 200 ng (lane 12) of nonlabelled GT oligomer.The

two probes were added to the sample at the same specific activity

( 10 000 c.p.m.) Labelled GT oligomer incubated without P1 (lane

13) and labelled CT oligomer incubated without P1 (lane 14) were used

as controls.After 20 min of incubation at room temperature, the

samples were loaded onto an 8% polyacrylamide gel in 0.5 · Tris/

borate/EDTA (TBE) buffer and electrophoresed at 4 C.The dried gel

was exposed to autoradiographic film.The arrow indicates the specific

complex.

Fig 4 Supershift assay experiments Proteins from CCRF-CEM cell nuclear extracts (0.5 lg) were incubated with or without the indicated amounts of specific polyclonal antibody (Ab eEF1A) or control rabbit total serum (CRS), for 2.5 h at room temperature Then, 2 ng of c32 P-labelled GT oligomer was added to the samples, as reported in the Materials and methods.After a further 30 min of incubation at room temperature, the samples were loaded onto a 7% polyacrylamide gel in 0.5 · Tris/borate/EDTA (TBE) buffer and electrophoresed at 4 C The gel was dried and exposed to Omat XAR Kodak film c 32 P-Labelled GT oligomer was incubated with buffer (lane 1), with 9 lg of polyclonal anti-eEF1A (lane 2), with 9 lg of total CRS (lane 3), with nuclear proteins and 9 lg of polyclonal anti-eEF1A (lane 4), with nuclear proteins and 0 9 lg of polyclonal anti-eEF1A (lane 5), with nuclear proteins and 9 lg of total CRS (lane 6), with nuclear proteins and 0.9 lg of total CRS (lane 7) or with nuclear proteins only (lane 8) The arrow indicates the supershift.

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(Fig.6A), and their nuclear proteins did not form the

CRC with the GT sequence (marked by arrow), as shown

by EMSA or UV cross-linking assays (Fig.6B,C) To

investigate the binding properties of the lymphocyte

eEF1A protein, SouthWestern blots were performed.It was found that the CCRF-CEM nuclear extracts con-tained higher amounts of eEF1A than those of human lymphocytes.In fact, Western blotting experiments dem-onstrated that the relative amount of eEF1A recovered from lymphocyte nuclear extracts was 2.7 ± 0.8-fold less than that obtained from cancer CCRF-CEM T lympho-blasts (mean of three independent experiments).For this reason, the SouthWestern assay was performed after

Fig 5 SouthWestern blot, Western blot and UV cross-linking analysis

of cytoplasmic extracts (A) SouthWestern blot.Twenty-five

micro-grams of total protein from cytoplasm or nuclear extracts, previously

normalized by comparison on a Coomassie-stained gel, were separated

by SDS/PAGE (8% gel) and transferred onto a nitrocellulose filter, as

described in the Materials and methods.The proteins were denatured,

renatured and the filter hybridized with a c32P-labelled GT probe at

4 C.After overnight incubation, the filter was rinsed and then

exposed to Omat XAR Kodak film, as described in the Materials and

methods.The same samples were used for Western blotting analysis

performed with the same amount of the cytoplasm and nuclear

pro-teins used in the SouthWestern blot.The specific protein was

con-firmed by using the monoclonal anti-eEF1A with the conditions

described in the Materials and methods.(B) UV crosslinking assay.

Two micrograms of total proteins derived from the cytoplasm or

nuclear extracts were incubated in buffer containing 25% glycerol,

with c32P-labelled GT probe in the presence of 1 lg poly(dIdC) and

1 lg of CT as competitors, as described in the Materials and methods.

After 25 min of incubation at room temperature, the samples were

cross-linked by UV exposure and then denatured and separated by

SDS/PAGE (12% gel).The dried gel was then exposed to Omat XAR

Kodak film.NE, nuclear extract; CE, cytoplasmic extract.

Fig 6 Effect of GT oligomer on cellular growth and on nuclear protein binding in human lymphocytes (A) Effect of GT oligomer on cellular growth or viability.A total of 10 4 CCRF-CEM cells or peripheral normal human lymphocytes were seeded in 100 lL of complete medium on 96-well microtiter plates.After 4 h of incubation, 7.5 l M of

GT oligomer or control CT sequence were added to the cells.The percentage of viable cells was assayed after 72 h of incubation by determining the incorporation of 3-(4,5-dimethylthiazol-2-yl)-2,5-di-phenyl-tetrazolium bromide, as described in Materials and methods (B) EMSA assay.Two micrograms of total nuclear proteins derived from CCRF-CEM cells or from human lymphocytes were incubated with 1.5 lg of poly(dIdC), 1 lg of CT and 1 ng of c32P-labelled GT oligomer in a buffer containing 25% glycerol, as described in the Materials and methods.After incubation at room temperature for

30 min, the samples were loaded onto a 7% polyacrylamide gel in Tris/ borate/EDTA (TBE) buffer and run at 4 C.(C) UV cross-linking assay.Two micrograms of total nuclear proteins derived from CCRF-CEM cells or from human lymphocytes were incubated with 1.5 lg of poly(dIdC), 1 lg of CT and 1 ng of c 32 P-labelled GT oligomer, as described in the Materials and methods.The samples were then exposed for 10 min to a 302 nm UV light, added to SDS/PAGE loading buffer and separated by SDS/PAGE (12% gel).The arrows indicated the specific cytotoxicity-related complex.

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normalizing the quantities of loaded proteins on a

Coomassie-stained gel by referring to the P1 band (known

to correspond to eEF1A) As reported in Fig 7A, in the

CCRF-CEM sample the GT oligomer recognized

nucleo-lin (marked by a black arrow), eEF1A (marked by a

white arrow) as well as the nonspecific 70 kDa protein

(marked by an asterisk).On the contrary, in human

lymphocytes the GT oligomer did not bind to eEF1A, but

it significantly recognized nucleolin.To rule out that

protein-degradation artefacts might account for the lack

of specific recognition, the same amounts of protein used

in SouthWestern experiments were assayed by Western

blotting.As shown in Fig.7B, the amount of eEF1A in

human lymphocytes was comparable to that in

CCRF-CEM cancer cells.On the contrary, b-actin showed

significant differences in the two samples, in agreement

with the higher quantity of total proteins loaded in the

lymphocyte sample, as mentioned above

Previous data demonstrated that the eEF1A protein is post-translationally modified [25,28,29].In order to detect whether this protein presented a different molecular nature

in normal and cancer cells, we performed a comparative bidimensional PAGE analysis of nuclear extracts coupled

to Western blotting analysis with an eEF1A mAb.As

an internal normalizer of loading amounts and focusing position, the nuclear protein, Ran-GTP, was used and identified by a specific mAb.The data reported in Fig.8A clearly showed, in T-lymphoblastic CCRF-CEM cancer

Fig 7 Comparative SouthWestern blot for CCRF-CEM cells and

normal lymphocytes (A) SouthWestern blot.Twenty-five micrograms

of total nuclear protein from CCRF-CEM cells and 50 lg of total

nuclear protein from normal human lymphocytes were separated by

SDS/PAGE (8% gel) and transferred onto a nitrocellulose filter, as

described in the Materials and methods.The proteins were denatured

and renatured as described above, and the filter was hybridized with

c32P-labelled GT probe at 4 C.After overnight incubation with the

probe, the filters were rinsed, as described in the Materials and

methods, and then exposed to Omat XAR Kodak film.(B)

Western-blotting analysis.Protein samples reported in (A) were analysed for

eEF1A and b-actin content.

Fig 8 Bidimensional PAGE analysis of nuclear elongation factor 1 alpha (eEF1A) (A) Thirty micrograms of nuclear extracts from CCRF CEM cells and normal human lymphocytes, calculated from evalua-tion of the protein content in a Coomassie-stained gel, were analysed

by bidimensional PAGE, as described in the Materials and methods The presence of eEF1A was tested by Western blot analysis by using the specific antibody anti-eEF1A.As an internal normalizer of loading amount and focusing position, the presence of the constitutive nuclear transporter, Ran-GTP, was also tested by using a specific monoclonal antibody.(B) Bidimensional PAGE analysis of other samples, con-firming the reproducibility of data obtained.Thirty micrograms of nuclear extracts from normal human lymphocytes were similarly analysed by bidimensional PAGE and compared with CCRF-CEM nuclear extracts.The presence of eEF1A was confirmed by Western blot analysis using the specific antibody, anti-eEF1A.Only the higher magnification of IEF of the eEF1A region is reported.

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cells, the presence of two different clusters of eEF1A

isoforms (cluster 1 and cluster 2).The apparent pI of cluster

1 ( pH 9.0), was calculated theoretically by considering

the pH gradient linear, as indicated by the manufacturer.In

nuclear extracts from lymphocytes, a similar species focused

near the same pH.Interestingly, cluster 2, which was absent

in lymphocytes, focused at an apparent pH of10.5 Thus,

it accounted for a more basic pI and for species different

from those present in lymphocytes.However, taking apart

the undoubtedly much more basic nature of the

faster-migrating isoform of eEF1A in cancer cells, the estimation

of its pI remains merely indicative.A magnified image of

this analysis, performed with a different nuclear extract, is

reported in Fig.8B It is clear that human lymphocytes

displayed only the main constitutive species that migrates

in correspondence to cluster 1 of CCRF-CEM cells (see

Fig.8B).To elucidate the GT oligomer binding behaviour

of the isoforms found in the cancer cell sample, a

SouthWestern assay was performed after analysis by

bidimensional PAGE.The antibody recognition of the

proteins performed on the same filter was prevented by

the SouthWestern treatment.Therefore, identification of the

eEF1A–oligomer interaction was carried out by matching

the SouthWestern results with those of the Western blotting

of bidimensional PAGE performed on the same sample,

under identical experimental conditions.The perfect match between the Western blot signals of bidimensional PAGE (Fig.9A) and the autoradiographic signals found in the SouthWestern blot (Fig.8B), unequivocally demonstrated that the protein reacting in SouthWestern blots was eEF1A Furthermore, the SouthWestern blot, reported in Fig.9B, showed that the labelled GT oligomer mainly recognized the more basic form of eEF1A, whereas a very weak interaction was found for the isoform of eEF1A focusing at a pH of

9.0 The recognition seemed highly specific because, under these experimental conditions, no other interactions were detected on the filter.Moreover, no significant interaction in bidimensional PAGE SouthWestern blots was found on human lymphocytes at the position corresponding to eEF1A (see Fig.10), once more indicating that normal eEF1A did not react with the GT oligomer

Fig 9 Comparative analysis of bidimensional PAGE analysis of

SouthWestern and Western blots for CCRF-CEM cells Two samples of

50 lg of total nuclear protein from CCRF-CEM cells were separated,

in parallel, by bidimensional PAGE and blotted onto nitrocellulose

filters, as described in the Materials and methods.(A) Western

blot-ting.The filter was assayed using anti-eEF1A mAb, as described in the

Materials and methods.The position of the eEF1A protein was

con-firmed by revealing the presence of the Ran–GTP protein.(B)

SouthWestern blotting.The filter was assayed for SouthWestern

blotting, as described in the experimental section using, as probe, c32

P-labelled GT oligomer and then exposed to Omat XAR Kodak film.

Fig 10 Comparative analysis of bidimensional PAGE, SouthWestern and Western blotting for human lymphocytes Two samples of 50 lg of total nuclear protein of normal human lymphocytes, previously nor-malized with respect to CCRF-CEM cell protein by a Coomassie-stained gel, were separated, in parallel, by bidimensional PAGE and blotted onto nitrocellulose filters, as described in the Materials and methods.(A) Western blotting.The filter was assayed for Western blot using anti-eEF1A mAb, as described in the Materials and methods The position of the eEF1A protein was focused by revealing the presence of the Ran–GTP protein.(B) SouthWestern blotting.The filter was assayed for SouthWestern blot as described in the Materials and methods using, as probe, c32P-labelled GT oligomer and then exposed to Omat XAR Kodak film.

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Eukaryotic EF1A is a protein belonging to the

binding elongation factor family, which promotes the

GTP-dependent binding of aminoacyl-tRNA to the A-site of

ribosomes during protein biosynthesis and the capture of

deacylated tRNA at the exit site and its delivery to synthase

[30].It has been suggested that eEF1A might serve also as a

downstream component of growth-signalling pathways,

possibly through its capability to interact with actin, thus

promoting cell transformation [31].An overexpression of

eEF1A has been shown in many tumours [32], and eEF1A

has been associated with a highly metastatic potential in

cancer cells [33].The regulation of eEF1A expression by

extracellular stimuli depends on human epidermal growth

factor (EGF) receptor family members that are widely

deregulated in human cancers [34]

eEF1A is the second most abundant protein in the cell;

whereas the b, c and d subunits of eEF1 are predominantly

located in the cytoplasm, a considerable fraction of the a

subunit can be found either in the cytoplasm or the nucleus

[35,36].The involvement of eEF1A in the regulation of

nuclear processes includes the accumulation of a nuclear

complex with vigilin, for exporting tRNA [37], and with

ZPR1, for inducing cell proliferation upon mitogen

stimu-lation [38].Thus, the elucidation of a possible role for the

nuclear fraction of eEF1A in modulating nuclear

func-tion and gene expression could gain new insights in

tumorigenesis

In this manuscript, we demonstrate that eEF1A, isolated

from nuclear extracts of CCRF-CEM cancer cells, is

specifically recognized by a cytotoxic GT sequence.This

protein was found to be the polypeptide component of the

CRC, based on MALDI-MS analysis, Western blotting

experiments and supershift assays.In contrast, the GT

oligomer did not bind to the eEF1A of normal human

lymphocytes and these cells were not sensitive to the

cytotoxic action of the GT.It should be noted that nucleolin

was also recognized by the GT oligomer [10,17].However,

under native conditions, the more abundant CRC observed,

migrated with an apparent mass not associated with the

nucleolin–oligomer complex [12–15], probably because the

GT sequence used does not form, in appreciable quantity,

the G-quartet structure specifically recognized by this

protein, as revealed by gel electrophoresis and circular

dichroism studies [12,14].Moreover, nucleolin, and not

eEF1A, was bound by the GT oligomer in lymphocyte

sample on one-dimensional SouthWestern assay; however,

lymphocyte viability was not affected by GT.In cytoplasmic

extracts, the nucleolin was found to bind to GT in a

SouthWestern assay, but not in EMSA or UV crosslinking

assays.Furthermore, we analysed a G-rich GT sequence

able to form the G-quartet structure and thus to bind to

nucleolin.We found that this oligomer did not elicit

cytotoxicity on CCRF-CEM cells, although it was

effi-ciently taken up by the cells.More interestingly, in UV

cross-linking competition experiments, this sequence did not

displace the labelled GT from the CRC but from the less

represented lower migrating complex (corresponding to

nucleolin) (data not shown).On this basis, we can

hypo-thesize a minor involvement of nucleolin in the mechanism

of cytotoxicity elicited by the GT oligomers [12].It seemed

probable that the reactivity of the nucleolin was related much more to the experimental conditions of the immobi-lized protein on the SouthWestern assay, than to a native binding affinity for the GT.Nevertheless, we cannot completely exclude that other, less-abundant proteins can contribute to this effect

Binding assays by SouthWestern experiments demon-strated that nuclear eEF1A affinity for GT oligomers was significantly higher than that measured for the control CT sequence.Moreover, in EMSA assays a significant quantity

of GT oligomer remained bound to the protein, derived from the excised P1 band, in the presence of a 50-fold molar excess of CT oligomer competitor, whereas only a fivefold molar excess of GT oligomer was sufficient to release all control CT oligomer from the complex.It is noteworthy that the P1 band excised from the Coomassie-stained gel of

a normal lymphocyte sample failed to form complexes in EMSA with GT oligomer (data not shown).Furthermore, overloaded protein samples from normal lymphocytes did not show significant interaction between the eEF1A protein and the cytotoxic GT oligomer in SouthWestern assays Accordingly, GT oligomers did not elicit cytotoxic action on these cells, and did not form the CRC with the nuclear proteins when a fourfold increase in protein content was loaded onto the gel (data not shown).These results underline that eEF1A from CCRF-CEM cell nuclear extracts displays specificity in recognizing GT oligomers, and the selective cytotoxic action on CCRF-CEM cells suggests a possible role for eEF1A in maintaining the viability and proliferative activity of cancer cells.One hypothesis may be that these oligomers exert their action by blocking the binding of eEF1A to its ligand in cancer cells, perhaps to zinc finger proteins involved in the modulation

of cell proliferation, as proposed by Gangwani et al [38] Bidimensional PAGE analysis of eEF1A combined with

a specific Western blotting assay showed the occurrence of two distinct clusters of spots in T-lymphoblastic CCRF-CEM cells, whereas normal lymphocytes presented only one cluster.In particular, the newly occurring components in cancer cells (cluster 2) focused at a more basic pH.This result could hypothetically explain the higher affinity of the protein towards oligonucleotides simply on the basis of a charge increase at specific amino acids in its nucleotide-binding site, but not its nucleotide-binding selectivity for the GT sequences

Different post-translational modifications have been reported to occur in the eEF1A polypeptide chain, such as phosphorylation, methylation and glyceryl-phosphoryl-ethanolamine addition [25,27,29,39,40] but, to date, their functional significance has not been totally solved.Differ-ences in the level of phosphorylation of eEF1A have already been reported to be associated with variation in binding affinity towards viral genomic RNA, as well as to regulative interconversion between active and inactive forms [41].Our findings should not sustain the hypothesis that eEF1A propensity for recognition of GT oligomers in CCRF-CEM cancer cells might be related merely to an increase of the phosphorylation state.On the contrary, the modification of eEF1A mobility on bidimensional PAGE by increasing its

pI value should be associated with the presence of other post-translational modifications.Methylation of eEF1A has been significantly associated with SV40 transformation in

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