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Báo cáo khoa học: Concerted mutation of Phe residues belonging to the b-dystroglycan ectodomain strongly inhibits the interaction with a-dystroglycan in vitro pot

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Solid-phase binding assays, performed with recombinant fragments corresponding to the C-terminal domain of a-DG harboring progressive deletions, have shown that the b-DG-binding epitope

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to the b-dystroglycan ectodomain strongly inhibits the

interaction with a-dystroglycan in vitro

Manuela Bozzi1,*, Francesca Sciandra2,*, Lorenzo Ferri2, Paola Torreri3, Ernesto Pavoni2,

Tamara C Petrucci3, Bruno Giardina2and Andrea Brancaccio2

1 Istituto di Biochimica e Biochimica Clinica, Universita` Cattolica del Sacro Cuore, Rome, Italy

2 CNR, Istituto di Chimica del Riconoscimento Molecolare c ⁄ o Istituto di Biochimica e Biochimica Clinica, Universita` Cattolica del Sacro Cuore, Rome, Italy

3 Dipartimento di Biologia Cellulare e Neuroscienze, Istituto Superiore di Sanita`, Rome, Italy

Dystroglycan (DG) is an adhesion molecule composed

of two subunits, a-DG and b-DG [1], encoded by a

single gene, dag1, which produces a unique polypeptide

precursor consisting of 895 amino acids A post-trans-lational cleavage, performed by a still unidentified pro-tease at the Gly653-Ser654 site, produces two subunits,

Keywords

alanine scanning; cell transfection;

dystroglycan; protein–protein interaction;

site-directed mutagenesis

Correspondence

A Brancaccio, CNR, Istituto di Chimica del

Riconoscimento Molecolare c ⁄ o Istituto di

Biochimica e Biochimica Clinica, Universita`

Cattolica del Sacro Cuore, Largo Francesco

Vito 1, 00168 Rome, Italy

Fax: +39 6 3053598

Tel: +39 6 3057612

E-mail: andrea.brancaccio@icrm.cnr.it

*These authors contributed equally to this

work

(Received 10 July 2006, revised 1 September

2006, accepted 6 September 2006)

doi:10.1111/j.1742-4658.2006.05492.x

The dystroglycan adhesion complex consists of two noncovalently interact-ing proteins: a-dystroglycan, a peripheral extracellular subunit that is extensively glycosylated, and the transmembrane b-dystroglycan, whose cytosolic tail interacts with dystrophin, thus linking the F-actin cytoskele-ton to the extracellular matrix Dystroglycan is thought to play a crucial role in the stability of the plasmalemma, and forms strong contacts between the extracellular matrix and the cytoskeleton in a wide variety of tissues Abnormal membrane targeting of dystroglycan subunits and⁄ or their aberrant post-translational modification are often associated with several pathologic conditions, ranging from neuromuscular disorders to carcinomas A putative functional hotspot of dystroglycan is represented

by its intersubunit surface, which is contributed by two amino acid stret-ches: approximately 30 amino acids of b-dystroglycan (691–719), and approximately 15 amino acids of a-dystroglycan (550–565) Exploiting alanine scanning, we have produced a panel of site-directed mutants of our two consolidated recombinant peptides b-dystroglycan (654–750), corresponding to the ectodomain of b-dystroglycan, and a-dystroglycan (485–630), spanning the C-terminal domain of a-dystroglycan By solid-phase binding assays and surface plasmon resonance, we have determined the binding affinities of mutated peptides in comparison to those of wild-type a-dystroglycan and b-dystroglycan, and shown the crucial role of two b-dystroglycan phenylalanines, namely Phe692 and Phe718, for the a–b interaction Substitution of the a-dystroglycan residues Trp551, Phe554 and Asn555 by Ala does not affect the interaction between dystroglycan subunits in vitro As a preliminary analysis of the possible effects of the aforementioned mutations in vivo, detection through immunofluorescence and western blot of the two dystroglycan subunits was pursued in dystro-glycan-transfected 293-Ebna cells

Abbreviations

DG, dystroglycan; DGC, dystroglycan–glycoprotein complex; EGFP, enhanced green fluorescent protein; SPR, surface plasmon

resonance.

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a-DG and b-DG a-DG is a highly glycosylated

per-ipheral membrane protein that interacts with several

extracellular matrix proteins such as laminin, perlecan

and agrin [2] b-DG spans the membrane and binds

a-DG in a noncovalent way, providing a connection

between the extracellular matrix and the cytoskeleton

inside the cells, where it interacts with dystrophin,

utrophin and other cytosolic proteins, such as rapsyn,

caveolin-3 and Grb2 [3–5] Together with sarcoglycans,

dystrobrevins, syntrophins, and sarcospan, DG forms

the dystrophin–glycoprotein complex (DCG), which

plays an essential role as a scaffold for cells in muscle

and in a wide variety of nonmuscle tissues [6,7],

inclu-ding the central and peripheral nervous systems, and

several epithelial tissues [8]

The importance of the DCG is dramatically

appar-ent in several forms of muscular dystrophy, where

mutations in DCG proteins lead to instability and

pro-gressive weakness of the muscle fibers [9] Although no

natural mutations have been detected in DG, it is

sub-stantially altered or absent in muscular dystrophies

For this reason, detailed molecular characterization of

the subunit interface should be considered of primary

importance for our understanding of the overall

stabil-ity of the DGG, and perhaps in the future for surgical

modulation of its function with the purpose of

allevi-ating severe human diseases [10]

Primary structure analysis and electron microscopy

have shown that a-DG has a dumbbell-like structure

organized in two globular domains, the N-terminal and

C-terminal domains, connected by an elongated central

mucin-like region that contains highly glycosylated

sequences, rich in prolines, serines and threonines [11]

A structural characterization of the N-terminal domain

was recently obtained by a crystallographic analysis

carried out on a murine a-DG N-terminal fragment,

and revealed the presence of two autonomous modules

connected by a long and flexible linker The N-terminal

module shows Ig-like folding, whereas the C-terminal

module appears to be very similar to the ribosomal

RNA-binding proteins [12] The only structural hints

concerning the C-terminal domain of a-DG come from

a sequence alignment approach, which has shown some

similarities with cadherin domains [13]

Previous studies, carried out employing a series of

independent techniques such as IR, CD [14] and NMR

spectroscopy [15], have revealed the absence of any

classic secondary structural element in the recombinant

b-DG ectodomain, which shows high conformational

plasticity, typical of a natively unfolded protein

The noncovalent interaction between the two DG

subunits occurs between the C-terminal region of

a-DG and the N-terminal ectodomain of b-DG, and is

apparently independent of glycosylation [16] Solid-phase binding assays, performed with recombinant fragments corresponding to the C-terminal domain of a-DG harboring progressive deletions, have shown that the b-DG-binding epitope resides between amino acids 550 and 585 [17], and further NMR analysis has narrowed this location to amino acids 550–565 [18] In addition, extensive NMR structural characterization

of our 15N⁄13C b-DG(654–750) recombinant fragment, spanning the b-DG ectodomain, suggested that the a-DG-binding epitope corresponds to an amino acid stretch located between positions 691 and 719 [15]

In order to identify the specific amino acids within the linear interacting epitopes involved in the complex between a-DG and b-DG, alanine scanning of some of the residues that were mainly influenced in NMR titra-tions [15] was performed on recombinant fragments a-DG(485–630) and b-DG(654–750) The reciprocal affinities of wild-type a-DG and b-DG peptides vs the panel of mutated recombinant fragments were meas-ured using two independent techniques: solid-phase binding assays, exploiting biotinylated recombinant lig-ands, and surface plasmon resonance (SPR), in which one peptide is covalently immobilized on a sensor chip while the other is used in soluble phase without labels Such mutations were also imported into full-length

DG constructs cloned into an appropriate vector to transfect eukaryotic cells, in order to set up a suitable cellular system to study the effect of site-directed mut-agenesis on the processing and targeting of DG in vivo

Results

Mutations within the b-DG(654–750) recombinant fragment

The phenylalanine in position 718, belonging to the putative a-DG-binding epitope (691–719) within the ectodomain of b-DG, was found to be one of the most influenced residues during the titration of [15N]b-DG(654–750) with thioredoxin-a-DG(485–620) [15] Therefore, we decided to mutate it to an alanine, together with two other phenylalanines, Phe692 and Phe700, the only other aromatic residues located within the a-DG-binding epitope that are highly con-served in all the species so far analyzed A more dras-tic alteration of the protein primary structure was produced by deleting six amino acids, located within the a-DG-binding epitope, between positions

701 and 706 A previous NMR characterization of the b-DG ectodomain [15] revealed that the amino acids between positions 701 and 704 are so flexible as to be undetectable under the experimental conditions used

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for NMR analysis We believed that it would be

inter-esting to verify whether such a flexible amino acid

stretch, located within the a-DG-binding epitope,

might play a role in the interaction between the a-DG

and b-DG subunits Three additional mutations were

introduced outside the putative a-DG-binding epitope

to check whether perturbing the b-DG ectodomain

elsewhere might also influence its interaction with

a-DG We produced two mutations upstream of the

a-DG-binding epitope, such as Trp659fi Ala, because

Trp659 is the only aromatic residue in this portion of

the protein, and Glu667fi Ala; only one mutation,

Val736fi Ala, was generated within the C-terminal

region of the b-DG ectodomain, downstream of

the a-DG-binding epitope A map of all the mutations

produced within the recombinant fragments

b-DG(654–750) and a-DG(485–620) is given in Fig 1

In order to measure the affinity of such mutants

for a-DG(485–630), a series of solid-phase binding

assays was carried out Typically, in solid-phase binding

assays, a-DG(485–630) was coated onto

micro-titer plates, whereas b-DG(654–750) and its

mutants, b-DG(654–750)Trp659fi Ala, b-DG(654–

750)Glu667fi Ala, b-DG(654–750)Phe692fi Ala, b-DG(654–

750)Phe700fi Ala, b-DG(654–750)Phe718fi Ala, b-DG(654–

750)Val736fi Ala, b-DG(654–750)Phe692fi Ala ⁄ Phe718 fi Ala,

b-DG(654–750)Phe692fi Ala ⁄ Phe700 fi Ala ⁄ Phe718 fi Ala and

b-DG(654–750)D(701)706), were biotinylated and used as

soluble ligand at increasing concentrations (up to 20 lm)

The apparent affinity for a-DG(485–630), exhibited

by the mutants b-DG(654–750)Glu667fi Ala and b-DG(654–750)Val736fi Alaand evaluated by solid-phase binding assays, was very similar to that displayed by b-DG(654–750) (Fig 2A, Table 1), whereas all the other single mutants, namely b-DG(654–750)Trp659fi Ala, b-DG(654–750)Phe692 fi Ala, b-DG(654–750)Phe700 fi Ala and b-DG(654–750)Phe718fi Ala, showed reduced affinity for a-DG(485–630) (Fig 2B) Also, the deletion mutant b-DG(654–750)D(701)706) was able to bind a-DG(485– 630) with the same affinity as the wild type, demonstra-ting that the highly flexible stretch corresponding to positions 701–706 is not involved in the interaction with a-DG(485–630) and does not alter significantly the b-DG ectodomain conformation (Fig 2A, Table 1) On the other hand, double and triple mutations, such as Phe692fi Ala ⁄ Phe718 fi Ala and Phe692fi Ala ⁄ Phe700fi Ala ⁄ Phe718 fi Ala, completely abolished the binding between b-DG(654–750) and a-DG(485– 630), at least in the ligand concentration range explored (Fig 2C) To rule out the possibility that the lower affinity for a-DG(485–630) exhibited by some b-DG mutants might be due to some major proteolytic event, all the samples used to perform solid-phase binding assays were checked by Tricine⁄ SDS ⁄ PAGE before and after biotinylation, and showed the same mobility as wild-type b-DG(654–750), indicating that no degrada-tion occurred within mutated recombinant fragments; similarly, we did not observe any evident aggregation behavior when analyzing the various mutated b-DG peptides by native gel electrophoresis (data not shown) The solid-phase binding assay data were confirmed

by SPR experiments, in which a-DG(485–630) was immobilized on a sensor chip, and b-DG(654–750) and its mutants were used in soluble phase as analytes First, the dissociation equilibrium constant KD was measured for the interaction between the two wild-type recombinant fragments a-DG(485–630) and b-DG(654–750) It should be noted that the affinity constant value for the b-DG(654–750)–a-DG(485–630) interaction, measured by immobilizing b-DG(654–750) and using a-DG(485–630) as analyte (KD2.73 lm) (Table 1, Supplementary Fig S1), was fully compar-able to the value obtained when a-DG(485–630) was immobilized and b-DG(654–750) was used as analyte (KD2.66 lm) (Table 1) The thermodynamic constant

KDwas also measured for the interaction between the wild-type recombinant fragment a-DG(485–630) and the mutant b-DG(654–750)Phe700fi Ala, and confirmed its reduced affinity for a-DG(485–630) with respect to the wild type (KD7.00 lm; Table 1)

The kinetic SPR profiles obtained for all the single mutants b-DG(654–750)Phe692fi Ala, b-DG(654–

Fig 1 A panel of mutations hitting the reciprocal a-DG–b-DG

bind-ing epitopes was generated In the C-terminal region of a-DG,

between amino acids 550 and 565, Trp551, Phe554 and Asn555

were mutated to alanine In the a-DG-binding epitope comprising

residues 691–719 of the b-DG ectodomain, the mutations

Phe692 fi Ala, Phe700 fi Ala and Phe718 fi Ala were generated

while the residues from 701 to 706 were knocked-in Three

addi-tional mutations were introduced: Glu667 fi Ala and Trp659 fi Ala

upstream, and Val736 fi Ala downstream, of the a-DG-binding

epi-tope.

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750)Phe700fi Ala and b-DG(654–750)Phe718fi Ala were in line with the reduction of affinity measured by solid-phase binding assays, indicating a lower association rate and a higher dissociation rate with respect to wild-type a-DG The only exception was the mutant b-DG(654–750)Phe700fi Ala, which showed a higher association rate but also a higher dissociation rate in comparison to the wild type; the double mutant b-DG(654–750)Phe692fi Ala ⁄ Phe718 fi Ala did not bind a-DG(485–630) at all (Fig 3)

Mutations within the a-DG(485–630) recombinant fragment

Our previous NMR analysis using a synthetic peptide corresponding to a-DG(550–585) and the recombinant fragment b-DG(654–750) indicated that the residues between positions 550 and 565 of a-DG belong to an amino acid stretch that is likely to be involved in the

A

B

C

Fig 2 Solid-phase binding assays a-DG(485–630) was immobilized

on plates, whereas b-DG(654–750) (black) and its mutants

b-DG(654–750) Glu667 fi Ala (blue), b-DG(654–750) Val736 fi Ala (red),

b-DG(654–750)D(701)706) (green) (A), b-DG(654–750) Trp659 fi Ala

(magenta), b-DG(654–750)Phe692fi Ala (green), b-DG(654–

750) Phe700 fi Ala (blue), b-DG(654–750) Phe718 fi Ala (yellow) (B),

b-DG(654–750) Phe692 fi Ala ⁄ Phe718 fi Ala

(cyan), and b-DG(654–

750)Phe692fi Ala ⁄ Phe700 fi Ala ⁄ Phe718 fi Ala(red) (C), were used as

biot-inylated ligands Every point is an average of three or more

inde-pendent experiments The continuous line represents fitting of

experimental data using a single class of equivalent binding sites

equation The maximal binding of control b-DG(654–750),

extrapola-ted by fitting experimental data, was set as 100% (see

Experimen-tal procedures).

Table 1 (A) Equilibrium dissociation constants (K D ) calculated by solid-phase binding assays and SPR Mean apparent K D values and relative standard deviations, calculated for the interaction between wild-type and mutated recombinant fragments, b-DG(654–750) and a-DG(485–630), by solid-phase binding assays The values are averaged over a number of independent experiments, indicated in parentheses For the b-DG mutants showing reduced affinity for a-DG(485–630), K D values cannot be calculated (ND, not determined; see Experimental procedures) (B) KD values for the interaction between wild-type recombinant fragments, b-DG(654–750) and a-DG(485–630), and b-DG(654–750) Phe700 fi Ala

and a-DG(485–630),

as measured by SPR.

(A) Solid-phase binding assays Immobilized protein ⁄ biotinylated protein Apparent KD(l M ) a-DGwt⁄ b-DG wt

2.8 ± 0.9 (9) a-DG wt ⁄ b-DG Glu667 fi Ala 3.5 ± 0.9 (3)

a-DGwt⁄ b-DG Val736 fi Ala

2.9 ± 2 (4)

a-DG wt ⁄ b-DG Phe700 fi Ala

ND (3) a-DGwt⁄ b-DG Phe718 fi Ala

ND (8) a-DG wt ⁄ b-DG Phe692 fi Ala ⁄ Phe718 fi Ala ND (3) a-DG wt ⁄ b-DG Phe692 fi Ala ⁄ Phe700 fi Ala ⁄ Phe718 fi Ala

ND (3) a-DGTrp551fi Ala⁄ b-DG wt

1.3 ± 0.8 (4) a-DG Phe554–Ala ⁄ b-DG wt 2.3 ± 0.9 (5) a-DG Asn555 fi Ala

a-DGTrp551fi Ala ⁄ Phe554 fi Ala⁄ b-DG wt

2.4 ± 0.7 (3) (B) SPR

a-DGwt⁄ b-DG Phe700 fi Ala

7.00

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interaction with b-DG(654–750), based on data

collec-ted at the level of their NH and CHa [18]

In order to test the role of individual amino acid

side chains at the a-DG–b-DG interface, alanine

scan-ning of positions Trp551, Phe554 and Asn555 was

carried out Solid-phase binding assays were carried

out, in which a-DG(485–630) and its mutants,

a-DG(485–630)Trp551fi Ala, a-DG(485–630)Phe554fi Ala,

a-DG(485–630)Asn555fi Ala and a-DG(485–

630)Trp551fi Ala ⁄ Phe554 fi Ala were coated onto the

microtiter plate and biotinylated b-DG(654–750) was

used as soluble ligand All the mutants showed the

same affinity for b-DG(654–750) as the wild type,

indi-cating that such mutations are not likely to have major

effects on the interaction between a-DG and b-DG

(Supplementary Fig S2) Accordingly, the apparent

dissociation constant values obtained by fitting the

experimental data are very similar to the values

calcu-lated for the interaction between the wild-type peptides

a-DG(485–630) and b-DG(654–750) (Table 1) To

fur-ther confirm that residues Trp551, Phe554 and Asn555

are not involved in the interaction with b-DG, the

affinities of some b-DG mutants for the mutants

a-DG(485–630)Trp551fi Ala, a-DG(485–630)Phe554fi Ala

and a-DG(485–630)Asn555fi Ala were also estimated

by solid-phase binding assays The affinities of

b-DG(654–750)Trp659fi Ala, b-DG(654–750)Phe692fi Ala,

b-DG(654–750)Phe700fi Ala, b-DG(654–750)Phe718fi Ala

and b-DG(654–750)Phe692fi Ala ⁄ Phe700 fi Ala ⁄ Phe718 fi Ala

for immobilized a-DG mutants were very similar to

the reduced affinity exhibited for wild-type a-DG(485–

630), indicating that the effect measured can be ascribed to the mutations within the b-DG ectodomain (data not shown) Interestingly, a western blot experi-ment showed that Trp551, Phe554 and Asn555 are also not likely to be key residues for the interaction with the mAb sx⁄ 3 ⁄ 50 ⁄ 25 directed against the b-DG-bind-ing epitope (residues 549–567 of a-DG) [19], as the antibody is able to recognize the bands relative to a-DG recombinant peptides in western blot experi-ments (Fig 4A) Moreover, the antibody is also able

to bind a-DG mutated peptides in solid-phase binding assays, as it inhibits the interaction between b-DG(654–750) and the mutant a-DG(485– 630)Phe554fi Ala (Fig 4B), as previously shown for wild-type a-DG(485–600) [19]

A

B

Fig 4 (A) Western blot on 12% SDS ⁄ PAGE of wild-type and mutated recombinant fragments of a-DG Recombinant fragments were detected using mAb sx ⁄ 3 ⁄ 50 ⁄ 25 Lane 1: a-DG(485– 630) Trp551–Ala ⁄ Phe554 fi Ala Lane 2: a-DG(485–630) Asn555 fi Ala Lane 3: a-DG(485–630) Phe554 fi Ala

Lane 4: a-DG(485–630) Trp551 fi Ala

Lane 5 (control): a-DG(485–630) (B) Solid-phase binding assays were performed by immobilizing a-DG(485–630) (d) and a-DG(485– 630) Phe554 fi Ala

(h) and using biotinylated b-DG(654–750) as soluble ligand, in the presence (empty symbols) and in the absence (full symbols) of mAb sx ⁄ 3 ⁄ 50 ⁄ 25.

Fig 3 SPR kinetic profiles of the interaction between immobilized

a-DG(485–630) and b-DG(654–750) (black) and its mutants,

b-DG(654–750) Phe692 fi Ala (green), b-DG(654–750) Phe700 fi Ala (blue),

b-DG(654–750)Phe718fi Ala(yellow), b-DG(654–750)Phe692–Ala⁄ Phe718 fi Ala

(cyan), used as analytes at a fixed concentration of 10 l M

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Transfection of 293-Ebna cells with wild-type and

mutated DG constructs

In order to verify the correct membrane targeting

of mutated DG, DNA constructs spanning the entire

DG gene, including its signal peptide, and carrying

the mutations analysed in vitro, such as Trp551fi

Ala, Phe554fi Ala, Asn555 fi Ala, Glu667 fi Ala,

Phe692fi Ala, Phe700fi Ala, Phe718fi Ala, Phe692fi Ala ⁄ Phe718 fi Ala and Val736fi Ala, were included in an appropriate mammalian expression vector and then transfected into human 293-Ebna cells The cytomegalovirus promoter drives the efficient tran-scription of the DG exogenous gene, which was strongly expressed in the transfected cells (Fig 5) None of the mutations seemed to significantly alter the

A

Fig 5 Immunostaining of wild-type DG and its mutants in transiently transfected 293-Ebna cells (A) The a-subunits were stained with a polyclonal antibody directed against the C-terminal domain of a-DG on intact 293-Ebna cells (B) Detection of b-DG was carried out using b-DG antibody in permeabilized 293-Ebna cells Both subunits of wild-type and mutated DG were clearly overexpressed with respect to non-transfected cells displaying a much lower and diffuse staining due to endogenous DG; the double mutation Phe692 fi Ala ⁄ Phe718 fi Ala does not alter the membrane targeting of a-DG.

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correct membrane localization of a-DG and b-DG, at

least 24 h after transfection, as all the mutants could

be stained with a polyclonal antibody directed against

the C-terminal region of a-DG [20] and with a

com-mercial antibody directed against the cytoplasmic tail

of b-DG (Fig 5A,B) Also, the double mutation

Phe692fi Ala ⁄ Phe718 fi Ala, which greatly reduces

the affinity of b-DG for the a-subunit in vitro, did not

influence the localization of the two DG subunits

(Fig 5A,B) In order to detect any effect of the double

mutation Phe692fi Ala ⁄ Phe718 fi Ala, which may

have evaded the immunostaining analysis [21], the entire DG carrying this mutation was cloned into the pEGFP vector, which codes for the enhanced green fluorescence protein (EGFP) fused at the C-terminus

of b-DG This vector was used to transiently transfect 293-Ebna cells Other two pEGFP vectors were produced, carrying wild-type DG and its mutant

DGPhe554fi Ala, respectively, to be used as a control (Fig 6)

EGFP increases the molecular mass of b-DG

by 25 kDa, allowing us to distinguish between the

B

Fig 5 (Continued).

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exogenous b-DG and the endogenous b-DG in western

blot experiments Western blot analysis carried out on

total protein extracts from 293-Ebna cells transiently

transfected with wild-type and mutated (Phe554fi Ala

or Phe692fi Ala ⁄ Phe718 fi Ala) DG genes did not

show any aberrant processing or glycosylation patterns

of DG Although lower expression of a-DG was

detected in all transfected cells (including those

transfected with empty pEGFP or wild-type pDG–

EGFP; Fig 7A), the amount of a-DG in the cells

transfected with the double-mutated (Phe692fi Ala ⁄

Phe718fi Ala) DG construct was similar to that

measured in wild-type DG-transfected cells (Fig 7)

Discussion

In vitro inhibition of the a-DG–b-DG interaction

via Phe to Ala mutations within the ectodomain

of b-DG

We investigated the interaction between a-DG and

b-DG recombinant peptides carrying a series of

site-directed mutations We performed amino acid

substitu-tions using alanine, because this residue does not show

any propensity for a specific secondary structure, and

therefore does not perturb the overall protein

confor-mation while highlighting the role of the side chain

functional group that it replaces [22,23] This

charac-teristic makes alanine the amino acid of choice for site-directed mutagenesis [22–26] For the first time, we have measured the affinity between recombinant pep-tides spanning the C-terminal domain of a-DG and the b-DG ectodomain by solid-phase binding assays and SPR, demonstrating that despite the intrinsic pit-falls of solid-phase binding techniques, extensively reviewed by Tangemann & Engel [27], the apparent

KDvalues measured with our ‘two-step’ biotin enzyme-linked streptavidin approach are in full agreement with those measured with an independent and accurate technique such as SPR, whose reliability has been dem-onstrated in recent years for protein–protein interac-tions displaying very low affinity [28] Our SPR measurements simply demonstrate that the apparent constants that we have estimated with the solid-phase binding approach are reliable In this case, it seems that even a complex displaying a relatively low affinity (KDabout 3 lm; Table 1) can be populated, when rap-idly washed without major perturbations and then titrated with streptavidin [17,29]

In previous studies, we had already estimated that the a-DG-binding epitope of b-DG might involve a relatively extended region of approximately 30 amino acids, between positions 691 and 719 [15] In order to obtain a deeper insight into the a–b interface, we have introduced a series of mutations within the b-DG ecto-domain located in three different protein regions:

D C

Fig 6 293-Ebna cells transiently transfected with the vector pEGFP, empty (A) or containing DNA constructs corresponding to wild-type DG (B) and its mutants DG Phe554 fi Ala (C) and

DGPhe692fi Ala ⁄ Phe718 fi Ala(D), where enhanced green fluorescent protein (EGFP) was fused at the C-terminus of b-DG All the images are magnified 10· EGFP alone was uniformly distributed throughout the cytoplasm, whereas DG–EGFP and its two mutants were mostly localized around the cellular periphery In order to better visualize the DG complex location at the cellular periphery, a 40· magnified image was obtained referring to wild-type DG–EGFP, which clearly shows the membrane targeting of the chimeric wild-type DG–EGFP construct [inset in (B), red arrowheads].

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upstream, downstream and inside the putative

a-DG-binding epitope By measuring the affinity of these

mutants for the recombinant fragment a-DG(485–630),

corresponding to the C-terminal domain of a-DG, via

solid-phase binding assays and SPR experiments, we

have found three different behaviors: some mutants,

namely b-DG(654–750)Glu667fi Ala, b-DG(654–

750)Val736fi Ala and b-DG(654–750)D(701)706), show the

same affinity for a-DG(485–630) as the wild-type

recombinant fragment; a second intermediate group,

comprising b-DG(654–750)Trp659fi Ala, b-DG(654–

750)Phe692fi Ala, b-DG(654–750)Phe700fi Ala and

b-DG(654–750)Phe718fi Ala, shows a reduced affinity

for a-DG(485–630); the double and triple mutants,

such as b-DG(654–750)Phe692fi Ala ⁄ Phe718 fi Ala and

b-DG(654–750)Phe692fi Ala ⁄ Phe700 fi Ala ⁄ Phe718 fi Ala are

completely unable to bind a-DG(485–630)

The behavior of b-DG(654–750)Glu667fi Ala and

b-DG(654–750)Val736fi Ala is not surprising, as these

point mutations are located upstream and downstream

of the a-DG-binding epitope, respectively, in por-tions of the protein that are not involved in the forma-tion of the a–b interface [15] However, this simple argument cannot be applied to explain the reduced affinity for a-DG(485–630) shown by the mutant b-DG(654–750)Trp659fi Ala, whose amino acid substitu-tion is located upstream of the a-DG-binding epitope

A possible interpretation of this result can be sugges-ted on the basis of previous studies showing that the recombinant fragment b-DG(654–750) is organized into an N-terminal region, consisting of approximately

70 amino acids, which is characterized by restricted conformational mobility, and a highly flexible C-ter-minal region of approximately 30 residues [15] In this context, an amino acid substitution introduced within the region of restricted mobility, such as Trp659fi Ala, although located outside the putative a-DG-binding epitope, may perturb the b-DG(654– 750) conformational equilibrium, driving it to adopt non-native conformations unable to efficiently bind a-DG(485–630)

All the point mutations located inside the puta-tive a-DG-binding epitope, namely b-DG(654– 750)Phe692fi Ala, b-DG(654–750)Phe700fi Ala and b-DG(654–750)Phe718fi Ala, result in reduced affinity between a-DG and b-DG recombinant peptides, which completely lose their ability to interact when two phenylalanines, Phe692 and Phe718, are simultaneously substituted with alanine Surprisingly, the deletion of six residues corresponding to amino acids 701–706, located between the two important phenylalanines Phe692 and Phe718, does not perturb the interaction between a-DG and b-DG recombinant peptides,

as can be deduced by comparing the values of the apparent KD for the b-DG(654–750)wt–a-DG(485–630) interaction and the b-DG(654–750)D(701)706) –a-DG(485–630) interaction, as measured by solid-phase binding assays (Table 1) It should be noted that the choice to delete these specific amino acids (701–706) is based on the observation that the residues between positions 701 and 704, although belonging to the region of restricted mobility, are so flexible to be unde-tectable under the experimental conditions used for NMR experiments [15]

The stretch 701–706 may be part of a flexible linker that could bring two separate regions of the a-DG-binding epitope (carrying Phe692 and Phe718, respect-ively) closer to each other when they bind a-DG Apparently, deleting the amino acid stretch 701–706 has no effect on the a–b interaction, so it is likely that the knock-in does not significantly alter the spatial distance between the two important phenyl-alanines

A

B

Fig 7 Immunoblot of total protein extracts from 293-Ebna cells

nontransfected (lane 1) or transfected with the empty pEGFP

vector (lane 2), or containing DG–EGFP (lane 3) and its mutants

DG Phe554 fi Ala

–EGFP (lane 4) and DG Phe692 fi Ala ⁄ Phe718 fi Ala

–EGFP (lane 5) (A) a-DG bound to the plasma membrane was probed

with the commercial antibody VIA4-1 (Upstate, Charlottesville, VA,

USA) (B) The amount of b-DG–EGFP (68 kDa) compared with that

of endogenous b-DG (43 kDa) was detected with the commercial

antibody directed against the cytoplasmatic tail of b-DG (upper

panel) and with antisera against EGFP (middle panel) Anti-actin

serum was used as loading control (lower panel).

Trang 10

Our previous results indicate that although the

ecto-domain of b-DG is a natively unfolded protein, its

conformation is still maintained by a delicate network

of long-range reciprocal interactions that govern major

structural–functional events [30], to which the two

phe-nylalanine residues, which are quite distant within the

b-DG ectodomain linear sequence, may make an

important contribution

When the binding experiments were performed with

a-DG(485–630) and its mutants, we found that

Trp551, Phe554 and Asn555 are not key residues

for the interaction with b-DG(654–750), because no

reduction of the affinity of the mutants a-DG

(485–630)Trp551fi Ala, a-DG(485–630)Phe554fi Ala,

a-DG(485–630)Asn555fi Ala and a-DG(485–

630)Trp551fi Ala ⁄ Phe554 fi Ala for b-DG(654–750),

com-pared to wild-type a-DG(485–630), was measured by

solid-phase binding assays (Supplementary Fig S2) It

should be pointed out that our previous NMR

experi-ments showed that a-DG residues Trp551, Phe554 and

Asn555, among others, were significantly influenced by

the presence of b-DG(654–750) at the level of the

pro-tein backbone (i.e at their NH and CHa), although at

that time no data were collected on their side chains,

which therefore could be substantially unaffected by

b-DG binding [18], as is now strongly suggested by the

results herein presented

A possible implication of our results is that the

specificity of a-DG(485–630) binding to b-DG(654–

750) could depend mainly on its local conformation

and only to a lesser extent on the chemical nature

of the amino acid side chains involved in the

bind-ing To further analyze this hypothesis, it will be

necessary to introduce, within residues 550–565 of

a-DG, amino acids that require stringent steric

con-straints, such as proline or isoleucine, which may

significantly perturb the local structural

characteris-tics of the b-DG-binding epitope Interestingly, the

amino acid substitutions that we analyzed do not

impair binding to a monoclonal antibody, mAb

sx⁄ 3 ⁄ 50 ⁄ 25, as suggested by the western blot in

Fig 4A Moreover, mAb sx⁄ 3 ⁄ 50 ⁄ 25 is able to

effi-ciently inhibit the interaction between wild-type

a-DG and b-DG peptides [19] and also between

mutated a-DG and b-DG (Fig 4B), suggesting that

other a-DG residues, belonging to the approximately

550–565 residues epitope, but located in the

C-ter-minal region downstream of those so far analyzed,

may be involved in the interaction both with mAb

sx⁄ 3 ⁄ 50 ⁄ 25 and b-DG(654–750) Therefore, additional

amino acid substitutions, such as Ser556fi Ala,

Gly563fi Ala and Pro565 fi Ala, will be tested in

the future [18]

Analysis of DG subunit targeting in vivo:

detection of DG subunits in 293-Ebna cells Few studies are currently available that focus on the identification and analysis of polymorphisms and⁄ or point mutations within the DG gene in human popula-tions [31,32]; nevertheless, it has been shown in a cellu-lar system that single mutations may strongly influence the processing of the DG precursor and targeting at the cell surface of its subunits [33] Mutations affecting some putative glycosylation sites lead to impaired membrane targeting of DG and also to defective clea-vage of the precursor into the two subunits [33] Fur-thermore, mutation at the precursor maturation cleavage site (Gly653-Ser654) induces muscular dystro-phy in mice [34]

To investigate whether the amino acid substitutions tested in vitro influence the stability and the localization

of DG at the plasma membrane, we transfected 293-Ebna cells with the full-length murine DG gene harboring the mutations Trp551fi Ala, Phe554 fi Ala, Asn555fi Ala, Glu667fi Ala, Phe692fi Ala, Phe700fi Ala, Phe718fi Ala, Val736fi Ala and Phe692fi Ala ⁄ Phe718 fi Ala Cell-staining experi-ments showed that none of these mutations significantly affects the subcellular trafficking and plasmalemmal tar-geting of exogenous murine DG in transfected human 293-Ebna cells (Fig 5) In fact, all the mutants were overexpressed, and a strong fluorescent signal was detec-ted at the plasmalemma, exploiting a monoclonal anti-body directed against the cytoplasmic tail of b-DG Apparently, even the double mutation Phe692fi Ala ⁄ Phe718fi Ala, which greatly impairs binding between the two DG subunits in vitro, has no evident effect on the plasmalemmal targeting of b-DG (Fig 5B) The cor-rect membrane targeting of DG was also confirmed by the immunodetection of the a-subunit in human cells transfected with all the mutants (Fig 5A) In order to further analyze possible effects of the double mutation Phe692fi Ala ⁄ Phe718 fi Ala in vivo, we also cloned the mutant DGPhe692fi Ala ⁄ Phe718 fi Alawithin the

pEG-FP vector, together with wild-type DG and the mutant

DGPhe554fi Alaas controls (Fig 6) Western blot analy-sis of total protein extracts from 293-Ebna cells, transi-ently transfected with these constructs, confirmed the results of cell-staining experiments (Fig 7) The amount

of a-DG in cells transfected with the mutant

DGPhe692fi Ala ⁄ Phe718 fi Ala is in fact fully comparable with that observed in cells transfected with the empty pEGFP vector or containing wild-type DG or

DGPhe554fi Ala(Fig 7A) The reduced amount of a-DG detected by VIA4-1 in all the 293-Ebna transfected cell lines probably results from reduction and⁄ or

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