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There-fore, as a first step toward understanding these mecha-nisms, we characterized a the pore-forming activity of PIN-a and a1-PTH in giant liposomes and b their toxicity to mammalian p

Trang 1

in giant liposomes but exert different toxic actions

on murine cells

Paola Llanos1, Mauricio Henriquez1, Jasmina Minic2, Khalil Elmorjani3, Didier Marion3,

Gloria Riquelme1, Jordi Molgo´2 and Evelyne Benoit2

1 Instituto de Ciencias Biome´dicas, Facultad de Medicina, Universidad de Chile, Santiago, Chile

2 Laboratoire de Neurobiologie Cellulaire et Mole´culaire, UPR 9040, Centre National de la Recherche Scientifique, Gif-sur-Yvette cedex, France

3 Biopolyme`res Interactions Assemblages, Institut National de la Recherche Agronomique, Nantes, France

Various cationic lipid-binding proteins, the folding of

which is stabilized by four or five disulfide bonds, have

been isolated from wheat endosperm They include

lipid-transfer proteins (LTPs), puroindolines (PINs)

and a⁄ b-purothionins (PTHs) [1] PINs are restricted

to Triticae and Avenae species [2,3], whereas LTPs and

PTHs are ubiquitous plant proteins found in most

plant organs [1,4,5] PIN-a and PIN-b, two isoforms

sharing 60% sequence homology, have been purified

from wheat seeds PIN-a displays a unique

trypto-phan-rich domain (WRWKWWK), which is slightly

truncated in PIN-b (WPTKWWK) The 3D structures

of LTPs and PINs are closely related and rich in

a-helices, as suggested by their cysteine pairing and

secondary-structure characterization [1,6], and they

dif-fer from the structure of the PTHs [5] Furthermore, in

contrast with LTPs, PINs and PTHs can be isolated

by Triton X-114 phase partitioning [7], an observation that is in agreement with differences in their lipid-binding properties Indeed, whereas LTPs bind lipid monomers in a hydrophobic cavity, PINs and PTHs interact with lipid aggregates, e.g micelles and lipid bilayers [1]

Because of their toxic activity against fungi, yeast and bacteria, PTHs have been suggested to play a role

in plant defence against microbial pathogens [4,5] PINs are also thought to have a role in plant defence because of their antifungal properties in vitro, and especially because they enhance the antimicrobial effects of PTHs [8] In addition, leaf extracts of trans-genic rice plants expressing genes encoding PINs (pinA and⁄ or pinB) reduce in vitro the growth of rice fungal

Keywords

a1-purothionin; giant liposomes; ion

channels; neuromuscular transmission;

puroindoline-a

Correspondence

E Benoit, Laboratoire de Neurobiologie

Cellulaire et Mole´culaire, UPR 9040, Centre

National de la Recherche Scientifique, baˆt.

32–33, 91198 Gif-sur-Yvette cedex, France

Fax: +33 169 82 41 41

Tel: +33 169 82 36 52

E-mail: benoit@nbcm.cnrs-gif.fr

(Received 20 July 2005, revised 13 February

2006, accepted 17 February 2006)

doi:10.1111/j.1742-4658.2006.05185.x

Puroindoline-a (PIN-a) and a1-purothionin (a1-PTH), isolated from wheat endosperm of Triticum aestivum sp., have been suggested to play a role in plant defence mechanisms against phytopathogenic organisms We investi-gated their ability to form pores when incorporated into giant liposomes using the patch-clamp technique PIN-a formed cationic channels ( 15 pS) with the following selectivity K+> Na+ Cl– Also, a1-PTH formed channels of  46 pS and 125 pS at +100 mV, the selectivity of which was Ca2+> Na+ K+ Cl– and Cl– Na+, respectively In isolated mouse neuromuscular preparations, a1-PTH induced muscle mem-brane depolarization, leading to blockade of synaptic transmission and directly elicited muscle twitches Also, a1-PTH caused swelling of differen-tiated neuroblastoma NG108-15 cells, membrane bleb formation, and dis-organization of F-actin In contrast, similar concentrations of PIN-a had

no detectable effects The cytotoxic actions of a1-PTH on mammalian cells may be explained by its ability to induce cationic-selective channels

Abbreviations

EPP, endplate potential; LTP, lipid-transfer protein; MEPP, miniature endplate potential; PIN, puroindoline; PTH, purothionin.

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pathogens [9] The generalized toxicity of PTHs may

be due to their ability to form ion channels in the

membrane of target cells, resulting in dissipation of

ion concentration gradients essential for the

mainten-ance of cellular homoeostasis [10–13] Also, b-PTH

extracted from wheat flour has been shown to form

cation-selective ion channels in artificial lipid bilayer

membranes and in the plasmalemma of rat

hippocam-pal neurons [14] PIN-a and a1-PTH have also been

reported to swell the nodes of Ranvier of frog

myeli-nated axons, and pore formation in the nodal

mem-brane has been suggested to be responsible for these

effects [15] In addition, PINs have also been shown to

be cytotoxic to Xenopus oocytes [16] However, the

mechanisms involved in the toxicity of PTHs and PINs

to mammalian cells remain poorly understood

There-fore, as a first step toward understanding these

mecha-nisms, we characterized (a) the pore-forming activity

of PIN-a and a1-PTH in giant liposomes and (b) their

toxicity to mammalian phrenic nerve⁄ hemidiaphragm

muscle preparations and cultured neuroblastoma

(NG108-15) cells A preliminary account of part of this

work has been published in abstract form [17]

Results

Molecular masses of purified PIN-a and a1-PTH

A typical electrospray mass spectrum of purified wheat

PIN-a (Fig 1A) reveals that its apparent heterogeneity

is related to complex post-translational proteolytic

maturation which leads to two major forms (Mr

12 750 and 12 919) and three minor ones (Mr

12 634.7, 12 803.5 and 13 083.6) However, as reported

by Blochet et al [18], all these polypeptides originate

from a unique polypeptide template with different

extensions at both the N-terminus and C-terminus

(Fig 1A) The mass spectrum of a1-PTH is depicted in

Fig 1B All the masses reported here fit very well with

the expected calculated molecular masses for native

PIN-a and a1-PTH

PIN-a forms ionic channels in giant liposomes

Seals of high-resistance and excised patches in an

‘inside out’ configuration were obtained from 19

prep-arations of giant liposomes containing PIN-a

Forty-five of 72 patches studied ( 60%) exhibited channel

activity Usually, multiple current levels corresponding

to a similar conductance were observed, and at least

two distinct levels were detected in 35 of the 45

pat-ches ( 78%) The unitary level was difficult to

observe in isolation, which suggested the presence of

substrates or clustering of channels in the patch How-ever, because it was not possible to distinguish between these two possibilities, we assume that each level above the baseline corresponds to a single channel, which opens and closes independently Unitary currents recorded at a holding potential of +100 mV are shown in Fig 2A, and the corresponding current amplitude distribution is depicted in Fig 2B Six chan-nels were present in the patch, as judged by the num-ber of simultaneous unitary current steps and histogram peaks A unitary conductance of 14.8 ± 0.6 pS (n¼ 17) was determined, between )80 and +80 mV, from the slope of the current–voltage rela-tionship (Fig 2C)

4,700 4,800 4,900 5,000 5,100 5,200

α1-PTH

4,921

B

12,600

DVA-(PIN)-GTIG

12,919

DVA-(PIN)-GTIGY

13,083.6

VA-(PIN)-GT

12,634.7

VA-(PIN)-GTIG

12,803.05

DVA-(PIN)-GT

12,750

A

Fig 1 MALDI-TOF mass spectrum of PIN-a and a1-PTH Deconvo-luted and reconstructed electrospray mass spectra from multi-charged ion spectra of the purified PIN-a (A) and a1-PTH (B) Note the homogeneity of the protein preparations.

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The selectivity of the channels for Na+ vs Cl– was

determined by increasing or decreasing the NaCl

con-centration in the bath solution In the presence of a

high NaCl concentration (440 mm instead of 140 mm)

in the bath, the reversal potential of the current

recor-ded in response to potential ramps shifted from 0 to

)25 ± 1 mV (n ¼ 3, Fig 2D), which is close to the

)28 mV theoretical equilibrium potential for Na+(the

equilibrium potential for Cl–was +29.6 mV under this

condition) Similarly, in the presence of a low NaCl

concentration (40 mm instead of 140 mm) in the bath,

the reversal potential of the current shifted from 0 to

+24 mV (data not shown), which is close to the

+30 mV equilibrium potential for Na+ The Na+ to

Cl– permeability ratio (PNa⁄ PCl) was 13 (n ¼ 5) To

determine the K+ to Na+ permeability ratio

(PK⁄ PNa), we replaced the bath NaCl with KCl When

140 mm KCl was perfused in the bath solution, the

current recorded in response to a potential ramp

showed an almost linear current–voltage

relation-ship, and it had a reversal potential of)9.2 ± 0.8 mV

(n¼ 8) Under these conditions, the permeability ratio

was 1.43 ± 0.04 (n¼ 8) These results indicate that

PIN-a forms a cationic channel, the permeability

sequence of which is K+> Na+ Cl–

a1-PTH forms ionic channels in giant liposomes Giant liposomes containing a1-PTH also produced excised patches with seals of high resistance Channel activity was found in 31 ( 41%) of 75 recorded pat-ches Single channels with a high unitary conductance and single channels with a low unitary conductance were detected in 32% (n¼ 10) and 68% (n ¼ 21) of the recordings, respectively In two independent experi-ments, low-conductance and high-conductance open-ings were detected simultaneously in the same patch, but these data have not been included in this study because of difficulties with their analysis

Typical current recordings through high-conduct-ance channels formed by a1-PTH are shown in Fig 3A The unitary conductance was 125 and 100 pS

at holding potentials of +100 and )100 mV, respect-ively Figure 3B depicts the current vs voltage plot at different holding potentials in the presence of 140 mm and 40 mm NaCl in the bath solution When the bath concentration of NaCl was decreased, the reversal potential of the current shifted from 0 to )20 mV, which is close to the )28 mV equilibrium potential for Cl– The calculated Cl– to Na+permeability ratio (PCl⁄ PNa) was  7, which indicates that the

high-500 ms

1 pA

500 ms

1 pA

5 s

1 pA

V (mV)

-1.5

-1.0

-0.5

0.5

1.0

1.5

C

I (pA)

100

-100 -50

50 100

V (mV)

D

I (pA)

I (pA)

1.5

Fig 2 Ion-channel activities exhibited by giant liposomes containing PIN-a (A) Unitary current traces recorded at a holding potent-ial of +100 mV The zero current level is indicated by the dotted line, and channel openings are indicated by upward deflect-ions The arrows show in an expanded time base the corresponding unitary currents (B) Time distribution of current amplitude corresponding to the recordings shown in (A) The time was expressed as a percent-age of the total recording time (C) Current– voltage relationship obtained from current amplitude distributions at various holding potentials A unitary conductance of 14.8 ± 0.6 pS (n ¼ 17) was determined from the slope of the relationship by linear regression between )80 and +80 mV (D) Representative currents recorded during potential ramps from )100 to +100 mV in the presence of either 140 or 440 m M NaCl

in the bathing solution Under these condit-ions, the voltages corresponding to zero current were 0 and )24.3 mV (arrow), respectively.

Trang 4

conductance channel formed by a1-PTH is an anionic

channel The Ca2+ selectivity of the channels was nil

Indeed, when the concentration of CaCl2was increased

from 2.6 mm to 10 or 20 mm in the bath solution, no

significant effect on current amplitude or reversal

potential values was detected in response to potential

ramps (data not shown)

Currents through low-conductance channels formed

by a1-PTH were recorded at holding potentials varying

from 0 to ± 80 mV in steps of 40 mV (Fig 4A)

Unit-ary conductances of 46 ± 5 and 34 ± 2 pS were

cal-culated from current potential relationships at holding

potentials of +100 and )100 mV, respectively

(Fig 4B), observed during 21 experiments using

sym-metrical NaCl (140 mm, n¼ 18) or sodium gluconate

(140 mm, n¼ 3) concentrations When the NaCl

concentration in the bath solution was decreased from

140 to 40 mm, the reversal potential of the current recorded in response to potential ramps shifted from 0

to +23 mV (Fig 4C), which is close to the Na+ equi-librium potential (+ 27.8 mV) A PNa⁄ PCl of 11 was calculated The low-conductance channels were almost equally selective to Na+ and K+ The PK⁄ PNa was

A

-60

-30

0

30

60

1 s

150 mV

50 mV

0 mV

-150 mV -50 mV

B

I ( pA)

V (mV)

-20 -15 -10 -5

5 10 15 20 25

-20 mV

I ( pA)

Fig 3 High-conductance channel activities exhibited by giant

lipo-somes containing a1-PTH (A) Unitary current traces recorded at

the indicated holding potentials (B) Current–voltage relationships in

the presence of either 140 m M NaCl (s) or 40 m M NaCl (d) in the

bathing solution Under these conditions, the voltages

correspond-ing to zero current were 0 and )20 mV (arrow), respectively.

A

-20 0 20

1 s

80 mV

40 mV

0 mV

-80 mV -40 mV

B

V (mV)

I (pA)

-4 -2

2 4 6 8

23 mV

V (mV)

I (pA)

-100 -50

50

100

C

Fig 4 Low-conductance channel activities exhibited by giant lipo-somes containing a1-PTH (A) Unitary current traces recorded in response to holding potentials varying from 0 to ± 80 in steps of

40 mV (B) Representative current–voltage relationship The calcula-ted unitary conductance was 51 and 35 pS at holding potentials of +100 mV and )100 mV, respectively (C) Representative currents recorded during potential ramps from )100 mV to +100 mV in the presence of either 140 or 40 m M NaCl in the bathing solution Under these conditions, the voltages corresponding to zero current were 0 and +23 mV (arrow), respectively.

Trang 5

1.10 ± 0.04 (n¼ 4), as calculated from changes in

the current reversal potential, e.g from 0 to

)2.5 ± 1.1 mV (n ¼ 4), brought about by replacing

NaCl (140 mm) with KCl (140 mm) in the bath

solu-tion These results indicate that the low-conductance

channel formed by a1-PTH is a cationic channel

The selectivity of the low-conductance channel to

bivalent cations was studied by changing the CaCl2

concentration in the bath solution Figure 5A shows

unitary currents, recorded at a holding potential of

0 mV, in the presence of 2.6 mm (control conditions)

and 20 mm CaCl2 In response to potential ramps,

the reversal potential shifted from 0 (Fig 5B) to

)8.0 ± 0.8 mV (n ¼ 4, Fig 5C) when the CaCl2

con-centration was increased from 2.6 to 10 mm, and it

was )13.3 ± 0.4 mV (n ¼ 5) when the CaCl2

concen-tration was 20 mm Under these conditions, the

expec-ted equilibrium potential calculaexpec-ted for Ca2+ was

)17.3 mV and )26.2 mV for 10 and 20 mm CaCl2,

respectively A Ca2+ to Na+ permeability ratio

(PCa⁄ PNa) of 5 was calculated from the changes in the

measured reversal potential Thus, the relative ionic

permeability sequence for the cationic channel formed

by a1-PTH is Ca2+> Na+ K+ Cl–

Effects of a1-PTH and PIN-a on isolated mouse

neuromuscular preparations

The addition of a1-PTH (0.01–1 lm) to the

physiologi-cal medium bathing isolated preparations produced a

concentration-dependent decrease in muscle twitches

and tetanic responses evoked by nerve stimulation at

0.2 and 40 Hz, respectively (Fig 6A) The

concentra-tion of a1-PTH that reduced the contracconcentra-tion amplitude

by 50% was 0.16 lm (Fig 6B) Complete blockade of

nerve-evoked muscle twitches and tetanic responses

occurred with 1 lm a1-PTH (n¼ 10), and the

block-ade was not reversed after extensive washing with the

standard physiological solution Similar concentrations

of a1-PTH also blocked twitches evoked by direct

electric stimulation of the muscle (Fig 6A,B) Thus,

a1-PTH is toxic to isolated mouse phrenic nerve⁄

hemi-diaphragm muscle preparations In contrast, when we

examined the ability of PIN-a (0.01–1 lm) to alter

muscle twitches and tetanic responses evoked by nerve

stimulation at 0.2 and 40 Hz, respectively, no

signifi-cant changes were detected in the contraction

ampli-tude (Fig 6B)

Membrane permeability changes caused by the

pore-forming ability of a1-PTH may explain the above

effects Therefore, we performed intracellular

record-ings to measure the effect of a1-PTH and PIN-a on

the resting membrane potential of mouse

hemidia-phragm muscle fibres When added to the standard medium, a1-PTH (0.05–1 lm) caused dose-dependent membrane depolarization (Fig 7A) A representative recording of the time course of 1 lm a1-PTH-induced depolarization of skeletal muscle fibres is shown in Fig 7B The time required by a1-PTH to exert

4 pA

0 pA

5 s

4 pA

0 pA

Control CaCl 2 (20mM in bath)

0 mV

min

A

V (mV)

I (pA)

-100 -50

50 100

-100 -50

50

100

I (pA)

V (mV)

B

C

Fig 5 Low-conductance channel selectivity for Ca2+ (A) Current traces recorded at a holding potential of 0 mV when the bath con-centration of CaCl2was increased from 2.6 m M (control) to 20 m M (arrow) The dotted lines indicate the zero current level The arrows show in an expanded time basis unitary currents (B,C) Representa-tive currents recorded during the same experiment in response to potential ramps from )100 mV to +100 mV in the presence of either 2.6 m M (B) or 10 m M (C) CaCl2in the bathing solution Under these conditions, the voltages corresponding to zero current were

0 (B) and )9 mV (C, arrow).

Trang 6

maximal depolarization was 3.5 ± 0.8 min (n¼ 4).

The magnitude of the depolarization was independent

of the external CaCl2 concentration between 0 and

2 mm (Fig 7C) However, when a1-PTH was added to

the standard medium in which the CaCl2concentration

was raised from 2 mm to 5 or 10 mm, no significant

change was detected in the resting membrane potential

of the muscle fibres (Fig 7B,C) In contrast with the

marked effect of a1-PTH, PIN-a (0.05–1 lm) did not

significantly alter the resting membrane potential of

the muscle fibres (Fig 7A) However, at a higher

con-centration (10 lm), the protein hyperpolarized the

muscle membrane by 21 ± 2.5 mV within about 5 min

(n¼ 4)

Analysis of synaptic transmission at single

neuro-muscular junctions revealed that a1-PTH (0.05–1 lm)

produced a dose-dependent decrease in endplate

poten-tial (EPP) amplitude Thus, in the presence of 0.25 lm

a1-PTH, EPPs had a subthreshold amplitude, being

unable to reach the threshold for action potential

gen-eration in muscle fibres, and were almost completely

blocked by 1 lm a1-PTH (Fig 8A) Parallel recordings

of spontaneous miniature endplate potentials (MEPPs) showed that 0.5 lm a1-PTH increased the frequency of MEPPs Thus, MEPP frequency was 0.7 ± 0.2 s-1 (n¼ 12) in control conditions and 6.7 ± 0.4 s1(n¼ 6) after the addition of 0.5 lm a1-PTH In addition, a1-PTH caused a marked decrease in MEPP ampli-tude, which attained the basal noise level with 1 lm a1-PTH (Fig 8B) This precluded the recording of

A

B

Fig 6 Effects of a1-PTH and PIN-a on nerve-evoked and directly

elicited muscle twitches (A) Superimposed tracings of muscle

twit-ches evoked by nerve stimulation (left panel, 0.2 Hz), tetanic nerve

stimulation (middle panel, 40 Hz), and direct muscle stimulation

(right panel) Tracings were recorded before and after 20 min

expo-sure to a1-PTH (0.05–1 l M ) (B) Dose–response curves of the

effects of a1-PTH (circles) and PIN-a (squares) on nerve-evoked

(filled symbols), and directly elicited muscle twitch (s) The twitch

tension is expressed with respect to controls and as means ± SEM

for n experiments (numbers beside data points) Note the complete

blockade of the twitch response in the presence of 1 l M a1-PTH,

and the quasi-absence of effect of similar concentrations of PIN-a.

Protein concentration

α1-PTH (2 m M CaCl2) PIN-a (2 m M CaCl2)

R -90

-80 -70 -60 -50 -40 -30 -20 -10 0

A

Control α1- PTH (1 µ M ) -90

-80 -70 -60 -50 -40 -30 -20 -10 0

C CaCl2 concentration

0 -10 -20 -30 -40 -50 -60 -70 -80

0 1 2 3 4 5 6 7 29 30 31 32

Time (min)

1 µ M α1-PTH (2 m M CaCl2)

1 µ M α1-PTH (10 m M CaCl2)

B

//

//

//

Fig 7 Effects of a1-PTH and PIN-a on the resting membrane potential of skeletal muscle fibres (A), and the influence of extracell-ular Ca 2+ concentration on the effect of a1-PTH (B and C) Note that in (A) only a1-PTH produces membrane depolarization, and in (B) and (C) increasing extracellular Ca 2+ concentration (from 2 to

10 m M ) markedly reduces a1-PTH-induced muscle depolarization, whereas decreasing extracellular Ca 2+ concentration (from 2 to

0 m M ) has no significant effect In (A) and (C), each column repre-sents the mean ± SEM obtained from 3 to 31 fibres In (B), the points represent the membrane potential of single muscle fibres as

a function of time after addition of a1-PTH to the medium.

Trang 7

MEPPs with concentrations higher than 0.5 lm

a1-PTH The above results indicate that a1-PTH,

within the range of concentrations studied, causes

per-meability changes in the presynaptic and postsynaptic

membranes of the neuromuscular junction In contrast,

MEPPs (Fig 8C) and EPPs were not significantly

affected by 1 lm PIN-a

Cytotoxic effects of a1-PTH and PIN-a on

neuroblastoma (NG108-15) cells

The effects of a1-PTH and PIN-a were studied on the

morphology of NG108-15 cells stained with the

fluor-escent dye FM1-43 and imaged with a confocal laser

scanning microscope (see Experimental procedures)

Images from each experiment were processed

identic-ally, and the effects were quantified using the same

cells examined before and during the action of the

proteins The 3D projected area of cells was measured

as an index of cell volume The addition of 10 lm a1-PTH to the standard mammalian physiological solution (e.g containing 2 mm CaCl2) produced, after

a latent period of about 15 min, a marked increase in the fluorescence intensity and a slight but significant (P¼ 0.0001) swelling of the cells (Fig 9Ab) Within 30–45 min, the 3D projected area of the cells reached a maximum increase of 128 ± 17% (n¼ 14), when com-pared with control values In addition, large membrane bleb formation followed by bleb dilation was consis-tently observed, and, in most cases, the blebs attained the size of the cells A similar increase in both fluores-cence intensity and 3D projected area occurred when the cells were exposed to 10 lm a1-PTH in a CaCl2 -free medium However, under these conditions, bleb formation was not observed (Fig 9Ad) In contrast, exposure to 10 lm PIN-a had no detectable effect on the morphology of NG108-15 cells (Fig 9Bc), although higher concentrations (50 and 100 lm) pro-duced a 10–15% decrease in the cells’ 3D projected area (Fig 9Bb,c)

Effects of a1-PTH and PIN-a on the actin network

of NG108-15 cells The significant membrane blebbing observed in the presence of a1-PTH, but not in the presence of

PIN-a, prompted us to determine whether the two pro-teins affect the cytoskeleton of NG108-15 cells Thus, immunofluorescence studies were performed to detect eventual changes in the actin network organization after exposure to a1-PTH (10 lm) or PIN-a (10 lm) for 2–4 h In comparison with control cells, and with cells treated with PIN-a, significant changes in fila-mentous actin immunolabelling distribution were observed in cells treated with a1-PTH (Fig 9C) Dis-organization and disarray of actin were reflected by disruption and clumping of actin filaments, which was depicted as a punctuate pattern throughout the cytoplasm (Fig 9Cb) Similar results were observed

in NG108-15 cells after AlexaFluor-594-conjugated phalloidin staining to visualize F-actin (data not shown)

Discussion

In this work, the ion channels formed by PIN-a and a1-PTH reconstituted into giant liposomes were characterized, and their toxicity examined in murine isolated neuromuscular preparations and cultured NG108-15 cells To our knowledge, this is the first study to demonstrate that highly purified a1-PTH

0.5 mV

1.00 µ M

5 ms

C

0.25 µ M

0.00 µ M

20 mV

1.00 µ M α1-PTH

5 ms

A

B 0.00 µ M

0.5 mV

5 ms

Fig 8 Effects of a1-PTH and PIN-a on nerve-evoked action

potent-ial, EPPs and MEPPs recorded from isolated hemidiaphragm

mus-cles (A) Single action potential recorded before (left trace), and

EPPs recorded after, 20 min exposure to 0.25 l M (middle trace)

and 1 l M (right trace) a1-PTH The arrow indicates the stimulation

artefact of the phrenic nerve (B) Average of 30 sequential MEPPs

recorded before (left trace) and after 20 min exposure to 0.5 l M

(middle trace) and 1 l M a1-PTH (right trace) (C) Average of 30

sequential MEPPs recorded before (left trace) and after 20 min

exposure to 1 l M PIN-a (right trace) Note the subthreshold EPP (A,

middle trace), the reduction and complete block of averaged

MEPPs induced by a1-PTH (B, right trace), and the absence of

effect of PIN-a on the amplitude of averaged MEPPs (C, right

trace) Note the different scales in A, B and C.

Trang 8

forms ion channels in biological and artificial

mem-branes In addition, we found that PIN-a forms a

cat-ion-selective channel with a 15 pS conductance This

channel is 13 times more permeable to a univalent

cat-ion (Na+) than to Cl– and 1.4-fold more permeable to

K+ than to Na+ These results considerably extend

those previously obtained on voltage-clamped Xenopus

oocytes [16]

In the case of a1-PTH, two types of channels with

different conductance and selectivity were detected

One of them is an anion channel with a conductance

larger than 100 pS (high-conductance channel), which

is 7 times more permeable to Cl– than to Na+ Our

results constitute the first description of single-channel

anion currents induced by a1-PTH The

low-conduct-ance channel formed by a1-PTH is a cationic channel

with single unitary conductance of 30–45 pS, which is

11 times more permeable to Na+than to Cl–, and has

a permeability ratio between Na+and K+ close to 1

However, this channel is 5 times more permeable to

Ca2+ than to Na+ Thus, the cation selectivity order

for this channel is the following: Ca2+> Na+ K+

These results are consistent with and extend

previ-ous observations suggesting that PTHs form

cation-selective ion channels, and in particular with data

obtained with b-PTH showing the formation of

cation-selective ion channels in artificial lipid bilayer

mem-branes and in the plasmalemma of rat hippocampal

neurons [14]

Although a concentration-dependent study of

a1-PTH has not been performed, it is possible that the

two different channel behaviours detected are the

con-sequence of protein–protein interactions in the

recon-stituted system, leading to channel clustering or similar

processes Thus, it is likely that progressive recruitment

of additional monomers will contribute to increase the pore size The formation of transmembrane chan-nels⁄ pores by bundles of amphipathic a-helices of a1-PTH and PIN-a polypeptides may occur via a ‘bar-rel-stave’ mechanism [19], in such a manner that their hydrophobic surfaces interact with the lipid core of the membrane and their hydrophilic surfaces point inward, producing an aqueous pore According to this model,

10 µm

10 µm

10 µ M α1-PTH (0 m M CaCl2)

Control (0 m M CaCl2)

Control 10 µ M α1-PTH 10 µ M PIN-a

* P > 0.02

* * P< 0.002

12

20

* *

16

* * 16

* * 34

21 20

Concentration (time of application)

10 µ M

(90 min)

50 µ M

(30min)

50 µ M

(60 min)

50 µ M

(120 min)

100 µ M

(15 min)

100 µ M

(30 min)

100 µ M

(90 min) 0.0

0.2 0.4 0.6 0.8 1.0 1.2 c

B A

5 µm

Fig 9 Effects of a1-PTH and PIN-a on NG108-15 cells In (A) and

(B), the cells were stained with 2 l M FM1-43 dye for 30 min, and

thereafter abundantly washed with dye-free solution before imaging

and the addition of a1-PTH or PIN-a to the medium Cells imaged

before (Aa) and after (Ab) exposure to 10 l M a1-PTH in a Ca 2+

-con-taining medium Note the marked increase in fluorescence intensity

in the cells’ cytosol, the large membrane blebs (arrows), and the

increase in projected area of the cells Cells imaged before (Ac) and

after (Ad) exposure to 10 l M a1-PTH in a Ca 2+ -free medium Note

the absence of blebbing, but a similar increase in cells’ cytosol

fluorescence intensity (B) Cells were imaged before (Ba) and after

(Bb) 50 l M PIN-a exposure to a Ca 2+ -containing medium In (Bc),

the bars indicate the relative projected area of the cells as a

funct-ion of PIN-a concentratfunct-ion and time of exposure (C)

Immunostain-ing of actin under control conditions (Ca) and after exposure of the

cells to either 10 l M a1-PTH (Cb) or 10 l M PIN-a In (Cb), note the

distinct distribution and clumping of the immunolabelling.

Trang 9

progressive recruitment of monomers would increase

the pore size Under our conditions, once the cationic

pore is formed, the aggregation of further monomers

would not only augment the pore size, but also, by

exposing some amino-acid residues, create a new

ani-onic-selectivity filter Although this may explain the

different channel behaviours detected with a1-PTH,

further experiments are needed to support this model

In isolated mouse hemidiaphragm preparations,

a1-PTH completely blocked directly and indirectly

electrical muscle twitches As a1-PTH caused

mem-brane depolarization, voltage-dependent sodium

chan-nels must be inactivated and unable to generate action

potentials in muscle fibres a1-PTH effects can be

rela-ted to its predominant ability to form low-conductance

cationic-selective channels, as reported in liposomes

The fact that increasing external Ca2+prevented

mus-cle depolarization by a1-PTH is not surprising because

pore formation induced by PTHs and PINs is inhibited

by high Ca2+concentrations [14,16] Also, a1-PTH

eli-cited permeability changes that may depolarize nerve

terminals supplying the neuromuscular junction Such

an action would explain the decrease in evoked

trans-mitter release (revealed by the decrease in EPP

ampli-tudes) and the increased spontaneous quantal release

(manifested by an enhanced MEPP frequency) Thus,

both presynaptic and postsynaptic permeability

chan-ges co-operate to block neuromuscular transmission

and muscle contraction evoked by nerve stimulation

In contrast, no changes were detected with PIN-a,

except for hyperpolarization of the muscle membrane

when high concentrations were used This is expected

if one considers that PIN-a increases membrane

per-meability mainly to K+ ions and that the reversal

potential for K+ions is more negative than the resting

membrane potential of muscle fibres Therefore, the

increased permeability induced by PIN-a will result in

K+ outflux and, as a consequence, in membrane

hyperpolarization

The consequences of the pore-forming ability of

a1-PTH and PIN-a were also evaluated in NG108-15

cells stained with the styryl dye FM1-43 This vital dye

partitions into the plasma membrane and does not

ordinarily ‘flip-flop’ across it [20] During exposure of

cells to a1-PTH action, the fluorescent staining of the

cell’s membrane by the FM1-43 dye was particularly

useful for delineating membrane blebbing and

follow-ing the 3D projected area of the cells The

develop-ment of blebs in the presence of a1-PTH is probably

related to the membrane permeability changes it

indu-ces, as, in other neuronal cells, blebbing has been

asso-ciated with raised intracellular Na+concentration [21]

Also, a1-PTH-treated NG108-15 cells exhibited an

increase in FM1-43 fluorescence intensity, similar to that previously observed at the nodes of Ranvier of myelinated axons [15] This may be due to dye entry into cells via a1-PTH-formed channels, as previously reported for mechanotransducer channels [22] Another possibility is that the increased fluorescence intensity reflects changes in membrane potential, as FM1-43 has also been used as a voltage-sensitive dye [20] In this case, a 3.3% fluorescence increase per 100 mV poten-tial change would be expected This value is too low to account for the marked increase in FM1-43 fluores-cence intensity observed in NG108-15 cells FM1-43 has also been reported to be a useful probe for monit-oring phospholipid scrambling [23] Taking into account that one of the earliest detectable events in cells undergoing apoptosis is phospholipid scrambling [24], the FM1-43 fluorescence increase detected during a1-PTH action, together with membrane blebbing and disorganization and disarray of cytoskeletal actin, may represent apoptotic events involved in a1-PTH cyto-toxicity

Experimental procedures

Extraction and purification of PIN-a and a1-PTH

PIN-a (Mr 12 920) and a1-PTH (Mr 4921.89) were puri-fied from wheat seeds of Triticum aestivum sp., using a modification of previously described procedures [18,25] Briefly, 4 kg wheat endosperm flour was extracted with a 10-L solution containing 100 mm Tris buffer, 100 mm NaCl, 5 mm EDTA and 5% Triton X-114 (pH 7.8) After stirring (12 h, 4C) and centrifugation (8000 g, 30 min),

the supernatants were heated at 30C to allow phase par-titioning, and the upper, detergent-poor phase was discar-ded The lower, detergent-rich phase was diluted with

5 vol water and loaded on a column packed with a cation exchanger (SP Biobeads; Pharmacia, Montigny-le-Breton-neux, France) Proteins were eluted by applying a gradient from 0.02 to 0.7 m NaCl in Tris buffer without Triton X-114 Analysis of the collected fractions by SDS⁄ PAGE indicated that the PTHs were eluted as a single peak just after the PINs Separate pools of the PTH-containing and PIN-containing crude fractions were dialyzed against de-ionized water and freeze-dried, and a1-PTH, a2-PTH and b-PTH were separated (at room temperature) by semipre-parative RP-HPLC The HPLC column was packed with Nucleosil C18 (5 lm, 300 A˚), the PTHs were eluted with

an acetonitrile gradient (0.1% trifluoroacetic acid in deion-ized water to 0.1% trifluoroacetic acid in acetonitrile), and the fractions containing a1-PTH were pooled and freeze-dried after dilution with deionized water PIN-a was puri-fied from the crude, freeze-dried, PIN-containing fraction

by cation-exchange chromatography on a 6 mL Resource

Trang 10

S column (Pharmacia), as previously described [26] The

homogeneity of the purified a1-PTH and PIN-a

prepara-tions was monitored by MS, as detailed by Elmorjani

et al [27]

Reconstitution of PIN-a and a1-PTH into giant

liposomes

Giant liposomes were prepared by subjecting a mixture

(2 mL) of the protein (100 lg either PIN-a or a1-PTH) and

asolectin lipid vesicles (13 mm, in terms of lipid

phospho-rus) to a partial dehydration⁄ rehydration cycle, as reported

previously [28] After the partial dehydration⁄ rehydration

cycle, the diameter of the resulting giant multilamellar

lipo-somes ranged from 5 to 100 lm

Patch-clamp measurements

Aliquots (3–15 lL) of giant liposome preparations, in Petri

dishes (3.5 cm diameter), were mixed with 1 mL of the

buf-fer of choice (the bath solution) for electrical recording,

and unitary current recordings were performed using the

patch-clamp technique in an excised patch ‘inside out’

con-figuration, as previously described [29] Giga seals were

formed on giant liposomes with glass microelectrodes of 5–

10 MW resistance After sealing, withdrawal of the pipette

from the liposome surface resulted in an excised patch

Current was recorded with an EPC-9 patch-clamp amplifier

(Heka Elektronic, Lambrecht⁄ Pfalzt, Germany) at a gain of

50–100 mVÆpA)1and a filter setting of 10 kHz The holding

potential was applied to the interior of the patch pipette

The bath potential was maintained at virtual ground via an

agar bridge (V¼ Vbath) Vpipette), and the junction

poten-tial was compensated for when necessary To study the

ionic selectivity of the protein-induced channels, we

deter-mined the relative ionic permeabilities from the reversal

potentials of the currents recorded in solutions of various

compositions, in response to potential ramps [ +150 to

)150 mV (60 mVÆs)1) or +100 to )100 mV (40 mVÆs)1)]

They were calculated from changes in reversal potentials,

brought about by ion replacement based on the Goldman–

Hodgkin–Katz flux equation [30,31] The reversal potential

of a cationic current as a function of the concentration or

activity and the permeability of each ion species was

calcu-lated as previously described [32,33]

Patch-clamp data were analyzed off-line with TAC

soft-ware (Bruxton Corporation, Seattle, WA, USA) and Pulse

Fit (Heka Elektronic) software All measurements were

made at  25 C, and the pipette and bath solutions

usu-ally had the following composition:140 mm NaCl, 2.6 mm

CaCl2, 1.3 mm MgCl2, and 10 mm Hepes (adjusted to

pH 7.4 with NaOH) In some experiments, NaCl was

replaced by either KCl or sodium gluconate All reagents

and chemicals were purchased from Sigma Biochemical Co

(St Louis, MO, USA) and Merck (Darmstadt, Germany)

Electrophysiological and mechanical recordings

in isolated mouse hemidiaphragm muscles

Left and right hemidiaphragm muscles with their associated phrenic nerves were isolated from adult Swiss-Webster mice (20–25 g) killed by cervical vertebrae dislocation followed by immediate exsanguination Phrenic nerve⁄ hemidiaphragm muscle preparations were mounted in a Rhodorsil-lined (Rhoˆne-Poulenc, St Fons, France) Plexiglas chamber (2-mL

or 4-mL capacity) and bathed in a standard physiological solution gassed with pure O2 and composed of 154 mm NaCl, 5 mm KCl, 2 mm CaCl2, 1 mm MgCl2, 11 mm glucose, and 5 mm Hepes (adjusted to pH 7.4 with NaOH) Lyophilized PIN-a and a1-PTH were dissolved in 100 mm Hepes buffer and stored as 1-mm stock solutions at)18 C The stock solutions were diluted with the standard physiolo-gical solution before experiments were performed at room temperature All experiments on mice were carried out in accordance with the European Communities Council Directive of 24 November 1986 (86/609/EEC), regarding the ethical use of animals for experimental procedures

Membrane potentials and synaptic potentials were recor-ded with intracellular microelectrodes filled with 3 m KCl (8–18 MW resistance), using conventional techniques and

an Axoclamp-2A system (Axon Instruments, Union City,

CA, USA) Recordings were made continuously from the same endplate before and during treatment with the pro-teins being tested Electrical signals after amplification were collected and digitized, at a sampling rate of 25 kHz, with the aid of a computer equipped with an analogue-to-digital interface board (DT 2821; Data Translation, Marlboro,

MA, USA) Computerized data acquisition and analysis were performed with a program kindly provided by

J Dempster (University of Strathclyde, Scotland, UK) For twitch tension measurements, one of the tendons of the hemidiaphragm muscle was tied with silk thread, via an adjustable stainless steel hook, to an FT03 isometric transdu-cer (Grass Instruments, West Warwick, RI, USA), and the other tendon was pinned to the Rhodorsil-lined chamber Twitches were evoked either by stimulating the motor nerve

of isolated neuromuscular preparations via a suction micro-electrode adapted to the diameter of the nerve, or by direct muscle stimulation via an electrode assembly placed along the length of the fibres Pulses were supplied by a S-44 stimu-lator (Grass Instruments) at frequencies of 0.2–40 Hz For each preparation investigated, the resting tension was adjusted to obtain maximal contractile responses Signals from the isometric transducer were amplified, collected, and digitized with the aid of a computer equipped with a DT

2821 analogue-to-digital interface board (Data Translation)

Cultured neuroblastoma cells

Rodent neuroblastoma (NG108-15) cells were grown in monolayer cultures on glass coverslips using Dulbecco’s

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