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Mu¨ller, Institut fu¨r Physiologische Chemie, Abteilung Angewandte Molekularbiologie, Universita¨t, Duesbergweg 6, 55099 Mainz, Germany Fax: +49 6131 3925243 Tel: +49 6131 3925910 E-mail

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Lubomirskia baicalensis

Role of okadaic acid produced by symbiotic dinoflagellates

Werner E G Mu¨ller1,2, Sergey I Belikov2, Oxana V Kaluzhnaya1,2, Sanja Perovic´-Ottstadt1,

Ernesto Fattorusso3, Hiroshi Ushijima4, Anatoli Krasko1and Heinz C Schro¨der1

1 Institut fu¨r Physiologische Chemie, Abteilung Angewandte Molekularbiologie, Universita¨t Mainz, Germany

2 Limnological Institute of the Siberian Branch of Russian Academy of Sciences, Irkutsk, Russia

3 Dipartimento di Chimica delle Sostanze Naturali, Universita` di Napoli ‘Federico II’, Italy

4 Department of Developmental Medical Sciences, Institute of International Health, The University of Tokyo, Japan

The taxon sponges (phylum Porifera) has been

surpris-ingly successful during evolutionary development This

metazoan phylum is the only one to have survived the

severe Varanger–Marinoan ice age (605–585 million years ago) of the Neo-Proterozoic eon (1000–520 million years ago), during which the earth was almost

Keywords

dinoflagellates; heat shock protein;

Lubomirskia baicalensis; okadaic acid;

protein phosphatase

Correspondence

W E G Mu¨ller, Institut fu¨r Physiologische

Chemie, Abteilung Angewandte

Molekularbiologie, Universita¨t,

Duesbergweg 6, 55099 Mainz, Germany

Fax: +49 6131 3925243

Tel: +49 6131 3925910

E-mail: wmueller@uni-mainz.de

Website: http://www.biotecmarin.de/

Database

The sequences from Lubomirskia

baicalen-sis reported here have been deposited in

the GenBank database under the accession

numbers AM392283 (protein phosphatase

LUBAIHSP70PP1) and AM392284 (heat

shock protein-70 LUBAIHSP70)

Note

This article is dedicated to Professor Michele

Sara`, Professor of Zoology at the University

of Genova, for his outstanding contributions

to marine biology, 1926–2006

(Received 16 August 2006, revised 21

October 2006, accepted 27 October 2006)

doi:10.1111/j.1742-4658.2006.05559.x

The endemic freshwater sponge Lubomirskia baicalensis lives in Lake Bai-kal in winter (samples from March have been studied) under complete ice cover at near 0C, and in summer in open water at 17 C (September) In March, specimens show high metabolic activity as reflected by the produc-tion of gametes L baicalensis lives in symbiosis with green dinoflagellates, which are related to Gymnodinium sanguineum Here we show that these dinoflagellates produce the toxin okadaic acid (OA), which is present as a free molecule as well as in a protein-bound state In metazoans OA inhibits both protein phosphatase-2A and protein phosphatase-1 (PP1) Only cDNA corresponding to PP1 could be identified in L baicalensis and sub-sequently isolated from a L baicalensis cDNA library The deduced poly-peptide has a molecular mass of 36 802 Da and shares the characteristic domains known from other protein phosphatases As determined by west-ern blot analysis, the relative amount of PP1 is almost the same in March (under ice) and September (summer) PP1 is not inhibited by low OA con-centrations (100 nm); concon-centrations above 300 nm are required for inhibi-tion A sponge cell culture system (primmorphs) was used to show that at low temperatures (4C) expression of hsp70 is strongly induced and hsp70 synthesis is augmented after incubation with 100 nm OA to levels measured

at 17C In the enriched extract, PP1 activity at 4 C is close to that meas-ured at 17C Immunoabsorption experiments revealed that hsp70 contri-butes to the high protein phosphatase activity at 4C From these data we conclude that the toxin OA is required for the expression of hsp70 at low temperature, and therefore contributes to the cold resistance of the sponge

Abbreviations

hsp70, heat shock protein-70; OA, okadaic acid; PP1, protein phosphatase-1; PP2A, protein phosphatase-2A.

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completely covered by ice; most organisms became

extinct during this period [1] As ‘living fossils’ [2],

spon-ges represent evolutionarily the oldest extant taxon, and

thus allow insight into the genome organization of

ani-mals that lived prior to the ‘Cambrian Explosion’ At

that time, sponges existed exclusively in the marine

envi-ronment, whereas later some taxa also occupied

fresh-water biotopes (during the Cenozoic period) From

cosmopolitan freshwater species, e.g Ephydatia

fluvia-tilis, endemic species branched off in ‘old lakes’ Lake

Baikal (Siberia), for example, harbors many prominent

endemic sponges [3] Major reasons for the recent rapid

evolution of the endemic sponge fauna in some areas,

that still continues, are: (a) successful adaptation to

environmental conditions, (b) dominance of sexual

reproduction over asexual reproduction in sponges, and

(c) differences in the habitats (littoral on rocks or on

calcifying algae, e.g Chara sp.) [4]

In Lake Baikal the dominant endemic sponge species

Lubomirskia baicalensis lives in a cold environment; in

March at an ambient temperature of)0.5 C and in

Sep-tember at around 17C [5] These animals, which grow

at depths of 1–20 m, maintain constant metabolic

activit-ies with pumping rates similar to those of specactivit-ies that live

at 15–20C [6,7] Surprisingly, L baicalensis produces

gametes and embryos in March when the lake is

com-pletely covered by 1 m of ice One major source of

essen-tial organic carbon for the animals during this season is

their ecological, symbiotic relationship with

chlorophyll-containing dinoflagellates [5] It has been reported

previ-ously that these symbiotic ‘Zoochlorellae’ exist in a 3-mm

thick external layer of the sponge [8] Field observations

revealed that, in the absence of light, the dinoflagellates

die and are removed from the sponge specimens which

likewise die (W E G Mu¨ller, University of Mainz,

unpublished results) In L baicalensis these protists,

which are closely related to Gymnodinium sanguineum,

produce glycerol and transfer this intermediate

metabo-lite via an aquaporin channel into the sponge cells

(W E G Mu¨ller, University of Mainz, submitted) This

raises two questions: how do the sponges live in the cold

environment; or, more specifically, (a) how do they solve

the problem of protein folding at low temperature, and

(b) how do they overcome the barrier of the required

acti-vation energy for the enzyme-mediated catalysis?

This study mainly addresses the first question It is

known that the growth of Escherichia coli at low

tem-perature is facilitated by chaperonins [9] The question

is, which sensor in these microorganisms regulates the

expression of the respective heat shock proteins? Here

we tested the hypothesis that secondary metabolites

produced by the symbiotic⁄ commensalic organisms in

sponges contribute to the cold stress response

The dinoflagellates of the taxon Gymnodinium identi-fied in L baicalensis are related to G sanguineum (Alve-olata; Dinophyceae; Gymnodiniales; Gymnodiniaceae; Gymnodinium), which has been described as a compo-nent of harmful algal blooms and has been found to be hemolytic and ichthyotoxic [10] One toxin often produced in these algae [11] is okadaic acid (OA), a polyether C38 fatty acid, originally isolated from Hali-chondria okadaii [12] The major targets of OA in all metazoans hitherto studied are the catalytic subunits of the proteins phosphatase-1 (PP1) and protein phos-phatase-2A (PP2A) which are sensitively inhibited at nanomolar concentrations (the 50% inhibitory con-centration for PP1 is 3–150 nm and that for PP2A is 0.03–0.2 nm) [11]

Here we show that OA is present in L baicalensis, where it is synthesized by the dinoflagellates In order

to perform functional studies between OA and PP1, the cDNA coding for PP1 had to be identified in L baical-ensis This polypeptide shares high sequence similarity with mammalian PP1 Antibodies against PP1 allowed its assessment during temperature-dependent expression

in vitro (cell culture) and in vivo (animals) At lower concentrations (< 100 nm), OA has no effect on the level and activity of the protein phosphatase(s) but induces the expression of heat shock protein-70 (hsp70) From earlier studies it is known that OA can trigger the expression of heat shock proteins in tissues [13] We applied the in vivo sponge cell culture system, the primmorphs [2], to demonstrate that in primmorphs

at 4C, OA upregulates both the expression of hsp70 transcripts and the amount of hsp70 protein to levels found at the ambient temperature of 17C Subsequent depletion experiments with antibodies against hsp70 showed that functionally active chaperon⁄ hsp70 mole-cules are required for full protein phosphatase activity

at low temperature From the data we conclude that at lower concentrations (< 100 nm) the secondary meta-bolite OA mediates⁄ controls in L baicalensis the cold stress defense, whereas higher concentrations are required to inhibit the protein phosphatase(s) It has been established that sponges, like Suberites domuncula [14] or L baicalensis, which contain symbiotic micro-organisms, display a stronger ‘resistance’ to OA; with regard to S domuncula only concentrations > 300 nm have a significant effect on protein synthesis

Results

L baicalensis specimens in winter and summer Animals were collected during September 2005 and March 2006 (Fig 1A,B) During these seasons, the

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animals have a bright green color, which is due to the

high abundance of dinoflagellates (Fig 1C,D) related

to the taxon G sanguineum (Alveolata; W E G Mu¨ller,

University of Mainz, submitted) Interestingly, during

winter the sponges form sexual propagation bodies,

reflecting an active metabolism Figure 1E shows one

spermatogenic cyst

Presence of OA in L baicalensis

The OA concentration in L baicalensis was determined

using HPLC⁄ MS analysis to be 83 ± 9 ngÆg)1 wet

weight (100 nm; March), whereas tissue from

speci-mens collected in September had a lower OA content

of 57 ± 6 ngÆg)1(70 nm) These values were confirmed

by competitive ELISA giving concentrations of

75 ngÆg)1(March) and 45 ngÆg)1(September)

Protein-coupled OA in L baicalensis

Protein extracts were prepared from specimen tissue

collected in March This preparation was subjected to

SDS⁄ PAGE (10% gel; Fig 2, lane a) After transfer,

blots were incubated with anti-OA sera (pAb-OA) This

revealed one prominent protein band of 14 kDa (Fig 2,

lane b) The specificity of the reaction was proven using

antibodies that had been adsorbed with OA bound to

the FID-33 peptide; under these conditions the

immu-noreaction of the 14 kDa band was strongly suppressed

(Fig 2, lane c) In contrast, the signal at 14 kDa was

of the same strength when membranes were incubated

with pAb-OA, which had been pretreated with FID-33

prior to use in the western blots (not shown)

Identification dinoflagellates in tissue using anti-OA sera

Slices of sponge tissue were prepared and reacted with pAb-OA The antibodies stained the dinoflagellates very brightly, whereas the sponge cells did not react

A

B

F

C

D

E

I

Fig 1 L baicalensis specimens during late summer (September) (A)

and the ice cover season (March) (B) In both seasons sponges

con-tain associated dinoflagellates (taxon Gymnodinium) Cross-sections

were prepared and examined using transmission electron

microsco-py (C, D) Sections through a branch from a September specimen

show the abundantly present dinoflagellates (d) that are assembled

at the rim of the green branches (E) Frequently the specimens

dur-ing the March season contain spermatogenic cysts (sc)

Identifica-tion of OA-producing dinoflagellates in L baicalensis (F–K) (F, I)

Slices were prepared from tissue of L baicalensis and the cells were

visualized Nomarsky interference contrast optics; dinoflagellates

(d) as well as sponge cells (s) are marked (G) In one series, the

slices were reacted with pAb-OA and then with Cy3-conjugated goat

anti-(rabbit IgG) and finally inspected by immunofluorescence

(wavelength ¼ 546 nm) (H) Autofluorescence of the chlorophyll in

the dinoflagellates was detected at a wavelength of 490 nm (J) In

parallel, the slices were reacted with pAb-OA, which had been

pretreated with OA, coupled to the FID-33 oligopeptide and then

with the labeled secondary antibodies (K) The same area was also

analyzed with a wave-length of 490 nm Scale bar ¼10 lm.

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(Fig 1G); using Nomarsky interference contrast optics

the granule-containing dinoflagellates could be

identi-fied (Fig 1F) As further evidence for the localization

of the dinoflagellates, slices were illuminated with

green fluorescent light (490 nm) to identify

dinoflagel-lates based on the autofluorescence of their chlorophyll

(Fig 1H) Again, the dinoflagellates were highlighted

in areas positive for pAb-OA In a parallel series,

sec-tions were treated with adsorbed antibodies against

OA; this preparation showed a slight signal only very

occasionally (Fig 1J) Dinoflagellates could again be

visualized by their autofluorescence (Fig 1K)

L baicalensis PP1 catalytic subunit

Complete cDNA encoding the L baicalensis PP1

pro-tein (LBPP1) was obtained from a cDNA library using

a degenerate primer against the Ser⁄ Thr-specific

pro-tein phosphatase signature of mammalian propro-tein

phosphatases The ORF between nucleotides 60–62

and 1057–1059(stop) codes for a 319 amino acid

polypeptide (PP1_LUBAI) with a predicted size of

36 802 Da (Fig 3A); the sequence was termed

PP1_LUBAI Like the related mammalian sequences,

the sponge protein comprises a characteristic Ser⁄

Thr-specific protein phosphatase signature (amino acids

121 and 126) and the conserved

matallophosphoest-erase (amino acids 57 and 252) The calcineurin-like

phosphoesterase (amino acids 57 and 252) overlaps

with the latter region Similarity between the sponge

molecule and other metazoan PP1 sequences is high;

the sponge PP1 shares 288 similar and 271 identical

amino acids with human PP1 (length: 323 amino acids), known to bind to OA (Fig 3A) The overall similarity⁄ homology to metazoan sequences is

 80% ⁄ 70% For the alignment in Fig 3A, the human protein with the highest similarity score was used (‘Expect value [E]’ 2e-162) [15]; this phosphatase is known to function as PP1 (catalytic subunit, gamma isoforms)

A phylogenetic tree was computed after alignment

of the metazoan sequences with yeast and plant-related PP1 (Fig 3B) The tree was rooted with the highest similar phosphatases from Arabidopsis thaliana (pro-tein phosphatase-type 1; NP_181514.1) and Saccharo-myces cerevisiae (type 1 Ser⁄ Thr protein phosphatase; NP_011059.1) Among the metazoan proteins, the sponge phosphatase clusters together with that of Dro-sophila melanogaster (Ser⁄ Thr protein phosphatase; CAA49594.1), while the Caenorhabditis elegans protein (even-like phosphatases family member (NP_001022616.1) forms a separate branch together with the human sequence Both branches are separated only with low significance

Relative PP1 content Because of the high sequence similarity between L bai-calensis PP1 and the corresponding mammalian phos-phatases it was possible to use a commercial antibody for the western blots Extracts were size-separated by SDS⁄ PAGE and either stained with Coomassie Brilli-ant Blue (Fig 3C, lane a) or the proteins were trans-ferred to poly(vinylidene difluoride) membranes and reacted with antibodies against PP1, as described in Experimental procedures Extracts from animals obtained in both March (Fig 3, lane b) and September (Fig 3, lane c) show a strong signal at  37 kDa, cor-responding to the size of sponge PP1 In contrast, if the blots were reacted with adsorbed antibodies, the signals were strongly reduced (lanes d and e)

Phosphatase activity in the extract Extracts were prepared from sponge tissue specimens collected in March or September and subjected to the protein phosphatase assay described in Experimental procedures The specific enzyme activities in tissues from winter and summer animals were almost identical (22.6 ± 4.7 versus 23.4 ± 4.2 nmolÆmin)1Æmg)1) If OA was added, the reactions in the two series of experi-ments were inhibited dose-dependently; at 100 nm the activity differed from that seen in the controls (March, 17.3 ± 3.9 nmolÆmin)1Æmg)1; September, 19.2 ± 4.3 nmolÆmin)1Æmg)1) However, at 300 nm the activity

Fig 2 Identification of protein-coupled OA in L baicalensis.

Extracts were prepared and the protein size separated by

SDS ⁄ PAGE (10% gel) Lane a, the gel was stained with Coomassie

Brilliant Blue The proteins were blot transferred and the filters were

either incubated with anti-OA sera (lane b) or with the antibody

pre-paration, which had been preincubated with FID-33-OA which had

been adsorbed with FID-33-OA (lane c) M, marker proteins.

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decreased to  80% (March, 3.7 ± 1.9 nmolÆmin)1Æ

mg)1; September, 5.2 ± 1.6 nmolÆmin)1Æmg)1)

Expression level of hsp70 in animals and

primmorphs

The semiquantitative steady-state level of hsp70

tran-scripts in animals was in the same range, regardless of

whether the RNA had been isolated from specimens

collected in March or in September For these

Nor-thern blot studies the EST probe for hsp70 from

L baicalensis(LUBAIHSP70) was used (Fig 4A)

In order to assess the expression level under

con-trolled laboratory conditions, in vivo primmorphs were

incubated for 24 h at 4 and 17C Primmorphs were

incubated in the dark to suppress the metabolic

activ-ity of the remaining symbiotic algae Setting the

expression level at 4C to onefold, the amount of

hsp70 transcripts in the primmorph cells incubated at

17C was much higher (10-fold; Fig 4A) However,

if primmorphs were incubated at 4C together with

100 nm OA the amount of hsp70 transcripts was the same as that measured for cultures maintained at

17C The toxin had no strong effect on hsp70 expres-sion in cells at 17C (Fig 4A) In controls, a-tubulin expression was determined using the L baicalensis probe LUBAITUB in a parallel Northern blotting experiment Almost identical signal intensities were seen, confirming that the same amount of RNA was loaded onto the gels From these results, we conclude that OA induces hsp70 expression at the lower incuba-tion temperature

To support these studies, comparative Northern and western blot experiments were performed using hsp70 (LUBAIHSP70) or antibodies (mAb-HSP70) as the respective probes (Fig 4B) Again, the Northern blot

A

Fig 3 PP1 from L baicalensis (A, B) The PP1 sequence from L baicalensis (A) Alignment of the sponge PP1 protein (PP1_LUBAI) with the human PP1 which binds to OA (PP1_HUMAN; accession number 1JK7_A) Amino acids, identical in both sequences, are in inverted type and those similar in both sequences are shaded The characteristic Ser ⁄ Thr-specific protein phosphatase signature (S ⁄ Tp) and the conserved metallophosphoesterase (MetPhoEsterase) regions are marked (B) The phylogenetic tree is constructed from the two abovementioned sequences as well as the PP1 from D melanogaster (PP1_DROME; CAA49594.1), from C elegans (seven-like phosphatases family mem-ber) (PP1 CAEEL; NP_001022616.1), from S cerevisiae (PP1_YEAST; NP_011059.1) as well as from A thaliana (PP1_ARATH; NP_181514.1), which was used as outgroup to root the tree After alignment the tree was built Scale bar indicates an evolutionary distance

of 0.1 amino acid substitutions per position in the sequence (C) Identification of PP1 in tissue from L baicalensis In all lanes 10 lg of pro-tein were separated Lane a, the separated propro-teins were identified with Coomassie Brilliant Blue Western blot experiments: lanes b and c, the membranes were reacted with antibodies against PP1 (PcAb-PP1) and then with labelled secondary antibodies to visualize the immuno-complexes with the BM chemoluminescence substrate kit Samples from March (lane b) and September (lane c) were analyzed In parallel, membranes with the extracts were treated with adsorbed PcAb-PP1 (lanes d and e) The size markers are given.

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studies showed low expression of hsp70 in primmorphs

incubated at 4C or in the absence of OA, in

compar-ison with those incubated with OA or at 17C

(Fig 4B,a) Steady-state expression of the a-tubulin

gene is shown using the same amount of RNA for

ana-lysis The data from western blot experiments showed a

similar expression pattern; low levels of hsp70 in

cul-tures incubated at 4C and without OA, in comparison

with those incubated with the toxin and at higher

tem-perature (Fig 4B,b) From these data, we conclude that

the level of hsp70 is controlled in primmorphs at both

a transcriptional and translation level

Effect of depletion of hsp70 from extracts on the

activity of protein phosphatase(s)

An immunodepletion study was performed as described

in Experimental procedures Extracts were prepared

from animals collected in September and incubated at 4

or 17C Unexpectedly, enzyme activity at 4 C was

only 20% lower (18.1 ± 4.2 nmolÆmin)1Æmg)1) than that measured at 17C (22.7 ± 5.1 nmolÆmin)1Æmg)1) However, after incubation of the extracts for 60 min with antibodies against hsp70 the activity of the protein phosphatase was reduced at 4C to 5.3 ± 2.9 nmolÆ min)1Æmg)1, whereas the antibodies had no effect on activity at 17C (Fig 5) The adsorbed mAb-HSP70

A

b

Fig 4 Expression of heat shock protein hsp70 transcripts in ani-mals and primmorphs (A) Northern blot analysis RNA was extrac-ted both from animals, collecextrac-ted in March or September, and from primmorphs cultivated in vitro As indicated, the primmorphs were cultivated either 4 C or at 17 C for 24 h in the absence (–) or presence of 100 n M of OA (+) Then, total RNA was isolated and fractionated by electrophoresis, transferred to nylon membrane, and hybridized with the respective labeled probes; hsp70 (LUBAIHSP70) or a-tubulin (LUBAITUB) 2 lg of total RNA were loaded into each slot The relative degree of expression was corre-lated with that seen for the minimal expression in primmorphs at

4 C (set to onefold) (B) Comparison of the level of hsp70 tran-scripts and hsp70 protein in primmorphs, incubated at 4 or 17 C

in the absence (–) or presence of OA (+) As marked, the primmorphs were incubated at these two temperatures for 24 h and - ⁄ +OA Then extracts were prepared for Northern blotting (RNA) or western blotting (protein) (a) Northern blot: after size fraction and transfer the filter was hybridized with the hsp70 probe: N1, incubation at 4 C in the absence of OA; N2, at 4 C in the presence of OA; N3, incubation at 17 C in the absence of OA; N4, incubation at 17 C in the presence of OA In parallel, a filter was hybridized with a a-tubulin probe (b) From the same samples the proteins were extracted and subjected to western blot analysis Samples from cultures incubated at 4 C in the absence (lane W1) or presence of OA (W2) or at 17 C without (lane W3) or with OA (lane W3) are loaded onto the gel, and after separation and transfer probed with the antibodies mAb-HSP70 The relative expression levels, correlated to the values assessed for cultures at 4 C and without OA (set to onefold), are given.

Fig 5 Effect of antibodies against hsp70 on the activity of the pro-tein phosphatase in extracts from animals Extracts were prepared from animals, collected in summer and tested for protein phospha-tase activity at 4 or 17 C, as described in Experimental proce-dures Where indicated the samples were pretreated either with mAb-HSP70 or with adsorbed mAb-HSP70.

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preparation did not show a significant effect on the

enzyme activities From these results we conclude

that: (a) hsp70 proteins, which are supposedly

func-tionally active, are present in sponge extracts together

with the enzyme; and (b) hsp70 is required for the

full enzyme activity during incubation at lower

temperature

Discussion

OA is a secondary metabolite produced by free-living

microalgae, primarily by Prorocentrum lima [16] Other

dinoflagellates, e.g Gymnodinium sp., are also

consid-ered to be producers [17] Secondary metabolites are

surely not without metabolic function for the producer

or the host, because then they would have been

elimin-ated during evolution They have, however, no direct

role in the growth of the producing organism and are

considered not to play a key role in the maintenance

of cellular function but in defense [18] It remains

unexplained, however, why some secondary

metabo-lites, like OA, are synthesized not only by one taxon,

but by a whole range of microorganisms These

dinoflagellates are harbored in a series of hosts, e.g

mussels [11] or sponges such as H okadaii [12],

S domuncula [14] and Geodia cydonium (W E G

Mu¨ller, University of Mainz, unpublished results), or,

as shown here, in L baicalensis This latter finding is

surprising, because L baicalensis is a freshwater

sponge, in contrast to the others which are marine

ani-mals These findings suggest that OA has a crucial role

in the maintenance of a symbiotic relationship between

algae and host With S domuncula it has been shown

that OA augments the concentration-dependent

immune defense system against bacteria [14], and as

described recently, kills symbiotic⁄ parasitic annelids

[19] The dinoflagellates present in L baicalensis are

related to G sanguineum, a species that has been found

worldwide, especially in coastal waters [20]

We have shown that the dinoflagellates (G

sangui-neum) produce OA in L baicalensis For identification,

we applied antibodies raised against OA, which have

been previously qualified as specific for this secondary

metabolite [14,19] In cross-sections though L

baical-ensisthese antibodies reacted specifically with the

dino-flagellates; their signals could be suppressed by

adsorption with free OA Analytical measurements

revealed that the concentration of OA in L baicalensis

is  50 ngÆg)1 of tissue (70 nm), a level comparable

with that found in other sponges [14] In addition,

western blot analysis has shown that, like in extracts

prepared from S domuncula and L baicalensis, OA

exists in a covalent linkage with a protein of 14 kDa

This finding, first described in S domuncula [19], can

be explained as a depot⁄ storage form of the free OA

It is not known whether OA is released from the sponge into the surrounding aqueous habitat Previous studies with S domuncula have shown that in this sponge OA accumulates in the epithelial layers of the aquiferous system within the animals, suggesting that

OA is involved in defense against microbial invaders [21] Because L baicalensis ingests⁄ feeds on microor-ganisms and plankton [7] it is very likely that OA is accumulated in the aquiferous canal system and acts

as a protecting metabolite

Based on existing data, it is increasingly evident that

OA in the symbiotic bacteria also affects the primary cell metabolism of the host Previously, the main focus

of research has been on the effect of OA on attacking

or commensalic organisms, via inhibition of enzymes (protein phosphatases) [11] In view of the data, the corresponding cDNA for one of these enzymes (PP1) needed to be identified first cDNA coding for PP1 was completely isolated and the corresponding protein deduced This polypeptide contains all the characteris-tic domains of other enzymes in this group, e.g the characteristic Ser⁄ Thr-specific protein phosphatase signature and the conserved metallophosphoesterase region Based on the high sequence similarity between the sponge protein phosphatase and mammalian enzymes an antibody against the latter could be used here Signals obtained by western blot analysis,

37 kDa, matched the expected size Enzyme activity in the prepared extract was  20 nmol inorganic phos-phate released per min and mg of protein in tissue extracts Inhibition studies with OA were performed which revealed that the toxin blocks the enzyme(s) significantly at OA concentrations > 300 nm; at

100 nm no inhibition was seen The sensitivity of the enzyme to OA was in the range published previously [11,14] In the plant Medicago sativa it could be shown that at low temperature hyperphosphorylation of proteins occurs and this is the result of inhibition of protein phosphatase(s) [22] It has been established that OA is a more sensitive inhibitor of PP2 than of PP1 [11] Therefore, we screened our EST database from L baicalensis, which comprises over 4000 sequences, and also performed extensive screening studies using degenerate primers, designed against the conserved regions within the PP2 nucleotide sequence,

to identify PP2 transcripts in the cDNA library from

L baicalensis However, these attempts were without success Therefore, we focused our studies at the protein and cellular level on PP1 only Nevertheless, the data presented here do not exclude that PP2 is involved in thermoregulation in L baicalensis

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As outlined earlier, L baicalensis lives in a biotope

with ambient temperatures between )0.5 C (March)

and 17C (August–September) To date, no data have

been available that could help in understanding which

protection system allows these animals to maintain

high metabolic activity during these extreme situations

The first series of experiments now demonstrates that

the relative level of enzyme(s) (protein phosphatase)

in the animals is the same in March or in September

Also, the sensitivities of the enzymes towards OA are

very similar Based on these results, we conclude that

OA has an inhibitory effect in the animals during both

seasons at concentrations > 300 nm

In multicellular organisms one major protection

sys-tem against sys-temperature stress is provided by the heat

shock proteins [23], with hsp70 being the most

thor-oughly studied example In contrast to the related

con-stitutively expressed cognate hsc70, which changes its

level only slightly upon differing stresses, hsp70 is

strongly upregulated upon exposure to stress [24] For

the marine sponges S domuncula or G cydonium we

were able to show that at both the gene-expression level

[25] and the protein level [26] expression of hsp70

increa-ses strongly after temperature change and also after

exposure to xenobiotics [27] The induction of the gene

with respect to the stressors proceeds with the same

kin-etics in the sponge and in fish [28] Focusing on Lake

Baikal sponges, hsp70 proved to be a suitable biomarker

for xenobiotics and temperature stress [29]

Few publications are available that describe the

effect of OA on the expression of heat shock proteins

[13,30] These authors demonstrated that injection of

300 ng of OA into 250 g rats resulted in notable

expression of hsp70⁄ 72 after an incubation of 72 h

More importantly, Joyeux et al [30] showed that OA

treatment results in a potentiation of hsp72 mRNA

expression In this study, we tested whether OA

chan-ges the level of hsp70 expression at both the gene

expression level and the protein level For these

stud-ies, the primmorph system was used, which allowed

the study of this toxin under controlled laboratory

conditions In earlier studies, primmorphs have proved

to be suitable for measuring these effects [31]

A hsp70 cDNA probe was used to measure

semiquan-titatively the steady-state expression hsp70 in animals

collected in March and September; there were no

signifi-cant changes As outlined, the sponges contain OA in

March and September However, if primmorphs, kept in

the dark to suppress the photosynthetic activity of

the algae, were cultivated at 4C the level of hsp70

transcripts was very low compared with primmorphs

cultivated at 17C, or animals in the biotope,

irrespect-ive of whether they were collected at )0.5 C or at

12C If primmorphs were cultivated at 4 C together with 100 nm OA the hsp70 level reached values seen in animals or primmorphs incubated at 17C Interest-ingly, the level of hsp70 protein also followed this pat-tern From these results we conclude that OA causes, at both the gene- and the protein level, increased expres-sion of this heat shock protein in primmorphs at 4 C Interestingly, expression of a-tubulin in primmorphs is low during incubation at 4C, and is upregulated in the presence of OA or at higher temperatures This suggests that OA plays an inducer role for hsp70 and tubulin in primmorphs under cold stress conditions

A set of immunodepletion experiments was per-formed Extracts from animals collected during the summer were prepared that, according to the above-mentioned data, contained greater amounts of hsp70 protein They were subjected to protein phosphatase activity determination in the presence or absence of antibodies raised against hsp70 Hsp70 is known to bind to target protein(s) in the presence of ATP [23,32,33], which was therefore added If the extracts were assayed for protein phosphatase(s) activity it was found that at lower temperatures (4C) enzyme activ-ity was close to that seen after incubation at 17 C However, if antibodies were added to the mixture and incubation was performed at 4C the activity was almost completely abolished At 17C the antibodies had no effect on the high expression level of hsp70 These results strongly suggest that native hsp70 binds

at lower temperature to the enzyme(s) and restored the activity to values seen at higher temperature

OA is a toxin present in dinoflagellates that coexist with marine animals⁄ sponges and, as described here, in freshwater sponges Quantitative determinations showed that the level of this toxin in the freshwater sponge L baicalensis was as high as in the marine sponge S domuncula As reported here, in these fresh-water animals OA is involved in processes that result

in a high steady-state expression of the chaperon– hsp70 system In addition, the data suggest that the hsp system contributes to the cold thermotolerance seen in L baicalensis, because the secondary metabo-lite OA functions as an inducer for hsp70 Therefore,

it can be postulated that OA contributes markedly to the survival strategies of these animals during unfavo-rable environmental conditions This view is outlined

in Fig 6 In animals, collected during winter and summer the level of hsp70 is high If extracts from these specimens were used for immunodepletion experiments the ‘activating’ effect of hsp70 on protein phosphatase activity could be demonstrated in extracts prepared from animals collected during the cold season This suggests that at low temperature

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ATP-dependent hsp70 molecules are required for the

pro-motion of folding, transport and⁄ or assembly of target

proteins participating in the primary metabolism or,

perhaps also, in the composition of the fluid

mem-branes Energetically, the dinoflagellates supply their

host with primary metabolites via their photosynthetic

activity, glycerol being the major compound We

recently identified that the dinoflagellates synthesize

glycerol which is then taken up by cells of L baicalensis

through the aquaporin channel (W E G Mu¨ller,

manuscript submitted) In conclusion, our data suggest

that OA causes induction of hsp70 at low⁄ cold

tem-perature stress; in turn, hsp70 contributes to the proper

activity of the protein phosphatase at low temperature

Experimental procedures

Chemicals and enzymes

Restriction enzymes, SNAP ‘Total RNA Isolation Kit’,

Superscript II and reagents for RACE procedure were

pur-chased from Invitrogen (Carlsbad, CA), TriplEx2 vector

from BD (Palo Alto, CA), TRIzol Reagent from

Gib-coBRL (Grand Island, NY), Hybond-N+nylon membrane

from Amersham (Little Chalfont, UK), mAb against hsp70

(bovine; H 5147) was obtained from Sigma (St Louis, MO),

polyclonal antibodies raised against PP1 were from Santa Cruz Biotechnology (Santa Cruz, CA), CDP from Roche (Mannheim; Germany), Technovit 8100 from Heraeus Kul-zer (Wehrheim, Germany), Sephadex G-20 from Pharmacia (Uppsala, Sweden), Lake Baikal water was obtained from

‘Lake’ Comp (Irkutsk; Russia), and the protein phospha-tase assay kit from Upstate Biotechnology (Lake Placid, NY) Okadaic acid was purchased from Alexis Biochemi-cals (Gru¨nberg; Germany), the toxin was dissolved in dimethylsulfoxide

Sponges, cells/primmorphs and cDNA libraries Specimens of L baicalensis (Porifera, Demospongiae, Haplo-sclerida) were collected in Lake Baikal (Russia) near the village Bolshiye Koty (5158 N, 10521¢E) from depths between 7 and 12 m during September 2005 and March 2006 Primmorphs were prepared by immerging sponge tissue into natural Lake Baikal water, supplemented with 50 mm EDTA Lake Baikal water was used to guarantee a suitable mineral composition [34] After gentle squeezing and subse-quent shaking for 30 min at 16C on a rotatory shaker, the solution was discarded and new Baikal water⁄ EDTA was added After 40 min the supernatant was collected and filtered through a 40-lm mesh nylon net; shaking in Baikal water⁄ EDTA and filtration were repeated once Single cells

Fig 6 Proposed function of OA in L baicalensis The toxin OA is produced by the dinoflagellates from the taxon Gymnodinium In both win-ter and summer the dinoflagellates produce primary metabolites via their photosynthetic activity; the metabolite is taken up by the sponge cells Using the primmorph system it could be shown that the level of hsp70 is low at the lower temperature (in primmorphs at 4 C) How-ever, the abundance of hsp70 increases in response to low concentrations of OA (100 n M ) to levels which are seen in primmorphs incubated

at a higher temperature (17 C) or in animals collected during March and September It is postulated that a sufficiently high level of hsp70 is one prerequisite for the promotion of folding, transport and⁄ or assembly of target proteins participating in the primary metabolism or in the composition of the fluid membranes during unfavorable environmental conditions (in nature, at )0.5 C) Only at higher concentrations (> 300 n M ) does OA inhibit protein phosphatase(s).

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were harvested by centrifugation (500 g for 5 min,

Eppen-dorf centrifuge 5702 with rotor A-8-17) and washed once

The cells of this pellet were resuspended in Baikal water,

supplemented with 5 lgÆmL)1 penicillin and 100 lgÆmL)1

streptomycin A cell suspension of 107 cells was added to

6 mL (final volume) of medium in 10 mL flasks (Nuclon

surface; #136196; Nunc Wiesbaden, Germany) Primmorphs

were obtained from these single cells; they reached sizes of

3–7 mm after two days in the dark The primmorphs were

incubated at 4 or 17C; during the summer season the

ambient water environment of L baicalensis can reach a

temperature of up 22C [35]

The cDNA library from L baicalensis was prepared in

TriplEx2vector

Preparation of antibodies against OA

Polyclonal antibodies against OA (pAb-OA) were raised in

female rabbits (White New Zealand) as described previously

[14] The antigen (OA) was covalently coupled via its

C-ter-minus to the FID-33 oligopeptide (sequence:

NH2-FIDA-VWKCVTPFIDAVWKTKFICVTPFIDAVWK-COOH),

using EDC

(1-ethyl-3-(3-dimethylaminopropyl)carbodi-imide; Sigma) as described previously [14] This OA

conju-gate was injected at 4-week intervals into the animals; after

three boosts serum was collected and the antibodies were

prepared [36] The titer of the antibodies was determined to

be 1 : 2000 Where indicated the antibodies (pAb-OA;

0.3 mL of undiluted serum) were adsorbed with FID-33

coupled to OA (1 mg) for 30 min at room temperature

The studies with animals (antibody production) have been

approved by the respective state authorities

Histological analysis

Tissue was fixed in paraformaldehyde, embedded in

Tech-novit 8100 and sectioned [37] The 4-lm thick slices were

incubated with pAb-OA (1 : 250 dilution) overnight Then

the slides were treated with Cy3-conjugated goat

anti-(rab-bit IgG) for 2 h Subsequently, the sections were inspected

by immunofluorescence with an Olympus AHBT3

micro-scope, using an excitation light wavelength of 546 nm In

addition, the slices were illuminated with light of a

wave-length of 490 nm, which detects the autofluorescence of

chlorophyll in the dinoflagellates In parallel, the slices were

inspected directly using Nomarsky interference contrast

optics In controls, the pAb-OA (10 lg) were preincubated

with OA, coupled to the FID-33 oligopeptide (10 lg)

Competitive ELISA

The ELISA was performed similar to the procedure

des-cribed earlier [14] OA, coupled to the FID-33 oligopeptide

was linked to 96-well plates (Covalink-primary amine;

Nunc) [14] After three washing steps with NaCl⁄ Pi (containing 0.05% Tween-20) the plates were blocked prior

to use with 3% of fatty acids-free bovine serum albumin in NaCl⁄ Pi Then 100 lL of pAb-OA were added at different dilutions to each well for 90 min Subsequently, the immu-nocomplexes were visualized using secondary antibodies, coupled to horseradish peroxidase (1 : 1000; Sigma, Dei-senhofen, Germany) under application of o-phenylenedi-amine as substrate The plates were read at 492 nm In the competitive ELISA procedure, OA was added at different concentrations (1 ngÆmL)1 to 1 lgÆmL)1 NaCl⁄ Pi) from a stock solution of 1 mgÆmL)1, dissolved in methanol Within the range of 10 ngÆmL)1 to 1 lgÆmL)1 the change of the absorbance was linear (logarithmic plot) For the determin-ation in the tissue of the sponge, extracts were prepared from the tissue with 80% methanol The values for the absorbance were extrapolated using the calibration curve obtained with the free toxin

Identification of OA-bound protein Extracts were prepared from tissue samples; they were homogenized in lysis buffer (1· Tris-buffered saline,

pH 7.5, 1 mm EDTA, 10 mm NaF, 0.1 lm aprotinin, 1 mm sodium orthovanadate) Total cell extracts (10 lgÆlane)1) were subjected to electrophoresis in 10% polyacrylamide gels containing 0.1% SDS⁄ PAGE as described previously [37] The gels were stained with Coomassie Brilliant Blue Subsequently, western-blotting experiments were performed after transfer of the proteins onto poly(vinylidene difluo-ride) membranes (Millipore-Roth) using pAb-OA (1 : 300 dilution) After incubation for 3 h, the blots were incubated with goat anti-(rabbit IgG), peroxidase-coupled (1 : 5000 dilution; New England Biolabs) Detection of the immuno-complex was carried out using the BM Chemoluminescence Blotting Substrate kit Where indicated the pAb-OA had been adsorbed with OA coupled to the FID-33 oligo-peptide

Relative PP1 content (western blotting) The relative content of PP1 in the extracts was determined

by western blotting First, the tissue extracts (see previous section) were size separated by electrophoresis (SDS⁄ PAGE⁄ 12% polyacrylamide); samples of 10 lg protein extract were loaded onto the gels In addition, the proteins were blot transferred and reacted with polyclonal antibodies raised against PP1 (PcAb-PP1; 1 : 2000 dilution) After incu-bation for 3 h, blots were incubated with peroxidase-coupled goat anti-(rabbit IgG); and the immunocomplexes were visualized using the BM Chemoluminescence Blotting Substrate kit In control experiments 10 lL of undiluted PcAb-PP1 was adsorbed with 10 lL of cell extract (1 mgÆmL)1; 30 min; 4C) prior to the use onto the blots

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