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We demonstrate the operation of the Sec and Tat pathways in cyanelles and show for the first time in vitro protein import across cyanobacteria-like thylakoid membranes and protease protec

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The cyanelle of Cyanophora paradoxa

Juergen M Steiner1, Juergen Bergho¨fer2, Fumie Yusa1, Johannes A Pompe1, Ralf B Klo¨sgen2 and Wolfgang Lo¨ffelhardt1

1 Max F Perutz Laboratories, University Departments at the Vienna Biocenter, Department of Biochemistry and Molecular Cell Biology and Ludwig Boltzmann Research Unit for Biochemistry

2 Martin-Luther-Universitaet Halle-Wittenberg, Institute for Plant Physiology, Vienna, Austria

The photosynthetic apparatus of cyanobacteria and

chloroplasts are organized in an analogous way, with

some differences in detail [1], and comprise stromal

proteins that temporarily attach to the thylakoid

surface, a number of integral thylakoid membrane

proteins, and some soluble or loosely

membrane-asso-ciated proteins of the thylakoid lumen In addition,

there are certain proteins that possess a thylakoid

membrane anchor but expose the bulk of the

poly-peptide chain and the prosthetic group involved in

electron transfer to the lumen In higher plants, the

chloroplast and nuclear genomes both contribute to

the complement of thylakoid proteins [2]

Nucleus-encoded precursors to integral proteins may contain a

transit sequence only so that information for thylakoid

integration is contained in the mature protein: the cab protein family is thought to use an exclusive mechan-ism, the post-translational signal recognition particle (SRP) pathway [3] Others possess a bipartite pre-sequence consisting of a stroma-targeting peptide fol-lowed by a signal peptide-like hydrophobic domain Such proteins as CF0-II integrate via the spontaneous (unassisted) pathway without the need for stroma fac-tors recepfac-tors, ATP, and DpH [4] Members of the group of (predominately) lumenal proteins are passen-gers of the Sec and DpH-dependent (or Tat) pathways, corresponding to their relatively unfolded or folded state during translocation, respectively Identified components of the chloroplast Sec machinery are SecY⁄ SecE (forming the translocation pore) and the

Keywords

Cyanophora paradoxa; cyanelles;

conservative sorting; Sec translocase; Tat

translocase

Correspondence

W Lo¨ffelhardt, Max F Perutz Laboratories,

University Departments at the Vienna

Biocenter, Department of Biochemistry and

Molecular Cell Biology and Ludwig

Boltzmann Research Unit for Biochemistry,

Dr Bohrgasse 9, 1030 Vienna, Austria

Fax: +43 14277 9528

Tel: +43 14277 52811

E-mail: wolfgang.loeffelhardt@univie.ac.at

(Received 6 September 2004, revised 11

November 2004, accepted 17 December

2004)

doi:10.1111/j.1742-4658.2004.04533.x

Higher plant chloroplasts possess at least four different pathways for pro-tein translocation across and propro-tein integration into the thylakoid mem-branes It is of interest with respect to plastid evolution, which pathways have been retained as a relic from the cyanobacterial ancestor (‘conserva-tive sorting’), which ones have been kept but modified, and which ones were developed at the organelle stage, i.e are eukaryotic achievements as (largely) the Toc and Tic translocons for envelope import of cytosolic pre-cursor proteins In the absence of data on cyanobacterial protein transloca-tion, the cyanelles of the glaucocystophyte alga Cyanophora paradoxa for which in vitro systems for protein import and intraorganellar sorting were elaborated can serve as a model: the cyanelles are surrounded by a pepti-doglycan wall, their thylakoids are covered with phycobilisomes and the composition of their oxygen-evolving complex is another feature shared with cyanobacteria We demonstrate the operation of the Sec and Tat pathways in cyanelles and show for the first time in vitro protein import across cyanobacteria-like thylakoid membranes and protease protection of the mature protein

Abbreviations

GFP, green fluorescent protein; SRP, signal recognition particle.

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translocation ATPase SecA which is a stromal protein

that binds to the pore during action Energy source:

ATP Inhibitor: sodium azide, acting on SecA Proteins

that fold rather quickly or must acquire their

pros-thetic groups in the stroma prior to translocation enter

the Tat pathway, in most cases indicated by a

‘twin-arginine’ motif preceding the hydrophobic core of their

signal sequences The known components Tat A

(Hcf106), TatB (Tha4) and TatC are all

membrane-bound Energy source is DpH at the thylakoid

mem-brane Inhibitor is nigericin, dissipating DpH [5] All

these data were collected using higher plant

chloro-plasts, with the exception of fucoxanthin⁄

chloro-phyll c-binding protein and the secondary plastids

(derived from endosymbiotic red algae) of the diatom

Odontella sinensis where indications for a SRP

path-way were obtained [6]

Cyanelles are the peptidoglycan-surrounded plastids

of glaucocystophyte algae [7], assumed to be the first

phototrophic eukaryotes [8] The protein import

appar-atus of the cyanelle envelope seems to function in an

analogous way as for rhodoplasts and chloroplasts [9]

Are all four pathways for further protein routing

inside the chloroplast also operative in a primitive

plastid? The meaning of ‘conservative sorting’ [10], i.e

the retainment of prokaryotic translocons in organelles

of endosymbiotic origin as first exemplified by the Sec

pathway, has changed during the past decade: the Tat

pathway was considered as an achievement of higher

plants until its occurrence in (cyano)bacteria was

dem-onstrated [5] On the other hand, the spontaneous

pathway now seems to be restricted to chloroplasts

since related insertion processes in bacteria were found

to depend on the novel translocon component YidC

[11,12]

In cyanobacteria, there are dual Sec translocons, in

the thylakoid membrane as well as in the inner

envel-ope membrane [13] Tat translocase is assumed to be

located in the inner envelope membrane of

cyanobac-teria: numerous periplasmic proteins were found where

the corresponding genes contained signal sequences

with the twin-arginine motif [14] and Tat signal

pep-tides directed green fluorescent protein (GFP) to the

periplasmic space of transgenic cyanobacteria [15] On

the other hand, the Tat passengers known from

chlo-roplasts are largely absent from several completely

sequenced cyanobacterial genomes: the two extrinsic

proteins from the oxygen evolving complex, PsbP and

PsbQ, are replaced in cyanobacteria by the unrelated

proteins PsbV and PsbU [16], respectively, that both

lack the twin arginine motif in the precursors Even

when a conserved lumenal protein like Hcf136 was

considered, the sorting signal appeared to have

changed after gene transfer to the nuclear genome: the precursor⁄ intermediate was shown to use the Sec pathway in cyanobacteria and the Tat pathway in higher plants [17]

One reason to investigate thylakoid transloca-tion⁄ integration in cyanelles is the bridge position of these organelles between chloroplasts and free-living cyanobacteria Cyanelle thylakoids resemble the cyano-bacterial ones in the composition of the OEC, the presence of phycobilisomes [18] as antenna system and the possibility of connections to the inner envelope membrane [19] In freeze-fracture experiments, cyanelle thylakoids also behaved cyanobacteria-like and upon isolation did not readily form closed vesicles as chloro-plast thylakoids do [20] In vitro experiments with cyanobacterial thylakoids are hampered through this problem: successful translocation is evidenced through protease protection of the mature (processed) protein which is not feasible when no tight vesicles can be pre-pared (C Robinson, personal communication) Assays that cannot be done ‘in thylakoido’ with cyanobacteria can be performed ‘in organello’ using intact, isolated cyanelles So phycobilisome assembly could be monit-ored via integration of imported, labeled core linker protein [18] The Sec pathway in cyanelles, which was made likely by the first demonstration of a functional organellar-encoded secY gene [21], was corroborated

by determining the energetic requirements for cyto-chrome c6, cytochrome c550 and PsbO import In this paper, we demonstrate Rieske Fe⁄ S protein as a Tat passenger, and, for the first time with phycobilisome-bearing thylakoids, we show protease protection of translocated, processed thylakoid lumenal proteins Another advantage of the cyanelle system is that pas-senger proteins can be studied that are different from the established chloroplast import systems (i.e that are not imported in vivo into chloroplasts) as AtpI

Results

Cytochrome c6uses the Sec pathway Using a modified cyanelle isolation procedure, the effi-ciency of homologous (envelope) import could be greatly increased [9,19] Import-competent cyanelles from Cyanophora paradoxa efficiently took up the

15 kDa pre-apocytochrome c6 and converted it into the protease-protected mature form of 9.2 kDa, comi-grating with the holoprotein (Fig 1, left panel) The time-course showed that the import was largely com-pleted after 3 min Prolonged incubation resulted in eventual degradation of the mature protein, presuma-bly through lumenal proteases [22] No intermediate

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was observed under these assay conditions, indicating

that envelope import is the rate-determining step

However, two-step processing, as reported for the

homologue from Chlamydomonas reinhardtii [23], could

be demonstrated when intermediate accumulated due

to the addition of the SecA inhibitor, sodium azide

(Fig 1, right panel), whereas nigericin, the inhibitor of

the DpH-dependent Tat pathway had no effect (data

not shown) The effect of azide was most pronounced

after 3 min compared with the control assay After

that time the intermediate is slowly imported and

pro-cessed, maybe because of intracyanellar ATP

genera-tion, as the azide-inhibition of SecA can be reverted by

a higher amount of ATP competing for the same

bind-ing sites [24] As sodium azide might inhibit

chloro-plast and cyanelle proteases (our own experiments and

K Cline, personal communication), it is somewhat

dif-ficult to compare the posterior time points Sodium

azide also appeared to impede the overall import

process of pre-apocytochrome c6 to some extent, since

a small amount of precursor protein was still bound to

the envelope (Fig 1, right panel) For a small

protein-like cytochrome c6 complete protease protection could

not be achieved [19] We therefore extended our

experiments to a heterologous system where tight

thylakoid vesicles can be obtained In vitro assays with

isolated spinach chloroplasts were performed including

competition experiments Saturating amounts of the

OEC23 (PsbP) precursor from spinach were used to

block the DpH-dependent Tat pathway [5] and – in

parallel – saturating amounts of the spinach OEC33

(PsbO) precursor, a well known Sec-passenger [24] to

inhibit the Sec-pathway (Fig 2) It could be clearly

shown that pre-apocytochrome c6 from C paradoxa

was readily imported into chloroplasts, processed to an intermediate form in the stroma and then translocated into the thylakoid lumen, where it was processed again

to its protease-protected mature form (Fig 2) In the heterologous system, the stroma-processing protease cleavage site obviously was not properly recognized leading to an intermediate of higher MW than that observed in the cyanelle system (Fig 1, right panel) When the OEC23 precursor was used as a competitor, the amount of mature protein was almost unchanged and its location in the thylakoid lumen could be pro-ven by protease protection (Fig 2) In competition experiments with the OEC33 precursor, the intermedi-ate accumulintermedi-ated in the stroma fraction by a factor of two (ImageQuant) and the amount of mature protein was reduced by a factor of two compared to the con-trol assay (Fig 2) The results of homologous and heterologous import experiments indicate that apocyto-chrome c6 is a Sec passenger in cyanelles (as its func-tional homologue plastocyanin in higher plants) in spite of the lack of protease protection due to system-inherent problems

Protease protection of lumenal proteins in cyanobacterial-type thylakoid vesicles

In order to identify additional Sec passengers and, eventually, to prove protease protection of a larger lumenal protein in cyanelle thylakoids, we cloned the psbO gene (GenBank accession number AJ784854) via

a PCR approach based on N-terminal sequence infor-mation [25] and used the labeled precursor to study the function of the cyanelle thylakoid translocons Figure 3 shows a typical import experiment in a time Fig 1 Time-course of import of35S-labeled pre-apocytochrome c6 into isolated cyanelles T, translation mix; –⁄ +, without ⁄ with addition of thermolysin; p, precursor; i, intermediate; m, mature protein Left panel: control; right panel: plus 10 m M sodium azide.

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course from 3 to 15 min Compared to

pre-apocyto-chrome c6, thylakoid import was retarded in the

stroma, whereas envelope translocation was almost

completed after 3 min The resulting intermediate form

of the OEC33 protein (iOEC33) appeared to be

trans-ported into the thylakoid lumen in a time-dependent

manner (Fig 3) When sodium azide was added,

mat-uration of iOEC33 was completely stopped (Fig 3)

These data do not unequivocally show if the mature

protein is internalized into the thylakoid lumen and

thus we wanted to demonstrate protease protection, at

least for larger proteins as OEC33 We established a

method to isolate tight thylakoid vesicles, which was

hitherto not achieved for phycobilisome-bearing,

cyanobacterial-type membranes When the novel

cyanelle fractionation procedure was applied after an

import experiment, the mature OEC33 localized to the thylakoid fraction (Fig 4) Thermolysin treatment digested the residual amount of precursor bound to the peptidoglycan-containing envelope membranes, which co-sedimented with the thylakoids and therefore served as internal controls for protease activity, whereas the internalized mature protein was protected

in the thylakoid lumen Sodium azide decreased the amount of precursor imported into the cyanelles (Fig 4), possibly due to inhibition of other ATP-dependent processes [26] iOEC33 accumulated in the stroma and even a small proportion of mature PsbO fractionated with the thylakoid membranes, possibly due to the longer incubation time (25min.) When this membrane pellet (containing also envelope membranes) was treated with thermolysin, the bound precursor as

Fig 2 Import of 35 S-labeled pre-apocytochrome c6of C paradoxa into isolated spinach chloroplasts Tr, translation mix; S, stroma; T–, thyl-akoid membranes; T+, thylthyl-akoid membranes treated with thermolysin; p, precursor; i, intermediate; m, mature protein Left panel, control; middle panel, saturation of the Tat-pathway by the 23-kDa protein; right panel, saturation of the Sec-pathway by the 33-kDa protein.

Fig 3 Time-course of import of 35 S-labeled pre-OEC33 into isolated cyanelles ivT, translation mix; p, precursor; i, intermediate;

m, mature protein (A) control; (B) plus

10 m M sodium azide; control + TL, plus thermolysin.

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well as the putative mature protein band disappeared,

indicating that PsbO protein generated in the presence

of azide is only bound to the thylakoid surface (or

rather arrested in a preliminary insertion stage that

allowed processing) but not internalized and thus not

protease-protected Nigericin also caused a drop in

over-all import efficiency, but did not lead to accumulation

of the intermediate in the stroma Furthermore, in

con-trast to the azide experiment, mature protein

fractionat-ing with the thylakoids was protease-protected (Fig 4)

All these data point towards a functional Sec translocase

with an azide-sensitive SecA homologue in the cyanelle

thylakoid membrane and that lumenal cytochrome c6as

well as OEC33 protein had used this pathway

The Rieske Fe/S protein is inserted into cyanelle

thylakoids via theDpH-dependent Tat pathway

In chloroplasts, Rieske Fe⁄ S protein, a

nuclear-enco-ded subunit of the cytochrome b6⁄ f complex, appeared

in the stroma after in vitro import and only slowly

translocated further into the thylakoid membrane

sys-tem It could also be shown, via competition

experi-ments and the sensitivity to nigericin, that thylakoid

translocation⁄ integration of this protein in chloroplasts

takes place through the DpH-dependent Tat pathway

[27] As the Rieske protein lacks a cleavable signal

peptide, its transport is mediated by the N-terminal

membrane anchor which does not contain the

twin-arginine motif typical of Tat transport signals Instead,

higher plant as well as cyanelle Rieske proteins contain

a lysin-arginine sequence at this position, whereas

cyanobacterial Rieske proteins do possess the

twin-arginine motif This renders the Rieske protein an

unusual Tat substrate and, concerning the evolutionary

position of the cyanelles, it was interesting which

pathway the authentic Rieske protein might use in the

cyanelle system For that reason we cloned two petC genes from C paradoxa via a PCR approach (petC1, GenBank accession number AJ784852 and petC2, GenBank accession number AJ784853) We performed

in organello experiments with isolated intact cyanelles and the precursor corresponding to petC1 in a time-course manner in the presence⁄ absence of specific translocase inhibitors (Fig 5) A striking feature in the targeting process of Rieske protein is the remarkably slow sorting of the protein within the cyanelles to its final destination, the thylakoid membrane system While the import of the Rieske precursor into the stroma proceeded within 5 min (Fig 5), only a minor fraction (20%) reached the thylakoids and was cor-rectly integrated during a total incubation time of

25 min (Fig 6) The majority of the processed mature protein of approximately 20 kDa accumulated in the

Fig 4 Fractionation of isolated cyanelles after import of 35 S-labeled pre-OEC33 ivT, translation mix; C, intact cyanelles; S, stroma; T–, thyla-koid membranes; T+, thylathyla-koid membranes treated with thermolysin; p, precursor; i, intermediate; m, mature protein; azide, plus 10 m M

sodium azide; nigericin, plus 2 l M nigericin.

Fig 5 Import of 35 S-labeled pre-Rieske-protein into isolated cya-nelles ivT, translation mix; p, precursor; m, mature protein; azide, plus 10 m M sodium azide; nig, plus 2 l M nigericin.

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cyanelle stroma Once the Rieske protein had

reached the thylakoids, it was to a large extent protected

against the activity of proteases that were added

exter-nally to the thylakoid vesicles, indicating that the

C-terminal hydrophilic domain had been completely

translocated into the lumenal space (Fig 6) Only the

utmost N-terminal residues preceding the membrane

anchor domain remained accessible to thermolysin

resulting in a decrease in apparent molecular mass of

approximately 0.5 kDa In the presence of nigericin,

thylakoid translocation of the Rieske protein was

com-pletely abolished, and the bulk of intracyanellar mature

protein localized with the stroma, while the thylakoid

membrane fraction contained only a minor amount of

loosely bound Rieske protein which disappeared after

thermolysin treatment Sodium azide reduced the

amount of membrane-integrated Rieske protein to

about 30% of the control assay This fraction of

mature protein was protease-protected and fully

integ-rated into the thylakoid membrane system through its

single membrane span A slight downward shift in

polypeptide mobility was best noticeable here due to

the removal of about four amino acids from the

stroma-exposed N terminus by thermolysin treatment,

indicating correct integration into the cytochrome b6f

complex In evaluating the azide effect on thylakoid

translocation of Rieske protein one should consider its

reported inhibitory action on numerous

nucleotide-binding proteins [28]: the azide-sensitive steps occur

very likely after the import of the apoprotein and prior

to membrane integration of the holoprotein [27] Thus

our interpretation of the experiments shown in Fig 6

is to name Rieske a bona fide Tat passenger: a similar conclusion was made in the chloroplast system [27]

The first precursor to a cyanelle lumenal protein (PsbU) containing the twin-arginine motif PrePsbU from the red alga Cyanidium caldarium was found to contain the twin-arginine motif in the thyla-koid transfer domain of the presequence [29]: this was the first incidence in algae containing ‘primitive’ plast-ids and prompted us to clone the counterpart from

C paradoxa based on sequence information from an EST collection (S Burey and H Bohnert, unpublished data) This completed the collection of cyanelle OEC component genes (GenBank accession number AJ784849) and presented another Tat passenger candi-date (Fig 7) Cyanelle import of prePsbU occurred as readily as that of the other small cyanelle protein, pre-cytochrome c6, with almost no envelope-bound precur-sor or intermediate (Fig 8) However, azide addition did not result in the accumulation of intermediate, excluding the Sec pathway Nigericin did not produce

a clear-cut effect either (except also increasing the amount of envelope-bound precursor) Small proteins obviously can escape from cyanelle thylakoid vesicles, thus mature PsbU localized to the stroma fraction in comparable amounts irrespective of any inhibitor used (Fig 8) Considering these experimental difficulties with regard to protease protection and the reported DpH-independence of Tat translocation in C reinhardtii chloroplasts [30] we propose that PsbU, i.e one of the three cyanelle OEC proteins, is a Tat passenger

Fig 6 Fractionation of isolated cyanelles after import of the 35S-labeled pre-Rieske-protein ivT, translation mix; C, intact cyanelles; S, stroma; T–, thylakoid membranes; T+, thylakoid membranes treated with thermolysin; p, precursor; m, mature protein; azide, plus 10 m M

sodium azide; nigericin, plus 2 lm nigericin.

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AtpI: SRP-dependent or spontaneous thylakoid

integration?

As other primitive plastids, cyanelles encode a higher

number of ATP synthase subunits than higher plant

chloroplasts, e.g atpG and atpD [32] However, in

con-trast to all sequenced plastid genomes, atpI is a nuclear

gene in C paradoxa [7] This means that a precursor

exceeding Cab protein with respect to hydrophobicity

has to be imported into cyanelles, must cross the

stroma and insert into the thylakoid membranes In the

case of Cab, the solution is the post-translational SRP

pathway involving a transit complex consisting of Cab,

SRP54 and SRP43 [3] We cloned two atpI genes via a

PCR approach based on highly conserved domains of

the protein They are listed in under the GenBank

accession numbers AJ784850 and AJ784851,

respect-ively The closely related sequences comprise four to

five putative transmembrane regions as candidates for

binding to SRP54 [33] and a hydrophilic loop with some resemblance to the ‘L18’ domain of Cab protein (Fig 9) which was shown to interact with SRP 43 [3] Highly hydrophobic precursor proteins pose problems upon in vitro import into isolated chloroplasts [34] This also applies for cyanelle envelope translocation: only a small fraction of AtpI is processed and internal-ized (Fig 10A) though a time course is noticeable Cya-nelle fractionation after incubation resulted in recovery

of substantial amounts of preAtpI in the thylakoid (and envelope) fraction Low amounts of mature pro-tein were detected in the thylakoid fraction: here no influence of added azide or nigericin became apparent Due to cleavage sites in the stromal loops thylakoid-inserted AtpI was degraded upon thermolysin treat-ment (Fig 10B) With regard to the insertion pathway, Sec and Tat do not seem to be involved In order to

Nucleus-encoded:

pre-cytochrome c6

KKGRREFVAAAGALFAAFAASPAAFA Plastid-encoded:

pre-cytochrome c550

MRKLFLLMFCLSGLILTTDIRPVRA Fig 7 Thylakoidal signal peptides of intermediates (precursors) to

cyanelle proteins that are imported into or synthesized within the

organelle, respectively Charged residues are underlined C,

C-ter-minal domain; H, hydrophobic core (bold); N, N-terC-ter-minal domain.

The signal sequences of nucleus-encoded precursors start with the

first amino acid after the putative SPP cleavage sites taken from

predictions of the CHLOROP program [31].

Fig 8 Fractionation of isolated cyanelles after import of the

35

S-labeled prepsbU-protein ivT, translation mix; S, stroma; T–,

thylakoid membranes; T+, thylakoid membranes treated with

thermolysin; p, precursor; m, mature protein; azide, plus 10 m M

sodium azide; nigericin, plus 2 lm nigericin.

Fig 9 Sequence comparison of a hydrophilic loop between the putative TM helices 3 and 4 of AtpI from C paradoxa to the ‘L18’ domain of pea LHCP Similarities are indicated by bold letters.

A

B

Fig 10 (A) Time-course of import of the35S-labeled preatpI-protein into isolated cyanelles T, translation mix; p, precursor; m, mature protein; 0, incubation for 20 min on ice; –, control; +, plus thermo-lysin (B) Fractionation of isolated cyanelles after import of the

35 S-labeled preatpI-protein ivT, translation mix; S, stroma; T–, thylakoid membranes; T+, thylakoid membranes treated with thermolysin; p, precursor; m, mature protein; azide, plus 10 m M

sodium azide; nigericin, plus 2 l M nigericin.

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assess an SRP-based mechanism, the import efficiency

will have to be increased first Spontaneous insertion is

less likely for a polytopic membrane protein as AtpI

but cannot be excluded at present

Discussion

Two of the four pathways operating in thylakoid

translocation⁄ integration in higher plant chloroplasts,

i.e the Sec and the Tat translocase could be

demon-strated to function in the cyanelles of C paradoxa

With respect to the hydrophobicity of the core

domains signal sequences from cyanelle genes surpass

those from nuclear genes (Fig 7) This has also been

observed with higher plants: the replacement (after

gene transfer) of leucine and phenylalanine by alanine

was interpreted as a measure to avoid interactions with

cytosolic SRP [35]

Interestingly, there seem to be relatively more

known Sec passengers in these primitive plastids than

Tat passengers, whereas the opposite was found for

chloroplasts [5] There are several reasons for the

observed prevalence of the Sec pathway in cyanelles:

one of them is the replacement of evolutionary ancient,

i.e cyanobacterial proteins by unrelated counterparts

in higher plants The cyanelle-encoded cytochrome c550

fulfills the function of the Tat passenger PsbP in the

OEC By analogy to the other c-type cytochromes it

should use the Sec pathway This was proven by

homologous and heterologous import experiments of a

construct containing the FNR transit sequence from

C paradoxa at the N terminus (T Ko¨cher and

J Steiner, unpublished data) Second, Tat passengers

like polyphenol oxidase, PsbT, PsaN and others

(with-out a cyanobacterial homologue) might be absent from

cyanelles Third, C paradoxa with its peculiar gene

distribution between the nuclear and cyanelle genomes

allows to test the hypothesis that rapidly folding

(small) polypeptides without prosthetic groups can be

Sec passengers in cyanobacteria and in primitive

plast-ids (when they are plastom-encoded) but should be

Tat passengers as nuclear gene products in higher

plant chloroplasts In the latter case, protein targeting

to the thylakoid lumen is much more time-consuming

and the intermediate should be rather tightly folded

upon arrival at the membrane [17] The

cyanelle-enco-ded Hcf136 homolog resembles its cyanobacterial

counterpart in the absence of the twin arginine motive,

i.e is a putative Sec passenger PsbU, on the other

hand, an OEC component of cyanobacteria and

chlo-rophyll b-less algae, is nucleus-encoded in the latter

Consequently, PsbU contains a twin-arginine motif in

its bipartite presequence and its translocation therefore

most likely is Tat-dependent In this case, evolutionary replacement through PsbQ in higher plants is not accompanied by a change in the translocase used Isolated cyanobacterial thylakoid vesicles do not allow in thylakoido import experiments or protease protection of luminal proteins, in contrast to spinach thylakoids [5,34] Therefore it was a considerable pro-gress to show protease protection at least for the

33 kDa PsbO protein after internalization into cyanelle thylakoids It is unknown, why these membranes are still leaky for smaller proteins as cytochrome c6 and PsbU Sodium azide appeared to be the diagnostic inhibitor of choice for in cyanello experiments Thyla-koid import was retarded for small Sec passenger proteins and completely blocked for larger ones, respectively This indicates high azide-sensitivity of cyanelle SecA Thus the Sec pathway can be excluded when no significant azide effect is observed, e.g in the case of PsbU

Nigericin completely abolished protease protection

of membrane-inserted Rieske protein However, azide addition resulted in a reduction of the amount of correctly assembled cyanelle Rieske protein as was observed with the chloroplast in organello system [27] There it was shown that although the Rieske protein is targeted exclusively by the DpH ⁄ Tat pathway, some azide-sensitive stromal factors, such as the Cpn60 chaperonin [36] might play a role in correct folding and⁄ or attachment of the Fe ⁄ S cluster to the Rieske mature (apo)protein Recently, an interaction and⁄ or regulation partner for the Rieske protein has been identified in Arabidopsis thaliana [37] A thylakoid lum-enal FKBP (immuno-suppressant FK506 binding pro-tein) was isolated, whereof only the precursor, but not the mature form, interacted with Rieske protein AtFKBP13 might serve as an ‘anchor’ chaperone that holds the Rieske protein in the cytoplasm or in the stroma so that excessive Rieske protein is not targeted

to the thylakoid, since its integration into the cyto-chrome b6f complex underlies complex regulation and coordination events It might well be that sodium azide blocks either one of those chaperones and⁄ or other factors necessary for the build-up of a functional cyto-chrome b6f complex, and the resulting malfunctioning

or only partially moulded unit fails to be translocated via the Tat-pathway The effects of nigericin on thyla-koid translocation of the other candidate Tat passen-ger, PsbU, were not clear-cut In this context it should be noted that the Tat translocase in the alga

C reinhardtii appeared to operate in the absence of a DpH [30], whereas proton efflux at the expense of the

pH gradient was a prerequisite for Tat-dependent translocation in higher plant chloroplasts [38]

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AtpI would be a candidate for the post-translational

SRP pathway in cyanelles In Escherichia coli, its

homologue, subunit a, needs the assistance of YidC for

integration into the inner membrane [39] Mitochondrial

Atp6 is also partially dependent upon Oxa1 in that

respect [40] In chloroplasts, by analogy, the

cotransla-tional SRP pathway and the Albino3 translocon

might be involved However, in the ac29 mutant of

C reinhardtii, where one out of the two albino3 genes is

inactivated, no effect on ATP synthase (at least on the a

subunit) could be observed [41] Thus far, there is no

evidence for ALB3 in the plastids of chlorophyll b-less

algae In C paradoxa, SecY is a component of two

different high molecular mass thylakoid-bound protein

complexes (F Yusa and W Lo¨ffelhardt, unpublished

data), a parallel to A thaliana where ALB3 is also

contained [42] Another crucial point will be to identify

SRP43 in nonchlorophytes, e.g diatoms that integrate

fucoxanthin chlorophyll a⁄ c-binding protein into their

thylakoid membranes [6] On the other hand, reports on

vesicle transport of cab protein from the inner envelope

membrane to the thylakoid membrane in C reinhardtii

[43] render the function of the transit complex and of

ALB3 questionable in this alga However this vesicle

transport must be different from that described for

higher plant chloroplasts that can be visualized upon

lowering the temperature and is sensitive to microcystin

[44]

The fourth pathway might also exist in cyanelles:

SecE from C paradoxa is not yet identified; in

chloro-plasts it was shown to use the spontaneous pathway

[11,12] Chloroplast and cyanelle thylakoids are both

rich in galactolipids which obviously support

unas-sisted integration of proteins in contrast to the

phos-pholipids of the E coli cytoplasmic membrane [12]

Experimental procedures

Materials

Cyanophora paradoxa LB555UTEX was grown as

previ-ously described [45] In general, cells were harvested in the

exponential growth phase Nucleic acids were isolated

according to published methods [45] Spinach (Spinacia

oleracea) was purchased from the local market and kept

overnight at 4C before isolating chloroplasts Pea

seed-lings (Pisum sativum) were grown for 8–10 days under a

16 h photoperiod

Protein import into isolated chloroplasts

Precursor proteins were synthesized by in vitro transcription

of the corresponding cDNA clones and subsequent in vitro

translation in cell-free wheat germ lysates in the presence of [35S]methionine Intact chloroplasts were isolated from pea

or spinach leaves by Percoll gradient centrifugation and were used in protein import experiments essentially as des-cribed [46] Competition experiments were performed with precursor proteins that were obtained by overexpression in Escherichia coli[47] and recovered from inclusion bodies by solubilization in a buffer containing 7 m urea, 30 mm Hepes,

pH 8.0 and 2 mm EDTA The solubilized proteins were included in the import assays at concentrations up to 4 lm, taking care that the concentration of urea in the assays never exceeded 300 mm Control assays contained the same amount of buffer lacking any such solubilized protein

Protein import into isolated cyanelles

Import-competent cyanelles were isolated as described in [19] They were used in protein transport experiments as described in [18]

Isolation of cyanelle thylakoid membranes

The import reaction was stopped by the addition of 1 mL ice-cold sorbitol resuspension medium (SRM) buffer (50 mm Hepes, 0.33 m sorbitol, pH 8.0) followed by centri-fugation at 800 g and 4C for 2 min The cyanelle pellet was washed in SRM and resuspended in 500 lL 2· SRM and incubated for 25 min at room temperature with 15 lL

of a 10 mgÆmL )1lysozyme stock solution in the presence of protease inhibitors (Complete, Roche), which led to diges-tion of the peptidoglycan wall, cyanelle lysis and release of the phycobilisomes from the thylakoid membrane After

centrifugation for 5 min at 9300 g in an Eppendorf

centri-fuge at 4C an aliquot of the deep-blue stromal superna-tant was precipitated with 100% (v⁄ v) acetone, the pellet containing the thylakoids and the peptidoglycan-linked outer envelope membrane was washed in 2· SRM and finally resuspended in 500 lL 2· SRM An aliquot (250 lL) was treated with thermolysin plus 10 mm CaCl2

for 30 min on ice After stopping the reaction with EDTA all aliquots were pelleted by centrifugation

Miscellaneous

Gel electrophoresis of proteins under denaturing conditions was carried out according to [48] Import data were ana-lyzed using a PhosphoImager and the molecular dynam-ics imagequant program (version 3.3), such that all the signals remained in the linear detection range

PCR, gene isolation

The nucleotide sequences determined via reverse translation

of highly conserved regions of the ATP synthase subunit

Trang 10

CF0-IV (AtpI) and of the Rieske iron–sulfur protein (PetC)

were used to design degenerate primers

AtpI: forward primer 5¢-GCNTAYTTYTAYGCNGG-3¢,

reverse primer 5¢-GGYTTNGTRAARTCYTC-3¢ (product

size: 111 bp); PetC: forward primer 5¢-CARGGNYTNAA

RGGNGAYCCNACNTA-3¢, reverse primer 5¢-TAYTGN

WSNCCRTGRCANGGRCA-3¢ (product size: 156 bp)

The PCR reaction mixture (50 lL) included 100 ng of

DNA from C paradoxa, 0.1 lm concentration of each

primer species, 10 mm Tris⁄ HCl (pH 8.3), 50 mm KCl,

1 mm MgCl2, 0.2 mm dNTPs, and 1 U of Taq DNA

polymerase (Dynazyme, Finnzymes Oy, Espoo, Finland)

The following thermal cycle was used: Step 1, 96C for

5 min; Step 2, 94C for 1 min; Step 3, 50 C for 2 min;

Step 4, 72C for 3 min; Step 5, repeat steps 2–4 35 times;

Step 6, 72C for 7 min The predominant PCR product

was cloned into pGEM-T and sequenced After

identifi-cation of the correct products the fragments were

labe-led with the Digoxigenin Labeling⁄ Detection System

(Boehringer Mannheim, Mannheim, Germany) and used

for screening of a C paradoxa cDNA library in the

vec-tor k-ZAP II (Stratagene, La Jolla, CA, USA) Plaque

hybridization was performed under high stringency

conditions [49]

Full-length cDNAs were cloned into the vector pBAT

[50] to allow sufficient translation efficiency psbO: forward

primer: 5¢-AANGGNACNCKYTCNCCNCC-3¢ The

for-ward primer was designed using a peptide sequence

(EGLTYDQ) obtained via Edman-sequencing [25] psbU:

forward primer: 5¢-AAGAATTCACGAGGCAGAAATG

GCGTTC-3¢, reverse primer: 5¢-AAGGATCCTGGGGAC

AGCAGAAACTTGG-3¢

The psbU gene was isolated by PCR with a proof-reading

polymerase (Pfu) using data from a C paradoxa EST

lib-rary (S Burey and H J Bohnert, unpublished data) and

directly cloned into the pBAT-vector via its EcoRI and

BamHI sites

Acknowledgements

We appreciate support from the Austrian Research

Fund (P15438-MOB, to W.L.) We thank Hans

Bohnert (Urbana, IL, USA) and Suzanne Burey for

providing EST data from Cyanophora paradoxa

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