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The protein contains an unusually long N-terminal domain, the pseudosubstrate site involved in binding and inactivation of the catalytic subunit, and two C-terminally located, closely sp

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The regulatory subunit of a cGMP-regulated protein kinase A of

Trypanosoma brucei

Tarek Shalaby, Matthias Liniger and Thomas Seebeck{

Institute of Cell Biology, University of Bern, Switzerland

This study reports the identification and characterization of

the regulatory subunit, TbRSU, of protein kinase A of the

parasitic protozoon Trypanosoma brucei TbRSU is coded

for by a single copy gene The protein contains an unusually

long N-terminal domain, the pseudosubstrate site involved

in binding and inactivation of the catalytic subunit, and two

C-terminally located, closely spaced cyclic nucleotide

binding domains Immunoprecipitation of TbRSU

copre-cipitates a protein kinase activity with the characteristics of

protein kinase A: it phosphorylates a protein kinase specific

substrate, and it is strongly inhibited by a synthetic protein

kinase inhibitor peptide Unexpectedly, this kinase activity could not be stimulated by cAMP, but by cGMP only Binding studies with recombinant cyclic nucleotide binding domains of TbRSU confirmed that both domains bind cGMP with Kd values in the lower micromolar range, and that up to a 100-fold excess of cAMP does not compete with cGMP binding

Keywords: sleeping sickness; protein kinase A; African trypanosomes; cyclic nucleotide signalling

The concept of cellular signaling by cyclic AMP (cAMP)

has been maintained throughout evolution, from bacteria to

mammals However, the only component of this signalling

pathway that has been strictly conserved is the second

messenger molecule itself, cAMP, while the enzymatic

machinery that generates and transduces the signal exhibits

great variety This is exemplified by the adenylyl cyclases,

which have developed into many different molecular

structures [1 – 3], although their function is invariably to

convert ATP to cAMP A similarly wide range of structure

and sequence diversity of functionally similar enzymes is

found within the cAMP-specific phosphodiesterases

(PDEs) On the basis of sequence comparison as well as

of pharmacological criteria, two distinct classes of

eukaryotic PDEs are currently distinguished, class I and

class II [4,5], with no significant sequence similarities

between them Besides these, many PDEs have been

identified in bacteria that share no significant sequence

homology with either the class I or the class II of the

eukaryotic PDEs [6]

An even greater variety is encountered with the

down-stream effectors of cAMP signalling cAMP can bind

directly to and regulate a number of different ion channels,

such as cyclic nucleotide gated ion channels [7,8] or

hyperpolarization-activated cyclic nucleotide gated chan-nels [9] On the other hand, cAMP can bind to and stimulate drug efflux pumps, e.g in the human erythrocyte [10] Furthermore, recent data have demonstrated that the guanine nucleotide exchange factor Epac is a cAMP-binding protein [11], and that binding of cAMP modulates its activity This interaction potentially allows a crosstalk between cAMP pathways and ras-mediated pathways in cell cycle control

In addition to its many roles as an intracellular messenger, cAMP also can act as an extracellular signalling molecule, either directly, as in the aggregation of the slime mold Dictyostelium discoideum [12], or indirectly via extracellu-lar conversion into adenosine and the subsequent activation

of adenosine receptors in the brain [13]

In mammalian systems, the most extensively studied downstream effector of cAMP is the cAMP-regulated protein kinase A (PKA) [14 – 18] According to the current paradigm, PKA is an R2C2heterotetramer consisting of two catalytic and two regulatory subunits The regulatory subunits contain a dimerization domain in their N-terminal regions, followed by an autoinhibitor sequence that resembles a PKA substrate This region binds to the active site of the catalytic subunit, inactivating it while it is in the

R2C2 complex The C-terminus of the regulatory subunit contains two adjacent cAMP-binding domains Domain A is not accessible for cAMP in the R2C2complex cAMP first binds to domain B, triggering a conformational change that renders domain A more accessible The two cAMP-binding domains are biochemically distinct, both in terms of binding kinetics and in their preference for substituted cAMP analogs The three-dimensional structure of the cAMP-binding domain of a bovine type I regulatory subunit has been determined [19] Binding of cAMP to the regulatory subunits releases the active catalytic subunits from the complex These proceed to phosphorylate a plethora of proteins, among them transcription factors such as CREB [20,21] The current view is that most of the downstream effects of cAMP in eukaryotic cells are mediated through

Note: a web site is available at

http://www.izb.unibe.ch/res/seebeck/sehome.html

Correspondence to T Seebeck, Institute of Cell Biology,

University of Bern, Baltzerstrasse 4, CH-3012 Bern, Switzerland.

Fax: 1 41 31 631 46 84, Tel.: 1 41 31 631 46 49,

E-mail: thomas.seebeck@izb.unibe.ch

(Received 27 June 2001, revised 20 September 2001, accepted

1 October 2001)

Abbreviations: PKA, protein kinase A; cGMP, cyclic guanosine

monophosphate; cAMP, cyclic adenosine monophosphate; cNMP,

cyclic nucleoside monophosphate; TbRSU, regulatory subunit of

trypanosomal PKA.

Eur J Biochem 268, 6197–6206 (2001) q FEBS 2001

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the alteration of transcription via PKA-mediated

phos-phorylation of transcription factors Interestingly, in at least

in some instances, the activity of mammalian PKA appears

to be stimulated by cGMP rather than by cAMP [22]

In the unicellular eukaryote Trypanosoma brucei, the

causative agent of human sleeping sickness in Africa, cAMP

signalling and its role in parasite proliferation and host/

parasite interaction are still poorly understood [23] A large

number of genes coding for different adenylyl cyclases have

been identified [3,24], and one of these enzymes, GRESAG

4.4B, has been further characterized [25] Also, several

cAMP-specific phosphodiesterases have recently been

iden-tified and characterized [26] (S Kunz, P Bern, A Rascon,

S H Soderling and J Beavo, personal communication;

A Rascon and J Beavo, personal communication,

University of Seattle, WA, USA) Little is currently known

about the biological role of cAMP signalling in these

organisms A role for cAMP in the differentiation of long,

slender to short, stumpy forms in the bloodstream of the

mammalian host has been proposed [27] PKA activity has

also been implicated in a mechanism by which T brucei

can remove bound host antibody from its cell surface [28]

The enzyme itself has not yet been characterized in any of

the kinetoplastids, although previous work demonstrated the

presence of a PKA-like kinase activity in T cruzi [29]

The current study describes the identification and

characterization of the regulatory subunit of trypanosomal

PKA (TbRSU) Many of the structural features are well

conserved between TbRSU and its mammalian counterparts

Despite this overall similarity between mammalian and

trypanosomal regulatory subunits, the trypanosomal

homo-log binds cGMP rather than cAMP, and the trypanosomal

PKA is activated by cGMP, but not by cAMP TbRSU thus

represents yet another facet in the amazing kaleidoscope of

cyclic nucleotide signalling

M A T E R I A L S A N D M E T H O D S

Materials

Enzymes were obtained from Roche Diagnostics (Rotkreuz,

Switzerland), and culture media were purchased from Difco

Radiochemicals were from Dupont-NEN (Regensdorf,

Switzerland), while chemicals were obtained from SIGMA

or Fluka (Buchs, Switzerland) Talonw immobilized-cobalt

resin was from Clontech (Basel, Switzerland) DNA

sequencing was outsourced to Microsynth GmbH, Balgach,

Switzerland where the reactions were run with BigDye

terminators (PE-Biosystems) and were analyzed on an ABI

Prism 377 instrument

Cell culture

T brucei strain 427 (derived form MiTat 15a), was grown as

procyclic forms at 27 8C in SDM medium [30]

Mono-morphic bloodstream forms of strain 221 (MiTat 1.2) were

cultivated as described by Hesse et al [31]

Drosophila Schneider 2 (S2) cells and expression vectors

were obtained from Invitrogen (Carlsbad, CA, USA) Cells

were passaged at cell densities between 6 and

20  106mL21 by splitting at a 1 : 2 to 1 : 5 dilution in

complete DESTM medium (Invitrogen) containing 10%

heat-inactivated fetal bovine serum S2 cells are

density-sensitive and do not proliferate when seeded at less than

5  105 mL21 Cells were cultured in a 22 – 24 8C incubator with no extra CO2 supplied Cell viability was checked using the Trypan Blue exclusion test and was routinely found to be between 95 and 99%

Transfection of S2 cells S2 cells were prepared for transfection by seeding 3  106 cells in 3 mL DESTMmedium into a 35-mm Petri dish The culture was incubated at 24 8C until a cell density of

2 – 4  106mL21 was reached (6 – 16 h) Immediately before transfection, the following two solutions were prepared separately (per 35-mm dish) Tube A: 36 mL 2M

CaCl2and 19 mg vector DNA, in a final volume of 300 mL

H2O Tube B: 300 mL 50 mM Hepes, pH 7.1, 1.5 mM

NaH2PO4, 280 mM NaCl The contents of tube A were added slowly (over 1 – 2 min) to tube B under continued mixing The final mixture was incubated at room temperature for 30 – 40 min to allow the precipitate to form The suspension was then well resuspended and added dropwise to the medium of the cell culture After incubation for 16 – 24 h, cells were washed twice with medium to remove the calcium-phosphate precipitate, suspended in fresh growth medium, and further incubated Expression of the recombinant protein was induced by the addition of

15 mL 100 mM CuSO4 per 3 mL culture medium (final concentration 500 mM), and protein expression was assayed

12 – 48 h after induction

When stable cell lines were desired, the cells were cotransfected with plasmid pCoHYGRO (Invitrogen) and were selected for growth in 300 mg:mL21hygromycin B Preparation of the PKA-specific substrate

An expression plasmid coding for a 28-kDa His6-tagged green fluorescent protein with a protein kinase A specific phosphorylation sequence (GFP227-RRRRSII) at its C-terminus was provided by K Shokat, Princeton University, NJ, USA [32] The plasmid was transfected into BL21DE, and positive colonies were identified by their fluorescence under UV light Liquid cultures were grown to

a D595of < 0.4 and were then induced for 4 h with 0.5 mM

isopropyl thio-b-D-galactoside Cells were suspended in

1 – 2% of the original culture volume of ice-cold 50 mM

sodium phosphate, pH 7.0, 300 mM NaCl, and were lysed

by sonication The lysate was cleared by centrifugation for

20 min at 7000 g, and the recombinant protein was adsorbed batchwise to Talonw immobilized-cobalt resin (Invitrogen) and purified according to the manufacturer’s protocol

Immunoprecipitation For the preparation of antibody-coated beads, protein

G – Sepharose beads (Amersham-Pharmacia) were washed twice in NaCl/Pi and then suspended as a 50% slurry in

100 mMphosphate buffer, pH 8.2 Fifty-microliter aliquots

of this slurry were incubated for 1 – 3 h at 4 8C in 500 mL phosphate buffer containing the antibody to be coupled (rat polyclonal antibody against TbRSU1 or a control polyclonal rat antibody directed against an irrelevant protein) Beads were then washed twice in 100 mM phosphate buffer and once in HB buffer (25 m Tris/HCl, pH 8.0, 50 m NaCl)

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For immunoprecipitation, 2  108 trypanosomes were

sedimented at 1300 g for 10 min and were washed twice in

ice-cold NaCl/Pi (137 mM NaCl, 2.7 mM KCl, 4.3 mM

Na2HPO4, 1.4 mM KH2PO4, pH 7.3) The final pellet was

suspended in 240 mL HB buffer and 30 mL Completew

protease inhibitor mix (Roche Molecular Biochemicals)

Thirty microliters lysis buffer (10% deoxycholate, 10%

NP40 in HB buffer) were added, and the mixture was

extensively vortexed After 30 min incubation on ice,

the lysate was centrifuged for 5 min at 10 000 g at 4 8C

200 mL of the supernatant was transferred to a fresh

tube containing 25 mL of the antibody-coated protein

G – Sepharose beads The slurry was gently rocked for 1 h to

overnight at 4 8C Beads were then washed on ice three

times with cold WBI buffer (0.5% NP 40, 0.05%

deoxycholate and 0.05% SDS in NaCl/Pi, pH 7.5), twice

with cold WBII buffer (125 mMTris/HCl, pH 8.2, 500 mM

NaCl, 1 mM EDTA, 0.5% NP40), and finally once with

500 mL kinase buffer (15 mM NaCl, 5 mM MgCl2, 10 mM

Hepes, pH 7.5)

Protein kinase assay

For assaying protein kinase activity in the

immunoprecipi-tates, the following reaction mix was prepared: 1 mL

[32P]gATP (5 mCi:mL21, 150 mMATP), 4 mL of 5  kinase

buffer (75 mM NaCl, 25 mM MgCl2, 50 mM Hepes,

pH 7.5), 1 mL kinase substrate (0.5 – 1 mg), further

additions as required, and H2O to a final volume of

20 mL These 20 mL were added to 10 mL washed

immunoprecipitation beads (corresponding to 2  106

trypanosomes), and the suspension was incubated at 30 8C

for 30 min The reaction was stopped by the addition of

5 mL 5  SDS sample buffer and boiling for 3 min

Expression of a recombinant GST – RSU fusion protein

A sequence fragment of the TbRSU gene recovered from the

T brucei genome project at The Institute for Genetic

Research (TIGR) was used to design two PCR primers

(RSU-1, 50-GAGAGTCGACGCTCAAGGTAGAAGGTA

CGG-30, and RSU-2, 50-AGACTCGAGCTACTTCCTCCC

CTCTGCCC-30; added SalI and XhoI restriction sites

underlined, respectively) The expected 600-bp fragment

was amplified from genomic DNA of T brucei, confirmed

by DNA sequencing and introduced into the multicloning

site of the expression vector pGEX-4T2

(Amersham-Pharmacia) The vector was transformed into Escherichia

coli BL21DE and the recombinant protein was expressed in

high amounts in an insoluble form The protein was

solubilized from the inclusion bodies in 100 mMTris/HCl,

pH 7.5, 5 mM EDTA, 6M urea For renaturation, several

procedures were tried, all of which lead to soluble fusion

protein unable to bind to glutathione – Sepharose Thus, the

fusion protein was purified by gel filtration on a Superdex

200 column, followed by gel electrophoresis After blotting

the protein to nitrocellulose (Schleicher & Schuell BA 85),

the 50-kDa fusion protein band was excised, dissolved in

dimethylsulfoxide and used for immunization

Expression of cNMP-binding domains inDrosophila S2 cells

For the expression of the cNMP-binding domains of TbRSU1 in S2 cells, the respective gene fragments were amplified and cloned into the pMT/V5-His B vector (Invitrogen) In this vector, expression is regulated by a metallothioneine promotor, and it allows induction of expression by the addition of Cu21to the growth medium The recombinant proteins carry a V5 immunological tag and

a His6-tag at their C-termini, which allow for easy detection and purification The cNMP-binding domain A (amino acids

231 – 367) was amplified using primers Adom-F [50 -TATACTAGTATGG(2531)CACTCATCTTGAAGTTGT-30, added Spe I site and start codon, bold underlined] and Adom-R [50-TATCTCGAGA(2938rev)AGGCCACTGAG GAAC-30, added Xho I site underlined] Domain B (amino acids 352 – 499) was amplified using primers Bdom-F [50-TATACTAGTATGC(2921)CGTTCCTCAGTGG-30, added SpeI site and start codon, bold underlined] and Bdom-R [50-TATCTCGAG(3334rev)CTTCCTCCCCT CTG-30, added XhoI site underlined] For amplification of the joint domains (amino acids 231 – 499), primers Adom-F and Bdom-R were used The PCR products were cloned into the pGEM T-Easy vector, verified by DNA sequencing and were finally subcloned into the expression vector pMT/ V5-His B

Purification of recombinant cNMP-binding domains from S2 Drosophilacells

Cells were collected by centrifugation at 500 g for 5 min at

4 8C The cell pellet was suspended in ice-cold lysis buffer (50 mL per mL cell culture; 50 mM Tris/HCl, pH 7.8,

150 mM NaCl, 1% Nonidet P-40; Completew protease inhibitor cocktail was added immediately before use) The lysate was incubated on ice for 20 – 30 min, briefly homogenized in a glass/Teflon homogenizer and finally centrifuged at 7000 g for 20 min at 2 8C To the cleared supernatant, 1/10 volume of a 50% (v/v) suspension of Talonw beads in NaCl/Piwas added, and the suspension was incubated on a rocking platform for 3 h at 4 8C After incubation, the suspension was poured into a small column and was washed extensively with 50 mMsodium phosphate buffer, pH 7.0, 300 mM NaCl Recombinant protein was finally eluted with four aliquots of 100 mL elution buffer (50 sodium phosphate, pH 7.0, 300 mM NaCl, 150 mM

imidazole) The protein containing fractions were pooled, aliquoted, snap-frozen and stored at 270 8C

Cyclic nucleotide binding assays Binding assays were performed in 5 mMsodium phosphate,

pH 6.8, 1 mM EDTA, 25 mM 2-mercaptoethanol, 0.2 mM

isobutyl-methyl-xanthine, 1.5 mg purified protein and increasing concentrations of [3H]cGMP (NEN, catalogue

no NET-337) adjusted to a specific activity of

1 mCi:nmol21 cAMP competition and kinetic experiments were carried out in the presence of 0.4 mM [3H]cGMP Initial experiments were carried out in the presence of

500 mg:mL21histone VIII-S, which increased the binding efficiency by about 50% Histone was omitted in later experiments The binding reactions were incubated on ice

qFEBS 2001 PKA regulatory subunit from T brucei (Eur J Biochem 268) 6199

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overnight Reactions were stopped by the addition of 1 mL

ice cold 10 mMsodium phosphate, pH 6.8, 1 mMEDTA and

were filtered immediately through prewetted Millipore

HAWP filters (0.45 mM) Filters were rinsed three times

with 1 mL ice-cold buffer each, thoroughly dried and

counted in a toluene-based scintillator Dissociation rate

constants were determined by overnight equilibration on ice

of the binding reaction containing 0.4 mM[3H]cGMP After

the addition of a 100-fold excess of unlabelled cGMP,

aliquots were withdrawn and processed for filtration at time

points between 0 and 30 min All reactions were done in

triplicate Binding parameters were determined by curve

fitting using thePRISMsoftware package of GraphPad Inc.,

San Diego, CA, USA

R E S U L T S

Identification of TbRSU1

The DNA database of the T brucei genome project was

searched for predicted proteins containing putative

cAMP-binding domains This search resulted in a 600-bp DNA

sequence which was predicted to code for the C-terminal

fragment of a protein with high similarity to the regulatory subunits of eukaryotic PKAs From the retrieved sequence, PCR primers were designed (see Materials and methods) and were used to amplify the corresponding fragment from genomic DNA of T brucei The resulting PCR fragment of

600 bp was cloned and verified by sequencing It was then used to hybridize genomic blots of T brucei DNA in order

to establish the number of corresponding genes present in the genome When genomic DNA was digested with enzymes that did not cut within the DNA sequence of the hybridization probe (Xho I, Stu I, Spe I, Pst I, Nhe I, Kpn I and HindIII), all digests resulted in a single hybridizing band (Fig 1A), strongly indicating that the new gene, TbRSU, is coded for by a single-copy gene The 600-bp PCR fragment was then used to screen a genomic library of

T brucei in a lambda phage vector [33] This screening resulted in several independent phages containing the same

Fig 1 TbRSU is a single-copy gene (A) Digests of genomic DNA of

T brucei were hybridized with a 600-bp PCR fragment representing the

conserved cNMP-binding domain of TbRSU (B) Map of the TbRSU

locus Nucleotides 1 – 483 code for the C-terminus of a protein of

unknown function (TbTAS ) Nucleotides 1838 – 3334 represent the open

reading frame of TbRSU Nucleotides 3335 – 3566 represent a part of the

30untranslated region of TbRSU The grey boxes designated A and B

represent the predicted cyclic nucleotide binding domains of the

TbRSU protein The sequence has been deposited at GenBank under the

accession number AF326975.

Fig 2 Gene and amino-acid sequence of TbRSU The pseudosub-strate sequence is indicated by the grey box The two cyclic-nucleotide binding domains A and B are boxed Shaded boxes in domain A: Glu311 (is Ala in all homologs, see Fig 3); Thr318 (is Arg in all homologs); Val319 (is Ala in cAMP and Thr in cGMP binding domains) Shaded boxes in domain B: Glu435 (is Ala in all homologs); Asn442 (is Arg in all homologs).

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locus A 3-kb Eco RI fragment was subcloned into

pBlueskriptSK1 and both strands were completely

sequenced The sequence analysis demonstrated that this

fragment contained the entire open reading frame of the

TbRSU gene (Fig 1B)

In parallel, a cDNA library of procyclic T brucei was also

screened with the same PCR fragment, resulting in three

independent phages that all contained a 1500-bp cDNA

fragment All three were sequenced and were shown to

contain a short 50 untranslated region, a complete open

reading frame of 1497 bp, and a 30 untranslated region

terminated by a polyA tract Although all three cDNA

clones were terminated with this sequence, this polyA tract

probably does not represent the polyA tail of the mRNA

because a sequence of 12 adenosine residues following

T3566 was is present in a genomic clone of the T brucei

genome project (accession number AQ 644384) that extends

beyond this region The sequences of the open reading

frames of all three cDNAs were identical to that obtained

from the genomic fragment Upstream of the TbRSU gene,

the 30 end of an open reading frame was identified

(nucleotides 1 – 486 of the genomic fragment), which coded

for an unidentified protein termed TbTAS The stop codon of

this open reading frame is separated from the start codon of

TbRSU by 1352 bp, including a pyrimidine-rich region

Predicted amino-acid sequence of TbRSU

The open reading frame of TbRSU predicts a protein of 499

amino acids, with a calculated Mr of 56 725 (Fig 2)

Overall, the protein shares extensive sequence homology

with mammalian PKA regulatory subunits type I The

N-terminal domain of TbRSU (amino acids 1 – 242) is

longer than the N-termini of its mammalian homologs, and it

bears no identifiable functional domains In analogy to

mammalian type I regulatory subunits, the cysteine residues

Cys15 and Cys67 may be involved in dimer formation,

although such dimers could not be detected in cell lysates

analysed by gel filtration chromatography (data not shown)

In these experiments, TbRSU always migrated as a monomer Residues 202 – 206 (-ArgArgThrThrVal-) rep-resent the pseudo-inhibitor site which is involved in the interaction with the catalytic domain [34] Amino acids

243 – 360 and 363 – 483 form the cyclic nucleotide binding domains A and B, respectively Based on the structural model of the bovine regulatory subunit RIa [17], Glu309 and Glu433 form a hydrogen bond with the 20 hydroxyl of the ribose of the bound cNMP, while Leu310 and Leu434 interact with a nitrogen of the pyrimidine ring of the base Tyr370 and Tyr482 are probably the functional homologs of Trp260 and Tyr371 in bovine RIa, allowing base-stacking with the purine residue Unexpectedly, a strongly conserved arginine residue, which forms a hydrogen bond to the phosphate group, is replaced by threonine (Thr318) and asparagine (Asn442) in domains A and B, respectively (Fig 3) Sequencing errors or allelic variation at these sites are unlikely as identical sequences have been obtained by independent sequencing of TbRSU from different trypano-some strains (accession nos AQ638897 and AF182823) A further difference between TbRSU and the PKA regulatory subunits from other eukaryotes is seen in Val319 All cAMP-binding domains of the regulatory subunits carry an alanine residue at this position, while the closely related cGMP-binding domains of protein kinase G always contain either threonine or serine residues

TbRSU mRNA is more abundant in bloodstream forms

To explore if TbRSU is differentially expressed in the different life stages of T brucei, total RNA was extracted both from bloodstream and from procyclic forms and was analyzed by Northern blotting and hybridization RNA loading was quantitated by ethidium bromide staining to visualize the ribosomal RNA before blotting the gel, and by hybridization of the filter with a DNA probe specific for b-tubulin [35] The extent of hybridization of both probes was quantitated using a PhosphorImager TbRSU mRNA is clearly detectable in both life cycle stages (Fig 4A)

Fig 3 Sequence comparison of cNMP-binding

domains of PKA regulatory subunits and of

protein kinase G cNMP-binding domains A and

B are indicated by grey boxes Amino-acid

numbering of the respective proteins is given A:

Rattus norvegicus type I (accession number

P09456); B: D melanogaster (P16905); C:

Caenorhabditis elegans (P30625); D:

D discoideum (P05987); E: S cerevisiae

(P07278); F: Schizosaccharomyces pombe

(P36600); G: TbRSU (AF326975); H:

Homo sapiens protein kinase G (O13237); I:

D melanogaster protein kinase G (O03043).

Filled circles denote amino acids conserved in all

sequences Open squares denote amino acids

which are conserved in all sequences, but differ in

TbRSU.

qFEBS 2001 PKA regulatory subunit from T brucei (Eur J Biochem 268) 6201

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However, the steady-state level of TbRSU mRNA in

blodstream forms is about five times higher than it is in

procyclic forms

The TbRSU protein is present both in bloodstream and in

procyclic forms

To follow up the results of the Northern blotting experiments

on the protein level, whole cell lysates were analyzed by

immunoblotting, using an affinity-purified polyclonal

antibody raised against recombinant TbRSU (see Materials

and methods) This polyclonal antibody not only recognizes

TbRSU in trypanosomes, but it also detects PKA regulatory

subunits in other organisms such as Saccharomyces

cerevisiae and mammalian cells (Fig 4B) The TbRSU

protein is readily detectable both in bloodstream and in

procyclic forms, and it migrates as a single band of a Mrof

55 000, in agreement with its calculated Mr of 56 726 Similarly to what was observed with TbRSU mRNA, the TbRSU protein is much more abundant in bloodstream than

in procyclic forms

Co-immunoprecipitation of PKA with TbRSU Sequence analysis clearly established TbRSU as a homolog

of the type I regulatory subunits of mammalian PKA In order to functionally verify if TbRSU is associated with a kinase in vivo, TbRSU was immunoprecipitated from whole cells lysates using the polyclonal rat antibody Immunopre-cipitates were first analyzed by immunoblotting with a polyclonal rabbit antibody against the catalytic subunit of bovine PKA In these experiments, the antibody detected a protein with a Mr of about 40 000, suggesting that the catalytic subunit of trypanosomal PKA does in fact coprecipitate with TbRSU Inspection of the T brucei databases identified several DNA sequences that code for a homolog of a PKA catalytic subunit The catalytic activity

of the immunoprecipitates was then analysed by incubation

in kinase reaction buffer in the presence or absence of a recombinant PKA-specific substrate [32] and 20 mMcAMP Analysis of the reaction products by gel electrophoresis and autoradiography (Fig 5) demonstrated that the coimmuno-precipitates did indeed contain a kinase activity which phosphorylated the PKA-specific substrate No phosphoryl-ation of the substrate was observed when either no antibody,

or an irrelevant antibody, was used for immunoprecipitation,

or when the TbRSU antibody was used in the absence of cell lysate Unexpectedly, the addition of 20 mM cAMP to the reactions did not stimulate the kinase activity, but had either

Fig 4 TbRSU is more abundant in bloodstream than in procyclic

forms (A) Northern blot analysis Ten-microgram aliquots of total

RNA of procyclic (PC) or bloodstream form (BSF) trypanosomes were

loaded per slot After transfer, the filter was successively hybridized

with a TbRSU probe (a) and a probe for b-tubulin (b) After

electrophoresis, the gel was stained with ethidium bromide to control

for equal loading (c) (B) Hybridization was quantified using a

PhosphorImager (a) Hybridization with TbRSU; (b) hybridization with

a b-tubulin probe Grey bars, procyclics; black bars, bloodstream forms.

(C) Immunoblot analysis (a) The polyclonal antibody raised against

recombinant TbRSU recognizes homologs in a wide spectrum of

species 1, Whole cell lysate from E coli expressing the GST – TbRSU

fusion protein used for raising the antibody; 2, whole cell lysate of

T brucei; 3, whole cell lysate of S cerevisiae; 4, whole cell lysate of

COS (monkey) cells (b) Immunoblot of equivalent amounts of whole

cell lysates of bloodstream (B) and procyclic (P) trypanosomes.

Molecular mass markers are indicated for each panel.

Fig 5 The TbRSU antibody coimmunoprecipitates a protein kinase activity which phosphorylates a PKA-specific substrate Protein kinase activity assays of immunoprecipitates (Top) Coomassie-stained gels, molecular mass markers are IgG heavy chain (50 kDa) and the PKA substrate (30 kDa); (bottom) corresponding autoradiographs, arrowheads indicate the position of the PKA substrate (A) Immunoprecipitation with no antibody; (B) immunoprecipitation with TbRSU antibody; (C) immunoprecipitation with irrelevant antibody (against the phosphodiesterase TbPDE1; S Kunz, personnal communi-cation); (D) immunoprecipitation with TbRSU antibody, but without cell lysate Beads were incubated for activity assays as follows: lanes 1: kinase buffer; lanes 2: kinase buffer plus 20 m M cAMP; lanes 3: kinase buffer plus PKA-substrate; lanes 4: kinase buffer plus PKA-substrate plus 20 m M cAMP

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no effect or inhibited it While the absence of stimulation by cAMP was consistent in all of the many independent experiments carried out (see also below), the inhibitory effect of cAMP was observed in some, but not in all experiments

Phosphorylation of the PKA-specific substrate by the immunoprecipitates was time-dependent, Mg21-dependent and was quenched by an excess of unlabelled ATP (data not shown) These results demonstrated that a protein kinase activity was coimmunoprecipitated with TbRSU under our conditions Phosphorylation of the PKA-specific substrate by this activity suggested that it represented PKA This was further corroborated by the observation that the co-immunoprecipitating kinase activity was inhibited

by the highly PKA-specific peptide inhibitor PKI [36] (Fig 6)

PKA activity is stimulated by cGMP, but not by cAMP When kinase activity of TbRSU immunoprecipitates was assayed in the presence or absence of 20 mM cAMP, no stimulation of phosphorylation of the PKA-specific substrate could be detected In contrast, control reactions using mammalian COS cell lysates precipitated by the same antibody, exhibited the expected stimulation of kinase activity by cAMP (Fig 7A) This unexpected absence of stimulation of trypanosomal PKA activity by cAMP was consistently observed over many independent experiments (see above) However, when similar experiments were performed with cGMP instead of cAMP, a marked stimulation of kinase activity was consistently observed (Fig 7B – D) The phosphorylation reactions followed a similar time course in the presence and in the absence of cGMP (Fig 7B), but the overall kinase activity was stimulated threefold to fourfold by cGMP The kinase reaction was stimulated to a similar extent in immunoprecipitates from procyclic and bloodstream form trypanosomes (Fig 7C,D), with maxi-mum stimulation reached around 20 mM cGMP These unexpected findings suggested that the trypanosomal TbRSU, in contrast to its homologs in all other eukaryotes analysed so far, is activated by cGMP rather than by cAMP

cGMP binding to the cyclic nucleotide binding domains A and B sites of TbRSU

In order to directly confirm if TbRSU does in fact bind cGMP, expression of the recombinant domains was attempted in E coli Expression of domain B alone produced ample recombinant protein, but all in insoluble form Expression of the combined A and B domains resulted

in much less protein (all insoluble) Expression of domain A alone proved impossible, despite much effort, in agreement with earlier observations that this domain is highly toxic for

E coli [37] Thus, domains A and B were expressed individually in the Drosophila cell line S2, under the control

of a Cu21-inducible metallothionein promoter Similarly to what was observed in E coli, domain B was well expressed, while domain A again resulted in very poor cell growth and

in low amounts of recombinant protein The individual domains A and B were purified by cobalt-affinity chromatography, and were assayed for cGMP binding

Fig 6 PKI inhibits the activity of coimmunoprecipitating kinase.

Immunoprecipitates were incubated for 10 min under phosphorylation

conditions with PKA substrate in the presence or absence of PKI

inhibitor peptide (10 mg per 30 mL reaction mix) (A) autoradiogram of

PKA substrate; (B) Coomassie-stained PKA substrate; (C)

Phosphor-Imager analysis of the gel shown in (A).

Fig 7 The kinase activity which coimmunoprecipitates with

TbRSU is stimulated by cGMP, but not by cAMP (A) Whole cell

lysates from mammalian COS cells and from T brucei were

immunoprecipitated with antibody against TbRSU, and the

immuno-precipitates were assayed for PKA activity in the presence or absence of

20 m M cAMP (B) Time course of kinase activity of immunoprecipitates

from T brucei in the presence (grey boxes) or absence (white boxes) of

cGMP (C and D) Effect of increasing cGMP concentrations on the

kinase activity of immunoprecipitates (autoradiographs) (C0and D0)

Coomassie stained PKA substrate bl, blank reaction incubated in the

presence of 20 m M cGMP, but without protein substrate (C and C 0 )

procyclics; (D and D0) bloodstream forms.

qFEBS 2001 PKA regulatory subunit from T brucei (Eur J Biochem 268) 6203

Trang 8

(Fig 8) Both domains exhibited very similar Kdvalues for

cGMP (domain A: 7.51 ^ 1.97 mM, n ¼ 3; domain B:

11.43 ^ 2.24 mM, n ¼ 3) For both domains, cAMP did

not measurably compete with cGMP binding up to a

100-fold excess of cAMP over cGMP Dissociation rate

constants for cGMP were also very similar between the two

domains (domain A 0.24 min21, n ¼ 3, and domain B

0.36 ^ 0.18 min21, n ¼ 3)

D I S C U S S I O N

The current study reports the identification of the regulatory

subunit of PKA from the parasitic protozoon T brucei,

TbRSU Several previous attempts to purify the PKA

holoenzyme from this organism had failed, although an

activity resembling the catalytic subunit could be identified

[29] Similarly, attempts in several laboratories, including

our own, to demonstrate cAMP-specific protein

phosphoryl-ation in T brucei were unsuccessful TbRSU was

originally identified by searching of the T brucei sequence

databases for putative cAMP-binding proteins The full

gene was then isolated by screening genomic and

cDNA libraries Sequence analysis demonstrated that

TbRSU is closely related to the mammalian type I

PKA regulatory subunits, with the only major difference

being the significantly longer N-terminus of the

trypanoso-mal protein

The two cyclic nucleotide binding domains exhibit

sequence similarities with both the cAMP-binding domains

of the PKA regulatory subunits from yeast to mammals, as

well as with the cGMP-binding domains of protein kinase

G Unexpectedly, one absolutely conserved arginine residue

in each of the two domains is replaced by Thr318 and

Asn442 in TbRSU In the bovine regulatory subunit, and by

inference also in all its homologs, these arginine residues

form a hydrogen bond to the phosphate group of the bound

nucleotide [19] Sequencing errors can be ruled out as a

simple reason for this variation, as this region was

independently sequenced by three different laboratories

using different trypanosome strains The functional

implication of this amino-acid substitution remains to be

explored Eight amino acids before Thr318 and Asn442,

another amino-acid substitution peculiar to TbRSU has

occurred: Glu311 and Glu435 replace otherwise invariant

alanine residues Thirdly, Val319 represents another

substitution that sets TbRSU apart from its homologs At

the equivalent position, the other PKA regulatory domains contain an alanine residue while protein kinases G contain serine or threonine The hydroxyl side chain of either one of these residues interacts with the C2 amino group of cGMP and is essential for full activation of cGMP dependent protein kinases [38]

The gene encoding TbRSU is expressed both in the bloodstream and in the procyclic forms of the parasite, but at much higher levels in the bloodstream form The TbRSU protein levels in both life cycle stages closely correspond to the mRNA levels

Immunoprecipitation of TbRSU consistently coprecipi-tated a protein kinase activity exhibiting many character-istics of the catalytic subunit of trypanosomal PKA The coprecipitated kinase is recognized by an antibody against the bovine PKA catalytic subunit, the enzyme phosphorylates a PKA-specific substrate [32], and its activity is strongly inhibited by the rabbit PKI inhibitor peptide [36]

While the protein kinase activity recovered in the immunoprecipitates exhibited all the characteristics of a canonical PKA catalytic subunit, no stimulation by cAMP could be detected On the contrary, cAMP appeared to inhibit the protein kinase activity in some, but not all, experiments Surprisingly, a marked stimulation of protein kinase activity was consistently found with cGMP This stimulation was concentration-dependent, reaching its maximum at < 20 mM cGMP The interaction of TbRSU with cyclic nucleotides was further investigated using the recombinant cNMP-binding domains A and B Both domains did bind cGMP with Kd values in the low micromolar range (7.5 and 11.4 mM, respectively) This value is unexpectedly high when compared to the Kdvalues determined for cAMP of mammalian PKA regulatory subunits (1.2 and 1.7 nMfor domains A and B, respectively [39]) However, the results are in good agreement with the PKA activation experiments presented in this study, which exhibited a maximal activation of the kinase at about 20 mM

cGMP This value is almost 200-fold higher than the apparent activation constant of mammalian PKA (120 nM; [17]) Binding of cGMP was not affected by cAMP, up to an excess of at least 100-fold Again, the results agree well with the observations that the kinase activity was not stimulated

by cAMP at concentrations of up to 20 mM In marked contrast to the mammalian regulatory subunit where the two domains differ considerably in their dissociation rate constants (0.15 min21vs 0.04 min21[17]), both domains

of TbRSU behave very similarly (0.24 min21for domain A and 0.36 min21for domain B)

The observation that protein kinase A in T brucei (and probably also in other kinetoplastids) is regulated by cGMP rather than by cAMP implies that cGMP has an important signalling role in this group of organisms Earlier work had demonstrated the presence of cGMP in T cruzi [40], and several members of a family of recently identified cAMP-specific phosphodiesterases of T brucei [26] (A Rascon,

S H Soderling & J Beavo, personal communication) contain one or two GAF-domains [41] that may be involved

in cGMP binding While these phosphodiesterases may represent an interconnection between the cAMP- and the cGMP-signalling pathways in T brucei, the cGMP-regu-lated TbRSU/PKA kinase may well represent the major effector of cGMP signalling in these organisms

Fig 8 The cNMP-binding domains of TbRSU bind cGMP, but not

cAMP Saturation binding of of cGMP to recombinant domains A and B

of TbRSU Data represent one of three very similar experiments.

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A C K N O W L E D G E M E N T S

We are grateful to Kevin Shokat (Princeton University, Princeton, NJ,

USA) for providing his plasmid for the expression of recombinant PKA

substrate, to Brian Hemmings (Friedrich Miescher Institute, Basel) for

his generous supply of antibody against bovine heart PKA catalytic

subunit, and to Ursula Kurath and Erwin Studer for producing the

trypanosomes Special thanks go to Min Ku for her careful reading of

the manuscript, and to Michael Boshart (Free University, Berlin) for

communicating unpublished results and for stimulating discussions.

This work was supported by grants 31-046760.96 and 31-058927.99 of

the Swiss National Science Foundation, grant C98.0060 of COST

program B9 of the European Union, and by the UNDP/World Bank/

WHO Special Programme for Research and Training in Tropical

Diseases

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