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Báo cáo khoa học: Characterization of the role of a trimeric protein phosphatase complex in recovery from cisplatin-induced versus noncrosslinking DNA damage potx

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After cisplatin treatment is terminated, pph3D, psy4D and psy2D mutants are delayed as compared with the WT strain in the dephosphoryla-tion of Rad53p.. [13] found that, during recovery

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phosphatase complex in recovery from cisplatin-induced versus noncrosslinking DNA damage

Cristina Va´zquez-Martin, John Rouse and Patricia T W Cohen

Medical Research Council Protein Phosphorylation Unit, College of Life Sciences, University of Dundee, UK

The chemotherapeutic agents cisplatin

(cis-diamminedi-chloroplatinum) and oxaliplatin are currently used for

the treatment of tumours in a variety of tissues, such

as testis, ovary, lung, bowel, head, and neck These

platinum-containing agents form adducts with DNA

that produce intrastrand and interstrand nucleotide

crosslinks [1], and are thought to be effective because

the DNA damage triggers apoptosis of cancerous cells

In response to these chemotherapeutic agents, ionizing radiation and chemical mutagens, activation of the DNA damage response pathways causes arrest of the cell cycle to allow time for cells to repair the DNA before the cell cycle resumes If the DNA cannot be repaired or the damage bypassed, apoptosis is initi-ated Protein phosphorylation plays a key role in the DNA damage response, but the protein phosphatases

Keywords

cisplatin; histone 2AX;

methylmethanesulfonate; PPH3;

protein phosphatase 4

Correspondence

P T W Cohen, MRC Protein

Phosphorylation Unit, College of Life

Sciences, Sir James Black Centre,

University of Dundee, Dow Street, Dundee

DD1 5EH, UK

Fax: +44 1382 223778

Tel: +44 1382 384240

E-mail: p.t.w.cohen@dundee.ac.uk

(Received 29 April 2008, revised 11 May

2008, accepted 23 June 2008)

doi:10.1111/j.1742-4658.2008.06568.x

Cisplatin (cis-diamminedichloroplatinum) and related chemotherapeutic DNA-crosslinking agents are widely used to treat human cancers Saccha-romyces cerevisiae with separate deletions of the genes encoding the trimeric protein serine⁄ threonine phosphatase (Pph)3p–platinum sensitivity (Psy)4p–Psy2p complex, are more sensitive than the isogenic wild-type (WT) strain to cisplatin We show here that cisplatin causes an enhanced intra-S-phase cell cycle delay in these three deletion mutants The C-termi-nal tail of histone 2AX (H2AX) is hyperphosphorylated in the same mutants, and Pph3p is found to interact with phosphorylated H2AX (cH2AX) After cisplatin treatment is terminated, pph3D, psy4D and psy2D mutants are delayed as compared with the WT strain in the dephosphoryla-tion of Rad53p In contrast, only pph3D and psy2D cells are more sensitive than WT cells to methylmethanesulfonate, a noncrosslinking DNA-alkylat-ing agent that is known to cause a Rad53p-dependent intra-S-phase cell cycle delay Dephosphorylation of Rad53p and the recovery of chromosome replication are delayed in the same mutants, but not in psy4D cells By com-parison with their mammalian orthologues, the regulatory subunit Psy4p is likely to inhibit Pph3p catalytic activity The presence of a weak but active Pph3p–Psy2p complex may allow psy4D cells to escape from the Rad53p-mediated cell cycle arrest Overall, our data suggest that the trimeric Pph3p– Psy4p–Psy2p complex may dephosphorylate both cH2AX and Rad53p, the differences lying in the more stable interaction of the Pph3 phosphatase with cH2AX as opposed to a transient interaction with Rad53p

Abbreviations

ATM, ataxia telangiectasia mutated; ATR, ataxia telangiectasia and RAD53 related; 4NQO, 4-nitroquinoline 1-oxide; FACS, fluorescent activated cell sorter; H2AX, histone 2AX; MMS, methylmethanesulfonate; PFGE, pulsed-field gel electrophoresis; Pph, Saccharomyces cerevisiae protein serine ⁄ theonine phosphatase; Ppp ⁄ PP, protein serine ⁄ threonine phosphatase in mammals and Drosophila; Ppp4c, protein phosphatase 4 catalytic subunit (also termed PP4, PPX); Psy, platinum sensitivity; WT, wild-type; cH2AX, phosphorylated histone 2AX.

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that participate in these pathways are not well

delin-eated Several studies have implicated complexes of

protein serine⁄ threonine phosphatase (Pph)3p in the

DNA damage response pathways in the budding

yeast Saccharomyces cerevisiae Cells lacking Pph3p

(Ydr075w) and an interacting protein Yln201c [2,3],

the yeast orthologues of mammalian protein

phospha-tase 4 catalytic subunit (Ppp4c) and its regulatory

subunit, R3, respectively [4], were reported to be more

sensitive to the chemical mutagen

methylmethanesulfo-nate (MMS), which alkylates DNA [5] These mutants

were also found to be more sensitive to cisplatin and

oxaliplatin, so Yln201c was designated platinum

sensitivity 2 (Psy2)p [6] Surprisingly, Ybl046w was not

identified being as sensitive to DNA-damaging agents

in this screen, although it had been identified in Pph3p

complexes by systematic analyses of the yeast proteome

[2,3], and its putative mammalian homologue R2 had

been identified as a core regulatory subunit in

com-plexes with Ppp4c [7] However, subsequent

investiga-tions showed that strains deleted for Pph3p, Psy2p and

Ybl046w were all sensitive to cisplatin [4,8], and

Ybl046w was designated Psy4p [9]

One of the earliest events in the cellular response to

many DNA-damaging agents is the phosphorylation of

histone 2AX (H2AX) at Ser129 in its C-terminal tail

and the accumulation of the phosphorylated histone

(cH2AX) at the sites of DNA damage [10,11] In the

deletion mutants pph3D, psy4D and psy2D, Keogh

et al [12] found that H2AX was hyperphosphorylated

as compared with the wild-type (WT) strain in both

the absence and the presence of ionizing radiation that

caused a G2⁄ M cell cycle arrest, implicating Ph3p–

Psy4p–Psy2p in the dephosphorylation of cH2AX and

efficient recovery from the checkpoint Substitution of

the H2AX Ser129 by Ala restored the ability of the

pph3D strain to turn off checkpoint signalling in a

timely manner and re-enter the cell cycle after DNA

repair of the double-strand break [12] Although the

studies of Hanway et al [5] showed that pph3D and

psy2D cells were more sensitive to MMS than were

WT cells, Keogh et al [12] reported that the pph3D,

psy4D and psy2D cells were only more sensitive than

WT cells to MMS if the cells also carried deletions of

genes involved in recombination and repair of DNA

While our studies were in progress, O’Neill et al [13]

found that, during recovery from MMS-induced DNA

damage, Rad53p dephosphorylation and resumption

of DNA synthesis are delayed in pph3D and psy2D

cells as compared with WT cells but not in psy4D cells

Consistent with this report, earlier studies had reported

that Rad53p, a key controller of the DNA damage

response pathways leading to intra-S-phase cell cycle

arrest, interacted with Psy2p in a yeast two-hybrid screen [14] Here we examine the roles of Pph3p, Psy2p and Psy4p in response to the DNA-crosslinking agent cisplatin and the noncrosslinking, alkylating agent MMS, and show that recovery after cisplatin-induced DNA damage is delayed in pph3D, psy4D and psy2D mutant cells, whereas it is only delayed in pph3D and psy2D cells after MMS-induced DNA damage

Results Role of Pph3p and its regulatory subunits Psy4p and Psy2p in the cell cycle arrest induced by cisplatin and MMS

In order to determine how the members of Pph3p complex affect the S cerevisiae cell cycle on treatment with cisplatin, we subjected the WT diploid BY4743 cells and the pph3D, psy4D and psy2D mutant cells to analysis on a fluorescent activated cell sorter (FACS) machine after incubation with 2 mm cisplatin for vari-ous times Figure 1A shows that at 90 and 120 min, the pph3D, psy4D and psy2D mutants were appreciably affected by the drug, with an increased fraction of cells accumulating in S-phase, whereas the WT cells were largely unaffected Although the evidence for an intra-S-phase cell cycle delay is less conclusive in psy4D cells than in pph3D and psy2D cells, examination of growth

on YPD plates demonstrates that deletion of any com-ponent of Pph3p–Psy4p–Psy2p decreases cell prolifera-tion in the presence of cisplatin, and that this trimeric Pph3p complex confers resistance to cisplatin (Fig 1B) [4,8,9]

MMS slows progression through S-phase in WT

S cerevisiae by methylation of DNA on N7 -deoxygua-nine and N3-deoxyadenine [15,16] The differing reports as to whether pph3D, psy4D and psy2D mutants were more sensitive than WT cells to MMS [5,12] led

us to compare the sensitivity of the mutants to increas-ing concentrations of MMS, and our results are in line with those of Hanway et al [5] We demonstrated that pph3D and psy2D mutants were more sensitive than the

WT strain when inoculated onto YPD plates contain-ing 0.03% MMS, whereas the psy4D mutant was no more sensitive than the WT strain to 0.03% MMS on YPD plates (Fig 1C) We also treated the cells in liquid culture (0.03% MMS) and plated them on YPD plates, obtaining the same results (data not shown) In addition, we investigated the sensitivity to another DNA-damaging agent, 4-nitroquinoline 1-oxide (4NQO), which also affects S-phase The pph3D and psy2D mutants were more sensitive than the WT strain

to the UV mimetic 4NQO (20 lgÆmL)1 on plates),

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whereas the psy4D mutant showed a similar sensitivity

to that of the WT strain (data not shown) These

results appear to support a role for Pph3p–Psy2p in

conferring resistance to MMS and 4NQO, and are in

contrast to the effects of cisplatin, which imply a role

for Pph3p–Psy4p–Psy2p in conferring resistance to

cisplatin (Fig 1B) [8,9]

S cerevisiaecells often respond to DNA damage by

activating a signal transduction pathway that leads to

phosphorylation of Rad9p by Mec1p Rad9p

phos-phorylation allows recruitment of Rad53p to Mec1–

Rad9, facilitating Rad53p phosphorylation by Mec1

Rad53p autophosphorylation then leads to an active

Rad53p that is multiply phosphorylated [17], and the phosphorylation can be detected by SDS⁄ PAGE and immunoblotting as bands that migrate more slowly than Rad53p As the protein kinase Rad53p was reported to interact with Psy2p [18], we investigated whether cisplatin treatment caused the activation of Rad53p in WT, pph3D, psy4D and psy2D cells, but we found that Rad53p was not phosphorylated in response to 2 mm cisplatin [9], although this concentra-tion could induce a cell cycle delay (Fig 1A) Use of higher concentrations can be a problem due to cisplatin insolubility, but we have now been able to demonstrate phosphorylation of Rad53p after

DNA content: 2C 4C 2C 4C 2C 4C 2C 4C

min

120 90 60 30

Untreated

B

1 2 3 4 5 6

WT MT

Cisplatin concentration

0 m M

5 m M

1 2 3 4 5 6

WT MT

10-fold yeast dilution

0%

0.01%

0.03%

1 3 5

WT MT

1 3 5

WT MT

MMS (v/v) concentration

1 3 4 6

WT MT

C

Fig 1 Pph3p complexes confer resistance

to DNA-damaging agents (A) The diploid

WT strain BY4743 and mutants pph3D,

psy4D and psy2D were grown to

mid-expo-nential phase in liquid culture and incubated

in the presence of cisplatin (2 mM) or left

untreated Samples for FACS analysis were

taken at the indicated time points (B, C)

The sensitivities of the same WT and

mutant (MT) cells to cisplatin and MMS

were examined Serial dilutions of

indepen-dent colonies (WT 1, 2 and 3) on all plates

are from the control BY4743 (Y20000)

strain Serial dilutions of independent

colo-nies (MT 4, 5 and 6) are from strains pph3D

(Y34010, left columns), psy4D (Y33072,

middle columns), and psy2D (Y32011, right

columns) The cisplatin and MMS

concentra-tion in each row of plates is indicated on

the right Plates were incubated at 30 C for

48 h.

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ment of yeast cells with 3 mm cisplatin (Fig 2A, top

left panel) On examining the recovery after different

times, we could see a slight decrease in the Rad53p

phosphorylation in the WT strain after 4 h, a

pro-nounced decrease at 6 h, and a return to the

unphos-phorylated basal state by 9 h In contrast, Rad53p was

phosphorylated at 4 h and remained at least partially

phosphorylated in pph3D, psy4D and psy2D mutants

during recovery up to 9 h The experiment was

per-formed five times

In response to MMS treatment, DNA

damage-induced phosphorylated forms of Rad53p occurred in

the WT strain and in pph3D, psy4D and psy2D mutant

cells (Fig 2B, top left panel) On examining the

recov-ery after different times, we saw a pronounced

decrease in Rad53p phosphorylation in the WT and

psy4D strains at 5–7 h In contrast, phosphorylated

forms of Rad53p remained in the pph3D and psy2D

strains during recovery between 5 h and 7 h This

experiment was performed four times

Our data suggest that a complex of Pph3p and

Psy2p may dephosphorylate Rad53p after it has been

activated and phosphorylated in response to MMS,

but that cisplatin-induced activation and

phosphoryla-tion of Rad53p may require a complex of Pph3, Psy4p

and Psy2p for dephosphorylation to occur as rapidly

as in WT cells Considering that Pph3p

dephosphory-lates Rad53p, we investigated the interaction between

Rad53p and Pph3p–Psy4p–Psy2p by coimmunoprecipi-tation In untreated AY925 cells, or cells treated with 0.03% MMS to induce Rad53p phosphorylation, Rad53p was not coimmunoadsorbed with HA3–Pph3p and Psy4p–MYC13 (Table 1, and data not shown), indicating that this interaction may be transient or too weak to withstand the isolation protocol

Pph3p–Psy4p–Psy2p dephosphorylates cH2AX The form of H2AX phosphorylated at Ser129 (termed cH2AX), which is induced in response to DNA-dam-aging agents, is normally removed before resumption

of the cell cycle, and Keogh et al [12] have presented evidence that Pph3p–Psy4p–Psy2p is involved in this process In untreated pph3D, psy4D and psy2D cells, we found that the phosphorylation of H2AX was mark-edly elevated as compared with the barely detectable levels of cH2AX in WT cells (Fig 3A,B) Treatment with cisplatin or MMS elevated cH2AX in WT cells and led to a further increase in the pph3D, psy4D and psy2D cells (Fig 3A, cisplatin treatment; Fig 3B, MMS 2 h recovery) After removal of cisplatin and MMS, the cH2AX levels returned to the near-zero basal levels in the WT cells after several hours but remain elevated in the pph3D, psy4D and psy2D cells (Fig 3A, 8 h; Fig 3B, 12 h) These results indicate that the three subunits of Pph3p–Psy4p–Psy2p acting

Rad53 Rad53P Rad53

Rad53P

Rad53 Rad53P

Rad53 Rad53P

Rad53 Rad53P

WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2

WT pph3 psy4 psy2 WT pph3 psy4 psy2

WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2

WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2

Rad53 Rad53P

Recovery 2 h

Rad53 Rad53P

A

B

Fig 2 Relationship between Rad53p and the Pph3p complex The diploid WT strain BY4743 and mutants pph3D, psy4D and psy2D were grown to mid-exponential phase in liquid culture and left untreated (UN) or incubated in the presence of 3 mM cisplatin (A) or 0.03% MMS (B) for 90 min Cells were filtered, washed free of cisplatin, and incubated at 30 C in YPD, and samples were taken at the indicated times during recovery Trichloroacetic acid extracts were prepared and subjected to immunoblot anal-ysis with antibodies against Rad53p, which detect the unphosphorylated Rad53p (92 kDa) and more slowly migrating phos-phorylated forms.

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together normally dephosphorylate cH2AX and are

essential for its complete dephosphorylation

Taking into account a role for Pph3p–Psy4p–Psy2p

in dephosphorylation of cH2AX, we investigated

whether there was any interaction between the

phos-phatase and the histone Employing lysates from the

S cerevisiae cells AY925 PSY4–MYC13 and

AY925HA3–PPH3, cH2AX was found in the anti-HA

immunopellets (Fig 3C bottom panel) and in the

anti-MYC immunopellets (data not shown), but not in the

immunopellets from the control cells that did not

express the tagged proteins (Fig 3C, top panel)

HA3–Pph3p interacted with increasing amounts of

cH2AX generated in the presence of increasing doses

of MMS (Fig 3C) and even with the low levels of cH2AX that were sometimes present in yeast cell ly-sates in the absence of DNA-damaging agents (data not shown) Most of the cH2AX is bound to the phos-phatase even after treatment with 0.5% MMS (Fig 3C, bottom panel) Given that endogenous Pph3p–Psy4p–Psy2p is also present in the cells, it appears likely that all of the cH2AX is bound to the phosphatase No increases in the levels of the catalytic subunit HA3–Pph3p or the regulatory subunit Psy4p– MYC13 (data not shown) were observed after DNA damage induced by MMS

Recovery 2 h Recovery 6 h Recovery 12 h

H2A/H2B H2AX

H2A/H2B H2AX

Recovery 2 h Recovery 4 h

H2A/H2B H2AX

WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2

WT pph3 psy4 psy2 WT pph3 psy4 psy2

WT pph3 psy4 psy2 WT pph3 psy4 psy2

WT pph3 psy4 psy2 WT pph3 psy4 psy2 WT pph3 psy4 psy2

H2A/H2B H2AX

Recovery 6 h Recovery 8 h

H2A/H2B H2AX A

B

C

Fig 3 The Pph3p complex is required for

dephosphorylation of cH2AX The diploid

WT strain BY4743 and mutants pph3D,

psy4D and psy2D were grown to

mid-expo-nential phase in liquid culture and left

untreated (UN) or incubated in the presence

of 2 mM cisplatin (CDDP) (A) or 0.03%

MMS (B) for 90 min Cells were filtered,

washed free of cisplatin, and incubated at

30 C in YPD, and samples were taken at

the indicated times during recovery

Trichlo-roacetic acid extracts were prepared and

subjected to immunoblot analysis with

anti-bodies against cH2AX

(H2AXphospho-Ser129) Lower panels are blots probed for

total H2A ⁄ H2B as a control (C) The Pph3p

complex associates with cH2AX Lysates

from control WT AY925 cells and AY925

HA3–Pph3p cells untreated or treated with

MMS at the indicated concentrations were

immunoadsorbed with antibodies to HA and

probed for cH2AX Lysate (L), 50 lg; the

supernatant (S, same volume as lysate)

and pellet (P, from 2 mg of lysate) were

obtained by centrifugation following the

immunoadsorption.

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Pph21p and Pph22p are protein phosphatases that

are highly related to Pph3p, and in some cases show

overlapping function with Pph3 [19] S cerevisiae

cells with deletions of the genes encoding both

Pph21p and Pph22p have extremely low viability As

the most abundant isoform is Pph21p, we examined

pph21D cells in order to determine whether Pph21p

may be partly responsible for the dephosphorylation

of cH2AX in yeast We treated WT and pph21D

cells with 2 mm cisplatin or 0.03% MMS, and also

examined the recovery after washing the cultures

extensively The levels of cH2AX phosphorylation

revealed no differences in the dephosphorylation of

cH2AX in pph21D cells as compared with the WT

cells, either before or after treatment or during

recovery (Fig 4)

Role of Pph3p and its regulatory subunits Psy4p

and Psy2p in recovery of chromosome replication

following MMS-induced DNA damage

cH2AX is believed to play a central role in the

recruitment and⁄ or retention of DNA repair factors

at the sites of DNA damage [20] In order to

investi-gate whether a Pph3p complex is required for the

recovery of chromosome replication following removal

of DNA-damaging agents, we employed pulsed-field

gel electrophoresis (PFGE) Cells were arrested in G1

with a-factor, released into S-phase, and then treated

with MMS for 90 min The drug was washed away

and cells were allowed to recover At various times,

chromosomes were prepared from WT, pph3D, psy4D

and psy2D cells, and separated by PFGE These gels

resolved a characteristic ladder of bands

correspond-ing to the 16 S cerevisiae chromosomes, visualized

after ethidium bromide staining (Fig 5) Treatment of

cells with MMS resulted in loss of chromosome bands (Fig 5, WT, pph3D, psy4D and psy2D, 0 h) due to the presence of forks and replication bubbles that prevent entry of the chromosomes into the gel [21,22] Treat-ment with MMS also sometimes resulted in the appearance of a ‘smear’ of low molecular mass DNA species that may represent some chromosome degra-dation (Fig 5, psy4D, 0 h) When WT cells were washed free of the DNA-damaging agents and allowed to recover, the intact chromosomes started to reappear after 2 h of recovery and were clearly visible

at 4 h (Fig 5, WT), indicating that the S-phase arrest had been overcome and chromosome replication had

UN CDDP MMS UN CDDP MMS

Treatment for 90 min

H2A/H2B H2AX

UN CDDP MMS UN CDDP MMS

Recovery 2 h

H2A/H2B H2AX

H2A/H2B H2AX

UN CDDP MMS UN CDDP MMS

Recovery 6 h

Fig 4 Pph21p (PP2Ac ortholog) is not involved in cH2AX dephosphorylation in yeast The WT strain BY4743 and the pph21D mutant were grown to mid-expo-nential phase in liquid culture and incubated

in the presence of cisplatin (CDDP) (2 mM)

or MMS (0.03%), or left untreated (UN), for

90 min Cells were filtered, washed free of the drug, and incubated at 30 C in YPD, and samples were taken at the indicated times during recovery Trichloroacetic acid extracts were prepared and subjected to immunoblot analysis with antibodies against cH2AX Lower panels: blots were stripped and immunostained for total H2A ⁄ H2B as a control.

Fig 5 The Pph3p complex is required for recovery of chromosome replication (A) The WT haploid strain BY4741 and mutants pph3D, psy4D and psy2D were grown to mid-exponential phase, arrested

in G1with a-factor, released into S-phase, and treated with 0.05% MMS for 90 min Cells were filtered, washed extensively, and incu-bated in YPD at 30 C for 6 h Samples for PFGE were taken after a-factor treatment (20 lgÆmL)1) (control), after MMS treatment and following removal of MMS after recovery for 2, 4 and 6 h.

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resumed and gone to completion When pph3D and

psy2D cells were allowed to recover from exposure to

MMS, intact chromosomes had barely reappeared

after 6 h of recovery, indicating that these mutants

were slower in the recovery of chromosome

replica-tion (Fig 5: pph3D, 6 h; psy2D, 6 h) In contrast,

recovery in psy4D cells was similar to that in WT

cells (Fig 5, psy4D, MMS 4 h) Thus, a correlation

was observed between delayed completion of

chromo-some replication and prolonged MMS-induced

Rad53p phosphorylation in pph3D and psy2D cells

Similar results were obtained in three independent

experiments

Further analysis of chromosome replication

follow-ing cisplatin-induced damage suggested that pph3D,

psy4D and psy2D cells were all slightly delayed as

compared with WT cells, but the small difference [at

concentrations of cisplatin (3 mm) near its maximum

solubility] was difficult to confirm (data not shown)

Discussion

In S cerevisiae, Pph3p has been shown to interact

with regulatory subunits Psy4p and Psy2p, and these

three proteins and their interactions have been found

to be conserved through evolution to Drosophila and

mammals [4] We have previously demonstrated that

deletion of any component of yeast Pph3p–Psy4p–

Psy2p causes hypersensitivity to the antitumour drug

cisplatin, indicating that all three proteins may

oper-ate as a functional unit in vivo, playing a role in the

cisplatin response [9] Cisplatin interferes with DNA

function by causing intrastrand and interstrand

cross-linking of nucleotide bases and, in replicating cells,

DNA damage usually induces an intra-S-phase cell

cycle arrest Accordingly, we show in this article that

treatment of pph3D, psy4D and psy2D mutant cells

with cisplatin causes enhanced accumulation of cells

in S-phase as compared with WT cells, although the

effect is less conclusive in the case of the psy4D cells

Nevertheless, the data suggest that a correlation is

observed between the slow growth of pph3D, psy4D

and psy2D cells in the presence of cisplatin [9] and

accumulation of cells in S-phase Delayed S-phase

progression is usually associated with activation of

the intra-S-phase checkpoint mediated by Rad53

phosphorylation, and indeed, treatment of cells with

3 mm cisplatin for 90 min resulted in phosphorylation

of Rad53p (Fig 2A), although slightly lower

concen-trations did not activate Rad53p [9] Notably,

recov-ery from cisplatin-induced Rad53p phosphorylation

was delayed in all three mutants: pph3D, psy4D and

psy2D

At sites of DNA damage, the Ser129-phosphorylated H2AX derivative, cH2AX, forms foci for the recruit-ment of factors involved in repair of DNA damage and maintenance of the cell cycle arrest H2AX was found to be hyperphosphorylated in pph3D, psy4D and psy2D strains in both the absence and the presence of ionizing radiation [12], and in the present study, in the absence and the presence of cisplatin In addition, we showed that Pph3p directly or indirectly binds to cH2AX, indicating that Pph3p–Psy4p–Psy2p forms a stable complex with H2AX when Ser129 is phosphory-lated and is therefore likely to be the phosphatase complex dephosphorylating the histone C-terminal tail Keogh et al [12] have provided evidence that cH2AX

is removed from the site of DNA damage before it is dephosphorylated If this is the case, removal from the action of the ataxia telangiectasia mutated (ATM)⁄ ataxia telangiectasia and RAD53 related (ATR) kinases at the site of DNA damage may decrease the kinase⁄ phosphatase ratio and allow the phosphatase to dephosphorylate cH2AX

In mammalian cells, PP2A isoforms, the orthologues

of S cerevisiae Pph21p and Pph22p, have been reported to dephosphorylate cH2AX [23], and in some cases, e.g in the mammalian target of rapamycin path-way, Pph21p and Pph22p have overlapping functions with Pph3p [24] It was therefore important to examine whether Pph21⁄ 22p might play a role in the dephos-phorylation of cH2AX Cells with deletion of the most abundant isoform, Pph21p, exhibit depletion of phos-phatase activity to 35% of the total attributable to Pph21 and Pph22 [25] In addition, these pph21D cells showed a significantly lower budding index and slightly slower growth than WT cells on nonfermentable carbon sources However, the pph21D cells showed no hyperphosphorylation of cH2AX and no delay in recovery from cisplatin and MMS as compared with

WT cells, supporting the idea that in S cerevisiae, cH2AX is dephosphorylated by Pph3p and not by Pph21p and its closely related isoform Pph22p

In contrast to the effects of cisplatin, which cross-links DNA strands, our studies in which yeast cells were treated with MMS, which mainly alkylates DNA but can cause double-strand breaks [26], showed delayed dephosphorylation of Rad53p and delayed recovery of chromosome replication only in pph3D and psy2D cells as compared with WT cells, but not in the psy4D mutant The results are in line with the competi-tive growth assays that identified the pph3D and psy2D cells as MMS hypersensitive [5] Recently, O’Neill

et al [13] found delayed recovery from MMS-induced Rad53 phosphorylation and decreased progression of replication forks along the DNA in pph3D and psy2D

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cells These authors conclude that a dimeric complex,

Pph3p–Psy2p, is responsible for the dephosphorylation

of Rad53p, and they further suggest that Rad53p

dephosphorylation at the replication fork is necessary

to allow the resumption of DNA synthesis Rad53p

has been shown to interact with the lagging strand

rep-lication apparatus regulating the phosphorylation of

DNA polymerase a-primase complex [27], and Psy2p

was found to interact with proteins at stalled

replica-tion forks in a yeast two-hybrid screen [28]

Our studies indicate that different Pph3 phosphatase

complexes or more likely different phosphatases are

responsible for the dephosphorylation of Rad53p after

cisplatin and MMS-induced DNA damage

Phosphory-lation of Rad53p is detected by a mobility shift after

gel electrophoresis, and multiple phosphorylation sites

in Rad53p are suggested by the several bands that can

sometimes be separated [13,29] Different

phosphoryla-tions of Rad53p may be triggered by the two

DNA-damaging agents, and the different phosphorylation

sites may then be dephosphorylated by different

phos-phatases The Mg2+-dependent phosphatases, Ptc2p

and Ptc3p, have been implicated in the

dephosphoryla-tion of Rad53p after a G2⁄ M arrest in response to

irreparable double-strand breaks in the DNA [29]

Keogh et al [12] have suggested that

dephosphoryla-tion of Rad53p during recovery from a repairable

double-strand break depends on the prior

dephos-phorylation of cH2AX by Pph3p–Psy4p–Psy2p [12]

Our results on recovery from cisplatin-induced DNA

damage are consistent with Rad53p phosphorylation

at a particular site being maintained by cH2AX, and

when the latter is dephosphorylated, Rad53p may be

dephosphorylated by Ptc2p and Ptc3p (Fig 6)

The question of whether Pph3p–Psy2p or Pph3p–

Psy4p–Psy2p is involved in the dephosphorylation of

Rad53p after DNA damage by MMS is interesting

An alternative explanation is presented by considering

the mammalian complex Ppp4c–R2–R3, which is

orthologous to Pph3p–Psy4p–Psy2p The isolation of

endogenous Ppp4c–R2 revealed that R2 inhibited

Ppp4c, and suggested that R2 may be a core

tory subunit that facilitates binding of further

regula-tory subunits to Ppp4c [7] The interaction of R3 with

Ppp4c was then shown to require prior preassembly of

Ppp4c and R2 [8] These observations suggest that if

the complexes are conserved through evolution, Psy4p

may be present in the complex that dephosphorylates

Rad53p In addition, by comparison with R2, the yeast

orthologue Psy4p may be an inhibitory regulatory

sub-unit for Pph3p, so that in psy4D cells, the active

Pph3p, weakly associated with Psy2p, may

dephos-phorylate Rad53p In psy4D cells, phosdephos-phorylated

Rad53p would therefore not be present at replication forks to stall DNA synthesis Our MMS sensitivity studies (Fig 1B) could also be explained by this mech-anism If we consider Psy4p as an inhibitory regulatory subunit of Pph3p, psy4D cells could escape from the Rad53p checkpoint, and grow similarly to WT cells; pph3D and psy2D cells would show slow growth because of the activation of the checkpoint

The stable interaction of Pph3p and Psy2p with cH2AX may require the presence of Psy4p The inter-action of Rad53p with a Pph3p complex, which we could not detect by coimmunoadsorption, would appear to be transient The different strengths of the interactions of the phosphatase complex with its sub-strates may underlie the nonessential nature of Psy4p for dephosphorylation of Rad53p by Pph3p in psy4D cells, although we cannot completely exclude the exis-tence of functional dimeric complexes in WT cells Overall, our studies are consistent with a role for Pph3p–Psy4p–Psy2p in the dephosphorylation of both cH2AX and Rad53p The complex may have an addi-tional function at stalled replication forks, but the data

do not necessitate such a role, as dephosphorylation of both cH2AX and Rad53p is likely to be a prerequisite for chromosome replication to resume A working model for the roles of Pph3p–Psy4p–Psy2p in the recovery from DNA damage induced by the crosslink-ing anticancer drug cisplatin and the noncrosslinkcrosslink-ing agent MMS is presented in Fig 6 Our data suggest that the sites phosphorylated on Rad53p and dephos-phorylated by different phosphatases may be depen-dent on the type of the DNA damage However, different levels of DNA damage cannot be entirely excluded, because cisplatin does not readily enter the yeast cell, and therefore it is possible that the overall amount of MMS-induced DNA damage may be higher than that caused by cisplatin

Experimental procedures Yeast strains and general methods All methods for the manipulation of yeast and preparation

of media were performed according to standard protocols [30] The growth conditions for the yeast strains and drug sensitivity studies were as described previously [9] The strains used in this study are listed in Table 1 The S cere-visiae strain AY925, in which Psy4p bears a C-terminal MYC13 epitope tag and Pph3p an N-terminal HA3 tag, was constructed by a PCR-based method as described in [9] The haploid and diploid strains with deletions of genes PPH3, PSY4 and PSY2 encoding ORFs YDR075w, YBL046w and YNL201c, respectively, were from Euroscarf

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(European Saccharomyces cerevisiae Archive for Functional

Analysis), Institute for Microbiology, Johann Wolfgang

Goethe-University Frankfurt, Germany

Yeast extracts, immunoblotting, and

immunoprecipitation

Extracts for immunoblot analysis were prepared either as

described previously [9] or by a slightly modified

trichlo-roacetic acid-lysis method [31] Briefly, in the

trichloro-acetic acid method, the cells were washed with 20%

trichloroacetic acid (v⁄ v) and were then disrupted with

0.5 mL of 20% trichloroacetic acid (v⁄ v) ⁄ 0.7 · 107

cells

by vortexing for 1 min in the presence of glass beads in

a mini-bead beater The lysates, separated from the

beads, were centrifuged for 5 min at 13 000 g The pellets

were resuspended in 200 lL of sample buffer adjusted to

0.3 m Tris⁄ HCl with 1 m Tris-HCl pH 8.8, boiled for

10 min, and clarified by centrifugation for 5 min at

13 000 g Proteins in the extracts were subjected to

SDS⁄ PAGE and transferred to nitrocellulose membranes

In coimmunoprecipitation experiments, aliquots of lysates

(2 mg of protein) prepared in the absence of trichloroacetic

acid from cells expressing Psy4p–MYC13 and HA3–Pph3p

were incubated with either anti-c-MYC or anti-HA agarose

beads (Sigma-Aldrich, Poole, UK) on a shaking platform at

4C for 2 h After centrifugation for 5 min at 13 000 g, the beads were washed two times in lysis buffer containing 0.15 m NaCl and twice in 50 mm Tris⁄ HCl (pH 7.5) and 0.1 mm EGTA The beads were boiled for 5 min in SDS sample buffer, and released proteins were subjected to SDS⁄ PAGE (4–12% polyacrylamide) and immunoblotting with either of the monoclonal antibodies anti-MYC (Roche Diagnostics, Indianapolis, IN, USA) or anti-HA (produced

in the Division of Signal Transduction Therapy, University

of Dundee) Rad53p immunoblots were performed using a mixture of two antibodies (yN-19 and yC-19, Santa Cruz Biotechnology Inc., Santa Cruz, CA, USA) Antibodies to histones H2A⁄ H2B and phosphoSer129-H2AX were from Abcam (Cambridge, UK)

FACS analysis Cells (1· 107) were resuspended in 70% (v⁄ v) ethanol and left for at least 2 h at 4C The cells were then washed in

50 mm Tris⁄ HCl (pH 7.8), treated with 0.2 mgÆmL)1 RNaseA (Sigma-Aldrich) at 37C overnight, and washed with 200 mm Tris⁄ HCl (pH 7.5), 211 mm NaCl, and 78 mm MgCl2; propidium iodide was then added to give a concen-tration of 50 lgÆmL)1 in the same buffer at least 1 h prior

Pph3 Psy2 Psy4 H2AX

DNA damage

Rad-53

Ptc2/Ptc3

Cisplatin

H2AX- P ( H2AX)

ATM/ATR kinases recruited

Rad53-Cell cycle delay

Recovery

P1

Pph3 Psy2 Psy4 P2

MMS

H2AX- P ( H2AX) DNA damage

ATM/ATR kinases recruited

Rad53-Cell cycle delay

Pph3 Psy2

Rad-53

Recovery

Fig 6 Schematic for the roles of Pph3p–Psy4p–Psy2p in recovery from cisplatin- and MMS-induced DNA damage Pph3p–Psy4p–Psy2p forms a stable complex with cH2AX via Psy4p During recovery from cisplatin- or MMS-induced DNA damage, cH2AX may be removed from the site of action of the ATM⁄ ATR kinases, allowing Pph3p–Psy4p–Psy2p to dephosphorylate cH2AX In the case of the cisplatin-induced DNA damage response, the site(s) phosphorylated (P1) on Rad53p are dephosphorylated by the phosphatases Ptc2 and Ptc3 In the case of the MMS-induced DNA damage response, the site(s) phosphorylated (P2) on Rad53p are distinct and are dephosphorylated by a transient interaction with Pph3p–Psy4p–Psy2p Psy4p is not absolutely essential for this dephosphorylation, allowing a weakly interacting Pph3p– Psy2p complex to dephosphorylate the P2 site(s) in the psy4D cells.

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to FACS analysis in a Becton Dickinson FACSort machine,

managed by R Clarke (University of Dundee, UK)

Analyses of chromosomes by PFGE

Cells were grown to early log phase (A600 nmof 0.5) in YPD

at 30C and arrested in G1 by addition of a-factor

(20 lgÆmL)1) When budded cells accounted for < 5% of

the population (confirmed by FACS analysis), the cells were

released from the G1arrest by filtration and extensive

wash-ing, and this was followed by incubation in prewarmed

YPD for 30 min to allow entry into S-phase before addition

of MMS (0.05%) or cisplatin (3 mm) After 90 min in MMS

or cisplatin, cells were filtered, washed extensively with YPD

containing 5% (w⁄ v) sodium thiosulfate, and incubated in

YPD at 30C At the times indicated, 1 · 108

cells were removed and fixed in 70% ethanol at 4C overnight before

preparation of chromosomes, exactly as described in the

CHEF DRII instruction manual (BioRad, Hemel

Hemp-stead, UK) PFGE was carried out using the BioRad

CHEF DRII apparatus at 14C in a 1% agarose (pulsed

field-certified BioRad) gel in 89 mm Tris, 89 mm boric acid

and 2 mm EDTA (pH 8) for 24 h at 6 VÆcm)1using a 120

included angle with a 6.8–158 s switch time ramp Gels were

stained with 1 lgÆmL)1 ethidium bromide for 30 min and

washed for 2 h in water before the DNA was visualized

Acknowledgements

We thank the Medical Research Council, UK for financial support

References

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M, Bauer A, Schultz J, Rick JM, Michon A-M, Cruciat C-M et al (2002) Functional organisation of the yeast proteome by systematic analysis of protein complexes Nature 415, 141–147

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et al.(2002) Systematic identification of protein com-plexes in Saccharomyces cerevisiae by mass spectrome-try Nature 415, 180–183

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JM (2004) Genome-wide identification of genes confer-ring resistance to the anticancer agents cisplatin, oxa-liplatin and mitocin C Cancer Res 64, 3940–3948

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Table 1 S cerevisiae strains used in this study Accession

num-bers for Euroscarf strains are cited at http://www.uni-frankfurt.de/

fb15/mikro/euroscarf/data.

AY925 MATa, ade2-1, his3-11, leu2-3,

trp1-1, ura3-1, can1-100

Fernandez-Sarabia

et al [32]

AY925

PSY4–MYC 13 ,

HA3–PPH3

AY925 PSY4–MYC 13 –HISMX6,

HA 3 –PPH3

Hastie

et al [9]

BY4741 (Y00000,

haploid)

MATa; his3D1; leu2D0;

met15D0; ura3D0

Euroscarf

BY4743 (Y20000,

diploid)

MATa ⁄ MATa; his3D1 ⁄ his3D1;

leu2D0 ⁄ leu2D0;

met15D0 ⁄ MET15;

LYS2 ⁄ lys2D0;

ura3D0 ⁄ ura3D0

Euroscarf

Y34010 BY4743pph3D::kanMX4 ⁄

pph3D::kanMX4

Euroscarf Y33072 BY4743psy4D::kanMX4 ⁄

psy4D::kanMX4

Euroscarf Y32011 BY4743psy2D::kanMX4 ⁄

psy2D::kanMX4

Euroscarf Y33831 BY4743pph21D::kanMX4 ⁄

pph21D::kanMX4

Euroscarf

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