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Cdk2⁄ cyclin A mediated phosphorylation of Cdc6 is thought to induce its translocation from the Keywords hypoxia; reoxygenation; Cdk2; replication; chromatin Correspondence M.. In order

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initiation after transient hypoxia in T24 cells

Dirk Stabenow, Hans Probst and Maria van Betteraey-Nikoleit

Interfakulta¨res Institut fu¨r Biochemie der Universita¨t Tu¨bingen, Germany

In eukaryotic cells, orderly cell cycle progression is

believed to be regulated by the action of Cdks and

their binding partners, i.e the cyclins, their inhibitors,

and the E2F family of transcription factors [1] The

initiation of the first replicons at the G1- to S-phase

transition, marks a key step of cell cycle progression

In living cells, the stepwise assembly of proteins at the

replication origins of replicons prepares for initiation

[2–5] First, the hexameric origin recognition complex

binds; this then recruits Cdc6 [6,7], Cdt1 [8,9] and the

minichromosome maintenance proteins [10] This

pre-replication complex (pre-RC) is built up during the

G1-phase The complex is suggested to be activated by

Cdk2 [11] and the Dbf4⁄ Cdc7 kinase [12] which is

required to load the initiation factor Cdc45 on the

pre-RC [13–15] Commonly, Cdk2 in association with cyclin E is thought to be essential for driving the cells through this transition Cdk2-mediated phosphoryla-tions are reported to be important in numerous steps preceding initiation of DNA replication; for example, together with Cdk4, the phosphorylation of pRb and the subsequent release of E2F results in the transcrip-tion of essential factors of the replicatranscrip-tion initiatranscrip-tion complex such as MCM and Cdc6 [16,17] Protein phosphorylations by Cdk2 were suggested to be important for initiation complex assembly and activa-tion [17,18] Cdk2⁄ cyclin A mediated phosphorylation

of Cdc6 is thought to induce its translocation from the

Keywords

hypoxia; reoxygenation; Cdk2; replication;

chromatin

Correspondence

M van Betteraey-Nikoleit,

Physiologisch-Chemisches Institut der Universita¨t

Tu¨bingen, Hoppe-Seyler-Straße 4,

D-72076 Tu¨bingen, Germany

Fax: +49 7071293339

Tel: +49 70712973329

E-mail: maria.van-betteraey@

uni-tuebingen.de

(Received 6 July 2005, revised 16 August

2005, accepted 5 September 2005)

doi:10.1111/j.1742-4658.2005.04957.x

We examined whether the fast release of replicon initiation after sudden O2 recovery of hypoxically incubated mammalian cells depends on kinase activity of Cdk2 We used a system based on starved⁄ refed T24 cells elab-orated previously for such investigations [van Betteraey-Nikoleit M, Eisele

KH, Stabenow D & Probst H (2003) Eur J Biochem 270, 3880–3890] Cells subjected to hypoxia concurrently with refeeding accumulate the G1 DNA content within 5–6 h In this state they are ready to perform, within 1–

2 min after O2recovery, a burst of replicon initiations that marks the start

of a synchronous S-phase We found that Cdk2 binds to the chromatin fraction within 4–6 h after refeeding with fresh medium, irrespective of whether the cells were incubated normoxically or hypoxically However, inhibition of Cdk2 by olomoucine, roscovitine or the Cdk2⁄ cyclin inhibi-tory peptide II had no influence on the synchronous burst of replicon initi-ations Cdc6 and pRb, possible targets of Cdk2 phosphorylation, behaved differentially Inhibition did not affect phosphorylation of Cdc6 after reoxygenation, whilst chromatin bound pRb remained hypophosphorylated beyond the initiation burst Thus, neither Cdk2 activity, though present at the end of the hypoxic period, nor pRb phosphorylation are necessary for releasing the burst of replicon initiations upon oxygen recovery Conse-quentially, Cdk2 dependent phosphorylation(s) cannot be a critical trigger

of replicon initiation in response to reoxygenation after several hours of hypoxia, at least in the T24 cells studied

Abbreviations

FITC, fluorescein isothiocyanate; PCNA, proliferating cell nuclear antigen; Pre-RC, prereplication complex.

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nucleus to the cytoplasm, thus preventing reinitiation.

Altogether, these observations suggest that Cdk2

activ-ity is necessary for progression of cells from G1to

act-ive DNA replication The importance of Cdk2 has

been substantiated by a number of different

approa-ches Microinjection of antibodies against Cdk2,

cyclin E or cyclin A and the antisense mRNA of Cdk2

block initiation of DNA synthesis in mammalian cells

[19,20] In vitro initiation in G1 nuclei is dependent on

Cdk2⁄ cyclin A and Cdk2 ⁄ cyclin E complexes [21]

Fur-thermore, in general, elevated levels of the Cdk2

inhib-itor p27 and decreased activity of Cdk2 in conjunction

with hypophosphorylated pRb have been shown to

result in growth arrest [22,23] However, these results

have been challenged by the finding that Cdk2

knock-out mice are viable [24] In addition, Cdk4 can

sub-stitute for Cdk2 in pRb phosphorylation, and

proliferation of cancer cells that do not contain pRb,

may be completely independent of Cdk2 or Cdk4

activity [25]

In order to reveal whether Cdk2 activity is also

involved in the very fast (requiring a few min only)

release of replicon initiations from the hypoxic arrest

described first by us [26], we studied the association of

Cdk2 with the chromatin fraction of T24 cells and its

enzymatic activity during the course of a starvation–

refeeding⁄ hypoxia–reoxygenation experiment As

out-lined in detail before and substantiated by

cytofluoro-metry, analysis of DNA replication at the level of

replicons and determination of the fraction of mitotic

cells [27] our especially elaborated starvation protocol

accumulates T24 cells in a G1 arrest, from which they

can be released by medium renewal Normally, the

cells then proceed to the S-phase within approximately

5 h, passing through a number of the above mentioned

regulatory steps until the start of orderly DNA

synthe-sis at the origins of replication (scheduled to be

activa-ted as the very first of the S-phase) We demonstraactiva-ted

[27] that subjecting the cells to hypoxic conditions

directly after restimulation with fresh medium

reversi-bly interrupts this process at a state situated extremely

close to the actual occurrence of replicon initiation

The cells accumulate in a state which we refer to as

the ‘hypoxic preinitiation’ state on the basis of prior

studies on DNA replication of a number of other cell

lines [27] and Simian virus 40 replication in vivo [28]

From this state, characterized by a still incomplete and

not yet functional set of replication proteins associated

with chromatin, they can be released within 1–2 min

by restoring atmospheric pO2, into a synchronous

wave of replicon initiations During the transition

trig-gered by the reoxygenation event, chromatin bound

replication proteins become completed [28] We have

demonstrated that, in the T24 system described before [27], most cells pass through a normal synchronous S-phase after reoxygenation

In the present study we found that substantial chro-matin associated Cdk2 emerged during the hypoxic period However, inhibitors of Cdk2 activity did not affect replicon initiation after reoxygenation in vivo Cdc6 phosphorylation in the course of initiation of DNA replication was also not affected, pRb remained hypophoshorylated for at least 30 min beyond the ini-tiation burst

Thus, at least in the T24 cells studied, Cdk2 activity

as well as Rb phoshorylation is dispensable for the fast release of hypoxically suppressed initiation of DNA replication at the beginning of the S-phase

Results

Hypoxia or reoxygenation do not interfere with the emergence of chromatin bound Cdk2 activity after restimulation by fresh medium

In [27] we found no Cdk2 protein in the chromatin fraction of starved T24 cells by western blot analysis However, significant amounts exist 7 h after medium renewal, irrespective of whether the cells were grown normoxically or hypoxically Immunofluorescence staining of the cells using a Cdk2 specific antibody (Fig 1D, final column) confirmed this result We then examined the protein kinase activity of Cdk2 from dif-ferent fractions of hypoxic and reoxygenated cells: The medium of two cultures with starved T24 cells was renewed and both were incubated hypoxically for a fur-ther 7 h One culture was subsequently reoxygenated for 30 min The immunoprecipitates of cytosolic, NP40-extractable nucleosolic, and salt eluted chromatin bound proteins were analysed for protein kinase activ-ity as described in Eperimental procedures The result-ing autoradiograph (Fig 1A) convincresult-ingly shows that the highest concentration (relative to total protein pre-sent) of kinase activity occurs in the chromatin bound fraction and (slightly less) in the cytosolic fraction The nucleosol exhibits the lowest activity There is obvi-ously no difference between Cdk2 precipitated from hypoxic and 30-min reoxygenated cells Western blot analysis of the same membrane (Fig 1B), exhibited analogous differences of general signal intensities, but revealed two bands of different electrophoretic mobil-ity, most probably reflecting two different phosphoryla-tion states We therefore suspect that chromatin bound Cdk2 differs from the cytosolic form by its preferential phosporylation state However, both forms obviously exhibit comparable protein kinase activity in vitro

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We next examined the inhibitory action of the Cdk2

inhibitors olomoucine, roscovitine and staurosporine,

all of which compete for the ATP-binding domain of

the kinase [29,30], and the Cdk2⁄ cyclin inhibitory

pep-tide II which is reported to inhibit specifically the

phosphorylation of substrates by Cdk2⁄ cyclin A and

Cdk2⁄ cyclin E complexes [31] in an in vitro kinase

assay All four inhibitors were used at medium

concen-trations reported by others to reliably inhibit Cdk2

[31–34] Starved T24 cells incubated normoxically after

medium stimulation were lysed Subsequently, Cdk2

was immunoprecipitated The kinase assay was

per-formed both in the absence and in the presence of the

inhibitors Figure 1C shows that Cdk2 activity is

signi-ficantly decreased in the presence of the inhibitors

Furthermore, to demonstrate that the Cdk2⁄ cyclin

inhibitory peptide II is cell permeable and localizes at

the sides of Cdk2, we used the Cdk2⁄ cyclin inhibitory

peptide II in a form carrying a fluorescence label at

the amino end (Fig 1D, middle column) Starved T24

cells were stimulated by medium renewal (except for

the culture designated N–), and hypoxic or normoxic gassing was started concurrently The labelled peptide was added (without interruption of the hypoxic incu-bation) 4 h after the start of gassing A further 3 h later, one hypoxic culture was reoxygenated for

30 min After this, cells were processed for Cdk2 immunostaining as described in Experimental proce-dures Finally, we found a strong fluorescence within the cells colocalized with the Cdk2 immunostaining (Fig 1D, last column) Starved T24 cells (N–) expres-sing barely detectable amounts of Cdk2 protein

A

B

C

D

Fig 1 Cdk2 activity does not decrease under hypoxia (A)

Phos-phorylation of histone H1 by immunoprecipitated Cdk2 obtained

from the cytosolic, nucleosolic and salt eluted chromatin bound

pro-teins, after 7 h hypoxia or reoxygenation, respectively

Immuno-precipitations and subsequent kinase assays were performed as

described The kinase reaction was stopped by boiling in protein

buffer, and proteins were separated by SDS ⁄ PAGE (12%

polyacryl-amide) After blotting, the membrane was autoradiographed (B)

Western blot analysis of immunoprecipitated Cdk2 from (A) H, 7 h

hypoxic incubation after medium renewal; 30¢, reoxygenated for

30 min after 7 h hypoxic incubation (C) Phosphorylation of histone

H1 by immunoprecipitated Cdk2 from cell lysate prepared after 7 h

normoxic incubation following medium stimulation

Immunoprecipi-tation was performed as described Subsequently, the kinase assay

was performed in the absence or presence of olomoucine (20 l M ),

roscovitine (7 l M ), staurosporine (100 n M ) or the Cdk2⁄ cyclin

inhibi-tory peptide II (50 l M ) The kinase reaction was stopped by boiling

in protein sample buffer, and the proteins were separated by

SDS ⁄ PAGE (12% polyacrylamide) After blotting, the membrane

was autoradiographed (upper row) Western blot analysis of the

membrane of immunoprecipitated Cdk2 was performed afterwards

(lower row) (D) Immunofluorescence staining of Cdk2 under

norm-oxic, hypoxic and reoxygenated incubation conditions in the

pres-ence of FITC labelled Cdk2⁄ cyclin inhibitor peptide II T24 cells

were grown on coverslips for 44 h The FITC labelled Cdk2⁄ cyclin

inhibitory peptide II was added 4 h before the end of the respective

incubation conditions After fixation of the cells, Cdk2 was

visual-ized by using a Cdk2 antibody, followed by an anti-mouse Ig

labelled with Alexa Fluor 568 Total DNA was stained with

bis-benzimide The respective incubation conditions are indicated

below the images N–, 7 h normoxic incubation without medium

renewal; N+, 7 h normoxic incubation after medium renewal; H,

7 h hypoxic incubation after medium renewal; R 30¢, reoxygenated

for 30 min after 7 h hypoxic incubation.

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showed significantly less fluorescence of the inhibitor

and as mentioned above Cdk2 immunofluorescence

Both increased dramatically after feeding the cells

Cdk2 inhibitors fail to prevent replicon initiation

after reoxygenation

As mentioned, our starvation–feeding⁄ hypoxia

proto-col arrests T24 cells very close before the effective

entry into S-phase During the hypoxic period, they

accumulate in a state separated by a few minutes only

from initiation of the replicons scheduled to be

repli-cated first [27] Readmission of O2to a thus pretreated

T24 culture triggers a subsequent synchronous burst of

replicon initiations Up to about 1 h thereafter, the

replicative activity in the reoxygenated culture is

gov-erned mainly by synchronous daughter strand growth

within the replicon cohort activated in response to the

reoxygenation event Afterwards, initiations of

repli-cons scheduled to be activated later in the S-phase

succeed, followed by G2, mitosis and a further

syn-chronous cell cycle [27] Alkaline sedimentation

analy-sis of the length distribution of pulse labelled daughter

strand DNA is suited to demonstrate the initial burst

as well as the succeeding synchronous daughter strand elongation On the basis of numerous prior studies [26,35–40], 8-min [3H]dThd pulses applied 20 and 40–50 min after reoxygenation, proved to be most con-venient for demonstrating initiation and succeeding elongation

We studied the influence of olomoucine, roscovitine and the Cdk2⁄ cyclin inhibitory peptide II on the sedi-mentation profiles of pulse labelled daughter strand DNA 20 and 50 min after reoxygenation (Fig 2) Starved T24 cells were stimulated by medium renewal, and hypoxic gassing was started concurrently The inhibitors were added (without interruption of the hyp-oxic incubation) 4 h after the start of gassing A fur-ther 3 h later, all cultures were reoxygenated After continuing normoxic incubation for 20 or 50 min, respectively, the cells were labeled by [3H]dThd pulses

In controls, inhibitor addition was omitted

The controls presented in the inset of Fig 2 serve to confirm the expected effect of hypoxia in the present experiment These alkaline sedimentation profiles represent pulse labelled DNA of cells which were

Fig 2 Inhibition of Cdk2 does not affect replicon initiation after reoxygenation Alkaline sedimentation patterns of pulse-labelled T24 DNA after lysis on top of the gradients Eight minutes before the end of the respective incubation conditions, nascent daughter strand DNA chains were pulse-labelled with 7 lCi [3H]dThdÆmL)1 Inset, Starved T24 cells were stimulated by medium renewal and incubated normox-ically (n) or hypoxnormox-ically (.) for 7 h; x, 14 C-labelled matured bulk DNA Main figure, T24 cells were stimulated by medium renewal, incubated hypoxically for 7 h and then reoxygenated for 20 min (open symbols) and 50 min (filled symbols), respectively Olomoucine (20 l M ), roscovi-tine (7 l M ) or the Cdk2 ⁄ cyclin inhibitory peptide II were added 3 h before reoxygenation s, d, Reoxygenated for 20 min and 50 min,

respectively, after 7 h hypoxic incubation; h, n, reoxygenated for 20 min and 50 min, respectively, after 7 h hypoxic incubation in presence

of olomoucine; e, r, reoxygenated for 20 min and 50 min, respectively, after 7 h hypoxic incubation, in presence of roscovitine; n, m, reoxy-genated for 20 min and 50 min, respectively, after 7 h hypoxic incubation, in presence of the Cdk2 ⁄ cyclin inhibitory peptide II.

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incubated 7 h after medium renewal normoxically

(open triangles) and hypoxically (filled triangles) The

mature DNA of these cells contained a prelabel

result-ing from [14C]Thd added 44 h before The 14C profile

obtained (crosses) typically exhibits a peak in the last

third of the gradient The 3H-profile of the

normox-ically incubated culture exhibits a sedimentation profile

attributable to asynchronously acting replicons and

reflects the normal steady-state of asynchronous

initi-ation, elonginiti-ation, and termination [26,38,41] The

gra-dient of hypoxic cells contains practically no3H-label,

indicating almost total absence of replicative activity

Twenty minutes after reoxygenation (Fig 2, main,

open symbols), four almost coincident prominent

radioactivity peaks at fraction 7–8 (35–41 S20w)

indi-cate the presence of growing daughter strands of about

35–50 kb length in both inhibitor treated and control

cells Assuming a bidirectional strand elongation rate

of 1.5 kbÆmin)1 at either end of strands, this size is

compatible with daughter strands of replicons initiated

10–20 min before Minor shoulders around fractions

11–12 (51–67 S20w) indicate the additional presence of

small portions of longer growing strands This

shoul-der was more or less prominent in different

independ-ent experimindepend-ents of this type (not shown) As in prior

studies, we attribute them to replicons in few cells

which could no more escape the late S-phase during

starvation and are hit by hypoxia in a still active state

Reoxygenation probably reactivates these late S-phase

replicons However, the shoulder is no more present in

the profiles obtained by analysing the cells 50 min after

reoxygenation (Fig 2, filled symbols) All four profiles

exhibit nearly identical narrow single peaks around

fraction 13 (about 62 S20w or 140–150 kb) Relative to

the main peaks obtained at 20 min, the observed shift

is again compatible with an elongation rate of about

1.5 kbÆmin)1 Thus, the inhibitors had no detectable

influence, neither on the replicon initiation burst

trig-gered by reoxygenation, nor on the succeeding growth

of daughter strands

Changes of chromatin bound pRb and Cdc6 after

reoxygenation

Starved T24 cells were stimulated by medium renewal

(except for the culture designated N–) and incubated

normoxically or hypoxically Further cultures were

reoxygenated after hypoxic incubation After

fraction-ation of the cells, chromatin bound proteins Cdc6 and

pRb were examined by western blot analysis

Western blot analysis of pRb using a pRb antibody

which recognizes an epitope between amino acids 332–

344 (Fig 3A, upper row) and an antibody specific for

underphosphorylated pRb (Figs 3A, row 2 from top) concurrently suggested that pRb is hypophosphorylated

in starved cells and becomes phosphorylated within

7 h after medium stimulation and further normoxic incubation (Fig 3B shows the effect of phosphatase

A

B

C

Fig 3 Phosphorylation of Cdc6 and pRb after reoxygenation (A) Western blot analysis of chromatin bound pRb, Cdc6, and PCNA from 7 h normoxic, hypoxic, and 30 min reoxygenated T24 cells (B) Lambda protein phosphatase digestion of immunoprecipitated Cdc6 and pRb (–), Immunoprecipitated Cdc6 and pRb prior phos-phatase digestion; (+), immunoprecipitated Cdc6 and pRb after phosphatase digestion according to the manufacturer’s instructions (New England Biolabs: Lambda protein phosphatase) (C) Western blot and subsequent immunological detection of chromatin bound PCNA and Cdc6 Staurosporine (10 l M ) was added 30 min before reoxygenation where indicated N–, 7 h normoxic incubation with-out medium renewal; N+, 7 h normoxic incubation after medium renewal; H, 7 h hypoxic incubation after medium renewal; 5¢, reoxy-genated for 5 min after 7 h hypoxic incubation; 30¢, reoxyreoxy-genated for 30 min after 7 h hypoxic incubation.

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digestion on pRb immunoprecipitated from N+ T24

cells) In comparison with normoxic cells, a larger

portion seems to remain hypophosphorylated in the

hypoxic cells Reoxygenation apparently causes no

detectable change of pRb phosphorylation, at least

during the following 30 min

Cdc6 protein was not detectable in starved cells and

appeared after medium stimulation, whereby more

Cdc6 accumulated during hypoxic than under

normox-ic incubation conditions (Fig 3A, row 3 from top)

After reoxygenation, the amount of chromatin bound

Cdc6 decreased within 30 min below the level of the

normoxic control Chromatin bound Cdc6 obtained

from hypoxic cells seems to migrate slightly faster

compared with that occurring in reoxygenated cells

Confirmed by the effect of phosphatase digestion

(Fig 3B), this points to a phosphorylation after

re-oxygenation The suspected phosphorylation could

(nonspecifically) be prevented by adding 10 lm

staurosporine before reoxygenation (Fig 3C) The

lat-ter experiment again clearly shows that the amount of

chromatin bound Cdc6 is high at the end of the

hyp-oxic period and distinctly decreases within 30 min after

reoxygenation The remainder is apparently converted

into the slower migrating form This significant

decrease and conversion to the slower migrating form

is inhibited by 10 lm staurosporine

The presence of substantial amounts of

chromatin-bound proliferating cell nuclear antigen (PCNA)

[27,28] can, in conformity with the function of PCNA

as processivity factor of polymerase delta, serves as an

indicator of active replicative DNA strand elongation

which, for its part, depends on successful replicon

initi-ation Therefore, its increase following reoxygenation

as shown in Fig 3A,C indicates successful replicon

ini-tiation Treatment with 10 lm staurosporine (Fig 3C)

abolishes this increase This suggests that, in

accord-ance with earlier findings of our group [42], replicon

initiation was suppressed by the elevated concentration

of staurosporine

Effects of Cdk2 inhibition on pRb, Cdc6 and

PCNA in vivo

In Fig 4 we analysed the effects of the Cdk2 inhibitors

olomoucine, roscovitine and staurosporine (at 100 nm)

on Cdk2 activity and its substrates pRb and Cdc6

in vivo Starved T24 cells were stimulated by medium

renewal (except for the culture designated N–)

Subse-quently, the cells were incubated normoxically or

hypoxically, or were reoxygenated with or without

prior addition of the inhibitors A concentration of

100 nm staurosporine suffices to inhibit Cdk2

accord-ing to [43], but does not suppress replicon initiation

in cultured cells [42] Accordingly, chromatin bound PCNA increased after reoxygenation under 100 nm staurosporine as well as under olomoucine and rosco-vitine

As already found in the experiment shown in Fig 3A, the hypophosphorylated form of pRb (migra-ting faster) is prominent in starved cells and mostly changes to a higher phosphorylation state after feeding with fresh medium (Fig 4A, top row) As before (Fig 3) this change is also suppressed by hypoxic gas-sing started concurrently with feeding Equally, the changes in appearance and mobility of Cdc6 were reproduced The decrease of Cdc6 in response to reoxy-genation is strengthened until 30 min, whereas chro-matin bound PCNA increases, reflecting increasing DNA strand elongation (Fig 4A, bottom row)

A

B

Fig 4 Western blot analysis of pRb, Cdc6 and PCNA after inhibi-tion of Cdk2 activity by olomoucine, roscovitine and staurosporine

in vivo (A) Western blot analysis of chromatin bound pRb, Cdc6, and PCNA from 7 h normoxic, hypoxic, 5 min, and 30 min reoxy-genated T24 cells Cdk2 inhibitors were added 3 h before reoxygen-ation where indicated (B) Western blot analysis of total cellular pRb, Cdc6, and PCNA from 7 h normoxic, hypoxic, 5 min, and

30 min reoxygenated T24 cells Cdk2 inhibitors were added 3 h before reoxygenation where indicated N–, Normoxic incubation without medium renewal; N+, 7 h normoxic incubation after med-ium renewal; H, 7 h hypoxic incubation after medmed-ium renewal; 5¢, reoxygenated for 5 min after 7 h hypoxic incubation; 30¢, reoxygen-ated for 30 min after 7 h hypoxic incubation.

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However, neither addition of olomoucine, roscovitine

or staurosporine (at 100 nm) before reoxygenation

pro-duced, until 30 min thereafter, any change of

chroma-tin bound pRb, Cdc6 or PCNA in comparison to the

untreated reoxygenated sample Application of the

Cdk2⁄ cyclin inhibitory peptide II in a separate

experi-ment according to the same schedule (data not shown)

yielded identical results This suggests that initiation

and further replication proceeded normally despite the

presence of the Cdk2 inhibitors

Figure 4B, on the other hand, shows that the

differ-ent treatmdiffer-ents of the cells in this experimdiffer-ent caused

no visible quantitative differences of total cellular pRb

and PCNA Both proteins, apparently, are relatively

abundant among total cellular proteins The change of

the electrophoretic mobility of pRb in response to

feeding with fresh medium (attributed by us to

phos-phorylation) obviously concerns the total cellular

pro-tein including the chromatin associated propro-teins On

the other hand the relative intensity of the Cdc6 signal

in Fig 4B is very low Because all wells of the gel for

Fig 4 were loaded with strictly equal amounts of

pro-tein and the fraction of chromatin associated propro-teins

represents only 8.2% of total proteins, the distinctly

higher Cdc6 signal intensities in Fig 4A indicate that,

in contrast to PCNA and pRb, a substantial portion

of Cdc6 was concentrated in the chromatin fraction

The high content of PCNA in the starved cells (N– in

Fig 4B) indicates that these cells rather reside in a

G1-arrest than in a G0-phase [44]

Discussion

This study continues prior work on molecular

mecha-nisms governing the initiation of replication units in

mammalian cells and its regulation in vivo The

dis-covery of the fast acting O2-dependent control of

mammalian replicon initiation [26,39] and the

suc-ceeding detailed evaluation of the relevant conditions

(ranges of O2 partial pressures, etc [38–40,45])

provi-ded a useful tool for this purpose: exposing cultures

of growing mammalian cells for several hours to

hyp-oxic conditions accumulates replicons (scheduled to

be initiated within the hypoxic period), in a state

from which they can easily be released within a few

minutes into a synchronous wave of initiations, by

abruptly restoring atmospheric pO2 The state of

repl-icon origins accumulated under hypoxia was

opera-tionally called by us ‘hypoxic preinitiation state’

Having characterized the changes occurring at the

level of the viral DNA replication in response to

reoxygenation [46], we developed a protocol for

analogous studies on cellular mammalian DNA

replication and its regulation, based on human T24 bladder carcinoma cells [27] Because we followed this protocol exactly in this study, we explicitly refer to the latter communication with respect to data charac-terizing cell cycle, DNA synthesis and cell fraction-ation into cytosolic, nucleosolic and chromatin associated material Clearly, T24 is an abnormal can-cer cell line having a permanently active H-ras [47] which conceivably could bypass some regulatory checkpoints of normal cells We choose these cells because they, best of all cell lines examined, permitted

a selective accumulation of a defined cohort of repli-cons (i.e that is scheduled to be activated as first of the S-phase) in the ‘hypoxic preinitiation state’, in preferable absence of other activated replicons [27] A main intention of this work was to study the mechan-ism of the transition of the latter state to actual initi-ation We emphasize that some of the results obtained, possibly, could only be valid for T24 cells and not for normal mammalian cells On the other hand, the hypoxic suppression of replicon initiation (situated very close before actual initiation), obvi-ously, is a widespread property of proliferating mam-malian cells, possibly serving basal functions, such as protection against metabolic catastrophes during embryonic development or wound healing and, unfor-tunately, also in tumour growth [38] So far, we found it in all types of cells examined in this respect during the past 20 years, ranging from cells replica-ting a virus (SV40) over a diversity of tumour cell lines to normal human primary explanted from umbi-lical cord vein (HUVEC) and nasal epithelium (HNEpC) (G Probst, H Probst & V Gekeler, unpub-lished observations) We suggest, therefore, that the data presented here have more general significance The ‘hypoxic preinitiation complex’ as defined by us [27] appears very similar to the preinitiation complex described by Dutta and Bell [2,48] We suspected that the mechanisms activating the ‘hypoxic preinitiation complex’ and the ‘classical prereplication complex’ are similar, and that hypoxia interferes with the switch from preinitiation to initiation The molecular mode of action of the suspected switch is, so far, completely obscure However, as mentioned, fast recruitment of regulatory proteins such as protein kinases to the ori-gins of replicons and⁄ or modifications of other pro-teins associated with them, by the still inactive initiation complex are involved A likely candidate was thus Cdk2 Numerous reports suggested that Cdk2 activity is essential for growth, and that the absence of Cdk2 activity leads to growth arrest In addition, hyp-oxia has been reported to suppress Cdk2 activity through elevated expression of the Cdk inhibitor p27,

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thus preventing pRb phosphorylation and activation

[49]

We found that Cdk2 associates with cellular

chro-matin within 4–6 h, when cells arrested in G1 are

re-stimulated by feeding under normoxic as well as under

hypoxic conditions Cdk2 protein kinase activity was

immunoprecipitable from the chromatin and cytosolic

fraction of hypoxic as well as of reoxygenated cells

Total cellular Cdk2 protein kinase activity was found

to be susceptible to inhibition by olomoucine,

roscovi-tine, staurosporine or the Cdk2⁄ cyclin inhibitory

peptide II in vitro However, administration of the

inhibitors in vivo before reoxygenation to the hypoxic

cells had virtually no influence on the DNA replication

occurring after reoxygenation, neither on the

synchron-ous burst of replicon initiations, nor on the succeeding

daughter strand elongation (Fig 2) The inhibitors had

no detectable influence on the behaviour of total

cellu-lar and chromatin associated pRb, Cdc6 and PCNA

after the reoxygenation either

Hypoxia, started concurrently with feeding with

fresh medium, suppressed pRb phosphorylation at

least until 30 min after reoxygenation (Figs 3 and 4),

despite the initiation burst occurring within these

30 min However, because the pRb phoshorylation

appearing after cell feeding without imposed hypoxia

emerges in the course of 6–7 h, it is possible

through-out that a pRb phoshorylation, susceptible to the

inhibitors, occurs some hours later after reoxygenation,

but then clearly cannot be causal for triggering the

ini-tiation burst already passed by Obviously, increased

Cdc6 accumulation occurred in the chromatin

associ-ated protein fraction when, after feeding, hypoxia was

imposed on the cells Subsequent reoxygenation

caused, within 30 min, a significant decrease of

chro-matin associated Cdc6 accompanied by a

phosphoryla-tion of a part of it The decrease of chromatin

associated Cdc6 as well as the phosphorylation, was

not prevented by 100 nm staurosporine (sufficient to

inhibit Cdk2), or by olomoucine, roscovitine or the

Cdk2⁄ cyclin inhibitory peptide II Staurosporine at

10 lm, however, distinctly inhibited this decrease and

the presumed phosphorylation At the same time, the

increase of chromatin associated PCNA, indicating

emerging processive DNA strand elongation after

reoxygenation, failed to appear (Fig 3C) The high

staurosporine concentration also suppressed the burst

of replicon initiations released by reoxygenation in the

T24 system observable by alkaline sedimentation (data

not shown) In this context it is tempting to speculate

that Cdc6 may be an in vivo substrate of a protein

kin-ase other than Cdk2, and its phosphorylation may be

involved in the eventual release of replicon initiation

This phosphorylation possibly abolishes binding of Cdc6 to the still incomplete initiation complex, thus, perhaps, allowing recruitment of still missing proteins However, despite the recent data that Cdk2 may be dispensable for proliferation in a mouse model [24], our data may seem contradictory to published studies

on the prerequisites of initiation of DNA replication starting from different states present in G1 or G0 nuclei

It has been reported that the initiation of DNA replication is dependent on the coordinate activity

of Cdk2⁄ cyclin E and Cdk2⁄ cyclin A complexes [18,21,50] The mentioned results are obtained with

in vitro replication systems from HeLa and⁄ or mouse 3T3 cells by mixing isolated nuclei and cytosolic extracts from different cell cycle phases Our in vivo situation is a quite different one: the relevant intervals

of time between mixing cytosolic extracts with nuclei and emergence of additional replicating nuclei are in the order of hours In contrast, our protocol produces,

in living cells, a defined state of replicons situated before origin unwinding (as shown in the SV40 system [46]) and characterized with respect to the absence of the proliferation marker PCNA in the chromatin frac-tion [27] Moreover, in the menfrac-tioned studies, syn-chronous cells for the preparation of nuclei and cytosolic extracts were obtained by different protocols

It can be asked whether the kind of synchronization is critical for the need of Cdk2⁄ cyclin complexes in initi-ation of repliciniti-ation

It was also demonstrated that Cdk2 activity is diminished in hypoxic cells [49,51,52] These studies examined Cdk2 preparations immunoprecipitated from whole cells The observed decrease in Cdk2 activity was probably mainly due to elevated levels of the Cdk2 inhibitory protein p27 obviously expressed under hypoxia in the studied cells and coimmunoprecipitated with Cdk2 With T24 cells we found did neither eleva-ted levels of p27 after several hours of hypoxic incuba-tion nor menincuba-tionable amounts of p27 coprecipitated with Cdk2 under any incubation condition (data not shown) This suggests that in T24 cells inhibition of the pRb pathway is not the direct cause of the hypoxic suppression of initiation in replicons Moreover, in cells replicating SV40 DNA pRb is inactivated by binding to the large T-antigen; nevertheless, their repli-cation of viral genomes obeys the fast O2 dependent control of replicon initiation [53]

The elucidation of the in vivo molecular processes leading from the hypoxic preinitiation state, within a few minutes, to actual initiation was the sole objective

of this work At the time, the T24 cell based protocol,

to our knowledge, accomplishes that comparatively

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well However, we may have observed phenomena that

are characteristic only of this cell line and possibly for

some further (abnormal) cells carrying comparable

genetic defects The general validity of our results

depends on the demonstration of the described effects

in a broader range of cell types, including noncancer

cells

Experimental procedures

Cell culture, transient hypoxia, reoxygenation,

and radioactive labelling

T24 cells (ATCC No HTB-4) were grown in plastic flasks

in DMEM supplemented with 10% (v⁄ v) fetal bovine

serum and 100 UÆmL)1 penicillin⁄ 100 lgÆmL)1

streptomy-cin The cells were subcultured when they reached

conflu-ence For synchronization, the desired number of glass

Petri dishes was seeded from an almost confluent large

cul-ture with 150 000 cellsÆmL)1 (35 mm, 1.5 mL; 145 mm,

25 mL) 44 h before the start of an experiment, as reported

previously [27] As a result, most cells were arrested in G1

due to starvation For prelabelling of DNA, the seeding

medium was supplemented with 5 nCiÆmL)1[14C]thymidine

Experiments were started by stimulation of the cells by

complete medium change, using prewarmed fresh medium,

supplemented with 10% (v⁄ v) fetal bovine serum Then, the

cultures were gassed by a continuous flow of humidified

artificial air containing 5% (v⁄ v) CO2in case of normoxic,

and with 0.0075% (v⁄ v) O2, 5% (v⁄ v) CO2, Ar ad 100% in

case of hypoxic incubations This hypoxic gassing protocol

diminished the pO2in the cultures within 1.5–2 h to about

0.1% and within 6–7 h to about 0.02% For gassing, the

equipment and the procedures described by [53] were used

For reoxygenation, 0.25 vols of medium equilibrated with

95% O2⁄ 5% CO2(v⁄ v) were added to hypoxic cell cultures,

and gassing was continued with artificial air⁄ 5% (v ⁄ v) CO2

Hypoxic addition of inhibitors or radioactive precursors

was performed by plunging a spatula carrying the

appropri-ate quantity into the culture medium without opening the

gassing vessel To stop incubations, medium was removed

by aspiration, and the cells were washed once with ice-cold

NaCl⁄ Pi

Alkaline sedimentation analysis of cellular DNA

To analyse the length distribution of growing daughter

strands of T24 DNA, cultures on 35-mm glass Petri dishes

were pulse labelled for 8 min with 7 lCi [methyl-3

H]deoxy-thymidineÆmL)1 Labelling was stopped by washing the cells

with ice cold NaCl⁄ Pi The cells were trypsinized and

layered onto the top of 15–30% alkaline sucrose gradients

After denaturation of the DNA for 6 h, centrifugation was

performed at 20 000 r.p.m., at 23C for 10 h in a Beckman

SW28 rotor (Krefeld, Germany) Fractions of 1.2 mL were collected from the top of the gradient and processed to ana-lyse acid insoluble radioactivity

Cell fractionation Fractions containing cytosolic, nucleosolic, and chromatin bound proteins of the cells were prepared as described pre-viously [27] Modified buffers were used for immunoprecipi-tation and kinase assays The cytosolic proteins were obtained after incubation of the cells in buffer A [50 mm Hepes pH 7.5; 20 mm b-glycerolphosphate; 1 mm dithio-threitol; containing aprotinin (1 lm); leupeptin (50 lm); 4-(2-aminoethyl)-benzenesulfonylfluoride HCl (AEBSF) (1 mm); NaF (10 mm); and Na3Vo4(1 mm)] and subsequent disruption of the cellular envelope with 20 strokes of a tight fitting pestle Nucleosolic proteins were obtained after incu-bation in buffer B (buffer A containing 0.1% NP40) The remaining chromatin bound proteins were solubilized by incubating the chromatin in IP buffer (buffer B containing

450 mm NaCl) for 1 h on ice and subsequent centrifuga-tion The fraction remaining after extraction of nuclei con-tains about 8.2% of total protein recovered and 96.6% of total DNA

Immunoprecipitation, kinase assay and phosphatase digestion

For immunoprecipitation of Cdk2 and the subsequent kin-ase assay, solutions of cytosolic, nucleosolic, solubilized chromatin bound or total cellular proteins were adjusted to equal protein content (300 lg) and incubated with 2 lg Cdk2 antibody (Santa Cruz, Clone M2; Santa Cruz, CA, USA) for 40 min on ice Then, 20 lL of a slurry of Protein G-agarose beads (Roche, Mannheim, Germany) equili-brated with IP buffer were added, and incubation was con-tinued overnight under continuous rotation

Subsequently, the beads were washed three times with

500 lL IP buffer and three times with 500 lL kinase buffer [50 mm Tris pH 7.5; 10 mm MgCl2; 1 mm dithiothreitol;

20 mm b-glycerolphosphate; containing aprotinin (1 lm); leupeptin (50 lm); AEBSF (1 mm); NaF (10 mm); and

Na3Vo4 (1 mm)] Excess solution was removed completely and beads were incubated for 30 min at 30C in a mix of

20 lL kinase buffer containing 2.5 lg H1; 0.2 mm ATP; and 10 lCi [32 (or33)P]ATP[cP] in the absence or presence of Cdk2 inhibitors

Incubation was stopped by adding 20 lL 2· protein sam-ple buffer After denaturation, the reaction products were separated by an SDS⁄ PAGE on a 12% polyacrylamide gel, blotted onto a Nylon-P membrane (Amersham, Bucks, UK) and subsequently exposed to Hyperfilm MP (Amersham) For immunoprecipitation and subsequent phosphatase digestion of Cdc6 or pRb, respectively, solutions of

Trang 10

solubilized chromatin bound proteins, containing 300 lg of

protein, were incubated with 2 lg Cdc6 antibody

(MoBi-Tec, Clone DCS-180), or pRb antibody (Pharmingen,

Clone G3-245; BD Biosciences Pharmingen, Canada) for

40 min on ice Then, 20 lL of a slurry of Protein A-agarose

beads (Bio-Rad, Hercules, CA, USA) equilibrated with IP

buffer were added, and incubation was continued for 3 h

(Cdc6) or overnight (pRb) under continuous rotation

Sub-sequently, the beads were divided in two equal parts and

washed three times with IP buffer Protein sample buffer

(20 lL) was added to one part afterwards The other part

was washed three times with phosphatase buffer (New

Eng-land Biolabs, Beverly, MA, USA) supplemented with

prote-ase inhibitors Phosphatprote-ase digestion was performed for

30 min at 30 with 200 U Lambda phosphatase (New

Eng-land Biolabs) After a final wash with IP buffer 20 lL

pro-tein sample buffer were added After denaturation, propro-teins

were separated on an 8% (49 : 1, Cdc6, PCNA and total

pRb) or 10% (149 : 1, chromatin bound-pRb) SDS⁄

poly-acrylamide gel, blotted onto Hybond-P (Amersham)

Pro-teins were visualized as described below

Immunofluorescence staining of Cdk2

Cells grown on coverslips and incubated with the

fluoresc-ein isothiocyanate (FITC) labelled Cdk2⁄ cyclin inhibitory

peptide II during the respective incubations, washed once

with ice-cold NaCl⁄ Pi For subsequent immunostaining of

Cdk2, cells were directly fixed with ice cold acetone⁄

meth-anol (1 : 1, v⁄ v) for 10 min at 4 C and processed for

detec-tion of Cdk2 after air drying Cells were blocked with 1%

(w⁄ v) BSA in NaCl ⁄ Pifor 20 min and incubated with the

Cdk2-antibody (Pharmingen, Clone 55) in NaCl⁄ Pi⁄ BSA

for 1 h at room temperature After washing three times

with NaCl⁄ Pi for 5 min they were further incubated for

30 min with a mouse-antibody labelled with Alexa Fluor

586 (Molecular Probes, dilution 1 : 200; Eugene, OR, USA)

in NaCl⁄ Pi⁄ BSA Cells were again washed three times for

5 min with NaCl⁄ Pi During the last wash total DNA was

stained with bisbenzimide (2 lgÆmL)1 in NaCl⁄ Pi) Finally

Cdk2, the Cdk2⁄ cyclin inhibitory peptide II and total DNA

(bisbenzimide stain) were visualized with a Zeiss

fluores-cence microscope (Axioskop; Jena, Germany) using the

appropriate filter combinations

Electrophoresis of proteins and western blotting

Cytosolic and nucleosolic proteins were precipitated from

the respective supernatants using the procedure described

by Wessel-Flu¨gge [54] Chromatin bound proteins for

west-ern blot analysis were either separated from the DNA by

treatment with 450 mm NaCl in buffer B and subsequent

Wessel-Flu¨gge precipitation as described above, or

chroma-tin was directly denatured and solubilized with SDS

electro-phoresis sample buffer

After determination of protein concentration (BioRad

DC protein assay) equal amounts were separated on appro-priate SDS⁄ polyacrylamide gels, blotted onto a Nylon-P membrane and subsequently immunodetected using the ECL western blotting procedure (both Amersham), accord-ing to the manufacturer’s instructions Dilution of antibod-ies used was as follows: Cdk2 (Pharmingen, Clone 55)

1 : 2,500, Cdc6 (Santa Cruz, 180.2) 1 : 500, pRb (Pharmin-gen, Clone G3-245) 1 : 1,000, hypophosphorylated pRb (Pharmingen, Clone G99-549), PCNA (Santa Cruz, clone PC10) 1 : 10 000

Acknowledgements

We thank Hubert Kalbacher for generous gift of the Cdk2⁄ cyclin inhibitory peptide II This work was sup-ported by the Wilhelm-Schuler Stiftung

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