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Tiêu đề DNA Modification With Cisplatin Affects Sequence-Specific DNA Binding Of P53 And P73 Proteins In A Target Site-Dependent Manner
Tác giả Hana Pivoňková, Petr Pečinka, Pavla Češková, Miroslav Fojta
Trường học Academy of Sciences of the Czech Republic
Chuyên ngành Biophysics
Thể loại Báo cáo khoa học
Năm xuất bản 2006
Thành phố Brno
Định dạng
Số trang 14
Dung lượng 538,41 KB

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Binding of both proteins to mutated p53 DNA-binding sites from which these motifs had been eliminated was only negligibly affected by cisplatin treatment, suggesting that formation of th

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DNA binding of p53 and p73 proteins in a target

site-dependent manner

Hana Pivonˇkova´1, Petr Pecˇinka1, Pavla Cˇ esˇkova´2

and Miroslav Fojta1

1 Institute of Biophysics, Academy of Sciences of the Czech Republic, Brno, Czech Republic

2 Masaryk Memorial Cancer Institute, Brno, Czech Republic

The tumor suppressor protein p53 is known as a

tran-scription factor involved in cell cycle control [1–3] It

plays a crucial role in preventing malignant

transfor-mation of a cell via induction of cell cycle arrest or

programmed cell death in response to stress conditions

(e.g DNA damage) The functions of p53 are closely

related to sequence-specific recognition of response

ele-ments [p53 DNA-binding sites (p53DBSs)] in

promot-ers of downstream genes such as p21WAF1⁄ CIP1

(involved in cell cycle arrest), Bax (apoptosis), and

mdm2 (negative feedback regulation of p53) [1–3]

Using chromatin immunoprecipitation combined with

a paired-end ditag DNA sequencing strategy, Wei

et al have recently established a global map of p53-binding sites encompassing over 540 loci in the human genome [4] A typical p53DBS consists of two tandem copies of the motif RRRCWWGYYY (where R¼ A

or G, Y¼ C or T, and W ¼ A or T), which may be separated by one or more base pairs [4,5] Natural p53 response elements exhibit surprisingly high sequence variability and may contain one or several nucleotides not fitting the above formula [6,7] The p53 protein binds to the response elements as a tetramer via its core domain The importance of p53 sequence-specific

Keywords

cisplatin; DNA damage; protein p73;

sequence-specific DNA recognition; tumor

suppressor protein p53

Correspondence

M Fojta, Institute of Biophysics, Academy

of Sciences of the Czech Republic,

Kra´lovopolska´ 135, CZ-612 65 Brno,

Czech Republic

Fax: +420 541211293

Tel: +420 541517197

E-mail: fojta@ibp.cz

(Received 25 April 2006, revised 18 July

2006, accepted 17 August 2006)

doi:10.1111/j.1742-4658.2006.05472.x

Proteins p53 and p73 act as transcription factors in cell cycle control, regu-lation of cell development and⁄ or in apoptotic pathways Both proteins bind to response elements (p53 DNA-binding sites), typically consisting of two copies of a motif RRRCWWGYYY It has been demonstrated previ-ously that DNA modification with the antitumor drug cisplatin inhibits p53 binding to a synthetic p53 DNA-binding site Here we demonstrate that the effects of global DNA modification with cisplatin on binding of the p53 or p73 proteins to various p53 DNA-binding sites differed signifi-cantly, depending on the nucleotide sequence of the given target site The relative sensitivities of protein–DNA binding to cisplatin DNA treatment correlated with the occurrence of sequence motifs forming stable bifunc-tional adducts with the drug (namely, GG and AG doublets) within the target sites Binding of both proteins to mutated p53 DNA-binding sites from which these motifs had been eliminated was only negligibly affected

by cisplatin treatment, suggesting that formation of the cisplatin adducts within the target sites was primarily responsible for inhibition of the p53 or p73 sequence-specific DNA binding Distinct effects of cisplatin DNA modification on the recognition of different response elements by the p53 family proteins may have impacts on regulation pathways in cisplatin-treated cells

Abbreviations

cisPt-DNA, cisplatin-modified DNA; CTDBS, C-terminal DNA-binding site; EMSA, electrophoretic mobility shift assay; fl, full length;

IAC, intrastrand crosslink; oligo, oligonucleotide; p53DBS, p53 DNA-binding site.

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DNA binding is underlined by the fact that most of

the cancer-related point mutations of p53 are located

in its core domain and the mutants are typically

unable to recognize the p53 response elements [1,8,9]

Besides the nucleotide sequence, binding of p53 to

the p53DBSs appears to depend on conformational

features of its target sites It has been proposed that

intrinsic bending of the p53DBSs contributes

signifi-cantly to the stability of the p53–DNA complexes [10]

In addition, interactions of the p53 protein with

cer-tain response elements can be controlled by changes in

DNA topology inducing formation of non-B DNA

structures within the binding sites [11,12] Interactions

of p53 with DNA are regulated mainly via

post-trans-lational modifications (phosphorylation, acetylation)

within the protein C-terminal domain [3,13,14]

Trun-cated forms of p53 lacking a negative-regulating

seg-ment at the protein C-terminus (residues 369–383 [15])

are constitutively active for sequence-specific DNA

binding [7,16] On the other hand, the C-terminus of

p53 was shown to be critical for its

conformation-selective DNA binding [11,12,17,18] and to favor p53

interactions with p53DBSs within long DNA molecules

[19,20]

The p73 protein has been identified as a p53

homo-log exhibiting 63% amino acid sequence identity in the

DNA-binding domain [21–23] In agreement with this

homology, the p73 protein can recognize the same

response elements as the p53 protein and activate an

analogous set of downstream genes Multiple splice

isoforms of the p73 protein have been found that differ

in the structure of their N-terminal and⁄ or C-terminal

domains [21,22] Although it was originally supposed

that the p53 homologs have redundant functions in the

regulation of gene expression, more recent data suggest

that p73 and p63 proteins do not act as ‘classic’ tumor

suppressors, but rather play important roles in the

regulation of cell development and differentiation

[21,23] Nevertheless, some observations suggest that

p73 is involved in the cellular response to DNA

dam-age and in apoptosis control [24,25]

Cisplatin [cis-diamminedichloroplatinum(II)] is a

clinically used anticancer agent [26,27] The drug binds

covalently to DNA, forming several kinds of adduct,

among which the most abundant are intrastrand

cros-slinks (IACs) between neighboring purine residues

The spectrum of cisplatin adducts identified in globally

modified chromosomal DNA comprises about 50%

of 1,2-GG IACs, 25% of 1,2-AG IACs, 10% of

1,3-GNG IACs and interstrand crosslinks, and another

2–3% of monofunctional adducts It has been found

that cisplatin cytotoxicity is related mainly to the IACs

that induce significant changes in the DNA

conformation, including bending and unwinding of the DNA double helix [26,28] The lesions are selectively bound by a variety of nuclear proteins, and it was pro-posed that these interactions are important for the anticancer activity of the drug [26,29,30]

Interactions of the p53 protein with cisplatin-modi-fied DNA (cisPt-DNA) have recently been studied [31– 36] In the absence of the p53DBS, enhancement of p53 sequence-nonspecific DNA binding due to DNA cis-platination was observed [33–36] On the other hand, the same DNA treatment resulted in inhibition

of p53 sequence-specific binding [31,32] An analogous inhibitory effect was observed with the anticancer tri-nuclear platinum complex BBR3464 but not with the clinically ineffective transplatin Quite recently, it has been shown that DNA modification with a transplatin analog, trans-[PtCl2NH3(4-hydroxymethylpyridine)], inhibits p53 binding to the same p53DBS similarly as does cisplatin [37] It has been proposed that the inhib-itory effects of the anticancer platinum complexes are due to the formation of platinum adducts within the p53DBS [31,32] To our knowledge, no analogous studies of the p73 protein interactions with chemically damaged DNA have been reported yet

In this work, we investigated the effects of global DNA modification with cisplatin on sequence-specific binding of p53 and p73 proteins to different target sites We demonstrated that the sensitivity of the pro-tein–DNA interactions to cisplatin DNA treatment correlated with the occurrence of sequence motifs forming the cisplatin IACs (namely GG and AG dou-blets) within the given p53DBS Binding of both pro-teins to mutated target sites not containing these motifs was not significantly affected by the DNA cis-platination Formation of the cisplatin adducts outside the p53DBSs did not apparently influence p53 sequence-specific DNA binding

Results

To analyze the sequence-specific DNA binding of p53 and p73 proteins, we designed 50-mer oligonucleotide substrates bearing various p53DBSs (Fig 1) In most experiments, we used a C-terminally truncated, consti-tutively active p53(1–363) to eliminate the sequence-nonspecific p53 interactions with the cis-platinated DNA, which have been shown to be mediated pri-marily by the p53 C-terminal DNA-binding site (CTDBS) [34] In the presence of competitor nonspe-cific DNA, sequence-spenonspe-cific binding of the p53(1– 363) protein to the 32P-labeled 50-mer targets resulted

in the appearance of a distinct retarded band R53 in the polyacrylamide gel (Fig 2) Binding of the p73b

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Fig 1 Scheme of DNA substrates used in this work All p53 DNA-binding sites (p53DBSs) were placed in the center of 50-mer oligonucleo-tides (oligos), being flanked with the sequences shown on the top (the same stretches flank the p53DBSs in the pPGM1 and pPGM4 plas-mids) The left part of the scheme shows two p53DBSs derived from natural p53 response elements in p21 (5¢-promoter) and mdm2 promoters, as well as the synthetic p53DBS PGM1 Motifs forming bifunctional adducts with cisplatin are highlighted (GG doublets are in bold and underlined, AG doublets are in bold, and GNG triplets are marked by brackets) The p53DBSs shown on the right are derivatives of p21 (p21a and p21b) or pPGM1 (pPGM4) In the latter targets, the incidence of the cisplatin-reactive sites was reduced or eliminated Bases not fitting the ‘canonical’ p53DBS [5] are denoted by lower-case letters.

Fig 2 Electrophoretic mobility shift assay of sequence-specific binding of p53 or p73 proteins to a 50-mer oligonucleotide (oligo) involving the p53 DNA-binding sites (p53DBSs) (A) The 32 P-labeled p21 target was incubated with the given protein in presence of competitor calf thymus DNA, and this was followed by electrophoresis on 5% polyacrylamide gel Lane 1 contains only DNA without any protein; lanes 2, 3 and 4 correspond to DNA complexes with p53(1–363), p73d and p73b, yielding retarded bands R53, R73dand R73b, respectively In lanes 5–7, the protein–DNA complexes are supershifted with monoclonal antibodies DO-1 (p53) or anti-HA (both p73 isoforms; the respective super-shifted bands are denoted as SR 53 , SR 73d and SR 73b ; the presence of two supershifted bands in each of the lanes 5–7 corresponds to two possible stoichiometries of the antibody–protein complexes) (B) Sections of an autoradiogram showing retarded bands due to binding of p53(1–363) or p73d proteins to 50-mer target oligos containing PGM1, PGM4, mdm2, p21, p21a and p21b sites Other details as in (A), lanes

2 and 3.

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and p73d proteins to the DNA targets caused the

for-mation of analogous retarded bands (denoted as R73b

or R73d, respectively; lanes 3 and 4 in Fig 2A) whose

mobilities reflected different molecular weights of the

p73 isoforms To verify the specificity of the band

shifts for DNA complexes with the proteins studied,

we used the band supershift assay with antibodies

against the p53 or p73 proteins Addition of the

DO-1 antibody [DO-17,38,39] mapping to the N-terminus of

the p53 protein resulted in further retardation of the

specific p53–DNA complexes (lane 5 in Fig 2A),

producing two supershifted bands (SR53; Fig 2A)

Formation of the two bands corresponded to two

possible stoichiometries of the antibody–p53 complex,

involving either one or two antibody molecules bound

per p53 tetramer [16,39] For supershifting of DNA

complexes with the p73 constructs, which were tagged

with hemagglutinin (HA), we used antibody to HA

and obtained analogous band patterns to those

obtained with p53 (Fig 2; lanes 6–7, bands SR73b

and SR73d), confirming the specificity of the observed

protein–DNA complexes All 50-mer substrates used

in this work were efficiently bound by the p53 and

p73 proteins [shown in Fig 2B for p53(1–363) and

p73d], although their affinities for the proteins

dif-fered to some extent (which was manifested by

differ-ent intensities of the R bands) To eliminate these

differences, the effects of DNA cis-platination on the

protein–DNA interactions were always normalized

with the intensity of the retarded band resulting from

protein binding to the same but unmodified p53DBS

Effects of cisplatin DNA modification on

sequence-specific binding of the p53 protein

Previously, it has been shown [31,32] that DNA

modi-fication with cisplatin causes dose-dependent inhibition

of the full-length (fl) p53 sequence-specific DNA

bind-ing to the synthetic target site PGM1 (Fig 1) Here,

we studied the effects of DNA treatment with cisplatin

on p53(1–363) binding to the p53DBSs PGM1, p21

and mdm2 (Fig 1) within the 50-mer oligonucleotides

(oligos) (Fig 3A) All targets were treated with the

drug in excess of nonspecific calf thymus DNA

Inter-action of the protein with any of these targets was

sig-nificantly affected by the cisplatin treatment, but the

levels of inhibition observed with individual p53DBSs

at the same degree of global DNA cis-platination

dif-fered significantly The steepest decrease in p53–DNA

binding with degree of DNA modification was

exhib-ited by the mdm2 target The R53 band due to the

p53–mdm2 complex exhibited only 10% intensity for

rb¼ 0.02, compared to the R53 band due to protein

binding to the same but unmodified substrate (the rb value refers to the number of platinum atoms per total DNA nucleotide) In contrast, the PGM1 and p21 tar-gets retained 75% and 53% of the p53-binding capa-city at rb¼ 0.02, respectively (Fig 3A) Increasing the DNA modification degree to rb¼ 0.04 resulted in a decrease of p53–p21 binding to 42%, whereas the PGM1 site bound only 16% of the protein, compared

to the same but unmodified p53DBS At rb¼ 0.06, all mdm2, PGM1 and p21 targets exhibited very weak p53 binding (about 4% for mdm2 and PGM1 and 10% for p21)

Sensitivity of the sequence-specific p53 DNA binding to DNA cis-platination depends on the incidence of cisplatin-reactive motifs within the p53DBSs

The mdm2, PGM1 and p21 target sites (Fig 1) differ significantly in the occurrence of sequence motifs known to form the cisplatin IACs [26,27] The p21 site, showing the weakest sensitivity of p53 binding to cisp-latin treatment, contains only one GGG triplet within the p53DBS The PGM1 site possesses two AGG tri-plets in one strand and two AG steps in the other The mdm2 target, whose interaction with p53 was most strongly affected by DNA cis-platination, contains

GG, GGG and AG motifs in one strand and GG and GTG motifs in the other, thus offering not only the highest total number of reactive motifs among the p53DBSs tested, but also the highest number of sites known to be modified most frequently (i.e the GG doublets)

For the subsequent experiments, we designed mutated p53 target sites from which the cisplatin-react-ive motifs were eliminated Two p53DBSs were dercisplatin-react-ived from the p21 target site (Fig 1); in p21a, the GGG triplet in the bottom strand was mutated into GAG This exchange resulted in elimination of the most reactive GG doublets and the introduction of less reactive AG and⁄ or GNG motifs [26] In p21b, the GGG triplet in the bottom strand was replaced by GAA, which contains neither RG nor GNG motifs (Fig 1); owing to this mutation, all sites suitable for formation of the bifunctional cisplatin adducts were removed from the p53DBS In addition, we derived another ‘unreactive’ p53DBS from the PGM1 target (PGM4; Fig 1) by replacing all guanine residues, except for those at the strictly conserved positions [4,5], by adenines All of these mutated p53DBSs (when cisplatin-unmodified) exhibited sequence-specific p53 binding comparable to that of the parent targets (Fig 2B)

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We studied how the cisplatin treatment influences

interaction of the p53(1–363) protein with the

mutated target sites The 50-mer oligos containing

sequences p21a, p21b or PGM4 were treated with

cisplatin as above DNA modification to rb¼ 0.02

resulted in a decrease of p53 binding to the p21a

tar-get by about 15%, which represented weaker

inhibi-tion than observed with the p21 target (25% decrease;

Fig 3) More conspicuous differences between the

p21a and p21 targets appeared at rb¼ 0.04 (35% or

58% inhibition, respectively) At rb¼ 0.06, the p21a

target retained 45% of the p53 binding, thus

exhibit-ing at least four times higher bindexhibit-ing capacity than

the natural p21 p53DBS treated in the same way

Binding of p53 to the mutated target p21b exhibited

even more remarkable resistance to the cisplatin

treat-ment For rb values of 0.02, 0.04 or 0.06, 100%, 91%

or 85% of the p21b target was bound by the protein,

respectively, when compared to the untreated p21b

The behavior of the PGM4 site was similar to that of p21b, showing practically no inhibition of p53–PGM4 binding for rb¼ 0.02 or 0.04 and about 10% inhibi-tion for rb¼ 0.06 The PGM4 site also exhibited practically no loss of its p53-binding capacity due to the DNA cis-platination when located within a

474 base pair fragment of the pPGM4 plasmid (not shown), in contrast to the behavior of the analogous pPGM1 fragment [31] These data revealed a clear correlation between the sensitivity of the p53 sequence-specific DNA binding to DNA treatment with cisplatin and the ability of the particular p53 target site to accommodate the cisplatin IACs The higher the probability of formation of the cisplatin IACs within the p53DBSs due to the occurrence of the GG, AG and⁄ or GNG motifs, the stronger the inhibition of the p53 sequence-specific DNA binding

to these targets caused by the DNA treatment with cisplatin

Fig 3 Effects of DNA modification with cisplatin on p53(1–363) binding to various target sites: (A), natural p53 DNA-binding sites (p53DBSs) mdm2 and p21, and the synthetic PGM1 sequence; (B) mutated p53DBSs PGM4, p21a and p21b (Fig 1) The top panels show sections of autoradiograms showing the R 53 bands corresponding to complexes of p53 with the 50-mer target oligonucleotides (oligos) (Fig 2) The extents of DNA modification with cisplatin (rb) are indicated Other details are as in Fig 2 The graphs show the dependence of relative p53 binding to the targets on the degree of DNA modification (data obtained from densitometric tracing of the autoradiograms; for each target site, the intensity of the R 53 band resulting from p53 binding to unmodified DNA was taken as 1.0, and the intensities of bands correspond-ing to p53 bindcorrespond-ing to the same but cisplatin-treated substrate were normalized to this).

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We also performed parallel experiments with fl p53

(expressed in insect cells) Like p53(1–363), the fl

pro-tein was able to recognize sequence specifically all of

the targets tested (not shown) The effects of the

degree of DNA cis-platination on recognition of the

particular target site by the fl p53 were analogous to

those observed with the C-terminally truncated p53(1–

363) (shown in Fig 4 shown for the mdm2, PGM1

and PGM4 targets)

Effects of DNA cis-platination on

sequence-specific DNA binding of p73 proteins

We tested the influence of DNA modification with

cisplatin on the binding of two p73 isoforms, p73d and

p73b, to the p21 target site (Fig 5) The intensity of

the resulting R73dband decreased almost linearly with

increase in the cis-platination level; for rb¼ 0.06,

about 90% inhibition of p73d–p21 binding was

observed Almost the same results were obtained when

interaction of the p73b isoform with the p21 target

was examined (Fig 5) In contrast, modification of

p21b to rb¼ 0.02 or 0.04 had no significant effect on

its interaction with either of the p73 isoforms; at rb¼

0.06, only slight (10–15%) inhibition of binding was

detected Thus, the p73d and p73b proteins exhibited

behavior upon binding to cisplatin-treated p21 and

p21b target sites that was very close to that of the p53

protein Analogous results were obtained with the

PGM1 and PGM4 target sites (not shown)

Competition experiments

We studied the influence of cisplatin DNA

modifica-tion on the competimodifica-tion between two p53 target sites

for the protein (Fig 6) The 474 base pair fragments

of plasmids pPGM1 or pPGM4 were used as the sequence-specific competitors, and changes in p53(1– 363) binding to the32P-labeled 50-mer targets were fol-lowed We first tested the effect of the presence of the competitor fragments (unmodified or treated with cisp-latin) on p53 binding to the unmodified PGM1 probe (Fig 6A) Addition of either of the unmodified frag-ments (70 ng per sample) resulted in a partial decrease (by 35–45%) of the R53band intensities due to binding

of a portion of the p53 molecule to the competitor p53DBS Modification of the pPGM1 fragment with cisplatin caused a reduction of its competitiveness, which was manifested by increasing relative intensity

of the R53 band yielded by the p53 complex with the radiolabeled PGM1 probe When the pPGM1 frag-ment was cis-platinated to rb¼ 0.04 or 0.06, its pres-ence had practically no effect on the R53 band intensity, suggesting that the modified pPGM1 frag-ment had lost its ability to compete for the protein (Fig 6A) In contrast, the competition ability of the pPGM4 fragment was not significantly influenced by its cis-platination This observation was in agreement with the resistance of p53 binding to the PGM4 target site to the cisplatin DNA treatment (see above)

In addition, we modified with cisplatin equimolar mixtures of the pPGM1 fragment with the 32P-labeled 50-mer targets p21 or p21b (in the presence of nonspe-cific competitor DNA), and performed a p53-binding assay (Fig 6B) In the unmodified DNA, the compet-itor pPGM1 fragment caused about 70% inhibition of p53(1–363) binding to either of the two targets Modi-fication of the p21⁄ pPGM1 mixture resulted in

rb-dependent inhibition of p53 binding to the p21 tar-get, but in contrast to the results shown in Fig 3 (where only the p21 target and nonspecific competitor DNA were present in the sample), the cisplatin inhibi-tion effect was detectable only at rb¼ 0.04 and 0.06 The apparent lack of the cisplatin effect at rb¼ 0.02 can be attributed to partial loss of the competitiveness

of the pPGM1 fragment due to its modification, which compensated for inhibition of p53 binding to the (rel-atively less reactive) p21 target When the mixture of the p21b target with the pPGM1 competitor fragment was treated with cisplatin in the same way, the inten-sity of the R53 band on the autoradiogram increased with the degree of DNA modification The increase was already significant at rb¼ 0.02 At rb¼ 0.04 or 0.06, the relative intensity of the R53 band reached about 90% of the value observed with unmodified DNA (Fig 6B) Such behavior reflected inhibition of p53 binding to the competitor pPGM1 fragment due

to its cis-platination, whereas interaction of the protein with the p21b target remained practically unaffected

Fig 4 Effects of DNA modification with cisplatin on full-length p53

binding to the mdm2, PGM1 and PGM4 targets For more details,

see Figs 2 and 3.

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under the same conditions The results of these model

competition experiments suggest that global

modifica-tion of DNA with cisplatin may shift the distribumodifica-tion

of the p53 protein among different target sites,

depend-ing on the susceptibility of the particular p53DBSs to

modification with the drug

Discussion

It has been demonstrated previously that interactions

of the tumor suppressor protein p53 with DNA are

influenced by covalent modification of the DNA by

antitumor platinum complexes [31–36]

Sequence-non-specific DNA binding (in the absence of the p53DBS)

of the p53 protein was significantly enhanced by DNA

modification with cisplatin [31,33,34] The ability of

p53 to recognize the cisPt-DNA was more pronounced

for the post-translationally unmodified (‘latent’) form

of the protein than for its ‘activated’ forms [33] Recently, it has been reported that accessibility of the p53 CTDBS is critical for (sequence-nonspecific) cisPt-DNA recognition [34] On the other hand, sequence-specific binding of p53 to the synthetic p53DBS PGM1 was inhibited in cisplatin-treated DNA [31,32] As the PGM1 site contains several sequence motifs known to form the most abundant cisplatin adducts (see Fig 1), the cisplatin inhibitory effects could be explained by DNA damage within the p53DBS It is known that the cisplatin IACs induce considerable DNA bending and untwisting as well as perturbation of hydrogen bond-ing within the base pairs [26–28] Cisplatin adducts occurring within p53DBS can therefore be expected to cause severe deformations of the binding site with con-comitant destabilization of the p53–DNA interaction (or even prevention of target recognition by the pro-tein)

DNA binding of the C-terminally truncated p53(1–363) protein

In this work, we studied the effects of cisplatin treat-ment of various p53DBSs on the sequence-specific binding of a truncated tetrameric p53 construct lacking the C-terminal DNA-binding site, p53(1–363) [18,34] This variant of the protein is known to be constitu-tively active for sequence-specific DNA binding [16] Models of p53 latency considering the (post-transla-tionally unmodified) p53 C-terminus solely as a negat-ive regulator of sequence-specific DNA binding [40,41] have recently been questioned [42–44] Instead, the p53 CTDBS has been proposed to cooperate with the core domain in complex p53–DNA interactions The CTDBS has been shown to be essential for p53 bind-ing to target sites adoptbind-ing non-B conformations (such

as stem–loop or cruciform structures) [11,12,45–47]

On the other hand, p53 constructs lacking the CTDBS are capable of efficient binding to short linear model DNA targets in which the p53DBS is present in its double-helical B-form Moreover, deletion of the CTDBS (amino acids 363–382) makes it possible to separate sequence-specific p53 DNA binding from other modes of p53–DNA interaction that are medi-ated by the protein C-terminus, particularly the sequence-nonspecific binding of p53 preferentially to cisPt-DNA [33,34] Another CTDBS-lacking tetrameric p53 construct, p53CT (spanning amino acids 94–360), has recently been used by Weinberg et al for evalua-tion of the protein-binding affinities for 20 natural p53 recognition elements [7] A comparative study invol-ving four of them showed practically the same cooper-ative binding of the fl p53 as exhibited by p53CT [7]

Fig 5 The effects of DNA modification with cisplatin on binding of

the p73 proteins to the p21 and p21b target sites In the graph,

squares correspond to p73b and triangles to p73d For other details,

see Figs 2 and 3.

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Likewise, our parallel experiments with fl p53 yielded

results that were very similar to those obtained with

p53(1–363) (Figs 3 and 4) Hence, the C-terminally

truncated constructs are suitable models for

comparat-ive studies of p53 sequence-specific DNA binding to

various and⁄ or variously modified target sites

Inhibition of p53 sequence-specific DNA binding

is linked to cisplatin adduct formation within the

p53DBSs but not outside these target sites

The 50-mer target DNA substrates were treated with

the drug in the presence of an excess of nonspecific

competitor calf thymus DNA mimicking

random-sequence natural genetic material that can

accommo-date the cisplatin adducts regardless of the reactivity

of the particular p53DBS The frequency of DNA modification within the p53DBSs could thus be expec-ted to reflect the known distribution of cisplatin adducts in globally modified chromosomal (genomic) DNA [26] Provided that the cisplatin inhibitory effect

on p53 sequence-specific DNA binding is linked pri-marily to the IACs formed within the target sites, the susceptibility of different targets to the drug treatment should correlate markedly with the incidence of the cisplatin-reactive motifs in the p53DBSs Such a corre-lation was indeed found: the sensitivity of the target sites to treatment with the drug followed the trend mdm2 > PGM1 > p21 > p21a > p21b  PGM4, in accordance with the number and kind of motifs suit-able for formation of the IACs inside the p53DBSs (Fig 1)

Fig 6 Competition between two different p53 target sites in globally cisplatin-modified DNA for the p53(1–363) protein In (A), 32

P-labeled, unmodified PGM1 50-mer was mixed with cisplatin-treated competitor frag-ments of plasmids pPGM1 or pPGM4 (and with unmodified calf thymus DNA) prior to addition of the p53 protein When the com-petitor fragment was unmodified, the p53 protein was distributed between it and the labeled probe target (a) Upon cis-platination

of the pPGM1 competitor fragment (b), its affinity for the protein was decreased due

to formation of cisplatin adducts within the p53 DNA-binding site (p53DBS), resulting in increased p53 binding to the labeled probe The pPGM4 fragment (c) contains cisplatin-resistant p53DBS, and its cis-platination did not change its competitiveness for p53(1– 363) In (B), the32P-labeled targets p21 (i) and p21b (ii) were treated with cisplatin together with the competitor pPGM1 frag-ment, and this was followed by the p53-binding assay Such treatment resulted in a decrease of p53 binding to the p21 target [in agreement with formation of the adducts within both p21 and pPGM1 p53DBSs; see (i)] In contrast, apparent p53 binding to the p21b target increased under the same con-ditions [because the cisplatin adducts were formed within p53DBS of the competitor but not within the p21b target; see (ii)] The graphs show the relative binding of p53 to the radiolabeled targets as a function of rb; the intensities of the R 53 bands observed for the unmodified targets in the absence of the competitor fragments (first samples of each set) were taken as 1 For other details, see Figs 2 and 3.

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In the p21 50-mer target and its derivatives p21a

and p21b, the 5¢-neighboring guanines in the ‘top’

strand form another GG doublet with the first guanine

of the p53DBS (Fig 1) Interestingly, the presence of

this reactive motif had no conspicuous effect on p53–

p21b binding in the cisplatin-treated DNA, as there

were no significant differences between the behavior of

p21b and that of PGM4 (lacking this boundary GG

doublet; Fig 1) The results presented in this article do

not make it possible to decide whether a single

cisplat-in IAC, wherever it is withcisplat-in the p53DBS, can fully

abrogate p53 sequence-specific DNA binding, or

whe-ther the protein can recognize such a cis-platinated

site, albeit with lower affinity Nevertheless, our data

show clearly that a single reactive motif located within

the 20 base pair recognition element (e.g in p21;

Fig 1) caused significant sensitivity of p53–p53DBS

binding to the DNA treatment with cisplatin, whereas

the presence of an overlapping GG doublet formed by

one guanine inside and the other outside the p53DBS

was practically without effect

Under the conditions used in this work, the

appar-ent sensitivity of p53 (or p73) DNA binding to

cis-pla-tination was influenced primarily by the probability of

adduct formation within the target sites, regardless of

the positions of the cisplatin adducts The adduct

posi-tioning may be nevertheless be important with respect

to the stereochemistry of the protein–DNA recognition

(cis-platination induces significant bending and

tor-sional deformations of the DNA double helix [28]) and

the availability of functional groups ensuring the

essen-tial protein–DNA contacts For example, formation of

the cisplatin crosslinks within the CWWG box (which

represents an area where the p53 Arg248 residue

inter-acts with the DNA via a minor groove [48]) might be

particularly critical The mdm2 site is the only

p53DBS analyzed in this work that involves an AG

doublet within the CWWG tetramer (Fig 1), which

may contribute to its high sensitivity to the cisplatin

treatment We tested this possibility using another

p53DBS containing a single AG doublet (and no other

reactive motif) derived from PGM4 by inverting the

TA pair at position 6 Inhibition of p53(1–363) binding

to this site due to its treatment with cisplatin did not

exceed the effect observed with the p21a site (also

involving a single AG motif but outside the CWWG

box), suggesting that the highest sensitivity of the

mdm2 site towards cis-platination was connected with

the abundance of the highly reactive GG motifs rather

than with the location of the AG doublet within the

CWWG tetranucleotide On the other hand, our

pre-liminary results (M Fojta et al., unpublished data)

suggest that the behavior of cisplatin-treated target

sites possessing a single GG motif at various positions may differ significantly (more details will be published elsewhere)

Altered sequence-nonspecific interactions of the p53 protein with DNA due to its cis-platination outside the p53DBSs might, in principle, influence recognition of the target sites by the protein Nevertheless, control tests of binding of the p53(1–363) protein to unmodi-fied PGM1, PGM4, p21 and p21b targets in the pres-ence of unmodified or cis-platinated (rb¼ 0.06) calf thymus competitor DNA revealed no apparent effect

of the competitor modification This observation was

in agreement with the recently reported lack of ability

of p53(1–363) to recognize the nonspecific cisPt-DNA [34] Furthermore, we were interested in whether the presence of cisplatin adducts within DNA stretches flanking the p53DBSs affects the ability of p53 to bind the specific sequence The flanking segments in all 50-mer substrates used in this work (Fig 1) contain three motifs expected to form the 1,2-IACs (one GG and two AGs) Another two sets of 50-mer substrates, in which the PGM1 or PGM4 sites were flanked by seg-ments either totally lacking the cisplatin-reactive motifs

or containing multiple guanine doublets and⁄ or triplets (Fig 7), were used to check the influence of cisplatin adducts in the vicinity of p53DBS Again, the effects

of DNA cis-platination on p53(1–363) binding to these substrates were dependent on the presence of cisplatin-reactive motifs within the p53DBS but not within the flanking stretches (Fig 7), suggesting that cisplatin adducts outside the binding site (albeit close to it) do not significantly affect sequence-specific DNA recogni-tion However, it should be emphasized that such conclusions need not be applicable to the post-translationally unmodified form of fl p53, which exhibits apparently weaker binding to p53DBS but sig-nificant sequence-nonspecific preferential binding to globally cis-platinated DNA [31,33,34]

Binding of p73 proteins to the recognition elements is affected by DNA cis-platination in a similar way to p53 binding

In agreement with the considerable homology between the p53 and p73 DNA-binding (core) domains, the p73 protein can bind to the p53 response elements [21,22] Among the known p73 splice isoforms [21,23], p73d (coded by exons 2–10 of the p73 gene) is most similar

to the p53 protein with regard to the protein domain structure as well as molecular size The p73b isoform differs from p73d in its C-terminal domain, which,

in p73b, is extended by a stretch coded by exons 11 and 12 In neither of the p73 isoforms has another

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DNA-binding site (besides the core domain) analogous

to the p53 CTDBS been identified Our results showed

that both p73d and p73b bound efficiently to all

(unmodified) p53DBSs used in this work, and that

cisplatin treatment of p21, p21b (Fig 5), PGM1 and

PGM4 (not shown) affected the p73 sequence-specific

DNA binding basically in the same manner as

observed with p53

Possible impacts on gene expression

in cisplatin-treated cells

It has been well established that modification of DNA

with cisplatin affects fundamental processes such as

DNA synthesis and transcription [26] The bifunctional

cisplatin DNA adducts slow down or block DNA or

RNA polymerization and can hamper the initiation of

DNA transcription [49] Strong differential inhibition

of marker gene expression was observed in cells treated

with cisplatin [50] Interestingly, expression of genes

with stronger promoters was strongly inhibited,

whereas some genes possessing weaker promoters were

induced It was proposed that the strong promoters

were associated with accessible chromatin and

there-fore more easily modified by the drug [50] However,

to our knowledge, no systematic study of the

sensitiv-ity of various promoters (and particularly those

con-trolled by the p53 family proteins), differing in the

occurrence of the cisplatin-reactive nucleotide sequence

motifs, to cisplatin treatment has been conducted to

date

In response to genotoxic stress, the wild-type p53

can activate two different response pathways with

quite different impacts on the fate of the cell The first

involves cell cycle arrest via p21WAF1⁄ CIP1 induction and activation of DNA repair processes that, in gen-eral, confer chemoresistance to cancer cells The other pathway leads to programmed cell death through acti-vation of proapoptotic genes such as Bax, PUMA and Noxa [1–3] The apoptosis trigger is the desired event

in cancer therapy Despite considerable recent progress

in understanding the functions of p53 and its homo-logs, it has not yet been clarified how the checkpoint proteins decide which pathway to activate Partic-ularly, no unambiguous correlation between wild-type p53 expression and cancer cell susceptibility to cisplat-in-induced apoptosis has been established Although some authors reported a clear p53-dependent

apoptot-ic response to cisplatin [51–54], other investigations revealed a less distinct link between p53 status and cell sensitivity to cisplatin, or even suggested opposite effects [55–57] Several observations suggest that apop-tosis in cisplatin-treated cells may be regulated via p53- and⁄ or p73-dependent or -independent pathways [24,56,58] Hence, the response of a cancer cell to cisp-latin seems to be rather complex, and its relationship

to the status of the p53 family proteins does not appear to be straightforward

The results of our in vitro binding experiments sug-gest that the expression of various p53 downstream genes might be differentially affected in the cisplatin-treated cells, due to different susceptibilities of the p53 response elements to modification with the drug The natural p53DBSs [6,7] differ significantly in this respect Among the 20 response elements recently characterized by Weinberg et al [7], GADD45 (a gene taking part in DNA repair) no GG, three AG doublets) and the p21 5¢-site (a single GGG triplet)

Fig 7 The effect of DNA modification with cisplatin on p53(1–363) binding to p53 DNA-binding sites (p53DBSs) flanked by stret-ches either totally lacking sites reactive to cisplatin (PGM1-AT, PGM4-AT) or involving multiple reactive motifs (PGM1-GC, PGM4-GC) The flanking stretches are shown at the top; for the p53DBS,s see Fig 1 The experimental conditions are as in Figs 2 and 3.

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