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Recently, we affinity purified several MLL complexes from human cells and demonstrated that MLL1 plays critical roles in his-tone H3 lysine-4 methylation and Hox gene regulation [21].. The

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upon exposure to a food contaminant mycotoxin,

deoxynivalenol

Khairul I Ansari1, Imran Hussain1, Hriday K Das2and Subhrangsu S Mandal1

1 Department of Chemistry and Biochemistry, The University of Texas at Arlington, TX, USA

2 Pharmacology & Neuroscience, University of North Texas Health Science Center, Fort Worth, TX, USA

Elucidating the regulatory network of proto-oncogenes

in normal healthy cells and under toxic stress is

impor-tant for understanding the mechanism of human

dis-eases [1–5] Mixed lineage leukemias (MLLs) are a set

of evolutionary conserved genes that are often

rear-ranged and misregulated in acute lymphoblastic and

myeloid leukemias [1,2,6] Humans encode several

MLL protein families, such as MLL1, MLL2, MLL3,

MLL4 and Set1 [1,7–14] In general, they are master

regulators of homeobox (Hox) genes which are critical

for cell differentiation and development [1,2,15,16]

Because of their importance in gene regulation and

dis-ease, researchers have purified MLL proteins from

human cells and have demonstrated that MLLs posses

histone H3 lysine-4-specific methyl-transferase activities

and play a critical role in gene activation [9,17–20]

MLLs exist as multiprotein complexes inside cells with

several common protein subunits such as Ash2, Wdr5,

Rbbp5 and CGBP [1,9,10,19,21] Recently, we affinity purified several MLL complexes from human cells and demonstrated that MLL1 plays critical roles in his-tone H3 lysine-4 methylation and Hox gene regulation [21] We also demonstrated that downregulation of MLL1 results in cell-cycle arrest in the G2⁄ M phase indicating its critical role in cell-cycle progression [22] Although recent discoveries of MLL-associated his-tone H3 lysine-4-specific methyl-transferase activities have shed significant light on the complex function of MLLs in gene regulation, little is known about their own regulation in normal cells or in cells under stress [1] However, it has been reported that certain chemo-therapeutic stresses result in MLL rearrangement and misregulation, leading to the development of secondary leukemias in humans [23,24] These observations indi-cated that MLL1 is stress-responsive gene Herein, we studied the effect of a potential carcinogenic

mycotox-Keywords

deoxynivalenol; mixed lineage leukemia;

MLL; mycotoxin; Sp1

Correspondence

S S Mandal, Department of Chemistry and

Biochemistry, The University of Texas at

Arlington, Arlington, TX 76019, USA

Fax: +1 817 272 3808

Tel: +1 817 272 3804

E-mail: smandal@uta.edu

(Received 2 February 2009, revised 29

March 2009, accepted 7 April 2009)

doi:10.1111/j.1742-4658.2009.07055.x

Mixed lineage leukemias (MLLs) are histone-methylating enzymes with critical roles in gene expression, epigenetics and cancer Although MLLs are important gene regulators little is known about their own regulation Herein, to understand the effects of toxic stress on MLL gene regulation,

we treated human cells with a common food contaminant mycotoxin, deoxynivalenol (DON) Our results demonstrate that MLLs and Hox genes are overexpressed upon exposure to DON Studies using specific inhibitors demonstrated that Src kinase families are involved in upstream events in DON-mediated upregulation of MLL1 Sequence analysis demonstrated that the MLL1 promoter contains multiple Sp1-binding sites and impor-tantly, the binding of Sp1 is enriched in the MLL1 promoter upon expo-sure to DON Moreover, antisense-mediated knockdown of Sp1 diminished DON-induced MLL1 upregulation These results demonstrated that MLL1 gene expression is sensitive to toxic stress and Sp1 plays crucial roles in the stress-induced upregulation of MLL1

Abbreviations

ChIP, chromatin immunoprecipitation; DON, deoxynivalenol; Hox, homeobox; MLL, mixed lineage leukemia.

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in, deoxynivalenol (DON) on the regulation of MLL1.

Notably, DON is a toxin produced by pathogenic

fungi during the infection of cereal crops and is often

linked with various acute and chronic human diseases,

including cancer [25–27] Herein, we report that MLL1

and its target Hox genes are upregulated upon

expo-sure to DON and transcription factor Sp1 plays

criti-cal roles in the DON-mediated upregulation of MLL1

Results

DON induces expression of MLL

To understand the effects of mycotoxic stress on MLL

expression, we treated cultured human cells

(H358 cells) with varying concentrations of DON (up

to 33 lm) for 7.5 h We isolated RNA from the treated

and untreated control cells and subjected it to

RT-PCR with primers specific to MLL1 and Set1 As seen

in Fig 1A,B, treatment with DON induced two- to five-fold overexpression of MLL1 and Set1 in a con-centration-dependent manner MLL1 overexpression

by DON was more dramatic (8.3-fold) at the protein level (lane 4, Fig 1C,D) The decrease in expression of MLL1 and Set1 at 10 h or longer (Fig 1C,D) is likely caused by cell death induced by DON Because MLL1

is upregulated upon exposure to DON, we analyzed the expression of several other proteins (such as Rbbp5, Wdr5 and Ash2) known to interact with MLL1 [9,21] We also analyzed the effect of DON on expression of some MLL1 target Hox genes (HoxA2, HoxA7, HoxB1, HoxB7, etc.) Importantly, similar to MLL1, Rbbp5 and Wdr5 were overexpressed upon treatment with DON, whereas Ash2 was not affected significantly (Fig 2) Similarly, HoxA7, HoxA2 and HoxB1were overexpressed, whereas HoxB7 was down-regulated upon exposure to DON (Fig 2 and data not shown) The upregulation of MLL1, its several

inter-Incubation time (h)

1 2 3 4 5 6

0 2.5 5 7.5 10 15

β -actin MLL1 Set1

0

2

4

6

8

10

0 h 2.5 h

5 h 7.5 h

10 h

15 h

1

2

3

4

5

6

0.33 µ M

3.3 µ M

33 µ M

β -actin

MLL1

Set1

1 2 3 4 5 6 7 8

0 0.33 3.3 33

DON (µ M )

B D

Fig 1 DON-induced expression of MLL 1 and Set1 (A) Human lung cancer cells (H358) were treated with varying concentra-tions (0–33 l M) of DON for 7.5 h Total RNA was subjected to RT-PCR analysis with primers specific to b-actin (control), MLL 1 and Set1 Each experiment was duplicated for accuracy (B) Quantification of MLL 1 and Set1 expression as seen in (A) Bars indi-cate SEM (C) Total protein extracts from DON (3.3 l M DON for various time points) treated H358 cells were analyzed by wes-tern blot using anti-actin (control), anti-MLL 1 and anti-Set1 Ig (D) Quantification of expressed proteins as seen in (C) relative

to actin.

Water DON

1 2 3 4 5 6 7 8

β -actin

Rbbp5

Ash2

Wdr5

HoxA7

HoxB7

0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0

A B

Fig 2 DON-induced expression of MLL 1- int-eracting and target genes (A) Human lung cancer cells (H358) were treated with 3.3 l M DON for 7.5 h Total RNA was subjected to RT-PCR analysis with primers specific for b-actin (control), Rbbp5, WDR5, Ash2, HoxA7 and HoxB7 Lanes 1–4, untreated control; lanes 5–8, treated with DON (B) Quantification of gene expression level as seen in (A) Bars indicate SEM.

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acting proteins or selected target Hox genes upon

exposure to DON indicated that expression of these

proteins is sensitive to toxic stress

Notably, we analyzed the effects of DON on cell

growth and determined the cytotoxicity (IC50) towards

H358 cells using a

3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl-tetrazolium bromideassay, as described

previ-ously [28] Upon treatment with 3.3 lm DON, up to 5,

47 and 68% of H358 cells were killed at 7.5, 24 and

72 h post treatment, respectively The IC50 value is

determined to be 1 lm These results demonstrated

that DON is significantly cytotoxic towards human

cells

Src kinase inhibitor suppressed the DON-induced

upregulation of MLL1

To understand potential mechanism of DON-mediated

upregulation of MLL1 and Hox genes, we examined

the involvement of different DON-responsive signaling

pathways Because DON is known to induce ribotoxic

stress that instigates various signaling cascades,

includ-ing MAP⁄ Src kinases [29–33], we initially examined

whether inhibition of MAP⁄ Src kinase activation had

any effect on DON-induced upregulation of MLL1

We treated cells with a Src kianse inhibitor (PP2) or a

MAP kinase inhibitor (PD98059) and then exposed the

cells to DON As expected, MLL1 was upregulated

upon treatment with DON (lanes 1 and 4–7, Fig 3)

However, upon treatment with PP2, DON-induced

expression of MLL1 and HoxA7 was suppressed in a

concentration-dependent manner at both the mRNA

and protein levels (compare lanes 4–7 with lane 1,

Fig 3A,B) These results indicated that Src kinases

play a critical role in regulating upstream events that

lead to MLL1 and HoxA7 upregulation by DON

Notably, PP2 has no significant effect on

DON-induced expression of Set1, Rbbp5, Ash2 and Wdr5

(data not shown) suggesting the involvement of

alter-nate pathways Because MLL1 induction was

sup-pressed by Src kinase inhibitor (PP2), we examined

whether MAP kinases are also involved in

DON-medi-ated MLL1 upregulation However, application of

PD98059 did not have any significant effect on

DON-induced upregulation of MLL1, indicating no

involve-ment of MAP kianses in this process (Fig 3C)

Sp1 plays a critical role in DON-induced MLL1

upregulation

To understand the mechanism of MLL1 upregulation

by DON, we analyzed the MLL1 promoter for the

presence of various cis-elements recognized by specific

transcription factors (such as Sp1, AP2), particularly those known to be activated by mycotoxins [27,29–36] Interestingly, we found the presence of multiple Sp1-binding sites in the MLL1 promoter ()3000 to +500 nucleotide region; Fig 4) To investigate possi-ble role of Sp1 in MLL1 gene regulation, we knocked down Sp1 in H358 cells by using Sp1-specific antisense and then analyzed the expression of MLL1 in the absence and presence of DON (3.3 lm) As seen in

Fig 5A,B, treatment with Sp1 antisense effectively knocked down Sp1 expression at both the mRNA and the protein level (compare lanes 1 with 3) Upon knockdown of Sp1, the basal level of MLL1 expression was not significantly affected at the mRNA or the

PP2 (µ M )

– –

1 2 3 4 5 6 7

β -actin MLL1

HoxA7 Ash2

10 0.1 1 10 25

A

+ + + +

PP2 (µ M ) 10 0.1 1 10 25

β -actin MLL1 Ash2

DON (3.3 µ M )

1 2 3 4 5 6 7

– – – + –

B

PD89059 (µ M )

1 2 3 4 5 6 7

β -actin MLL1

– – – –

25 1 5 25 50

C

Fig 3 Effect of DON on expression of MLL 1 and HoxA7 genes in presence of MAP ⁄ Src kinase inhibitor PP2 and PD98059 H358 cells were treated 0.1, 1, 10 and 25 l M PP2 and 1, 5, 25 and

50 l M PD98059 for 1 h prior to treatment with 3.3 l M DON for an additional 7.5 h (A) RT-PCR analysis of RNA extract from cells treated with PP2 with primers specific to b-actin (control), MLL1, Ash2 and HoxA7 (B) Western blot of the total proteins extract of the cells treated with PP2 with antibodies specific for b-actin, MLL 1 and Ash2 (C) RT-PCR analysis of RNA extract from cells treated with PD98059 with primers specific to b-actin (control) and MLL1 Each experiment was performed in duplicate.

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protein level (Fig 5A,B, lanes 1 and 3) Interestingly,

however, DON-induced upregulation of MLL1

(mRNA and protein level) was suppressed to almost

normal levels under an Sp1 knocked down

environ-ment (Fig 5A,B, lanes 2 and 4) These results

indi-cated that Sp1 is critical for MLL1 regulation,

especially in presence of DON

Because the MLL1 promoter contains multiple

Sp1-binding sites and our results demonstrated that Sp1 is

critical in regulating MLL1 on exposure to DON, we

hypothesized that DON modulates binding of Sp1 to

the MLL1 promoter To confirm our hypothesis, we

treated H358 cells with 3.3 lm DON and subjected

them to chromatin immunoprecipitation (ChIP) using

anti-Sp1 Ig (Fig 5C,D) In parallel, we also performed

ChIP with an unrelated antibody (actin antiserum)

The immunoprecipitated DNA fragments were PCR

amplified using primers specific for MLL1 promoter

regions R1 ()497 to )593), R2 ()5 to )105),

MLL1-ORF (as control) and b-actin-MLL1-ORF (a second

unre-lated control) Our results demonstrated that no Sp1

was bound to the ORF region of actin in either the

absence or presence of DON (Fig 5C, upper, lanes

5 and 6) Similarly, Sp1 binding was not enriched in

the MLL1-ORF region in the presence of DON

(MLL1-ORF; Fig 5C, lanes 5 and 6) Interestingly,

however, the binding of Sp1 was significantly enriched

in the Sp1-binding sites of the MLL1 promoter regions

R1 and R2 in the presence of DON, although more

enrichment was observed in the R2 region (closer to

the transcription start site) (Fig 5C,D, lanes 5 and 6)

ChIP analysis showed no binding of b-actin to the

MLL1 promoters and ORF region, irrespective of the presence or absence of DON (Fig 5C, lanes 3 and 4) These results demonstrated that binding and enrich-ment of Sp1 to the MLL1 promoter regions (R1 and R2) in the presence of DON is specific and this dem-onstrates that Sp1 is crucial for transcriptional activa-tion of MLL1 under DON treatment

Furthermore, because phosphorylation of Sp1 is well known to be associated with toxic stress, we analyzed the state of Sp1 phosphorylation upon DON exposure [33,37] We performed immunoprecipitation of Sp1 using anti-Sp1 Ig (nonphosphorylated) from DON-treated and unDON-treated cells We analyzed the immuno-precipitates by western blot using both anti-Sp1 Ig (nonphosphorylated) and anti-phosphotyrosine Ig that recognize tyrosine-phosphorylated proteins Interest-ingly, upon DON treatment, the protein level of Sp1 was not significantly affected, although, the level of tyrosine-phosphorylated Sp1 was increased (Fig 5E) These results indicated that DON induces phosphory-lation of Sp1 and this might be linked with MLL1 upregulation

Discussion Because MLLs are proto-oncogenes and are known to

be rearranged or misregulated under chemotherapeutic stress, leading to secondary leukemias [23,24], elucidat-ing the stress responsive regulatory mechanism of MLL is important Herein, our studies showed that exposure to mycotoxin DON-induced expression of MLL1, several MLL interacting proteins and MLL target Hox genes Notably, MLL1 exists as a multipro-tein complex inside the cell with subunits like Ash2, Wdr5 and Rbbp5, and MLL1 executes its histone methyl-transferase activity and regulates target Hox genes in the context of the multiprotein complex [1,9,10] Therefore, because MLL1 and several Hox genes (HoxA7, HoxA2, etc.) were overexpressed upon exposure to DON, we anticipated that MLL-interact-ing proteins might be upregulated in a similar fashion However, our results demonstrated that although several MLL1-interacting proteins such as Wdr5 and Rbb5 were upregulated upon exposure to DON, Ash2 expression was not significantly affected These observations suggest that Ash2 is a unique component

of MLLs and may have other distinct functions that are yet to be revealed It is also possible that Ash2 is normally distributed in different protein complexes which may be redistributed (without being induced) under stress to compensate for the higher expression of MLL1 This aspect needs further investigation for complete understanding Similarly, although the MLL1

Fig 4 Sp 1- binding sites in the MLL 1 promoter MLL 1 gene

pro-moter (from )3000 to +500 bp) sequence was analyzed for

pres-ence of Sp 1 -binding sites (GGGCGG, GGCGGG, CCCGCC and

CCGCCC) using http://www.ifti.org/ promoter screening tool

Puta-tive Sp 1 Binding sites are underlined Transcription start site (ATG)

is shown as +1.

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target genes HoxA7, HoxA2 and HoxB1, along with

MLL1, were upregulated upon exposure to DON, we

observed that HoxB7expression decreased These

results suggested that the mechanism of regulation,

especially in presence of DON, is different for HoxB7

(as well as HoxA2 and HoxB1) and HoxA7, although

they are all targets of MLL1 in normal circumstances

(without DON) Nevertheless, our results showing the

DON-induced upregulation of MLL1 and related

pro-teins indicated that MLL1 and its associated genes are

sensitive to toxic stress

The effect of DON is very well studied in plants

[38,39] In mammalian cells, DON induces oxidative

stress, activates MAP⁄ Src kinases and induces

inflam-mation and oxidative stress-responsive genes such as

interleukins and cyclooxygenase [32,36,40–42] Using

RT-PCR analysis, we also observed that

interleukin-8 and cyclooxygenase are overexpressed in H35interleukin-8 cells upon exposure to DON, indicating the induction of oxidative stress in human cells, as reported earlier (data not shown) [36,41] Furthermore, using Src kinase inhibitor (PP2), we demonstrated that DON-induced MLL1 and HoxA7 gene upregulation were alleviated in the presence of PP2 These observations demonstrated that Src kinases are involved in upstream events in DON-mediated upregulation of MLL1 and HoxA7 Notably, our results demonstrated that application of PP2 has no significant effect on the DON-induced upregulation of other proteins such as Set1, Wdr5 and Rbbp5 (data not shown), suggesting the involvement of alternate pathways in the regulation

of these genes

Our sequence analysis demonstrated that the MLL1 promoter contains multiple binding sites for Sp1, a

Water DON Water DON Water DON Input Actin Sp1

Anti-serum

MLL1 ( ORF ) MLL1 ( R1 ) (R2)

β -actin

1 2 3 4 Water DON Water DON

Scramble antisense

28S rRNA Sp1 MLL1

Sp1 antisense

1 2 3 4 Water DON Water DON

Scramble antisense

β -actin Sp1 MLL1

Sp1 antisense

Sp1

Sp1-p

0 0.33 3.3 33 DON

(µ M )

0.0 0.2 0.4 0.6 0.8 1.0

Actin Sp1 Actin Sp1 Actin Sp1 Actin Sp1 Actin (ORF) MLL (ORF) MLL1 (R1) MLL1 (R2)

Water DON

ChIP anti-sera Target DNA region

A B

C E

D

Fig 5 Effect of knockdown of Sp 1 on

DON-induced upregulation of MLL1.

H358 cells were treated with Sp 1- specific

phosphorothioate antisense for 48 h

fol-lowed by treatment with 3.3 l M DON for

7.5 h (A) RT-PCR analysis of Sp 1 and MLL 1

using specific primers 28S rRNA was used

a quantitative control (B) Total protein was

analyzed by western blot using anti-actin

(control), anti-Sp 1 and anti-MLL 1 Ig (C)

DON-induced recruitment of Sp 1 in the

MLL 1 promoter H358 cells treated with

3.3 l M DON for 7.5 h were subjected to

ChIP assay using Sp 1 and actin antibodies.

Actin ChIP was used as a nonspecific

anti-body control ChIP DNA fragments were

PCR amplified using primer specific to

dif-ferent Sp 1- binding sites in the MLL 1

promot-ers b-actin (ORF): PCR-amplified ‘+712 to

+1011’ of b-actin (unrelated control); MLL 1

(ORF): PCR-amplified ‘+3190 to +3380’ of

MLL 1 gene (control); MLL 1 (R1 and R2)

PCR-amplified ‘ )497 to )593’ and ‘)5 to

)105’ of the MLL 1 promoter (D)

Quantifica-tion of Sp 1 recruitment as seen in (C) (E)

Western blot analysis of phosphorylated Sp 1

upon DON treatment H358 cells were

trea-ted 0–33 l M DON for 7.5 h The whole-cell

extracts were immunoprecipitated with

anti-Sp 1 Ig The Sp1 immunoprecipitate was

ana-lyzed by western blot using both anti-Sp 1

and anti-phosphotyrosine Ig.

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transcription factor that is well known to be activated

and phosphorylated under stress [29,33,34,36,43] The

literature relating to mycotoxin-mediated activation of

Sp1 and our results showing the presence of multiple

Sp1-binding sites in the MLL1 promoter, prompted us

to hypothesize that Sp1 plays a critical role in the

reg-ulation of MLL1, especially under mycotoxic stress

[33,37,43] Our studies demonstrated that

antisense-mediated knockdown of Sp1 suppressed the effects of

DON on upregulation of MLL1 In addition, the level

of Sp1 is enriched in the Sp1-binding regions of the

MLL1 promoter upon exposure to DON These results

demonstrated that Sp1 acts a mediator in translating

the effects of DON on MLL1 gene upregulation

Notably, cells respond to stress by activating signaling

pathways that regulate defense responsive genes

[36,38,39] An early step in the stress response includes

phosphorylation of the MAP⁄ Src kinases leading to

their activation [36] Sp1 and other Sp1 family

mem-bers are differentially acetylated, phosphorylated

and⁄ or glycosylated, and bind variants of a GC-rich

box in promoter of target genes Because the MLL1

promoter contains multiple Sp1-binding sites and is

regulated by Sp1, as well as the Src family of kinases

on DON treatment, we hypothesized that Sp1 is likely

phosphorylated and recruited to the MLL1 promoter,

resulting in its upregulation Our studies demonstrated

that Sp1 is phosphorylated upon exposure to DON

Although, at this point we could not directly analyze

recruitment of the phosphorylated Sp1 into the MLL1

promoter because of the unavailability of the

phospho-Sp1-specific antibody, the increased recruitment of the

Sp1 in the MLL1 promoter may be linked with

phos-phorylation of Sp1

In conclusion, we demonstrated that MLL1, several

MLL-associated proteins and Hox genes are

upregulat-ed upon exposure to mycotoxin DON via involvement

of Src kinase activation The transcription factor Sp1

plays critical role in upregulating MLL1 gene

expres-sion under mycotoxic stress Although further analysis

is needed to understand the detailed mechanism of

MLL gene (and other DON-responsive genes)

regula-tion in normal cell or under stress, our studies

estab-lished a novel link between MLL gene regulation, the

stress response and DON, and revealed critical

stress-responsive MLL1 gene regulatory pathways Although,

the mechanism is not clear, MLL is well known to be

rearranged and misregulated in various cancers and it

is likely that different types of stresses cause MLL

mis-regulation and rearrangement As exposure to DON

induces upregulation of MLL1, we hypothesize that

this may be one of the possible mechanism by which

DON exerts is carcinogenic action in human cells

Experimental procedures

Cell culture and treatments with DON Human cells (H358, a lung cancer, ATCC) were grown on RPMI media supplemented with 10% fetal bovine serum,

l-glutamine (1%) and penicillin⁄ streptomycin (0.1%) (Sigma, St Louis, MO, USA) For the toxin treatment, cells were grown to 80% confluence and treated with varying concentrations of DON (Sigma) for different times, as needed Total RNA and proteins were isolated from the treated and untreated cells and subjected to RT-PCR and western blot analysis For the RT-PCR analysis, each experiment was performed in two to four replicates in par-allel For the western blot analysis, proteins from replicate experiments were pulled together prior to SDS⁄ PAGE

Preparation of RNA, nuclear proteins and whole-cell extract

DON-treated and untreated cells were harvested by centrifu-gation at 500 g, resuspended in diethyl pyrocarbonate-treated buffer A (20 mm Tris⁄ HCl, pH 7.9, 1.5 mm MgCl2,

10 mm KCl, 0.5 mm dithiothreitol and 0.2 mm phenyl-methanesulfonyl fluoride), incubated on ice for 10 min and then centrifuged at 3500 g for 5 min The supernatant containing the cytoplasmic extracts was subjected to phenol– chloroform extraction followed by LiCl precipitation of cytoplasmic mRNA by incubating overnight at)80 C The mRNA was washed with diethyl pyrocarbonate treated 70% EtOH, air dried and resuspended in diethyl pyrocarbonate-treated water Nuclear proteins extracts were prepared from the nuclear pellets, as descried previously [21,22] For prepa-ration of whole-cell protein extracts cells were incubated in whole cells extract buffer (50 mm Tris⁄ HCl pH 8.0, 150 mm NaCl, 5 mm EDTA, NP-40, 0.2 mm phenylmethanesulfonyl fluoride, 1· protease inhibitors) for 20 min on ice The whole cell extract was separated from histone protein by centrifugation at 12 000 g for 10 min

RT-PCR and western blots Reverse transcription reactions were performed in a total volume of 25 lL containing 1 lg of total RNA, 2.4 lm of oligo-dT, 100 U of MMLV reverse transcriptase (Promega, Madison, WI, USA), 1· first strand buffer (Promega),

100 lm dNTPs, 1 mm dithiothreitol and 20 U of RNaseOut (Invitrogen, Carlsbad, CA, USA) This cDNA (1 lL) was used for PCR with primer pairs listed inTable 1 Each of the experiments was performed in two replicates for three times The normality of the data was analyzed by using t-test and analyses of the variants (ANOVA) were performed at 5% level of significance

Equivalent amount of proteins were analyzed in SDS⁄ PAGE and subjected to western blot analysis with

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specific antibodies MLL1, MLL2, Set1, Ash2 and Rbbp5,

antibodies were purchased from Bethyl laboratory

(Mont-gomery, TX, USA)

Immunoprecipitation and western blotting of Sp1

and phosphorylated Sp-1

For western blot analysis of the Sp1 expression, equivalent

amounts of whole-cell extract (DON-treated and untreated)

were separated in 8% SDS⁄ PAGE and subjected to western

blot analysis using anti-Sp1 Ig (Upstate, Waltham, MA,

USA) For the analysis of DON-induced phosphorylation of

Sp1, we performed immunoprecipitation of Sp1 from the

whole-cell protein extract using anti-Sp1 Ig, as described

ear-lier [21] The Sp1 immunoprecipitates were electrophoresed

in 8% SDS⁄ PAGE and subjected to western blot using both

anti-Sp1 (nonphosphorylated) and anti-phosphotyrosine Ig

(Upstate) that recognize tyrosine phosphorylated proteins

Antisense-mediated knockdown of Sp1

The Sp1 antisense (5¢-CTGAATATTAGGCATCACTCC

AGG-3¢) was transfected into H358 cells using Maxfect

transfection reagent (MoleculA) In brief, H358 cells were

grown to 60% confluence, washed twice with fetal bovine

serum-free RPMI media and then incubated with

transfec-tion reagent–antisense complex for 5 h in serum-free RPMI

prior to the addition of complete growth medium (with 10%

serum) Cells were then incubated for 48 h followed by

treat-ment with 3.3 lm DON for 7.5 h Cells were then harvested

for RNA, nuclear protein extraction or ChIP analysis A

scramble antisense without any sequence homology with Sp1

(5¢-CGTTTGTCCCTCCAGCATCT-3¢) was used as control

ChIP experiment

The ChIP assay was performed using H358 cells and

anti-Sp1 mAb (Bethyl lab) using EZ Chip chromatin

immuno-precipitation kit (Upstate) as described previously [21,22]

Immunoprecipitated DNA obtained from the ChIP was PCR amplified with different primers (specific to Sp1 rich sites in MLL1 promoter, Table 1)

Acknowledgements This work was supported by grants from Texas Advanced Research Program (00365-0009-2006) and American Heart Association (SM 0765160Y) We also thank Saoni Mandal and other Mandal lab members for critical discussions

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