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Resveratrol Inhibits Drug-Induced Apoptosis in Human Leukemia Cells byCreating an Intracellular Milieu Nonpermissive for Death Execution Kashif Adil Ahmad,1Marie-Veronique Clement,2Ismai

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Resveratrol Inhibits Drug-Induced Apoptosis in Human Leukemia Cells by

Creating an Intracellular Milieu Nonpermissive for Death Execution

Kashif Adil Ahmad,1Marie-Veronique Clement,2Ismail Muhamad Hanif,1and Shazib Pervaiz1

Departments of 1 Physiology and 2 Biochemistry, Faculty of Medicine, National University of Singapore, Singapore

ABSTRACT

Efficient apoptotic signaling is a function of a permissive intracellular

milieu created by a decrease in the ratio of superoxide to hydrogen

peroxide and cytosolic acidification Resveratrol (RSV) triggers apoptosis

in some systems and inhibits the death signal in others In this regard, the

inhibitory effect on hydrogen peroxide-induced apoptosis is attributed to

its antioxidant property We provide evidence that exposure of human

leukemia cells to low concentrations of RSV (4 – 8M ) inhibits caspase

activation, DNA fragmentation, and translocation of cytochrome c

in-duced by hydrogen peroxide or anticancer drugs C2, vincristine, and

daunorubicin Interestingly, at these concentrations, RSV induces an

in-crease in intracellular superoxide and inhibits drug-induced acidification.

Blocking the activation of NADPH oxidase complex neutralized

RSV-induced inhibition of apoptosis Furthermore, our results implicate

intra-cellular hydrogen peroxide as a common effector mechanism in

drug-induced apoptosis that is inhibited by preincubation with RSV.

Interestingly, decreasing intracellular superoxide with the NADPH

oxi-dase inhibitor diphenyliodonium reversed the inhibitory effect of RSV on

drug-induced hydrogen peroxide production These data show that low

concentrations of RSV inhibit death signaling in human leukemia cells via

NADPH oxidase-dependent elevation of intracellular superoxide that

blocks mitochondrial hydrogen peroxide production, thereby resulting in

an intracellular environment nonconducive for death execution.

INTRODUCTION

The effector components of apoptotic death signaling and their

intricate networking have been unraveled during the past couple of

decades (1–3) Consequently, it is now well established that

depend-ing on the level of activation of the initiator caspase, such as

caspase-8, the death signal can recruit directly downstream effector

caspases or engage the mitochondria with the resultant release of

death amplification factors, such as cytochrome c, apoptosis inducing

factor, and Smac/DIABLO (2, 4, 5) Death signaling by anticancer

drugs generally relies on positive input from the mitochondria, as is

evidenced by the resistance of tumor cells overexpressing the

death-inhibitory protein Bcl-2 that is localized to the membranes of

mito-chondria, endoplasmic reticulum, and nucleus (6 – 8) Therefore, by

implication, an intracellular milieu permissive for caspase activation/

activity and recruitment of mitochondria-derived amplification factors

is critical for efficient apoptotic execution To that end, we have

demonstrated the critical role of cellular redox status in the regulation

of death signaling (9 –12) Whereas an overwhelming accumulation of

intracellular reactive oxygen species could create an oxidatively

stressed environment leading to necrosis, a slight increase is a

stim-ulus for cellular proliferation (13, 14) Pro-oxidant intracellular milieu

is a hallmark of many tumor cells and is believed to endow tumor cells

with a survival advantage over their normal counterparts (15, 16)

Furthermore, we have demonstrated that a slightly elevated intracel-lular concentration of superoxide (O2⫺) inhibited apoptotic signaling, irrespective of the trigger (17, 18) Contrarily, our data and that of others have highlighted the critical role of intracellular H2O2 in rendering the cytosolic milieu permissive for efficient apoptotic exe-cution (19 –21) Thenceforth, we hypothesize that a critical balance between intracellular H2O2 and O2⫺dictates the response of tumor cells to apoptotic stimuli (9, 10, 12), and any stimulus/signal that inhibits the ability of intracellular H2O2, triggered on drug exposure,

to reduce the intracellular environment could potentially favor the acquisition of the resistant phenotype

One area of recent interest in cancer biology is the chemopreventive potential of natural products Among the compounds being evaluated for their cancer inhibiting activity is a phytoalexin, resveratrol (RSV), found in grapes and wines and known for its diverse biological activities, including antioxidant property (22–24) We reported previ-ously that the chemopreventive activity of RSV could be the result of its ability to induce apoptotic death in human leukemia and breast carcinoma cells (25) However, depending on the cell type and the concentration used, RSV has been shown to induce or inhibit cellular proliferation and death signaling (25–29) Our present study was stimulated by a recent report that H2O2-induced apoptosis was inhib-ited in the presence of RSV and the implication that this could be a function of its antioxidant activity (30) Given our recent findings that drug exposure of human leukemia cells resulted in H2O2-dependent apoptosis, we set out to investigate the mechanism by which RSV inhibited apoptotic signaling triggered by exogenous H2O2 or by exposure to three anticancer agents, namely, C2, vincristine, or dauno-rubicin, that induce apoptotic death in cancer cells (21)

MATERIALS AND METHODS

Determination of Cell Viability and DNA Fragmentation Human

pro-myelocytic leukemia (HL60) cell line was purchased from American Type Culture Collection (Manassas, VA) and maintained in RPMI 1640 supple-mented with 10% fetal bovine serum, 1%L-glutamine, and 1% S-penicillin In

a typical survival assay, HL60 cells (1⫻ 105cells/well) plated in 96-well plates were preincubated with RSV (4 – 8␮M) for 2 h and then treated with 100

␮M of H2O2, 50 ␮g/ml of C2, 1.25 ␮g/ml of vincristine, or 0.2 ␮g/ml of

daunorubicin for 18 h Cell survival was determined by 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT) assay as described previously or

by the␤-galactosidase (␤-gal) survival assay described below (31)

Propidium iodide staining was performed for analyzing DNA fragmentation

as described previously (25) Stained cells were analyzed by flow cytometry (Coulter EPICS Elite ESP; Beckman Coulter, Fullerton, CA) with the excita-tion and emission wavelengths at 488 nm and 610 nm, respectively At least 10,000 events were analyzed by WinMDI software

Determination of Caspase-3 and -9 Activity Caspase-3 and -9 activity

was determined using the Bio-Rad fluorescent assay kit (Hercules, CA) for the two caspases Cells (1⫻ 106) were preincubated for 2 h with RSV (4 – 8␮M) and then incubated for 12 h with 100␮MH2O2, 50␮g/ml of C2, 1.25 ␮g/ml

of vincristine, or 0.2␮g/ml of daunorubicin Fifty ␮l of 2⫻ reaction buffer

with 10 mM DTT and 5 ␮l of the conjugate substrate (DEVD-AFC for

caspase-3 and LEHD-AFC for caspase-9) were added to cell lysates Caspase activity was determined by the relative fluorescence intensity at 505 nm

Received 8/5/03; revised 12/9/03; accepted 12/10/03.

Grant support: Research grants from the NMRC, Singapore (R-185-000-032-213) to

S Pervaiz and from the BMRC, Singapore (R-185-000-048-305) to S Pervaiz and

M-V Clement.

The costs of publication of this article were defrayed in part by the payment of page

charges This article must therefore be hereby marked advertisement in accordance with

18 U.S.C Section 1734 solely to indicate this fact.

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activity relative to untreated cells (1⫻) In addition, cleavage of the caspase-3

substrate, poly(ADP ribose) polymerase (PARP), was assessed by Western

blot analysis using anti-PARP (clone C-2–10; PharMingen, San Diego, CA) as

described previously (9)

Measurements of Intracellular O 2and pH Intracellular O2⫺was

as-sayed by a lucigenin-based chemiluminescence assay as described previously

(11) Data are shown as percentage change (% change) in the intracellular O2⫺

concentration compared with untreated cells and are the mean⫾ SD of three

independent measurements

For measurement of cytosolic pH, cells were loaded with 10␮M2

⬘,7⬘-bis(2-carboxyethyl)-5,6-carboxyfluorescein (BCECF-AM; Sigma, St Louis, MO),

and the fluorescence ratio of 525:610 nm was used to derive cytosolic pH using

a standard pH calibration curve as described previously (11)

Flow Cytometric Analysis of Intracellular H 2 O 2 Cells were exposed to

the apoptotic triggers for 4 –12 h, loaded with 5-(and-6)-chloromethyl-2

⬘,7⬘-dichlorofluorescin diacetate (CM-H2DCFDA; Molecular Probes, Eugene, OR;

5␮M) (32) at 37°C for 15 min, and analyzed by flow cytometry (Coulter

EPICS Elite ESP) using an excitation wavelength of 488 nm as described

previously (21) At least 10,000 events were analyzed

Determination of Mitochondrial ⌬⌿m and Cytosolic Cytochrome c.

Potential-sensitive probe 3,3⬘dihexyloxacarbocyanine iodide was used to

measure mitochondrial⌬␺mas described previously (31) Briefly, 1⫻ 106

cells were incubated with 3,3⬘dihexyloxacarbocyanine iodide (40 nM) for 15

min at 37°C As a positive control, cells were incubated separately with an

uncoupling agent, carbonyl cyanide m-chlorophenylhydrazone (CCCP) (100

␮M) At least 10,000 events were analyzed by flow cytometry with excitation

set at 488 nm

Cytochrome c was detected in cytosolic extracts from 30⫻ 106cells by

Western blot analysis using anti-cytochrome c (7H8.2C12; PharMingen) as

described previously (33)

Transient Transfection with pIRESRacN17 and ␤-Gal Survival Assay.

Transient transfections of CEM cells were performed using the SuperFect

transfection reagents from Qiagen (Hilden, Germany), and survival of

trans-fected cells was assessed by the␤-gal survival assay as described recently (34)

Cell survival was calculated as [(␤-gal activity ␮g⫺1protein of transfected

cells incubated with the apoptotic trigger)/(␤-gal activity ␮g⫺1 protein of

transfected cells incubated without the trigger)].␤-Gal activity was measured

using the Galacto-Star mammalian reporter kit (Applied Biosystems, Foster

City, CA) Protein concentration was determined using the Coomasie Plus

protein assay reagent from Pierce (Rockford, IL)

Data Analysis Data presented are mean⫾ SD of at least three independent

experiments performed in triplicate, unless otherwise indicated Statistical

significance was determined by the Student’s t test.

RESULTS Low Doses of RSV Inhibit H 2 O 2 -Induced Apoptosis Upstream

of the Mitochondria Corroborating earlier findings on the

death-inducing activity of H2O2in cancer cells, exposure of HL60 cells to

H2O2(100␮M) resulted in a significant decrease in cell survival (Fig

1A) The cytotoxic activity of H2O2was a function of activation of the apoptotic death pathway as evidenced by the significant increase in caspase activity, cleavage of the caspase-3 substrate PARP, and appearance of the sub-G1fraction (Fig 1, B–D) Interestingly,

prein-cubation of cells with 4 – 8 ␮MRSV for 2 h before the addition of

H2O2 for 18 h resulted in an increase in cell survival (Fig 1A),

significant inhibition of caspase-3 activity and PARP cleavage (Fig 1,

B and C), and inhibition of DNA fragmentation (Fig 1D) Moreover,

preincubation with RSV prevented H2O2-induced decrease in mito-chondrial ⌬␺m (Fig 2A) and significantly blocked H2O2-induced

cytosolic translocation of cytochrome c from the mitochondria (Fig 2B) One possible explanation for the observed inhibitory effect of

RSV could be that RSV functioned as an efficient scavenger of H2O2 However, addition of RSV and H2O2simultaneously to the culture medium (RSV/H2O2) had no effect on H2O2-induced cell death (Fig

2C), whereas previous incubation with RSV for 2 h (RSV⫹ H2O2)

significantly (P ⬍ 0.05) inhibited apoptotic signaling (Fig 2C) These

data indicate that the death-inhibitory effect of RSV is not simply a function of its ability to scavenge H2O2but involves mechanism(s) upstream of the mitochondria or signals that engage the mitochondrial death machinery

RSV Inhibits H 2 O 2 -Induced Decreases in Intracellular O 2and Cytosolic pH We have shown that H2O2induces a decrease in O2⫺ and cytosolic acidification, thereby creating an intracellular milieu permissive for apoptotic execution (18, 34, 35) Therefore, we ques-tioned if the inhibitory effect on H2O2-induced apoptosis was caused

by the ability of RSV to create an intracellular environment

noncon-Fig 1 Preincubation with resveratrol (RSV)

in-hibits H2O2-induced caspase activation and DNA

fragmentation in HL60 cells A, HL60 cells

(1 ⫻ 10 6 cell/ml) were incubated with 100 ␮ M

H2O2for 18 h with or without preincubation for 2 h

with RSV (4 and 8 ␮ M ) Cell viability was

deter-mined by the MTT assay B, caspase-9 and -3

activity was determined by fluorimetric assays, and

(C) poly(ADP ribose) polymerase cleavage was

assessed by Western blot analysis D, DNA

frag-mentation was determined by propidium iodide

staining and the appearance of sub-G1fraction.

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ducive for death execution Preincubation with RSV not only induced

a slight increase in intracellular O2⫺but also blocked the inhibitory

effect of H2O2 on intracellular O2⫺levels (Fig 3A) Interestingly,

preincubation with RSV before the addition of H2O2 consistently

resulted in higher intracellular O2⫺than RSV alone In addition, the

significant decrease in cytosolic pH (P⬍ 0.01) triggered by H2O2was

inhibited by previous incubation with RSV (Fig 3B).

RSV-Induced Inhibition of Apoptosis Can Be Reverted by

Blocking NADPH Oxidase Activation Considering the reports on

the antioxidant potential of polyphenolic compounds, such as RSV,

we were intrigued by our observation that low concentrations of RSV

induced an increase, rather than a decrease, in intracellular O2⫺

concentration (30, 36 –38) Therefore, we investigated the effect of

blocking NADPH oxidase complex, one of the major sources of

intracellular O2⫺, on RSV-induced increase in O2⫺ Pharmacologic

inhibition of NADPH oxidase with diphenyleneiodonium chloride

(DPI) completely blocked RSV-induced increase in intracellular O2⫺

in HL60 cells (Fig 3C) Furthermore, incubation of cells for 1 h with

DPI before the addition of RSV significantly (P⬍ 0.004) restored the

sensitivity of HL60 and CEM leukemia cells to H2O2(Fig 3D; data

not shown) To provide additional evidence that this was a function of

NADPH oxidase activation, CEM cells were transfected transiently

with a dominant negative mutant of Rac (RacN17), which inhibits

NADPH oxidase-dependent increase in intracellular O2⫺(34) Similar

to DPI, transient transfection with RacN17 completely neutralized the

death-inhibitory activity of RSV and restored the sensitivity of

leu-kemia cells to H2O2(Fig 3E).

RSV Inhibits Apoptosis Triggered by Anticancer Drugs C2,

Vincristine, and Daunorubicin In our earlier reports, we

demon-strated that exposure of human leukemia and melanoma cells to C2, a

purified photoproduct of MC540, triggered mitochondrial generation

of H2O2 that was responsible for the release of cytochrome c and

downstream activation of the caspase cascade (21) Similar to the data

obtained with H2O2, preincubation of cells with RSV before the

addition of C2 resulted in an increase in cell survival compared with

the cells treated with C2 alone (Fig 4A) Whereas exposure of

leukemia cells to C2 resulted in robust increases in caspase-3 and -9

activity, preincubation with RSV significantly inhibited both caspases

and the cleavage of the caspase-3 substrate PARP (Fig 4B) That this

translocation of cytochrome c in cells preincubated with RSV before the addition of C2 (Fig 4C) In addition, similar to the results obtained

with H2O2, previous incubation with RSV (RSV⫹ C2) was required

for the inhibitory effect of RSV on C2-induced death signaling, whereas simultaneous exposure to RSV and C2 (RSV/C2) had no effect on C2 signaling (data not shown)

We next questioned whether the inhibitory effect of RSV on

C2-induced apoptosis also was mediated by its ability to (a) create a pro-oxidant intracellular milieu; and (b) inhibit cytosolic acidification.

Results indicate that preincubation of HL60 cells with RSV inhibited

H2O2production triggered by exposure to C2 (Fig 5A) Similar to the

results obtained with H2O2, preincubation of HL60 cells with RSV for

2 h resulted in an increase in intracellular O2⫺concentration, which

was even more pronounced on subsequent addition of C2 (Fig 5B) It

should be noted that a slight increase in intracellular O2⫺also was observed on exposure of cells to C2 alone; however, unlike RSV, this was accompanied by a surge in intracellular H2O2 production In addition, cytosolic acidification triggered on exposure to C2 was

inhibited completely on previous exposure to RSV (Fig 5C)

Further-more, incubation of cells with DPI before the addition of RSV and C2 resulted in a decrease of intracellular O2⫺ (data not shown) and

restored death signaling in response to C2 (Fig 5D).

To gain additional insight into the death-inhibitory effect of RSV and its potential clinical implications, we next investigated the effect

of RSV on apoptosis induced by two chemotherapeutic agents, vin-cristine and daunorubicin (39) Corroborating the results obtained with H2O2 and C2, results indicate a dose-dependent (up to 8␮M)

inhibitory effect of RSV on vincristine-induced cell death (Fig 6A)

together with significant inhibition of caspase-9 and -3 activity (Fig

6B) That the apoptosis inhibitory effect of RSV was linked to its

ability to create a pro-oxidant intracellular milieu was supported additionally by the ability of DPI or transient transfection with RacN17 to revert the sensitivity of leukemia cells in the presence of

RSV to vincristine-induced apoptosis (Fig 6, C and D).

The inhibitory effect of low concentrations of RSV on drug-induced apoptosis was not exclusive to C2 or vincristine Preincuba-tion of leukemia cells to RSV for 2 h resulted in a significant increase

in cell survival (Fig 7A), inhibition of caspase activity (Fig 7B), and

Fig 2 Inhibitory effect of resveratrol (RSV) on

H2O2-induced death signaling is upstream of the

mitochondria A, HL60 (1⫻ 10 6 ) cells were

ex-posed to 100 ␮ M H2O2for 4 h with or without

previous incubation for 2 h with RSV (8 ␮ M ), and

⌬␺ m was determined as described in “Materials

and Methods.” B, cytosolic cytochrome c was

as-sessed by Western blot analysis

Staurosporin-treated HL60 cytosolic extract was used as positive

control C, HL60 cells (1⫻ 10 6 /ml) were incubated

simultaneously with RSV (8 ␮ M ) and H2O2(100

␮ M) for 18 h (RSV/H 2 O 2) or preincubated for 2 h

with RSV (8 ␮ M ) before the addition of 100 ␮ M

H2O2(RSV ⫹ H 2 O2) Cell viability was

deter-mined by MTT assay.

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Fig 3 Inhibition of NADPH oxidase activation prevents resveratrol (RSV)-induced increase in intracellular O2⫺and overcomes its death-inhibitory effect A, cytosolic pH was

determined with the pH-sensitive probe 2⬘,7⬘-bis(2-carboxyethyl)-5,6-carboxyfluorescein B, 2 ⫻ 106 cells were treated with RSV (8 ␮ M ) for 2 h or H2O2(100 ␮ M ) for 4 h with or without 2 h of previous incubation with RSV (8 ␮ M ) Intracellular O2⫺was measured by a lucigenin-based chemiluminescence assay C, HL60 (2⫻ 10 6 ) cells were incubated with

8 ␮ M RSV for 4 h in the presence or absence of DPI (1.25 ␮ M ), and intracellular O2⫺was measured as described previously D, HL60 cells (1⫻ 10 6 /ml) were preincubated with DPI (1.25 ␮ M ) or with DPI (1.25 ␮ M ) ⫹ RSV (8 ␮ M ) for 4 h before the addition of 100 ␮ M H2O2for 18 h Cell survival was assessed by the MTT assay E, CEM cells (1⫻ 10 6 /ml) cotransfected with pCMV-␤-galactosidase (␤-gal) and pIRES-RacN17 were exposed to 100 ␮M H2O2for 18 h with or without previous incubation for 2 h with 8 ␮ M RSV Cell survival was assessed by the ␤-gal survival assay Mean of two independent transfections done in duplicate is shown.

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Decrease in Intracellular O 2Overrides the Inhibitory Effect

of RSV on Drug-Induced H 2 O 2 Production Thus far, we have

shown that the inhibitory activity of RSV on drug-induced apoptosis

was linked to its ability to increase NADPH oxidase-dependent

intra-cellular O2⫺production Interestingly, all of the drugs used in this

study resulted in an intracellular increase in H2O2 production (Fig

NADPH oxidase complex had no effect on intracellular H2O2increase (21) Similar to the results reported with C2, preincubation of HL60 cells with DPI did not affect intracellular H2O2production on expo-sure to vincristine and daunorubicin, thus strongly suggesting mito-chondria as the cellular source on drug exposure (data not shown) More importantly, decreasing intracellular O2⫺with DPI restored the ability of C2, vincristine, and daunorubicin to trigger intracellular

H2O2production even in the presence of RSV (Fig 7C).

DISCUSSION RSV Inhibits Apoptosis by Altering Cellular Redox Status.

Taken together, our data provide strong evidence that contrary to its proapoptotic activity atⱖ25␮M, low micromolar concentrations (4 – 8

␮M) inhibit apoptotic signaling (25, 40, 41) This divergent signaling

by RSV is intriguing and could be explained by our earlier observa-tions that at concentraobserva-tions of ⱖ32␮M, apoptosis induced in HL60 cells is mediated by up-regulation of CD95 (Fas/Apo1)-CD95L inter-action (25) This effect on up-regulation of the death receptor ligand

is not observed at concentrations of RSV⬍16␮M, hence the inability

to trigger apoptosis in these cells (data not shown) Contrarily, at these concentrations, RSV inhibits apoptotic signaling upstream of the mitochondria, thus blocking the recruitment of mitochondrial-derived

amplification factors, such as cytochrome c We also provide evidence

that RSV has a potent effect on the intracellular redox status, a critical determinant of the efficacy of the death signal (9, 42, 43) In that respect, it has been shown previously that maintaining a slightly elevated intracellular O2⫺promotes cellular proliferation (14, 44) and inhibits apoptotic signaling (18, 42) A pro-oxidant intracellular mi-lieu is an invariable finding in cancer cells and has been shown to endow cancer cells with a survival advantage over their normal counterparts (15) Because a decrease in intracellular O2⫺and cyto-solic pH is critical for efficient death execution, our results suggest that low concentrations of RSV could enable cancer cells to evade death signaling by creating a pro-oxidant intracellular milieu and inhibiting cytosolic acidification

RSV Induces Increase in O 2via NADPH Oxidase Activation.

Considering the earlier reported ability of RSV to inhibit mitochon-drial complex III-induced reactive oxygen species production, our paradoxical findings provide evidence for a pro-oxidant effect of RSV

at concentrations that do not trigger apoptosis (45) Such pro-oxidant activity of polyphenolics, such as RSV, has been reported recently in different systems (46, 47) In one model, reactive oxygen species generation at concentrations of RSV that triggered cell death in human cancer cells was proposed to be responsible for its cytotoxic activity (47) In addition, our results implicate the membrane NADPH oxidase complex as a potential source of O2⫺on incubation with low doses of RSV Inhibition of the NADPH oxidase complex not only restored death signaling but also resulted in reverting the negative effect of RSV on drug-induced intracellular H2O2production This fits in well with our hypothesis that a balance between intracellular O2⫺ and

H2O2could be a critical factor in the response of cells to apoptotic triggers, with a tilt toward the former favoring survival and a pre-dominance of the latter facilitating death execution (10) A careful

look at the data shown in Fig 5B reveals that, similar to RSV alone,

exposure of cells to the anticancer drug C2 also results in a slight elevation in intracellular O2⫺ However, it is important to note that C2-induced O2⫺ is accompanied by a surge in intracellular H2O2, which is not observed with low concentrations of RSV In addition, preincubation with RSV completely blocks C2-induced H2O2 produc-tion and maintains a significantly elevated intracellular O2⫺level By

Fig 4 Resveratrol (RSV) inhibits apoptosis triggered by a novel anticancer drug, C2.

A, HL60 cells (1⫻ 10 6 /ml) were incubated simultaneously with RSV (8 ␮ M ) and C2 (50

␮g/ml) for 18 h (RSV/C2) or preincubated for 2 h with RSV (8 ␮M ) before the addition

of C2 (RSV⫹ C2) Cell viability was determined by MTT assay B, activity of caspase-3

and -9 was determined by fluorimetric assays Poly(ADP ribose) polymerase (PARP)

cleavage and (C) cytosolic cytochrome c were detected by Western blot analyses.

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inhibiting the decrease in intracellular pH It is intriguing as to how an

increase in intracellular O2 ⫺blocks mitochondrial-derived H2O2 One

possibility could be inhibition of upstream caspase activation, as has

been shown previously, or other proapoptotic factors, such as

death-promoting Bcl-2 family members, required for the engagement of the

mitochondrial pathway (48) Impeding these upstream pathways could

account for the inhibition of drug-induced mitochondrial H2O2

pro-duction and downstream cytochrome c release observed in cells

preincubated with RSV This in turn fails to amplify downstream

caspase cascade (caspase-9 and -3) and leads to a substantial decrease

in the sensitivity of cells to apoptotic stimuli that require mitochon-drial amplification factors Taken together, these results indicate that the increase in intracellular O2⫺on exposure of leukemia cells to RSV was mediated through the activity of NADPH oxidase complex and linked directly or indirectly to the apoptosis-inhibitory activity of RSV In addition, data presented here not only implicate mitochon-drial H2O2production as a critical effector mechanism during drug-induced apoptosis but also demonstrate the ability of an increase in intracellular O2⫺to prevent H2O2production and thereby impede the recruitment of the mitochondrial death pathway

Fig 5 Resveratrol (RSV) creates a pro-oxidant

intracellular milieu and inhibits C2-mediated

de-crease in cytosolic pH and cell death A, HL60

(1 ⫻ 10 6 ) cells were treated with 50 ␮g/ml of C2

for 4 h with or without previous incubation with 8

␮ M RSV, and intracellular H2O2was determined.

B, 2⫻ 10 6 cells (in 2 ml) were treated with RSV (8

␮ M ) for 4 h or 50 ␮g/ml of C2 for 4 h with or

without 2 h of previous incubation with RSV (8

␮ M ), and intracellular O2⫺was determined C, cells

were treated as in (A), and cytosolic pH was

as-sessed with 2

⬘,7⬘-bis(2-carboxyethyl)-5,6-carboxy-fluorescein D, HL60 cells (1⫻ 10 6 /ml) were

pre-incubated with DPI (1.25 ␮ M ) or with DPI (1.25

␮ M ) ⫹ RSV (8 ␮ M ) for 4 h before the addition of

50 ␮g/ml C2 for 18 h Cell survival was assessed

by the MTT assay.

Fig 6 The inhibitory effect of resveratrol (RSV)

on vincristine-induced apoptosis can be neutralized

by inhibition of the NADPH oxidase complex A,

HL60 cells (1⫻ 10 6 cell/ml) were preincubated

with RSV (2, 4, or 8 ␮ M ) for 2 h before treatment

with 1.25 ␮g/ml of vincristine for 18 h Cell

viability was determined by the MTT assay B,

caspase-9 and -3 activity was determined by

fluo-rimetric assays C, HL60 cells (1⫻ 10 6 /ml) were

preincubated with DPI (1.25 ␮ M or 2.5 ␮ M ) ⫹ RSV

(8 ␮ M ) for 4 h before the addition of 1.25 ␮g/ml of

vincristine for 18 h Cell survival was assessed by the

MTT assay D, CEM leukemia cells (1⫻ 10 6 /ml)

were cotransfected with pCMV- ␤-galactosidase

(␤-gal) and pIRES-RacN17 and exposed to 1.25 ␮g/ml

of vincristine for 18 h with or without previous

incu-bation for 2 h with 8 ␮ M RSV Cell survival was

assessed by the ␤-gal assay.

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Potential Implications These findings could be potentially

im-portant in light of the recent interest in the biological activity of

flavonoids or flavonoid-like molecules, such as RSV, for their

possi-ble use in combination chemotherapy regimens Although in vitro

exposure of tumor cells to RSV at relatively high concentrations

results in apoptotic cell death, because of the low bioavailability of

RSV, plasma levels as high as 50 –100␮Mmay not be physiologically

attainable (49, 50) Our data suggest death-inhibitory and/or

prosur-vival activity of RSV in leukemia cells at doses that may be relevant

physiologically (49, 50) Thus, the use of RSV in combination with

drugs such as C2, vincristine, or daunorubicin could be a dangerous

mixture because the slight pro-oxidant effect may provide tumor cells

with not only a survival advantage but also impede death signals This

could present an ideal environment for the propagation and

prolifer-ation of tumor cells

ACKNOWLEDGMENTS

We thank Kartini Bte Iskander and M Ali Shazib for technical assistance

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Fig 7 Resveratrol (RSV) inhibits

daunorubicin-induced apoptosis, and preincubation with DPI

re-verts the effect of RSV on drug-induced H 2 O 2

production A, 1⫻ 10 6 cell/ml were incubated with

RSV (8 ␮ M ) for 2 h, followed by 18 h of exposure

to 0.2 ␮g/ml of daunorubicin Cell viability was

determined by the MTT assay B, caspase-9 and -3

activity was determined by fluorimetric assays C,

HL60 (1 ⫻ 10 6 ) cells were preincubated with 1.25

␮ MDPI before the addition of RSV (DPI/RSV),

followed by treatment with C2 (50 ␮g/ml),

dauno-rubicin (0.2 ␮g/ml), or vincristine (1.25 ␮g/ml) for

4 h Intracellular H 2 O 2 was determined by flow

cytometry.

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