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Báo cáo khoa học: Inhibitor of nuclear factor-kappaB alpha derepresses hypoxia-inducible factor-1 during moderate hypoxia by sequestering factor inhibiting hypoxia-inducible factor from hypoxia-inducible factor 1a ppt

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Nội dung

Under aerobic conditions, HIF-1a is hydroxylated by dioxygenase members [the HIF-prolyl-hydroxylases Keywords factor inhibiting hypoxia-inducible factor FIH; hypoxia-inducible factor-1 H

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hypoxia-inducible factor-1 during moderate hypoxia by

sequestering factor inhibiting hypoxia-inducible factor

from hypoxia-inducible factor 1a

Dong Hoon Shin1,*, Shan Hua Li1,*, Seung-Won Yang1, Byung Lan Lee2, Myung Kyu Lee3and Jong-Wan Park1

1 Department of Pharmacology Ischemic ⁄ Hypoxic Disease Institute, Seoul National University College of Medicine, Korea

2 Department of Anatomy, Ischemic ⁄ Hypoxic Disease Institute, Seoul National University College of Medicine, Korea

3 Omics and Integration Research Center, KRIBB, Yuseong, Daejeon, Korea

Hypoxia-inducible factor (HIF)-1 plays a crucial role

in tumor promotion by switching on many genes that

are required to overcome oxygen and nutrient

defi-ciency HIF-1 is composed of HIF-1a and HIF-1b

(HIF-1b is also called ARNT) [1] HIF-1a enables

mRNA synthesis through its own transactivation domains (TADs), whereas ARNT assists the stabiliza-tion and binding between HIF-1a and DNA [2] Under aerobic conditions, HIF-1a is hydroxylated by dioxygenase members [the HIF-prolyl-hydroxylases

Keywords

factor inhibiting hypoxia-inducible factor

(FIH); hypoxia-inducible factor-1 (HIF-1);

IjBa; nuclear factor-kappaB (NF-jB); protein

interaction

Correspondence

J.-W Park, Department of Pharmacology,

Seoul National University College of

Medicine, Seoul, Korea

Fax: +82 2 7457996

Tel: +82 2 7408289

E-mail: parkjw@snu.ac.kr

*These authors contributed equally to this

work

(Received 11 January 2009, revised 17

March 2009, accepted 21 April 2009)

doi:10.1111/j.1742-4658.2009.07069.x

Hypoxia and inflammation often develop concurrently in numerous diseases, and both hypoxia-inducible factor (HIF)-1a and nuclear factor-kappaB (NF-jB) are key transcription factors of stress response genes

An NF-jB inhibitor, inhibitor of NF-jBa (IjBa), was found to interact with factor inhibiting HIF (FIH) and to be hydroxylated by FIH How-ever, FIH did not functionally regulate IjBa, and the consequence of the FIH–IjBa interaction thus remains uncertain In the present study, we tested the possibility that IjBa regulates FIH FIH–IjBa binding was confirmed by yeast two-hybrid and coimmunoprecipitation analyses Functionally, IjBa expression further enhanced the transcriptional activity

of HIF-1a under hypoxic conditions Furthermore, IjBa knockdown repressed HIF-1a activity Mechanistically, IjBa derepressed HIF-1a activity by inhibiting the FIH-mediated Asn803 hydroxylation of HIF-1a

It was also found that IjBa activated HIF-1a by sequestering FIH from HIF-1a However, the effect of IjBa on HIF-1a activity was only observed in atmospheres containing 1% or more of oxygen After tumor necrosis factor-a treatment, IjBa downregulation, Asn803 hydroxylation and HIF-1a inactivation all occurred up to 8 h, but subsided later On the basis of these results, we propose that IjBa plays a positive regula-tory role during HIF-1-mediated gene expression Therefore, IjBa, owing

to its interactions with NF-jB and HIF-1a, may play a pivotal role in the crosstalk between the molecular events that underlie inflammatory and hypoxic responses

Abbreviations

ARD, ankyrin repeat domain; CAD, C-terminal transactivation domain; EPO, erythropoietin; FIH, factor inhibiting hypoxia-inducible factor; GFP, green fluorescent protein; HA, hemagglutinin; HIF, hypoxia-inducible factor; IjBa, inhibitor of nuclear factor-kappaB alpha; NF-jB, nuclear factor-kappaB; PHD, prolyl-hydroxylase; SD, standard deviation; sHIF-1a, stable hypoxia-inducible factor-1a; siRNA, short interfering RNA; TAD, transactivation domain; TNF-a, tumor necrosis factor-a; b-gal, b-galactosidase.

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(PHD1–3)], ubiquitinated by von Hippel–Lindau

pro-tein-containing E3-ubiquitin ligase complex, and

conse-quently degraded by 26S proteasomes [3] In addition,

the transcriptional activity of HIF-1a is

oxygen-depen-dently regulated by another dioxygenase member,

fac-tor inhibiting HIF (FIH) [4] HIF-1a harbors two

TADs, an N-terminal TAD (amino acids 531–575) and

a C-terminal TAD (CAD, amino acids 786–826) [5]

Furthermore, CAD predominantly affects gene

expres-sion in an oxygen tenexpres-sion-dependent manner

How-ever, when Asn803 of CAD is hydroxylated by FIH,

CAD cannot recruit p300⁄ CBP coactivator, and thus

loses its transcriptional activity [4] Furthermore, as

both proline and asparagine hydroxylases require

molecular oxygen to function, HIF-1a becomes

stabi-lized and activated under oxygen-deficient conditions

FIH was first shown to interact with HIF-1a by

yeast two-hybrid screening [6] However, FIH has also

been found to bind and hydroxylate asparagines in

several proteins other than HIF-1a For instance,

immunoprecipitation and MS analyses revealed that

SOCS Box protein 4 (ASB4) and Notch-1⁄ 2 were

tar-geted and hydroxylated by FIH [7,8] Ankyrin repeat

domains (ARDs) in these proteins have been found to

be FIH-binding sites Moreover, Asn246 of ASB4 and

Asn1945⁄ 2012 of Notch-1 have been identified as the

amino acids hydroxylated by FIH In terms of the

bio-logical significance of FIH interaction, the

FIH-medi-ated asparagine hydroxylation promoted vascular

differentiation under aerobic conditions by activating

ASB4 or accelerated myogenic differentiation by

inhib-iting Notch [7,8] However, the role of FIH in Notch

signaling (FIH fi Notch) is controversial, because

there was another report demonstrating that FIH had

no significant effect on Notch activity [9] Interestingly,

in both reports, it was also examined whether Notch-1

affects FIH activity (Notch fi FIH), which is the

reverse of the former mechanism It was found that

the intracellular domain of Notch-1 blocked the

FIH-mediated HIF-1 repression by sequestering FIH

through its ARD Taken together, these findings

sug-gest that FIH mediates cross-coupling between the

Notch and HIF-1 signaling pathways

The FIH interaction with inhibitor of nuclear

fac-tor-kappaB alpha (IjBa) or p105 [the precursor of p50

nuclear factor-kappaB (NF-jB)] was discovered before

its interactions with ASB4 and Notch-1 By using yeast

two-hybrid screening, Ratcliffe et al identified two

ARD-containing proteins, p105 and uveal autoantigen

with coiled-coil domains and ankyrin repeats They

also found that ARD-containing IjBa was targeted by

FIH and hydroxylated at Asn210⁄ 244 [10] However,

as FIH expression and knockdown both failed to

affect IjBa binding to NF-jB or NF-jB activity, the biological significance of the FIH–IjBa interaction was not identified In the present study, we investi-gated the consequence of the FIH–IjBa interaction in the opposite direction, namely, IjBa fi FIH As FIH controls HIF-1a CAD activity, we focused on the roles of IjBa in HIF-1 activation and hypoxic gene regulation

Results

IjBa associates with FIH

To search for FIH-interacting proteins, we screened a HeLa cDNA library by using the yeast two-hybrid method, using full-length FIH as bait Of 22 positive clones representing four different cDNAs, IjBa cDNA alone was shown to be fused to Gal4–TAD in the right frame, whereas Notch cDNAs were not fished out (Fig S1) Hemagglutinin (HA)–FIH and Flag–IjBa were immunoprecipitated from HEK293 cells coex-pressing HA–FIH and Flag–IjBa, and Flag–IjBa and HA–FIH were then copurified in the precipitates (Fig S2A) To determine whether FIH and IjBa asso-ciate endogenously, FIH or IjBa was immunoprecipi-tated in untransfected HEK293 cells It was found that endogenous FIH and IjBa were coimmunoprecipitated

by either anti-FIH or anti-IjBa serum (Fig S2B) In agreement with what has been reported previously [10], binding of FIH to IjBa was confirmed in our experi-mental setting

FIH does not affect IjBa expression or NF-jB activity

We first examined whether or not FIH regulates IjBa expression by binding IjBa However, IjBa levels were not changed by FIH overexpression or knock-down (Fig 1A) Furthermore, when IjBa was over-expressed or knocked down, FIH levels were unchanged (Fig 1B) Next, we checked the possibility that FIH regulates NF-jB activity by interacting with IjBa However, both basal and stimulated activities of NF-jB were unaffected by FIH expression or knock-down (Fig 1C) On the basis of these results, we suggest that FIH does not affect the expression or the NF-jB-inhibitory function of IjBa

IjBa positively regulates HIF-1 activity by antagonizing FIH

As the FIH–IjBa interaction did not affect NF-jB activity, we checked the possibility that this interaction

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affects HIF-1 activity, which is known to be regulated

by FIH HIF-1 activities were evaluated using a

lucif-erase reporter plasmid containing the HIF-1-targeting

erythropoietin (EPO)-enhancer segment Reporter

activity was found to increase under 5% O2 hypoxia,

and this activity was markedly enhanced by IjBa

expression (Fig 2A) Furthermore, the effect of IjBa

on HIF-1 activity was found to be attenuated by FIH

expression in a gene dose-dependent manner In

addi-tion, when endogenous IjBa was knocked down, the

hypoxic activation of HIF-1 was significantly inhibited, but this was rescued by FIH inhibition (Fig 2A) To verify the HIF-1 dependencies of the effect of IjBa or FIH on the reporter activity, we analyzed the activity

of a reporter containing EPO-enhancer segment lack-ing the HIF-1-bindlack-ing site, and confirmed that IjBa and FIH did not affect the reporter lacking the HIF-targeted segment (Fig 2B) As FIH is known to repress the activity of HIF-1a CAD by hydroxylating Asn803, we examined whether CAD activity is regu-lated by the FIH–IjBa interaction using the Gal4– CAD⁄ Gal4–Luc reporter system Figure 2C shows that IjBa noticeably increased the hypoxic activation of wild-type CAD, but that it failed to increase the activ-ity of the CAD N803A mutant IjBa is likely to acti-vate HIF-1a CAD in an Asn803-dependent manner

As Asn803 of CAD plays a critical role in the interac-tion between HIF-1a and p300⁄ CBP coactivator, we examined whether IjBa regulates HIF-1a and p300 binding As expected, p300 was found to associate with HIF-1a under hypoxic conditions, whereas this binding did not occur under normoxic conditions Moreover, HIF-1a and p300 binding was enhanced by IjBa expression and inhibited by IjBa knockdown (Fig 2D) This result indicates that IjBa positively regulates the p300 recruitment by HIF-1a

HIF-1 derepression by IjBa occurs in 1–5% O2but not under more severe hypoxia

Because molecular oxygen is an essential substrate of PHDs and FIH, the activities of PHDs and FIH should be restricted under oxygen-deficient conditions, although FIH has a much higher affinity for oxygen than PHDs, and thus can retain its activity under moderate hypoxia [11] Furthermore, although HIF-1a

is stabilized in moderately hypoxic conditions, it is not fully activated, owing to hydroxylation by FIH, which suggests that the IjBa-dependent regulation of HIF-1a activity, which depends on FIH, might occur only under moderate hypoxia, when sufficient oxygen is still available for FIH To confirm the oxygen dependency

of the activity of IjBa, we incubated HEK293 cells in 1% or 0.5% oxygen In the EPO-enhancer reporter system, HIF-1 activity was modulated by IjBa expres-sion or knockdown in 1% oxygen (Fig 3A, left panel),

as was observed in 5% oxygen However, IjBa did not regulate HIF-1 activity at an oxygen level of 0.5% (Fig 3A, right panel) To rule out the possibility that the effect of IjBa on HIF-1 activity is related to the oxygen-dependent regulation of HIF-1a, we analyzed the transcriptional activity of stable HIF-1a (sHIF-1a), which is stably expressed oxygen-independently, owing

A

C

B

Fig 1 FIH does not affect IjBa expression and NF-jB activity (A)

FIH does not affect IjBa expression HEK293 cells were

transfect-ed with the HA–FIH plasmid (0.2 or 0.4 lg) or FIH siRNA (40 or

80 n M ) The empty vector (Mock) and green fluorescent protein

(GFP) siRNA (80 n M ) were transfected as transfection and siRNA

controls, respectively After being stabilized for 48 h, the cells were

prepared for the analysis of cellular levels of IjBa and FIH by

immunoblotting b-Tubulin levels were analyzed as loading controls.

(B) IjBa does not affect FIH expression HEK293 cells were

trans-fected with the Flag–IjBa plasmid (0.2 or 0.4 lg) or IjBa siRNA

(40 or 80 n M ) After being stabilized for 48 h, the cells were

pre-pared for the analysis of cellular levels of FIH and IjBa by

immuno-blotting (C) NF-jB activity was not regulated by FIH NF-jB

reporter plasmid (0.02 lg) and b-gal plasmid (0.1 lg) were

cotrans-fected with FIH plasmid (0.2 lg) or siRNA (40 n M ) Flag–IjBa

plas-mid was transfected to test the NF-jB-specific expression of the

reporter luciferase To stimulate NF-jB, cells were also stimulated

with 10 ngÆmL)1 TNF-a or 2 ngÆmL)1interleukin-1b (IL-1b) for 8 h

before harvesting Luciferase activities were measured using a

Biocounter LB960 luminometer, and transfection efficiencies were

normalized by b-gal activity Each bar represents the mean ± SD

(n = 4); NS, not statistically significant.

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to the deletion of both PHD-targeted and

ARD1-tar-geted motifs Expression of sHIF-1a stimulated

EPO-enhancer activity even under normoxia, and further

enhanced the reporter activity under hypoxia More

importantly, the sHIF-1a activity was also positively

regulated by IjBa in 1% oxygen but not in 0.5% oxy-gen (Fig S3) Also in the Gal4 reporter system, the HIF-1a CAD activity was modulated by IjBa expres-sion or knockdown in 1% oxygen but not in 0.5% oxygen (Fig 3B) These results suggest that IjBa

Fig 2 IjBa enhances the hypoxic activity of HIF-1 by antagonizing FIH (A) IjBa is required for the hypoxic activation of HIF-1 EPO-enhan-cer–luciferase plasmid (0.1 lg) and b-gal plasmid (0.1 lg) were cotransfected with Flag–IjBa plasmid (0.2 lg), HA–FIH plasmid (0.2 lg), IjBa siRNA (40 n M , si-IjBa), or FIH siRNA (40 n M , si-FIH) After being stabilized for 48 h, cells were incubated under normoxia or hypoxia for

16 h, and then harvested for the analysis of luciferase activity (B) IjBa enhances the EPO reporter activity HIF-1-dependently Mutated reporter plasmid (0.1 lg) lacking the HIF-1 target sequence and b-gal plasmid (0.1 lg) were cotransfected with Flag–IjBa plasmid (0.2 lg) or HA–FIH plasmid (0.2 lg) After 16 h of normoxic or hypoxic incubation, luciferase activity was measured (C) IjBa stimulates the transcrip-tional activity of HIF-1a CAD in an Asn803-dependent manner Wild-type or N803A Gal4–CAD (amino acids 776–826) plasmids (0.1 lg) and Gal4–luciferase reporter plasmid (0.1 lg) were cotransfected with b-gal plasmid (0.1 lg) or ⁄ and Flag–IjBa plasmid (0.2 lg) into HEK293 cells After 16 h of normoxic or hypoxic incubation, luciferase activity was measured Each bar represents the mean ± SD from four indepen-dent experiments *P < 0.05, NS, no significance (D) IjBa positively regulates the interaction between HIF-1a and p300 The HIF-1a–p300 interaction was examined using a coimmunoprecipitation assay HEK293 cells were cotransfected with HA-tagged stable HIF-1a plasmid (HA–sHIF-1a, 1 lg) and p300 plasmid (1 lg), Flag–IjBa plasmid, and ⁄ or IjBa siRNA (80 n M ) Cells were incubated under normoxic or hypoxic conditions for 8 h, and then homogenized p300 was immunoprecipitated with anti-p300 serum (a-p300) and protein G ⁄ A beads (IP), and coprecipitated HA–sHIF-1a was identified by immunoblotting (IB) Input levels were measured by immunoblotting using specific antibodies.

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functionally stimulates the transcriptional activity of

HIF-1a at moderate levels of hypoxia (1–5% O2) but

not at a more severe level (0.5% O2)

IjBa inhibits FIH-mediated Asn803 hydroxylation

under moderate hypoxia

As shown in Fig 2C, Asn803 was found to be required

for CAD activation by IjBa, which suggests that

FIH-dependent Asn803 hydroxylation is related to the

activity of IjBa To test this possibility, we analyzed

Asn803 hydroxylation in CAD using a specific

anti-body against hydroxylated Asn803 in HEK293 cells

Under normoxic conditions, Asn803 hydroxylation

could be detected, although HIF-1a was negligibly expressed In 1% oxygen, HIF-1a was robustly expressed and Asn803 was partially hydroxylated IjBa overexpression noticeably inhibited the Asn803 hydroxylation, which was rescued by FIH coexpression (Fig 4A, left panel) When IjBa was knocked down, Asn803 hydroxylation was enhanced, and this was attenuated by FIH knockdown (Fig 4A, right panel)

On the other hand, in 0.5% oxygen, Asn803 was negli-gibly hydroxylated, and IjBa or FIH overexpres-sion⁄ knockdown failed to affect Asn803 hydroxylation (Fig 4B) Next, we checked the expression of three HIF-1-targeted genes, namely, those encoding vascular endothelial growth factor-A, aldolase-A, and lactate

A

B

Fig 3 The IjBa-mediated activation of HIF-1 occurs in moderate hypoxia (A) IjBa stimulation of HIF-1 activity occurs only in 1% oxygen EPO-enhancer–luciferase plasmid (0.1 lg) and b-gal plasmid (0.1 lg) were cotransfected into HEK293 cells with Flag–IjBa plasmid (0.2 lg), IjBa siR-NA(80 n M , si-IjBa), or GFP siRNA (80 n M , si-GFP) (B) IjBa stimulates HIF-1a CAD activity only in 1% oxygen Wild-type Gal4– CAD plasmid (0.1 lg), Gal4–luciferase reporter plasmid (0.1 lg) and b-gal plasmid (0.1 lg) were cotransfected into HEK293 cells with Flag–IjBa plasmid (0.2 lg), IjBa siRNA (80 n M , si-IjBa), or GFP siRNA (80 n M , si-GFP) After cells were incubated

in 1% or 0.5% oxygen for 16 h, luciferase activities (mean ± SD, n = 4) were analyzed.

*P < 0.05, NS, no significance.

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dehydrogenase-A In 1% oxygen, the hypoxic

expres-sion of these genes was regulated positively by IjBa

but negatively by FIH (Fig 4C) However, the

expres-sion of these genes was unaffected by IjBa or FIH in

0.5% oxygen (Fig 4D) These results suggest that

IjBa inhibits FIH-dependent Asn803 hydroxylation

under moderate hypoxia, but not under severe

hypoxia

IjBa competes with HIF-1a in FIH binding

To understand the interplay between HIF-1a, FIH,

and IjBa, we coexpressed these proteins in HEK293

cells and examined protein interactions by performing immunoprecipitation and immunoblotting assays Figure 5A shows the effect of IjBa on the interaction between HIF-1a and FIH FIH and HIF-1a proteins were coimmunoprecipitated, but this was noticeably reduced by IjBa expression, which suggests that IjBa interferes with FIH binding to HIF-1a Next, we checked whether IjBa–FIH binding is disrupted by HIF-1a It was found that HIF-1a inhibited IjBa–FIH binding (Fig 5B) As FIH binding affinities for HIF-1a and IjBa are likely to be similar, it appears that HIF-1a and IjBa compete for FIH binding

Fig 4 IjBa stimulates HIF-1-dependent gene expression by inhibiting Asn803 hydroxylation (A, B) IjBa inhibits FIH-mediated Asn803 hydroxylation HEK293 cells were transfected with Flag–IjBa plasmid (0.2 lg), HA–FIH plasmid (0.2 lg), IjBa siRNA (80 n M , si-IjBa), and ⁄ or FIH siRNA (80 n M , si-FIH) pcDNA (0.2 lg) and GFP siRNA (80 n M , si-GFP) were used as transfection controls After cells had been incu-bated in 1% or 0.5% oxygen for 16 h, protein levels were analyzed by immunoblotting Asn803-hydroxylated HIF-1a was detected using an antibody against hydroxylated asparagine (N803-OH) (C, D) HEK293 cells were transfected as described above and then incubated in 1% or 0.5% oxygen for 16 h Vascular endothelial growth factor (VEGF), aldolase, lactate dehydrogenase (LDH) and b-actin mRNA levels were analyzed by semiquantitative RT-PCR and autoradiography.

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HIF-1a CAD becomes inactivated shortly after

tumor necrosis factor-a (TNF-a) stimulation

What is the biological significance of the

IjBa-medi-ated HIF-1 activation? If FIH-mediIjBa-medi-ated HIF-1a

inac-tivation is antagonized by IjBa, the HIF-1a CAD

activity might be regulated IjBa-dependently during

inflammation As IjBa is dynamically regulated

dur-ing inflammation, the CAD activity needs to be

exam-ined in the time course of inflammation Therefore,

we analyzed CAD activity and Asn803 hydroxylation

4, 8 and 16 h after TNF-a stimulation CAD activity

was increased by hypoxia in a time-dependent

man-ner, and was generally inhibited by TNF-a treatment

The inhibitory effect of TNF-a on hypoxic CAD

activity was more significant after 4 h (42.1%

inhibi-tion) or 8 h (30.5% inhibiinhibi-tion) of incubation than

after 16 h of incubation (6.9% inhibition) (Fig 6A,

upper panel) Also, CAD activity was inhibited by

TNF-a even under normoxic conditions Under the

same conditions, IjBa expression was found to be

noticeably downregulated 4 and 8 h after TNF-a

stimulation, but to be somewhat restored after 16 h

of incubation (Fig 6A, lower panel) However,

Asn803 hydroxylation of Gal4–CAD was stimulated

4 h after TNF-a treatment and was abolished in a

time-dependent manner Asn803 hydroxylation

appears to be inversely correlated with IjBa

expres-sion On the basis of these results, the

HIF-1-medi-ated hypoxic responses are likely to be repressed at

the early phase of inflammation, and this may be attributed to IjBa downregulation and subsequent activation of FIH

Discussion

In the present study, we tested the possibility that the interaction between FIH (HIF-1 inhibitor) and IjBa (NF-jB inhibitor) participates in crosstalk between the HIF-1 and NF-jB signaling pathways FIH–IjBa binding was confirmed by yeast two-hybrid assays and coimmunoprecipitation analyses Functionally, IjBa was found to regulate the transcriptional activity of HIF-1 positively, whereas FIH did not affect NF-jB activity Mechanistically, IjBa derepressed HIF-1a CAD activity by inhibiting the FIH-mediated Asn803 hydroxylation of CAD It was also found that IjBa inhibited FIH by competing with FIH for HIF-1a binding Furthermore, IjBa affected HIF-1a activity only in moderately hypoxic conditions, under which FIH remains functional When cells were treated with TNF-a, IjBa downregulation, Asn803 hydroxylation and HIF-1a inactivation all occurred up to 8 h, but subsided after 16 h On the basis of these results, we propose that IjBa plays a pivotal role in the crosstalk between the HIF-1 and NF-jB signaling pathways This hypothesis is summarized in Fig 6B

Hypoxia and inflammation often codevelop in immunological, ischemic and cancerous diseases Inflammation stimulates oxygen consumption, which

Fig 5 IjBa and HIF-1a compete with each other in FIH binding (A) IjBa inhibits the FIH–HIF-1a interaction HEK293 cells were

cotransfect-ed with HA–HIF-1a plasmid (0.7 lg), HA–FIH plasmid (0.3 lg), and ⁄ or Flag–IjBa plasmid (0.2 or 0.4 lg) HIF-1a or FIH protein was precipi-tated using their specific antibodies, and then FIH or HIF-1a coprecipitation was identified by immunoblotting (B) HIF-1a inhibits the IjBa–FIH interaction HEK293 cells were cotransfected with Flag–IjBa plasmid (0.3 lg), HA–FIH plasmid (0.3 lg), and ⁄ or HA–HIF-1a plasmid (0.2 or 0.4 lg) FIH or IjBa protein was precipitated using specific antibodies, and then IjBa or FIH coprecipitation was identified by immunoblotting.

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results from increased energy metabolism of resident

cells and from respiratory bursting of infiltrating

phagocytes These events lead to the establishment of

a hypoxic microenvironment around inflamed tissue

[12] Conversely, hypoxia stimulates inflammation,

because immune cells gather around hypoxia-injured

tissues [13] Given that HIF-1a and NF-jB are key

factors of the hypoxic and inflammatory responses,

respectively, the possibility of crosstalk between two

factors is of growing interest

Many lines of evidence support the notion that

sub-stantial crosstalk occurs between the HIF-1a and

NF-jB pathways under pathological circumstances associated with hypoxia and inflammation [14] For example, HIF-1 has been reported to be activated under nonhypoxic conditions by a number of proin-flammatory cytokines, such as TNF-a, interleukins, lipopolysaccharide, and reactive oxygen⁄ nitrogen species [15] In terms of mechanisms underlying HIF-1a induction by inflammatory stimuli, Frede et al [16] previously demonstrated that NF-jB mediated the transcription of the HIF1A gene during lipopolysac-charide stimulation of human monocytes Recently, the role of NF-jB in HIF-1a mRNA expression was further investigated, using the HIF-1a promoter– luciferase reporter and electrophoretic mobility-shift analyses [17] Rius et al [18] also showed, in macro-phages of IkB kinase-b knockout mice, that NF-jB plays a critical role in transactivation of the HIF1A gene and that basal activity of NF-jB is required for hypoxic induction of HIF-1a In addition to its posi-tive role in HIF-1 regulation, NF-jB can negaposi-tively control HIF-1a expression by inducing an HIF-1a-silencing micro-RNA, miR-155 [19] Although HIF-1a

is under the control of NF-jB, HIF-1a is also required for NF-kB activation Walmsley et al [20] demon-strated that NF-jB induction in response to hypoxia was significantly attenuated in neutrophils of HIF-1a knockout mice and that NF-jB signaling activated by HIF-1a contributed to neutrophil survival in hypoxia

In addition, HIF-1a overexpression in keratinocytes was found to activate NF-jB in the mouse skin and to augment the skin inflammation in response to 12-O-tetradecanoylphorbol-13-acetate Mechanistically, it was suggested that HIF-1a is involved in IjBa degra-dation and NF-jB activation by extracellular signal-related kinase-mediated phosphorylation [21] Given these reports, HIF-1a is likely to regulate NF-jB-med-iated inflammatory responses positively However, we did not observe the reciprocal regulation between HIF-1a and NF-jB Even when IjBa was overexpressed or knocked down, HIF-1a protein levels were not signifi-cantly changed (Figs 4 and 5A) Also, HIF-1a overex-pression did not affect IjBa exoverex-pression (Fig 5B) We here transiently expressed or silenced HIF-1a or IjBa and performed all experiments within 2 days after transfection A distinct change in HIF-1a or IjBa expression may require a longer incubation time than

2 days

In the present study, we found that an NF-jB inhi-bitor, IjBa, activated HIF-1a by sequestering an HIF-1a inhibitor, FIH During inflammation, IjBa is phosphorylated at Ser32 and Ser36 by IkB kinase complex and then degraded by proteasomes [22] Our results suggest that IjBa degradation may reinforce

A

B

Fig 6 HIF-1a is functionally inhibited by inflammatory stimulation.

(A) HIF-1a CAD is inactivated shortly after TNF-a stimulation

Wild-type Gal4–CAD plasmid (0.1 lg), Gal4–luciferase reporter plasmid

(0.05 lg) and b-gal plasmid (0.1 lg) were cotransfected into

HEK293 cells Cells were treated with 10 ngÆmL)1TNF- and

incu-bated under normoxic or hypoxic conditions for 4, 8, or 16 h Each

bar represents the mean ± SD (n = 4), and the percentage

inhibi-tion by TNF-a is marked above the corresponding bars (B)

Sum-mary of IjBa roles in inflammatory and hypoxic responses As IjBa

inhibits NF-jB and FIH through direct interaction, it inhibits

inflam-matory responses but stimulates hypoxic responses.

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the FIH-mediated repression of HIF-1a, which would

negatively affect cellular adaptation to hypoxia Indeed,

we found that IjBa was noticeably downregulated 4

and 8 h after TNF-a stimulation (Fig 6A) However,

its expression recovered after 16 h of incubation, which

suggests that IjBa is resynthesized by NF-jB activated

by TNF-a [22] Likewise, both HIF-1a CAD

inactiva-tion by TNF-a and Asn803 hydroxylainactiva-tion showed a

similar time course (Fig 6A) Therefore, HIF-1a

inacti-vation by IjBa suppression seems to occur transiently

during the early stage of inflammation, and HIF-1a

activity may subsequently resume, owing to IjBa

resynthesis

ARD, which consists of 30–34 amino acids, is one of

the most common motifs in nature, and functions

exclu-sively to mediate protein–protein interactions [23]

Three thousand six hundred and eight proteins have

been identified as containing ARD sequences in the

non-redundant smart protein database [24], but only Notch

and IjBa have been found to regulate HIF-1a by

inter-acting with FIH However, the high affinity of FIH for

ARD suggests that other ARD-containing proteins also

affect HIF-1-mediated hypoxic responses by interacting

with FIH Furthermore, given the diverse functions of

ARD-containing proteins, such as transcriptional

regu-lation, cell cycle reguregu-lation, differentiation, cytoskeletal

organization, and stress response [23], it is possible that

the ARD–FIH interaction could lead to various hypoxic

responses other than inflammation

Here, we suggest that IjBa derepresses HIF-1a

activ-ity by inhibiting FIH If this is the case, this action of

IjBa can only occur when FIH is functional, and this

functionality requires molecular oxygen To determine

the minimal oxygen tension required for FIH activity,

we analyzed cellular levels of Asn803-hydroxylated

HIF-1a in 1% or 0.5% oxygen (Fig 5) In 1% oxygen,

HIF-1a was found to be stabilized but to be still

hydroxylated at Asn803 Moreover, ectopically

expressed FIH increased the amount of Asn803

hydroxylation These results suggest that FIH remains

functional in 1% oxygen However, in 0.5% oxygen,

Asn803 hydroxylation was found to be almost

com-pletely inhibited, and under this condition, FIH

overex-pression failed to increase Asn803 hydroxylation levels,

which suggests that FIH is inactivated in 0.5% oxygen

Furthermore, the oxygen-dependent action of IjBa was

also confirmed by our reporter and mRNA analyses

Does IjBa, then, regulate HIF-1a in hypoxic and

inflammatory tissues? Given that the oxygen tension in

tissues rarely falls below 1% (7.6 mmHg), even in

hyp-oxic or inflammatory diseases [25], we believe that IjBa

may positively regulate HIF-1a by inhibiting FIH in

most hypoxia-related diseases

We conclude that IjBa is likely to function as a positive regulator of HIF-1a under moderately hypoxic conditions, and this action of IjBa appears to be attributable to its ability to sequester FIH from HIF-1a However, little is known of the significance of the IjBa– FIH interaction during the progress of diseases associated with hypoxia and inflammation On the basis

of our results, we suggest that IjBa plays a pivotal role

in shifting the cell response from NF-jB-mediated inflammation to HIF-1-mediated hypoxic adaptation

Experimental procedures

Reagents and antibodies Culture media and fetal bovine serum were purchased from Invitrogen (Carlsbad, CA, USA) Anti-HIF-1a serum was raised in rabbits against glutathione S-transferase-tagged human HIF-1a (amino acids 418–698), and a monoclonal antibody against hydroxylated Asn803 of HIF-1a was raised in mice immunized with a peptide containing a hydroxylated asparagine residue, as previously described [26,27] Anti-IjBa and anti-FIH sera were purchased from SantaCruz Biotech (Santa Cruz, CA, USA) Other chemi-cals were purchased from Sigma-Aldrich (St Louis, MO, USA)

Cell culture and hypoxic incubation The HEK293 cell line was obtained from the American Type Culture Collection (ATCC; Manassas, VA, USA), and cultured in DMEM, supplemented with 10% heat-inac-tivated fetal bovine serum in a humidified 5% CO2 incuba-tor For hypoxic incubation, cells were incubated in a hypoxic chamber (5% CO2and 5%⁄ 1% ⁄ 0.5% O2)

Preparation of short interfering RNAs (siRNAs) and plasmids

To knock down IjBa and FIH, siRNA duplexes were designed on the basis of cDNA sequences provided by the NCBI (NM_020529 for IjBa, and NM_017902 for FIH), and synthesized by Samchully Pharm (Seoul, Korea) The sequences for IjBa siRNA duplex are 5¢-GAGUACGA GCAGAUGGUCA-3¢ and 5¢-UGACCAUCUGCUCGUA CUC-3¢, and those of FIH siRNA duplex are 5¢-GAAUC CCAGUUGCGCAGUUAUAGCU-3¢ and 5¢-AGCUAUA ACUGCGCAACUGGGAUUC-3¢ cDNAs of IjBa, FIH and HIF-1a were cloned by RT-PCR using Pfu DNA poly-merase and inserted into pcDNA–Flag or pcDNA–HA plasmid by blunt-end ligation The plasmid for sHIF-1a mutant was made by deleting three degradation motifs (amino acids 397–405, 513–553, and 554–595), using a

Trang 10

PCR-based mutagenesis kit (Stratagene, Cedar Creek, TX,

USA), as previously described [28]

Reporter assays

Luciferase reporter genes containing EPO enhancer,

hypoxia-response element-mutated EPO enhancer or

Gal4-binding promoter were constructed as previously described

[29] An jB reporter plasmid, which contains 5·

NF-jB response elements fused to luciferase, was purchased

from Stratagene (La Jolla, CA, USA) HEK293 cells were

cotransfected with 1 lg each of reporter gene and plasmid

cytomegalovirus–b-gal and⁄ or plasmid of HIF-1 or Gal4–

CAD, using the calcium phosphate method pcDNA was

added to ensure that the final DNA concentrations in both

the control and experimental groups were similar After

being stabilized for 24 h, the cells were incubated under

normoxic or hypoxic conditions, and then lysed to

deter-mine luciferase and b-galactosidase (b-gal) activities

Lucif-erase activity was analyzed using a Lumat LB960

luminometer (Berthold Technologies, Bad Wildbad,

Germany), and a b-gal assay was performed to normalize

transfection efficiency

Immunoprecipitation and immunoblotting assay

HEK293 cell lysates were incubated with specific antibodies

or nonimmunized serum at 4C for 4 h The immune

com-plexes were further incubated with protein G–Sepharose

beads (GE Healthcare Bio-science, Piscataway, NJ USA)

at 4C for 4 h After washing of the beads,

immunocom-plexes were eluted with an SDS buffer containing 200 mm

Tris⁄ HCl (pH 6.8), 40% glycerol, and 10%

b-mercaptoeth-anol For immunoblotting assays, cells were lysed with an

SDS buffer, separated on SDS⁄ polyacrylamide gels, and

transferred to an Immobilon-P membrane (Millipore,

Bed-ford, MA, USA) Membranes were blocked with 5% nonfat

milk in NaCl⁄ Tris containing 0.1% Tween-20 at room

tem-perature for 30 min, and then incubated overnight at 4C

with a primary antibody b-Tubulin was used as a loading

control

Semiquantitative RT-PCR

Total RNAs were isolated from HEK293 cells by Trizol

reagent (Invitrogen) RNA was quantified by measuring

absorbance at 260 nm RNAs (1 lg) were reverse

tran-scribed at 48C, and the resulting cDNAs were amplified

over 18–23 PCR cycles in 20 lL of reaction mixture

con-taining 0.185 MBq [32P]dCTP[aP] and 250 nm each primer

set The PCR products were electrophoresed on a 4%

poly-acrylamide gel, and dried gels were autoradiographed The

nucleotide sequences of primer pairs have been described

previously [26]

Statistical analysis All data [means and standard deviations (SDs)] were ana-lyzed using excel 2003 software (Microsoft, Redmond,

WA, USA) Two-sided, Student’s t-tests were used for two-group comparisons, and P < 0.05 was considered to be significant

Acknowledgements

This work was supported by a Korea Research Foundation Grant (2008-E00054) and by a Bone Metabolism Research Center Grant (R11-2008-023-02001-0) provided by the Korea Science and Engi-neering Foundation We thank E Huang (University

of Utah) for kindly providing us with gene constructs

References

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4 Lando D, Peet DJ, Whelan DA, Gorman JJ & White-law ML (2002) Asparagine hydroxylation of the HIF transactivation domain: a hypoxic switch Science 295, 858–861

5 Ruas JL, Poellinger L & Pereira T (2002) Functional analysis of hypoxia-inducible factor-1 alpha-mediated transactivation Identification of amino acid residues critical for transcriptional activation and⁄ or interaction with CREB-binding protein J Biol Chem 277,

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