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Tiêu đề Identification of membrane-bound serine proteinase matriptase as processing enzyme of insulin-like growth factor binding protein-related protein-1 (IGFBP-rP1/angiomodulin/mac25)
Tác giả Sanjida Ahmed, Xinlian Jin, Motoki Yagi, Chie Yasuda, Yuichiro Sato, Shouichi Higashi, Chen-Yong Lin, Robert B. Dickson, Kaoru Miyazaki
Trường học Yokohama City University
Chuyên ngành Cell Biology, Molecular Biology
Thể loại Research article
Năm xuất bản 2006
Thành phố Yokohama
Định dạng
Số trang 13
Dung lượng 366,88 KB

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Of nine human cell lines tested, seven cell lines secreted IGFBP-rP1 at high levels, and two of them, ovar-ian clear cell adenocarcinoma OVISE and gastric carcinoma MKN-45, highly produc

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matriptase as processing enzyme of insulin-like growth factor binding protein-related protein-1

(IGFBP-rP1/angiomodulin/mac25)

Sanjida Ahmed1,2, Xinlian Jin1, Motoki Yagi1,2, Chie Yasuda1, Yuichiro Sato1,2, Shouichi Higashi1, Chen-Yong Lin3, Robert B Dickson3and Kaoru Miyazaki1,2

1 Division of Cell Biology, Kihara Institute for Biological Research, Yokohama City University, Japan

2 Graduate School of Integrated Sciences, Yokohama City University, Japan

3 Lombardi Comprehensive Cancer Center, Georgetown University Medical Center, Washington, DC, USA

Insulin-like growth factor (IGF) binding proteins

(IGFBPs) regulate cellular proliferation by modulating

the actions of insulin and IGFs [1,2] Recent studies

have revealed a group of IGFBP-related proteins (IGFBP-rPs), which have low affinity for IGFs⁄ insulin and low structural homology to IGFBPs [3]

Keywords

angiomodulin; insulin-like growth factor;

insulin-like growth factor binding

protein-related protein-1; matriptase; proteolytic

processing

Correspondence

K Miyazaki, Division of Cell Biology, Kihara

Institute for Biological Research, Yokohama

City University, 641–12 Maioka-cho,

Totsuka-ku, Yokohama 244–0813, Japan

Fax: +81 458201901

Tel: +81 458201905

E-mail: miyazaki@yokohama-cu.ac.jp

(Received 25 August 2005, revised

15 November 2005, accepted 8 December

2005)

doi:10.1111/j.1742-4658.2005.05094.x

Insulin-like growth factor (IGF) binding protein-related protein-1 (IGFBP-rP1) modulates cellular adhesion and growth in an IGF⁄ insulin-dependent or ininsulin-dependent manner It also shows tumor-suppressive activity

in vivo We recently found that a single-chain IGFB-rP1 is proteolytically cleaved to a two-chain form by a trypsin-like, endogenous serine protein-ase, changing its biological activities In this study, we attempted to iden-tify the IGFBP-rP1-processing enzyme Of nine human cell lines tested, seven cell lines secreted IGFBP-rP1 at high levels, and two of them, ovar-ian clear cell adenocarcinoma (OVISE) and gastric carcinoma (MKN-45), highly produced the cleaved IGFBP-rP1 Serine proteinase inhibitors effect-ively blocked the IGFBP-rP1 cleavage in the OVISE cell culture The con-ditioned medium of OVISE cells did not cleave purified IGFBP-rP1, but their membrane fraction had an IGFBP-rP1-cleaving activity The mem-brane fraction contained an 80-kDa gelatinolytic enzyme, which was identified as the membrane-type serine proteinase matriptase (MT-SP1)

by immunoblotting When the membrane fraction was separated by SDS⁄ PAGE, the IGFBP-rP1-cleaving activity comigrated with matriptase

A soluble form of matriptase purified in an inhibitor-free form efficiently cleaved IGFBP-rP1 at the same site as that found in a naturally cleaved IGFBP-rP1 Furthermore, small interfering RNAs for matriptase efficiently blocked both the matriptase expression and the cleavage of IGBP-rP1 in OVISE cells These results demonstrate that IGFBP-rP1 is processed to the two-chain form by matriptase on the cell surface

Abbreviations

AEBSF, 4-(2-aminoethyl)benzenesulfonyl fluoride hydrochloride; AGM, angiomodulin; FBS, fetal bovine serum; HAI-1, hepatocyte growth factor activator inhibitor-1; HGF, hepatocyte growth factor; HLE, hepatocellular carcinoma; IGF, insulin-like growth factor; IGFBP, IGF-binding protein; IGFPB-rP1, IGFBP-related protein-1; MMP, matrix metalloproteinase; MT-SP1, membrane-type serine proteinase matriptase; PSF, prostacyclin-stimulating factor; TAF, tumor-derived cell adhesion factor; siRNA, small interfering RNA; tPA, tissue plasminogen activator uPA, urokinase-type plasminogen activator.

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Angiomodulin (AGM) was initially purified as a

tumor-derived cell adhesion factor (TAF) from human

bladder carcinoma cells [4,5] Its cDNA was cloned

from human leptomeningial cells as mac25 [6] and from

human fibroblasts as prostacyclin-stimulating factor

(PSF) [7] Since AGM has a relatively low structural

homology to IGFBPs, the name of IGFBP-related

pro-tein-1 (IGFBP-rP1) has recently been proposed for

AGM⁄ mac25 ⁄ PSF AGM ⁄ IGFBP-rP1 exerts a weak

cell adhesion activity through heparan sulfate

proteog-lycans on the cell surface [4,5,8] and stimulates cell

growth in culture medium containing insulin or IGFs

[9,10] The IGFBP-rP1 mRNA is expressed in a wide

range of normal tissues including the heart, spleen,

ovary, small intestine and colon [11]

Immunohisto-chemical analysis has shown that IGFBP-rP1 is highly

expressed in the blood vessels of various human cancer

tissues [5] and in invading tumor cells [12] On the other

hand, other studies have shown that IGFBP-rP1

exhib-its a tumor-suppressive activity when overexpressed in

cancer cells [13–15] Thus, exact biological functions of

IGFBP-rP1 remain to be clarified

Various extracellular proteinases regulate cellular

functions by degrading or processing protein

sub-strates including extracellular matrix proteins, growth

factors and cell surface proteins For example,

mat-rix metalloproteinases (MMPs), such as membrane

type-1 matrix metalloproteinase (MT1-MMP),

matri-lysin (MMP-7) and gelatinases A⁄ B (MMP-2 ⁄ 9), are

known to play important roles in the process of

tumor invasion and metastasis [16–18] Serine

pro-teinases such as plasminogen activators, plasmin and

trypsin also contribute to expression of malignant

phenotypes in tumor cells [19,20] Recently,

consider-able attention has been focused on the physiological

and pathological functions of a membrane-bound

serine proteinase, matriptase (MT-SP1) [21–23] It is

well known that IGFBPs often undergo proteolytic

processing in various kinds of biological fluids such

as blood, synovial fluid and interstitial fluid, as well

as culture media [24,25] Several types of proteinases,

such as pregnancy-associated plasma proteins [26,27],

prostate specific antigen [28] and MMP-3 [29], have

been reported to cleave IGFBPs The proteolysis of

IGFBPs is thought to modulate the actions of IGFs

towards cells [29]

We recently found that IGFBP-rP1 is converted

from a single-chain form to a two-chain form by the

action of a trypsin-like serine proteinase [10] The

pro-teolytic processing of IGFBP-rP1 greatly reduced its

insulin⁄ IGF-dependent growth promoting activity but

enhanced its syndecan-1-mediated cell adhesion activity

[10] We report here that the membrane-bound serine

proteinase matriptase is responsible for the processing

of IGFBP-rP1

Results

Expression and processing of IGFBP-rP1

in various cell lines

We have reported that IGFBP-rP1 is proteolytically converted to a two-chain form during purification [10] The cleavage of IGFBP-rP1 leads to complete loss

of insulin⁄ IGF-1-dependent cell growth-stimulatory activity due to its loss of insulin⁄ IGF-binding ability

To examine whether the specific cleavage of IGFBP-rP1 also occurs in cultured cell systems, we tested expression and processing of IGFBP-rP1 in eight human cancer cell lines and one immortalized epithe-lial cell line (HEK293) When the conditioned media were analyzed by immunoblotting after reducing SDS⁄ PAGE, seven of the nine cell lines tested were found to secrete IGFBP-rP1 protein (Fig 1) Among them, OVISE ovarian adenocarcinoma cells and MKN-45 gastric adenocarcinoma cells secreted signifi-cant levels of the 25-kDa, cleaved form of IGFBP-rP1

On nonreducing SDS⁄ PAGE, IGFBP-rP1 in the two-conditioned media was separated to a single band of

33 kDa (data not shown), indicating that the cleaved IGFBP-rP1 was a two-chain form consisting of a

25 kDa chain and an 8 kDa chain [10] These results suggested that OVISE and MKN-45 cells expressed a high level of proteinase(s) responsible for the process-ing of IGFBP-rP1

To determine the class of the IGFBP-rP1-cleaving proteinase, OVISE cells were cultured in the presence

of various proteinase inhibitors and the processing of IGFBP-rP1 was analyzed As shown in Fig 2, serine proteinase inhibitors, 4-(2-aminoethyl)benzenesulfonyl fluoride hydrochloride (AEBSF) and aprotinin, signifi-cantly inhibited the production of the cleaved form of IGFBP-rP1 (25 kDa), whereas a cysteine proteinase inhibitor (leupeptin), an aspartic proteinase inhibitor (pepstatin) and a metalloproteinase inhibitor (N-(R)- (2-(hydroxyaminocarbonyl)methyl)-4-methylpentanoyl-l-3-(2¢-naphthyl)alaninyl-l-alanine 2-aminoethyl amide; TAPI-1) did not affect the processing A commercially available proteinase inhibitor mixture containing AEBSF, aprotinin and some other inhibitors inhibited the processing to the same extent as AEBSF alone

As trypsin-type serine proteinases, but neither chymotrypsin-type nor elastase-type, are susceptible to the AEBSF inhibition, a trypsin-type serine proteinase was thought to be responsible for the IGFBP-rP1 cleavage

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Analysis of serine proteinases secreted

by various cell lines

Trypsin-type serine proteinases present in the

condi-tioned media of the nine cell lines were analyzed by

gelatin zymography (Fig 3A) To eliminate the activit-ies of metalloproteinases, the renatured gel was first treated with 1 mm EDTA and then incubated in the presence of 10 mm CaCl2, as described in Experimental procedures Of the nine cell lines tested, OVISE,

Fig 1 Analysis of noncleaved and cleaved

forms of IGFBP-rP1 in conditioned media of

eight cancer cell lines and one immortalized

cell line (HEK293) Concentrated conditioned

media were prepared from the cultures of

the nine indicated human cell lines, and

each sample containing the same amount of

protein (5 lg) was subjected to SDS⁄ PAGE

under reducing conditions on a 14% gel,

followed by immunoblotting with the

anti-TAF ⁄ IGFBP-rP1 antibody (upper panel) Bars

indicate the noncleaved form (33 kDa) and

the cleaved form (25 kDa) The cleaved form

is detected highly in OVISE and MKN-45 cell

lines and slightly in HLE and HEK293 cell

lines As a loading control, the same

vol-umes of conditioned media as those for the

immunoblotting were subjected to SDS ⁄

PAGE followed by protein staining with

Coomassie Brilliant Blue R-250 (lower

panel) Bars indicate the molecular size in

kDa Other experimental conditions and the

types of the cell lines used are described in

‘Experimental procedures’.

Fig 2 Effects of proteinase inhibitors on

processing of IGFBP-rP1 in culture of OVISE

cells OVISE ovarian carcinoma cells were

incubated in a serum-free culture medium

supplemented without (None) or with one

of the following proteinase inhibitors:

AE-BSF (100 l M ), aprotinin (75 n M ), leupeptin

(10 l M ), pepstatin A (1 l M ), TAPI-1 (2 l M ),

and a mixture (100 l M AEBSF, 75 n M

aprotinin, 5 l M bestatin, 1.5 l M E-64, 2 l M

leupeptin, and 1 l M pepstatin A) After

incubation for 2 days, IGFBP-rP1 in each

conditioned medium was analyzed by

immunoblotting, as described in Fig 1 The

upper panel shows immunoblots for

matriptase Bars indicate the noncleaved

form (33 kDa) and the cleaved form

(25 kDa) of IGFBP-rP1 The lower panel

shows protein staining patterns of

conditioned media Bars indicate the

molecular size in kDa.

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MKN-45 and DLD-1 cells commonly expressed a

major gelatinolytic activity at approximately 75 kDa

and additional weak activities at 95 kDa, 105 kDa and

lower molecular weight positions The 75 kDa activity

was faintly detected in HSC-4 and HEK293 cells

To date, several families of type II transmembrane

serine proteinases have been identified [30] Among

them, MT-SP1 is known to be expressed in many types

of epithelial cell lines and carcinoma cell lines, and to

be proteolytically released from the cell membranes

[21,31,32] The molecular size of a major form of

sol-uble matriptase is approximately 75 kDa To

deter-mine whether or not the 75 kDa proteinase in Fig 3A

was matriptase, the conditioned media of the nine cell

lines were subjected to immunoblotting with an

anti-matriptase antibody (M32) As shown in Fig 3B, the

conditioned media of OVISE, MKN-45 and DLD-1

cells clearly showed doublet bands at approximately

75 kDa and two minor bands at 95 and 110 kDa The

conditioned media of HSC-4 and HEK293 cells also

showed weak immunoreactive bands at the same

posi-tions These results attributed the gelatinolytic activit-ies at 75, 95 and 105 kDa in Fig 3A to matriptase The 75 kDa doublet has been reported to result from glycosylation [33] The glycosylation is thought to increase the stability of this protein against trypsin and other proteinases [34]

To further characterize the gelatinolytic activities in the OVISE cell conditioned medium, we examined effect of a serine proteinase inhibitor, AEBSF, on the proteinase activities (Fig 4) The sample was treated with 2 mm AEBSF before and⁄ or after SDS ⁄ PAGE and subsequent renaturation of separated proteins The pretreatment of the sample with the inhibitor par-tially blocked only the 75 kDa activity, whereas the inhibitor treatment after the protein renaturation strongly blocked the activities at 75, 95 and 110 kDa This indicated that only a part of the 75 kDa enzyme existed in an inhibitor-free active form in the concen-trated conditioned medium A weak activity of 40 kDa was not inhibited by the inhibitor, suggesting that it might be a metalloproteinase It has been reported that

110 95 75

EJ-1 ECV

-304 HT1080 OV

IS E MKN-45 HLE HSC-4 DLD-1 HEK293

110 95 75

EJ-1 ECV

-304

HT1080 OV

IS E MKN-45 HLE HSC-4 DLD-1 HEK293

A

B

Fig 3 Analysis of serine proteinases secre-ted by nine human cell lines Conditioned media were prepared from the cultures of the indicated, nine human cell lines The concentrated conditioned media containing the same amount of protein (5 lg) were subjected to gelatin zymography (A) and immunoblotting with the antimatriptase antibody M32 (B) as described in ‘Experi-mental procedures’ In the gelatin zymogra-phy, metalloproteinase activities were eliminated by incubating the renatured gel with 1 m M EDTA for 30 min (A) Gelatin zymograms of the conditioned media from the nine cell lines The conditioned media of OVISE and MKN-45, which showed high IGFBP-rP1 cleavage in Fig 1, showed a major activity at 75 kDa and minor activities

at 95 and 110 kDa, which were indicated by bars (B) Immunoblots for matriptase The

75 kDa major band seems to correspond mainly to a single-chain, latent matriptase, while the 95 and 110 kDa bands seem to correspond to two-chain, active forms complexed with HAI-1 [18,32].

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membrane-bound matriptase is shed into culture

med-ium in some different forms [21] The soluble

matrip-tase includes a 70 kDa single-chain, latent form as a

major component, a two-chain, active enzyme

com-plexed with two different sizes of hepatocyte growth

factor (HGF) activator inhibitor (HAI-1) (total

molecular sizes of 95 and 110 kDa), and a trace of an

inhibitor-free active enzyme [21,31,32] The 95 and

110 kDa matriptase⁄ HAI-1 complexes are expected

not to react with AEBSF, because their active serine

residues are bound to HAI-1 Based on these facts,

the 95- and 110-kDa bands in zymography (Figs 3A

and 4) and immunoblotting (Fig 3B) are most likely

to correspond to the matriptase⁄ HAI-1 complexes

The 95- and 110-kDa gelatinolytic activities seemed to

result from partial dissociation of an active matriptase

from its inhibitor HAI-1 after SDS⁄ PAGE Similarly,

the 75-kDa activity that was not inhibited by the

pre-treatment with AEBSF was thought to be an active

matriptase, which had been dissociated from HAI-1 by

the SDS treatment In addition, immunoblotting under

reducing conditions suggested that the majority of the

75-kDa immunoreactive band was a single-chain latent

matriptase (data not shown) [32]

The correlation between the IGFBP-rP1-cleaving activity (Fig 1) and the expression of matriptase in MKN-45 and OVISE cell lines suggested matriptase as

a candidate for the IGFBP-rP1-processing enzyme Moreover, it has been reported that matriptase prefers basic P1, P3 and P4 residues to cleave substrates [33] This consensus sequence is found in the cleavage site sequence of IGFBP-rP1, where Lys97, Lys95 and Arg94 residues are located at P4, P3 and P1 sites, respectively [10] These facts prompted us to examine whether or not matriptase is the IGFBP-rP1-processing enzyme However, when purified IGFBP-rP1 was incubated with the conditioned medium of OVISE or DLD-1 cells, the latter of which contained the highest amount of matriptase, its processing to a two-chain form was not observed (data not shown)

IGFBP-rP1-cleaving activity of membrane fraction from OVISE cells

As IGFBP-rP1 is cleaved in cultured OVISE cells, we next examined the possibility that cell-associated serine proteinase(s) might cleave IGFBP-rP1 A membrane fraction of OVISE cells was prepared as described under ‘Experimental procedures’ and incubated with purified IGFBP-rP1 Figure 5A (lanes 1 and 2) shows that the cleaved form of IGFBP-rP1 significantly increased during the incubation This cleavage was inhibited effectively by aprotinin, suggesting that a serine proteinase(s) catalyzed this processing (Fig 5A, lane 3) We further analyzed serine proteinase activit-ies in the membrane fraction of OVISE cells by gelatin zymography This analysis revealed the presence of a gelatinolytic enzyme, with an approximate molecular size of 80 kDa, in the membrane fraction (Fig 5B, lane 1) When analyzed on the same gel, the apparent molecular size of the gelatinolytic activity in the membrane was slightly higher than the 75 kDa activity found in the conditioned medium (data not shown) Immunoblotting with the antimatriptase antibody showed an immunoreactive band at the same position

as the gelatinolytic activity (Fig 5B, lane 2), suggest-ing that the 80-kDa serine proteinase was a mem-brane-bound matriptase

To verify that the 80 kDa proteinase has the IGFBP-rP1-cleaving activity, we separated the proteins

in the membrane fraction of OVISE cells by SDS⁄ PAGE After electrophoresis, the proteins on the gel were renatured and the gel was horizontally divided into eight equal parts Each piece of the gel was then incubated with purified IGFBP-rP1 and the cleavage

of the protein was analyzed as described under Experi-mental procedures As shown in Fig 6A, gel fractions

Fig 4 Effect of serine proteinase inhibitor AEBSF on gelatinolytic

activities of OVISE cell conditioned medium AEBSF was added to

make a final concentration of 2 m M into the OVISE cell conditioned

medium before SDS ⁄ PAGE (lanes 2 and 4) and ⁄ or into the reaction

buffer after the SDS ⁄ PAGE and subsequent renaturation (lanes 3

and 4) –, No addition, +, addition Ordinate indicates the molecular

size in kDa Arrowheads show the matriptase bands Other

experi-mental conditions are described in ‘Experiexperi-mental procedures’ and

in the legends to Fig 3A.

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4–6 had the IGFBP-rP1-cleaving activity and fraction

6 showed the highest activity When the proteins in

the gel pieces were analyzed by immunoblotting, an

80 kDa matriptase was also detected in fraction 6

(Fig 6B), indicating that this membrane-bound serine proteinase is the prime candidate for the IGFBP-rP1-cleaving proteinase in OVISE cells

IGFBP-rP1-cleaving activity of purified matriptase The results of the SDS⁄ PAGE separation of the mem-brane-bound enzyme suggested that the soluble form

of matriptase might cleave IGFBP-rP1 if separated from inhibitors To test this possibility, the condi-tioned medium of DLD-1 cells, which contained the highest activity of matriptase, was separated by SDS⁄ PAGE and assayed for the IGFBP-rP1-cleaving

80

B

80

33 25

Fig 5 Analysis of IGFBP-rP1-cleaving enzyme present in

mem-brane fraction of OVISE cells A memmem-brane fraction was prepared

from OVISE cells as described in ‘Experimental procedures’ and

used for the following assays (A) IGFBP-rP1-cleaving activity

Puri-fied IGFBP-rP1 (500 ng) was incubated with the membrane fraction

(20 lg protein) in the presence (lane 3) or absence (lane 2) of

75 n M aprotinin (serine proteinase inhibitor) The incubated samples

were subjected to immunoblotting under reducing conditions with

the anti-TAF ⁄ IGFBP-rP1 antibody Lane 1, no incubation Bars

indi-cate the noncleaved form (33 kDa) and the cleaved form (25 kDa).

(B) Gelatin zymography (lane 1) and immunoblotting with the

anti-matriptase antibody M32 The membrane fraction containing 15 lg

protein was run on a gelatin-containing gel under nonreducing

con-ditions for the zymography (lane 1), and the same sample

contain-ing 10 lg protein was subjected to immunoblottcontain-ing with the

antimatriptase antibody M32 The bar indicates a gelatinolytic band

at approximately 80 kDa in lane 1 and a matriptase band at almost

the same position in lane 2 Other experimental conditions are

des-cribed in ‘Experimental procedures’.

Fig 6 Fractionation of IGFBP-rP1-cleaving enzyme and matriptase present in OVISE cell membrane by SDS ⁄ PAGE The membrane fraction (20 lg proteinÆlane)1) of OVISE cells was separated by non-reducing SDS ⁄ PAGE on two lanes of a 7.5% gel After the gel was washed with 1% Triton X-100 for protein renaturation, each of the two lanes was divided into eight fractions and used for one of the two following assays (A) IGFBP-rP1-cleaving activity Each gel frac-tion was incubated with IGFBP-rP1 (500 ng) at 4 C for 24 h fol-lowed by 37 C for 24 h The incubated samples were subjected to immunoblotting under reducing conditions with the anti-TAF ⁄ IGFBP-rP1 antibody (None), IGFBP-rP1 incubated without gel frac-tion Bars indicate the noncleaved form (33 kDa) and the cleaved form (25 kDa) Fraction 6 shows the highest activity (B) Fraction-ation of matriptase Gel fractions from another lane were used to detect matriptase Each gel fraction was extracted with the SDS sample buffer and applied to SDS ⁄ PAGE under nonreducing condi-tions on a 10% gel and immunoblotted with the antimatriptase anti-body M32 An arrow indicates an immunoreactive band of matriptase MF, the membrane fraction before separation Other experimental conditions are described in ‘Experimental procedures’.

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activity The IGFBP-rP1-cleaving activity was detected

at fractions corresponding to approximately 75 and

95 kDa, which also showed immunoreactive bands to

the antimatriptase antibody in immunoblotting (data

not shown) A similar result was also obtained when

the conditioned medium of OVISE cells was separated

by SDS⁄ PAGE (data not shown) These results

strongly suggested that soluble forms of matriptase are

able to cleave IGFBP-rP1 in the absence of HAI-1 or

other inhibitors

To further confirm this possibility, we purified an

inhibitor-free, soluble form of matriptase from the

conditioned medium of DLD-1 cells, as described in

‘Experimental procedures’ The purified matriptase

preparation contained the 75-kDa matriptase and a

few minor proteins, as analyzed by SDS⁄ PAGE

(Fig 7A) Gelatin zymography under nonreducing

conditions confirmed that the 75 kDa matriptase had a

proteolytic activity (Fig 7B) Immunoblotting analysis

under nonreducing conditions showed a single

immuno-reactive band for matriptase at 75 kDa, but under

reducing conditions it was split into a major 75-kDa

band of the single-chain, latent enzyme and a minor

50 kDa band of the two-chain, active enzyme (Fig 7C) [10] Based on the relative band intensity, the percent-age of the active enzyme to the total matriptase was estimated to be approximately 30%

We previously reported that trypsin cleaves IGFBP-rP1 at the same site as an endogenous processing enzyme [10] The IGFBP-rP1-cleaving activities of matriptase and trypsin were compared at varied con-centrations (Fig 8) Fifty nanograms of the 33 kDa IGFBP-rP1 was almost completely cleaved to the

25 kDa form by 5 ng of the total matriptase, which contained the active enzyme as a minor component

On the other hand, 10 ng of trypsin converted a major part of the 33 kDa IGFBP-rP1 to the 25 kDa form, but an increased amount (50 ng) of trypsin nonspecifi-cally degraded both forms of IGFBP-rP1 These results indicated that the two-chain, active matriptase has a much higher IGFBP-rP1-cleaving activity than trypsin Furthermore, we tried to identify the cleavage site of IGFBP-rP1 by the purified matriptase The 25 kDa form of IGFBP-rP1 obtained by the treatment with matriptase was applied to an automated protein sequencer The N-terminal amino acid sequence of the

25 kDa band of IGFBP-rP1 was determined to be

A98GAAAGGPG106, suggesting that this protein had been cleaved between K(Lys)97 and A(Ala)98 This cleavage site was identical to that previously deter-mined for a naturally cleaved IGFBP-rP1

All these results demonstrate that the soluble form

of active matriptase cleaves IGFBP-rP1 but HAI-1

or some other inhibitors block its activity in culture medium

Effects of matriptase siRNAs on IGFBP-rP1 cleavage in OVISE cells

To show that matriptase is an endogenous IGFBP-rP1-processing enzyme in OVISE cells, we designed three siRNAs for matriptase and examined their effects

on the IGFBP-rP1 cleavage As negative controls, OVISE cells were treated with a scrambled RNA or with the lipofectamine reagent alone Although the scrambled RNA had some cytotoxic effect, there was

no significant difference in the profiles of secreted pro-teins among the control and siRNA-treated cultures (Fig 9A) Immunoblotting with the antimatriptase antibody showed that all of the three siRNAs decreased the amount of soluble matriptase to less than 20% of the control levels (Fig 9B) When the IGFBP-rP1 secreted into culture medium by OVISE cells was analyzed by immunoblotting, contrasting patterns of the secreted IGFBP-rP1 were obtained

Fig 7 Electrophoretic analyses of purified matriptase Soluble

mat-riptase was purified from the conditioned medium of DLD-1 cells

as described in the text The purified matriptase (approximately

200 ng of total proteins) was subjected to the following analyses.

(A) SDS ⁄ PAGE under nonreducing conditions followed by silver

staining Arrowhead indicates the matriptase band Bars indicate

the molecular size in kDa (B) Gelatin zymography Arrowhead

indi-cates the gelatinolytic activity by matriptase (C) Immunoblotting

with the antimatriptase antibody M32 under nonreducing conditions

(lane 1) and reducing conditions (lane 2) In lane 2, the 75-kDa band

corresponds to the single-chain, latent enzyme, while the 50 kDa

band corresponds to the heavy chain of the two-chain, active

enzyme Other experimental conditions are described in

‘Experi-mental procedures’.

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between the control and siRNA-treated cultures

(Fig 9C) In the two control cultures, the 33-kDa,

uncleaved IGFBP-rP1 was faintly detected compared

with the 25-kDa, cleaved form, whereas in the

siRNA-treated cultures, the uncleaved IGFBP-rP1 was a

major component This indicated that the cleavage of

IGFBP-rP1 was effectively reduced by the siRNA

treatment These results confirmed that matriptase acts

as an IGFBP-rP1-processing enzyme in the culture of OVISE cells

Discussion

In this study, we first identified the type II membrane-bound serine proteinase matriptase as a processing enzyme of IGFBP-rP1⁄ AGM Matriptase was initially

Fig 8 Cleavage of IGFBP-rP1 by purified matriptase and trypsin (A) Matriptase IGFBP-rP1 (50 ng) was incubated with the indicated amounts of purified matriptase at 37 C for 5 h in 10 lL of a reaction mixture containing 20 m M Tris ⁄ HCl (pH 7.5), 0.1 M NaCl and 10 m M

CaCl2 The original concentration of matriptase was determined for the total 75-kDa protein based on the band intensity relative to that of bovine serum albumin as standard (Fig 7A) (B) Trypsin IGFBP-rP1 was incubated with the indicated amounts of TPCK-trypsin under the same conditions except for the absence of CaCl 2 in the reaction mixture The proteolytic cleavage of IGFBP-rP1 in (A) and (B) was analyzed

by immunoblotting as described in Fig 1 Bars indicate the 33 kDa, uncleaved form and the 25 kDa, cleaved form of IGFBP-rP1.

Fig 9 Effects of matriptase siRNAs on IGFBP-rP1 processing in culture of OVISE cells OVISE cells at 50–60% confluence in 60 mm culture dishes were transfected with 200 pmol of each of three siRNAs (si973, si1513 and si2578) using Lipofectamine 2000 reagent As negative controls, the cells were treated with a scrambled RNA (sc) or with the lipofectamine reagent alone (Cont.) These cultures were incubated in serum-containing medium overnight, and then in serum-free medium for 2 days The resultant conditioned media were collected and con-centrated The concentrated samples containing 10 lg protein were subjected to reducing SDS ⁄ PAGE followed by the Coomassie Brilliant Blue staining (A), nonreducing immunoblotting to detect matriptase (B), and reducing immunoblotting to detect IGFBP-rP1 (C) Bars indicate the molecular sizes of marker proteins in (A), the 110-, 95- and 75-kDa bands of matriptase in (B), and the 33-kDa, uncleaved form and the 25-kDa, cleaved form of IGFBP-rP1 in (C) The scrambled RNA-treated culture (2nd lane) was low in the total band intensity of matriptase (B) and IGFBP-rP1 (C) as compared with the control or siRNA-treated cultures This seemed due to the cytotoxic effect of the scrambled RNA Other experimental conditions are described in Experimental procedures.

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found as a trypsin-like serine proteinase secreted by

human breast cancer cells [35] and later purified as a

complex with its natural inhibitor HAI-1 from human

milk [21] Matriptase is expressed in normal epithelial

tissues such as the skin, stomach, colon, kidney, breast,

ovary and pancreas, but not in mesenchyma [36,37] A

recent study with matriptase-deficient mice has shown

that matriptase plays critical roles in the epidermal

barrier function, hair follicle development and thymic

homeostasis [38] Matriptase is also expressed in cancer

tissues of the breast, ovary, uterus and colon and also

by some mammary and ovarian carcinoma cell lines

in vitro[36] Since matriptase is able to degrade

extra-cellular matrix proteins and to activate

urokinase-type plasminogen activator (uPA) [33,39], hepatocyte

growth factor (HGF) [39] and protease-activated

receptor-2 (PAR-2) [33], it is expected to play some

roles in the growth, invasion and metastasis of human

carcinoma cells

We previously reported that IGFBP-rP1 is cleaved

to a two-chain form by a trypsin-like serine proteinase

[10] In the present study, we found that OVISE

ovar-ian carcinoma cells cleaved endogenous IGFBP-rP1,

and their membrane fraction cleaved exogenous

IGFBP-rP1 in a cell-free solution The

IGFBP-rP1-cleaving activity in the OVISE cell membrane

comi-grated with membrane-bound matriptase on SDS⁄

PAGE Furthermore, the treatment of OVISE cells

with matriptase siRNAs efficiently blocked both

mat-riptase expression and the cleavage of IGFBP-rP1 It

is also noted that the cleavage sequence of IGFBP-rP1

is consistent with the most preferable sequence in

sub-strate proteins of matriptase [33] Indeed, a soluble

form of matriptase purified in an inhibitor-free form

efficiently cleaved IGFBP-rP1 at the same site as that

found in a naturally cleaved IGFBP-rP1 All these

facts indicate that the membrane-bound matriptase is

a natural processing enzyme of IGFBP-rP1 On the

other hand, soluble forms of matriptase, which are

released from cell membranes by proteolysis, were

detected in the conditioned media of at least 5 cell

lines out of 9 cell lines tested The processing of

endo-genous IGFBP-rP1 was correlated with the amount of

soluble matriptase in the conditioned media Although

the purified soluble matriptase could cleave

IGFBP-rP1, the conditioned media of OVISE and DLD-1 cells

did not show the IGFBP-rP1-processing activity unless

they were separated by SDS⁄ PAGE Our recent

analy-sis has detected soluble matriptase in 19 of 24 human

carcinoma cell lines tested, which included carcinomas

of the breast, lung, stomach and colon [32] The

sol-uble matriptase mostly existed in a single-chain, latent

form as a major component and two-chain forms

complexed with its inhibitor HAI-1, in agreement with the past reports [18,30] Therefore, soluble matriptase released from cell membrane is expected to have a very low, if any, proteolytic activity The IGFBP-rP1-clea-ving activities of the SDS⁄ PAGE fractions and the matriptase purified from DLD-1 conditioned medium indicate that the soluble form of activated matriptase can cleave IGFBP-rP1, but its activity is masked by HAI-1 in culture medium It was recently reported that the matriptase zymogen might be auto-activated by interacting with HAI-1 on the cell surface [40] The proteolytic action of matriptase, including the process-ing of IGFBP-rP1, seems to be restricted to the cell surface and its close vicinity

Although the present study demonstrates that mat-riptase cleaves IGFBP-rP1, our data do not exclude the possibility that other proteinases, especially serine proteinases, also cleave IGFBP-rP1 We previously reported that many human cancer cell lines secrete an active or latent form of trypsin and a 75-kDa serine proteinase [20], the latter of which was identified as matriptase in a recent study [32] We have also repor-ted that OVISE cells secrete uPA, but neither trypsin nor tissue plasminogen activator (tPA) [41] In addi-tion, it was previously found that trypsin cleaves IGFBP-rP1 to the same two-chain form as that found

in conditioned media [10] In the present study, we examined whether or not uPA and tPA cleave IGFBP-rP1 in test tubes, but the IGFBP-IGFBP-rP1 cleavage was seen with neither uPA nor tPA (data not shown) There-fore, matriptase seems to be a major IGFBP-rP1-pro-cessing enzyme, at least in OVISE cells, and possibly

in MKN-45 cells Recent studies have revealed the presence of four families of type II transmembrane ser-ine proteinase [30] The matriptase subfamily consti-tutes three members (matriptase, matriptase 2 and matriptase 3) It is conceivable that some of these mem-brane-bound serine proteinases or their soluble forms are also involved in the processing of IGFBP-rP1

It is well known that some IGFBPs undergo proteo-lytic cleavage [24,25] In biological fluids, IGFBPs bind IGFs with high affinity, protecting the growth factors from proteolytic degradation The proteolytic cleavage

of IGFBPs is thought to contribute to the release of IGFs from IGF⁄ IGFBP complexes to interact with IGF receptors on the cell surface This mechanism may not be directly applicable to the case of IGFBP-rP1, because IGFBP-rP1 has a far lower affinity for IGFs than IGFBPs The high affinity binding of IGFs

to IGFBPs limits the interaction of the growth factors with the cell surface receptors Therefore, IGFBPs gen-erally inhibit IGF-stimulated cell growth in vitro [25]

In contrast, IGFBP-rP1 stimulates cell growth in the

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presence of insulin or IGF-1 in vitro, presumably due

to its low affinity for the factors [9,10] On the other

hand, some studies have shown that IGFBP-rP1

exhib-its a tumor-suppressive activity when overexpressed in

cancer cells [13–15] The apparent discrepancy between

the in vitro and in vivo studies is not clearly explained

IGFBP-rP1 also shows IGF⁄ insulin-independent

activ-ities It has affinity for heparin, type IV collagen and

syndecan-1 [5,8,10] These activities seem to be

respon-sible for the cell adhesion activity of IGFBP-rP1

in vitroand its dense deposition on the basement

mem-brane of blood vessels in tumor tissues [5] These

IGF⁄ insulin-dependent and independent activities of

IGFBP-rP1 are notably altered by its proteolytic

clea-vage [10] For example, IGFBP-rP1 loses its IGF⁄

insulin-binding activity and IGF⁄ insulin-dependent

growth-stimulating activity but acquires high cell

adhe-sion activity by proteolytic cleavage It seems

conceiv-able that matriptase regulates tumor growth by

modulating biological activities of IGFBP-rP1, as well

as other growth-regulating proteins, in vivo

In this study, we identified a new substrate of

mat-riptase Matriptase may exert a broad range of

func-tions in regulating cellular growth, apoptosis and

differentiation by degrading or processing a variety of

extracellular proteins

Experimental procedures

Materials

The sources of materials used are as follows: aprotinin,

leu-peptin, pepstatin A, AEBSF and proteinase inhibitor mixture

that contains AEBSF, aprotinin, bestatin, E-64, leupeptin

and pepstatin A from Wako Pure Chemical Industries

(Osaka, Japan); gelatin from Difco (Detroit, MI, USA);

N-(R)-(2-(hydroxyaminocarbonyl)methyl)-4-methylpentanoyl-l-3-(2¢-naphthyl)alaninyl-l-alanine 2-aminoethyl amide

(TAPI-1) from Peptide Institute (Osaka, Japan) IGFBP-rP1

was purified from the conditioned medium of the human

bladder carcinoma cell line EJ-1, as described previously [10]

An anti-TAF⁄ IGFBP-rP1 monoclonal antibody (#88) [5]

and an antimatriptase monoclonal antibody (M32) [21] were

raised against purified IGFBP-rP1 and purified matriptase,

respectively All other chemicals were of analytical grade or

the highest quality commercially available

Cell cultures and preparation of conditioned

medium

Types of human cancer cell lines used are as follows:

HSC-4, tongue squamous cell carcinoma; HT1080, fibrosarcoma;

EJ-1 and ECV-304, bladder carcinomas; DLD-1, colon

adenocarcinoma; OVISE, ovarian clear cell adenocarcino-ma; MKN-45, adenosquamous carcinoma of the stomach; HLE, hepatocellular carcinoma The source and properties

of OVISE cells were described before [41] The human embryonic kidney cell line HEK293 (ATCC CRL-1573) was purchased from American Type Culture Collection (ATCC, Rockville, MD, USA) The other cell lines were obtained from Japanese Cancer Resources Bank (JCRB) in National Institute of Biomedical Innovation (Osaka, Japan) To prepare conditioned medium, each cell line was grown to semiconfluence in 90-mm culture dishes contain-ing a 1 : 1 mixture of Dulbecco’s modified Eagles medium and Ham’s F12 medium (Gibco; Grand Island, NY, USA), DME⁄ F12, supplemented with 10% fetal calf serum (FCS) The cells were rinsed three times with serum-free DME⁄ F12, and the culture was further continued in the presence or absence of various proteinase inhibitors in serum-free DME⁄ F12 After incubation for 2 days, the resultant conditioned medium was collected, clarified by centrifugation and dialyzed against distilled water at 4C The dialyzed sample was then lyophilized and dissolved in

a 100th volume of 10 mm Tris⁄ HCl (pH 7.5) to the original conditioned medium

Preparation of membrane fractions

OVISE cells were grown to confluence in the serum-contain-ing medium, rinsed three times with ice cold NaCl⁄ Piand then scraped in the presence of 20 mm Hepes (pH 7.5) con-taining 250 mm sucrose at 4C The cell suspension was then homogenized with a Dounce homogenizer The homogenate was centrifuged at 1500 g for 7 min to remove the nuclei The postnuclear supernatant was further centrifuged at

50 000 g for 30 min The resultant pellet was then dissolved

in 20 mm Tris⁄ HCl (pH 7.5) containing 0.5 m KCl, 0.15 m NaCl and 1% Triton X-100, and the insoluble substances were removed by centrifugation at 14 000 g for 20 min The supernatant was used as a crude membrane fraction

SDS–polyacrylamide gel electrophoresis (SDS/PAGE) and immunoblotting

SDS⁄ PAGE was performed on 7.5, 10, or 14% polyacryl-amide gel slabs (85 mm wide, 1 mm thick, and 70 mm long) under reducing or nonreducing conditions Separated pro-teins were stained with silver Immunoblotting was per-formed as described previously [42] Briefly, proteins on gels were transferred onto nitrocellulose membranes (Schlei-cher & Schuell, Keene, NH, USA) The membrane was blocked with skimmed milk and successively treated with

an anti-TAF⁄ IGFBP-rP1 monoclonal antibody (#88) or an antimatriptase monoclonal antibody (M32) as the first anti-body, the second antibody (biotinylated antimouse IgG, Vector Laboratory, Burlingham, CA, USA), and alkaline

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