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Likewise, processed MMP-2 was observed in the conditioned medium of K-562, NCI-H460 and Hep G2 cells, and their incubation with the metallo-protease inhibitors did not result in the prev

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activation of pro-matrix metalloprotease-2 by proprotein convertases

Bon-Hun Koo, Hee-Hyun Kim, Michael Y Park, Ok-Hee Jeon and Doo-Sik Kim

Department of Biochemistry, College of Life Science and Biotechnology, Yonsei University, Seoul, South Korea

Introduction

Matrix metalloproteases (MMPs) constitute a family

of 23 zinc-dependent endopeptidases They are

involved in many biological processes and diseases,

and catalyze the proteolysis of extracellular and

non-extracellular matrix molecules [1] For example,

MMP-2 is associated closely with organ growth,

endometrial cycling, wound healing, bone remodeling, tumor invasion and metastasis [2] Its functions are executed through the degradation of components of the basement membrane, including type IV collagen, fibronectin, elastin, laminin, aggrecan and fibrillin [1,3]

Keywords

furin; membrane type-1 matrix

metalloprotease (MT1-MMP); pro-matrix

metalloprotease-2 (pro-MMP-2); pro-MMP-2

activation; proprotein convertases

Correspondence

B.-H Koo, Department of Biochemistry,

College of Life Science and Biotechnology,

Yonsei University, 134 Sinchon-Dong

Seodaemun-Gu, Seoul 120-749, South Korea

Fax: 82 2 312 6027

Tel: 82 2 313 2878

E-mail: k4119@yonsei.ac.kr

D.-S Kim, Department of Biochemistry,

College of Life Science and Biotechnology,

Yonsei University, 134 Sinchon-Dong

Seodaemun-Gu, Seoul 120-749, South Korea

Fax: 82 2 312 6027

Tel: 82 2 2123 2700

E-mail: dskim@yonsei.ac.kr

(Received 14 July 2009, revised 26 August

2009, accepted 28 August 2009)

doi:10.1111/j.1742-4658.2009.07335.x

Matrix metalloprotease-2 is implicated in many biological processes and degrades extracellular and non-extracellular matrix molecules Matrix metalloprotease-2 maintains a latent state through a cysteine–zinc ion pairing which, when disrupted, results in full enzyme activation This pairing can be disrupted by a conformational change or cleavage within the propeptide The best known activation mechanism for pro-matrix metalloprotease-2 occurs via cleavage of the propeptide by membrane type-1 matrix metalloprotease However, significant residual activation of pro-matrix metalloprotease-2 is seen in membrane type-1 matrix meta-lloprotease knockout mice and in fibroblasts treated with metameta-lloprotease inhibitors These findings indicate the presence of a membrane type-1 matrix metalloprotease-independent activation mechanism for pro-matrix metalloprotease-2 in vivo, which prompted us to explore an alternative activation mechanism for pro-matrix metalloprotese-2 In this study, we demonstrate membrane type-1 matrix metalloprotease-independent propep-tide processing of matrix metalloprotease-2 in HEK293F and various tumor cell lines, and show that proprotein convertases can mediate the processing intracellularly as well as extracellularly Furthermore, processed matrix metalloprotease-2 exhibits enzymatic activity that is enhanced by intermolecular autolytic cleavage Thus, our experimental data, taken together with the broad expression of proprotein convertases, suggest that the proprotein convertase-mediated processing may be a general activation mechanism for pro-matrix metalloprotease-2 in vivo

Abbreviations

Con A, concanavalin A; dec-RVKR-cmk, dec-Arg-Val-Lys-Arg-chloromethyl ketone; FITC, fluorescein isothiocyanate; GAPDH, glyceraldehyde-3-phosphate dehydrogenase; MMP, matrix metalloprotease; MT1-MMP, membrane type-1 matrix metalloprotease; MTT, 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl-tetrazolium bromide; PC, proprotein convertase; pro-MMP-2, pro-matrix metalloprotease-2; TGN, trans-Golgi network; TIMP, tissue inhibitor of metalloprotease.

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Because of its potential for tissue destruction,

MMP-2 activity is regulated at multiple points, such

as gene expression, compartmentalization, zymogen

activation and enzyme inactivation by extracellular

inhibitors [e.g tissue inhibitors of metalloproteases

(TIMPs)] [1] Like other MMPs, pro-MMP-2

main-tains a latent state via an interaction between a

thiol group of a propeptide cysteine residue and the

catalytic zinc ion in the active site [4] Disruption of

this cysteine–zinc ion pairing, such as through

confor-mational changes [5] or proteolysis within the

propep-tide [e.g by plasmin, thrombin or membrane

type-MMPs (MT-MMPs)] [6–12], is required for the

activation of the latent enzyme The most studied

acti-vation mechanism for pro-MMP-2 is cleavage of the

propeptide by MT1-MMP, which requires cooperative

activity between MT1-MMP and TIMP-2 [7,13–15]

However, residual activation of pro-MMP-2 is

observed in MT1-MMP knockout mice, even though

the activation is reduced significantly [16,17] Thus,

these data suggest that an MT1-MMP-independent

activation mechanism for pro-MMP-2 may also exist

in vivo

Proprotein convertases (PCs), a family of Ca2+

-dependent serine proteases of which furin is the most

ubiquitous, have a major role in molecular maturation

[18–20] Most PCs reside within the trans-Golgi

net-work (TGN), but some are present at the cell surface

via a transmembrane domain (e.g furin) [21,22] or the

extracellular matrix (e.g PACE4 and PC5A) [23] Like

other PCs, furin cleaves its substrates immediately

downstream of the consensus sequence

Arg-Xaa-Arg⁄ Lys-Arg (where Xaa is any amino acid) in the

TGN [18,19,24] or at the cell surface [25] The

signifi-cance of furin in many biological processes is

attri-buted to its widespread expression [26] and the

developmental lethality of furin knockout mice [27]

Furthermore, elevated expression of PCs is frequently

observed in various human cancers and tumor cell

lines, implicating the importance of PCs in tumor

progression [28]

The presence of activated MMP-2 in MT1-MMP

knockout mice prompted us to explore an

MT1-MMP-independent activation mechanism for

pro-MMP-2 In this study, we demonstrate

MT1-MMP-independent propeptide processing of MMP-2 in

HEK293F and various tumor cell lines, where PCs

could mediate this processing Furthermore,

PC-pro-cessed MMP-2 showed enzymatic activity, which was

enhanced following intermolecular autolytic cleavage

Thus, these results strongly suggest a potential role

of PCs in pro-MMP-2 activation in PC-expressing

cells

Results

MT-MMP-independent processing of pro-MMP-2 Previous studies have shown that MT1-MMP is a major activator of pro-MMP-2 [29–31] Furthermore, TIMP-2 and integrin avb3 have been shown to play important roles in MT1-MMP-mediated pro-MMP-2 activation [13–15,32] Thus, prior to investigating the role of MT1-MMP in pro-MMP-2 activation, expres-sion of MT1-MMP, TIMP-2 and integrin avb3 was characterized in COS-1, HCT116, HEK293F, MCF-7, MDAH 2774, K-562, NCI-H460 and Hep G2 cells MT1-MMP protein was undetectable by immunoblot-ting with anti-MT1-MMP rabbit polyclonal IgG in all cell types (data not shown), whereas semi-quantitative RT-PCR detected its mRNA in HCT116, K-562, NCI-H460 and Hep G2 cells (Fig 1A) Because other MT-MMPs have also been demonstrated to process pro-MMP-2 [8–11], their expression was also examined

in these cells Although protein expression was not determined, different levels of MT-MMP mRNA were observed in the cells (Fig 1A) Immunoblotting with mouse anti-TIMP-2 IgG2a showed that COS-1 cells possessed the highest levels of TIMP-2, whereas the expression of this inhibitor was absent or much lower

in HCT116, HEK293F, MCF-7, MDAH 2774, K-562, NCI-H460 and Hep G2 cells (Fig 1B) Variable cell surface expression of integrin avb3 was assessed by flow cytometric analysis (Fig 1C), although its expres-sion was undetectable in HCT116, K-562 and Hep G2 cells (data not shown) These data demonstrate that different cell types have different cellular components for MT-MMP-mediated pro-MMP-2 activation

To test the MT-MMP-independent processing of pro-MMP-2, cells were incubated with metalloprotease inhibitors (e.g GM6001 and TIMP-2), and the condi-tioned medium was analyzed by zymography TIMP-2

is a strong inhibitor of MT1-MMP at high concentra-tions [33], although it activates pro-MMP-2 with MT1-MMP at low concentrations [34] Thus, we used a high concentration of TIMP-2 (5 lgÆmL–1) to completely inhibit the enzymatic activities of MT1-MMP and other TIMP-2-sensitive MMPs The data showed that the processed MMP-2 was clearly seen in the condi-tioned medium of HEK293F, MDAH 2774 and

MCF-7 cells (Fig 2A) However, processing was not affected

by incubation with the inhibitors in these cells (Fig 2A) Likewise, processed MMP-2 was observed

in the conditioned medium of K-562, NCI-H460 and Hep G2 cells, and their incubation with the metallo-protease inhibitors did not result in the prevention of processing even though pro-MMP-2 accumulated

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slightly in the conditioned medium of K-562 cells

trea-ted with the inhibitors (Fig 2B) As a control, the

con-ditioned medium of concanavalin A (Con A)-treated

HT-1080 cells showed that MT1-MMP-mediated

pro-cessing of pro-MMP-2 was completely inhibited in the

presence of the metalloprotease inhibitors (Fig 2C)

Unlike HT-1080 cells, endogenous MMP-2 expression

in all the cell lines used was low, so that lytic bands

could hardly be seen in the zymograms without

con-centrating the conditioned medium (Fig 2A and not

shown in Fig 2B)

MT-MMPs cleave pro-MMP-2 at the Asn66–Leu

[7–10] or Asn109–Tyr peptide bond [11] Therefore, to

further investigate the role of MT-MMP in

pro-MMP-2 activation, pro-MMP-pro-MMP-2 mutants incapable of

cleav-age by MT1-MMP and⁄ or autolysis were generated

(N66I⁄ L67V, N109I ⁄ Y110F and N66I ⁄ L67V ⁄ N109I ⁄

Y110F) (Fig 3) In agreement with the data using

metalloprotease inhibitors, transient transfection of

these mutants into HEK293F, MCF-7 and

MDAH 2774 cells did not prevent cleavage, as

pro-cessing of the mutants persisted (Fig 4A) By contrast,

processing was increased significantly in the cells

expressing the pro-MMP-2 N66I⁄ L67V and

N66I⁄ L67V ⁄ N109I ⁄ Y110F mutants by unknown mechanisms (Fig 4A) As a control, COS-1 cells expressing the mutants with MT1-MMP showed that the pro-MMP-2 N66I⁄ L67V and N66I ⁄ L67V ⁄ N109I ⁄ Y110F mutants were not cleaved by MT1-MMP, and that the pro-MMP-2 N109I⁄ Y110F mutant was not processed autocatalytically following MT1-MMP cleavage (Fig 4B) Overall, these results suggest the presence of an MT-MMP-independent activation mechanism for pro-MMP-2 in some cell types

PCs mediate propeptide processing of MMP-2

To further explore the MT-MMP-independent activa-tion mechanism of pro-MMP-2, cells were incubated with various inhibitors targeted towards serine (e.g aprotinin, chymostatin, and leupeptin) and aspartyl (e.g pepstatin) proteases, and the conditioned medium was analyzed by zymography As shown in Fig 5A, this processing was not affected by effective concentrations

of these protease inhibitors in HEK293F, MCF-7 and MDAH 2774 cells These data suggest that pro-MMP-2 processing may be mediated by proteases other than serine and aspartyl proteases in these cells

A

C

B

Fig 1 Cellular expression of MT-MMPs,

TIMP-2 and integrin avb3 (A) Analysis of

MT-MMP mRNA in various cell lines The

data represent semi-quantitative RT-PCR

analysis of MT-MMP mRNA in HCT116,

HEK293F, MCF-7, MDAH 2774, K-562,

NCI-H460 and Hep G2 cells PCR products

(25 cycles) were resolved by agarose gel

electrophoresis and visualized by ethidium

bromide staining Arrowheads indicate PCR

products of MT-MMPs or GAPDH (B)

Wes-tern blotting of conditioned medium with

mouse anti-TIMP-2 IgG2a The conditioned

medium from the cells on 12-well plates

was concentrated prior to SDS-PAGE Arrow

indicates TIMP-2 protein (C) Flow

cytometric analysis for cell surface

expression of integrin avb3 The percentage

changes in fluorescence intensity by the

presence of integrin avb3 are shown.

A sample lacking primary antibody was used

as a control (n = 3 representative

experi-ments).

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A previous study has shown the furin processing

of pro-MMP-2 through cleavage of a consensus PC

cleavage site in the propeptide of MMP-2

(Arg98-Lys-Pro-Arg101) [35] We initially examined the enzymatic

activities of PCs in various cells using an enzymatic

activity assay The results showed PC activities in the

cell lysates from HEK293F, MCF-7, MDAH 2774,

K-562, NCI-H460 and Hep G2, whereas negligible

amounts of PC activity were detected in COS-1 and

HCT116 cells (Fig 5B) Next, we investigated whether

PCs play a crucial role in pro-MMP-2 processing by incubating cells with increasing concentrations of the membrane-permeable PC inhibitor dec-Arg-Val-Lys-Arg-chloromethyl ketone (dec-RVKR-cmk) As shown

in Fig 5C, D, pro-MMP-2 processing was reduced significantly in the PC inhibitor-treated cells, suggesting that PCs are major processing enzymes for pro-MMP-2

in these cell types The cells did not undergo apoptosis

at the doses of inhibitor used, which was confirmed

by 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl-tetrazolium bromide (MTT) assay (data not shown) Next, experi-ments were performed to identify which PCs associated with the constitutive secretory pathway mediated this processing When pro-MMP-2 was expressed in COS-1 and HCT116 cells, mainly the intact MMP-2 zymogen was detectable, whereas the processed form was negli-gible in the conditioned medium (Fig 5E) However, processed MMP-2 was seen in the conditioned medium

of cells co-expressing pro-MMP-2 and PCs (Fig 5E) Parallel experiments performed in HEK293F and MCF-7 cells showed endogenous processing of pro-MMP-2, which was enhanced following the transfection

of PCs (Fig 5E) The substitution of Arg101 with Ala decreased PC processing significantly, as well as the endogenous processing of pro-MMP-2 However, par-tially and fully processed MMP-2 was marginally detect-able in the conditioned medium of the cells expressing the mutant (Fig 5E) As such, PCs may be the major processing enzymes for pro-MMP-2 in these cells

PACE4- and PC5A-expressing cells exhibit intracel-lular and extracelintracel-lular processing of pro-MMP-2 Intracellular processing of pro-MMP-2 by furin has been shown previously in COS-1 cells [35] Despite

A

B

C

Fig 2 MT-MMP-independent processing of pro-MMP-2 in various

cell types (A) Effect of metalloprotease inhibitors on the propeptide

processing of MMP-2 in HEK293F, MDAH 2774 and MCF-7 cells.

Cells were treated with GM6001 (20 l M ) or TIMP-2 (5 lgÆmL –1 ) in

500 lL of 293 SFM-II medium on 24-well plates After 14 h of

incu-bation, MMP-2 was captured from 500 lL of the conditioned

med-ium using gelatin–Sepharose according to the manufacturer’s

recommendations (Amersham Biosciences) and eluted in 30 lL of

SDS sample buffer, and the eluted sample was analyzed by

zymog-raphy; 10 lL of the conditioned medium (pre-column sample,

unconcentrated) was loaded on the first lane Arrows indicate

pro- and processed MMP-2 (MMP-2) (B) Effect of metalloprotease

inhibitors on the processing of pro-MMP-2 in K-562, NCI-H460 and

Hep G2 cells Cells were treated as described above MMP-2 was

concentrated from 125 lL of the conditioned medium using

gela-tin–Sepharose and the eluted sample was used for zymographic

analysis Conditioned medium from HT-1080 cells was used as a

positive control for pro-MMP-2 (C) Validation of the

metallopro-tease inhibitors to prevent MT1-MMP-mediated processing of

pro-MMP-2 HT-1080 cells were treated with Con A (50 lgÆmL –1 ) in

the presence and absence of the metalloprotease inhibitors for

14 h (n = 3 representative experiments).

Fig 3 Structures of pro-MMP-2 mutants.

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this, the cellular localization of pro-MMP-2 processing

by other PCs, including PACE4 and PC5A, remains

unknown Therefore, whether PACE4- or

PC5A-medi-ated processing of pro-MMP-2 occurs intracellularly

was investigated using a variety of approaches First,

we examined the enzymatic activities of PCs in

condi-tioned medium and cell lysates using the enzymatic

activity assay The results showed PC activities in the

conditioned medium and cell lysates from COS-1 cells

expressing PCs (Fig 6A) We further verified whether

the activitie cell lysates with the PC inhibitor (1 s

shown reflected exclusively the presence of PCs by

treating the conditioned medium and 00 lm) The

enzymatic activities were almost completely inhibited

(more than 98%) in the PC inhibitor-treated samples

(data not shown), excluding the enzymatic activities of

other proteases in the conditioned medium and cell

lysates Next, pro-MMP-2-expressing COS-1 cells were

co-cultured with cells expressing furin, PACE4, PC5A

or MT1-MMP, and zymographic analysis of the

condi-tioned medium was performed Although soluble furin

was detected in the conditioned medium (Fig 6A) and

furin cell surface expression was also confirmed by

flow cytometry and cell surface biotinylation (Fig 6C),

furin-expressing COS-1 cells did not show extracellular

processing of pro-MMP-2 (Fig 6B) Moreover, when

purified pro-MMP-2 was incubated with purified furin

under cell-free conditions, processing did not occur (data not shown) By contrast, the presence of PACE4, PC5A or MT1-MMP resulted in extracellular cleavage

of pro-MMP-2 (Fig 6B) Moreover, substitution of Arg101 with Ala abolished the extracellular processing

of pro-MMP-2 by PACE4 and PC5A completely (Fig 6B), suggesting the direct cleavage of pro-MMP-2

by these enzymes

To further compare PACE4 and PC5A processing

of pro-MMP-2 with that of furin, cell lysates from the co-transfected cells were analyzed by zymography, in which cells were pretreated with trypsin⁄ EDTA to remove MMP-2 from the cell surface (Fig 6E) Cell lysates from furin-expressing cells showed dramatically larger amounts of processed MMP-2 than did those from cells expressing PACE4 or PC5A (Fig 6D) Interestingly, processed MMP-2 was also seen in cell lysates from HEK293F and MCF-7 cells expressing pro-MMP-2 alone (Fig 6D)

To further verify the intracellular localization of PC-processed MMP-2, a FLAG-tagged pro-MMP-2 mutant, in which the FLAG epitope was inserted imme-diately downstream of Arg98-Lys-Pro-Arg101, was gen-erated In these experiments, PC-processed MMP-2 with

a free N-terminal FLAG tag was detected by western blotting with mouse anti-FLAG M1 IgG2b The anti-FLAG M1 IgG2b only recognizes proteins with a free

A

B

Fig 4 (A) Zymograms of conditioned

medium from cells expressing pro-MMP-2

(WT), pro-MMP-2 N66I⁄ L67V mutant

(N66I ⁄ L67V), pro-MMP-2 N109I ⁄ Y110F

mutant (N109I ⁄ Y110F) and pro-MMP-2

N66I⁄ L67V ⁄ N109I ⁄ Y110F mutant

(N66I ⁄ L67V ⁄ N109I ⁄ Y110F) The conditioned

medium was analyzed without

concentra-tion The bar graph shows the ratio of

processed MMP-2 to unprocessed

pro-MMP-2 Arrows indicate pro- and

processed MMP-2 (MMP-2) (B) Zymogram

of conditioned medium from COS-1 cells

expressing pro-MMP-2, pro-MMP-2

N66I⁄ L67V mutant, pro-MMP-2

N109I ⁄ Y110F mutant and pro-MMP-2

N66I⁄ L67V ⁄ N109I ⁄ Y110F mutant with or

without MT1-MMP Note that COS-1 cells

expressing pro-MMP-2 N66I ⁄ L67V and

N66I⁄ L67V ⁄ N109I ⁄ Y110F mutants show

prominent processing of the propeptide

without MT1-MMP expression Arrows

indicate pro-, intermediate and processed

MMP-2 (MMP-2) Data are the means and

standard deviations of n = 3 experiments.

*P < 0.05 versus wild-type.

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N-terminal FLAG tag These results demonstrated that

furin-processed MMP-2 was recognized specifically by

the anti-FLAG M1 antibody (Fig 7B), whereas

pro-MMP-2 and processed pro-MMP-2 were detected by the

anti-MMP-2 antibody (Fig 7A) Furthermore,

muta-tion of Arg101 to Ala resulted in the complete loss of

FLAG-tagged MMP-2, further supporting the

specific-ity of the anti-FLAG M1 antibody and validating this

experimental approach (Fig 7B) Immunofluorescence

of fixed and permeabilized COS-1 cells stained with

anti-MMP-2 antibody revealed MMP-2 localization to

be mostly intracellular (Fig 7C) Staining with

anti-FLAG M1 antibody also showed the intracellular

local-ization of PC-cleaved MMP-2, even though cells

expressing PACE4 or PC5A stained weakly (Fig 7C)

Cells expressing MMP-2 alone exhibited little staining

with the anti-FLAG M1 antibody (Fig 7C) Further-more, no signal was observed in cells expressing the pro-MMP-2-RKPA(101)-FLAG mutant with PCs, providing additional evidence for the specificity of the anti-FLAG M1 antibody (data not shown) Taken together, these results demonstrate that furin-expressing cells undergo exclusive intracellular processing of pro-MMP-2, whereas cells expressing PACE4 or PC5A exhibit both intracellular and extracellular processing

of pro-MMP-2

Pro101 regulates excessive PC processing of pro-MMP-2

Because Arg98-Lys-Pro-Arg101 in the propeptide of MMP-2 is a minimal recognition motif for PC

cleav-A

C

E

D

B

Fig 5 PC-dependent processing of pro-MMP-2 (A) Effect of various inhibitors

on the propeptide processing of MMP-2

in HEK293F, MCF-7 and MDAH 2774 cells Cells were treated with aprotinin (20 lgÆmL –1 ), chymostatin (10 lgÆmL –1 ), leupeptin (20 lgÆmL –1 ) and pepstatin (2 l M ) After 8 h of incubation, the conditioned media were analyzed by zymography Arrows indicate pro- and processed MMP-2 (MMP-2) (B) Protease activities of PCs in cell lysates from the cells indicated (C) Inhibition of pro-MMP-2 processing by a PC inhibitor dec-RVKR-cmk in HEK293F, MCF-7 and MDAH 2774 cells Cells were incubated with 0–100 l M of the inhibitor for 8 h, and the conditioned medium was analyzed by zymography The bar graph shows the ratio

of processed MMP-2 to pro-MMP-2 in the conditioned medium of cells treated with

100 l M of the PC inhibitor Data are the means and standard deviations of n = 3 experiments *P < 0.05 versus untreated control (D) Inhibition of pro-MMP-2 processing by the PC inhibitor in K-562, NCI-H460 and Hep G2 cells Cells were incubated with 100 l M of the inhibitor Note that almost complete inhibition of

pro-MMP-2 processing is seen in the conditioned medium of the inhibitor-treated cells (E) Zymograms of conditioned medium from cells expressing pro-MMP-2 or pro-MMP-2 R101A mutant with furin, PACE4 or PC5A (n = 3 representative experiments).

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age [18,19,24], and Pro100 is highly conserved in the

MMP family, we investigated whether this amino acid

residue can play a role in regulating the PC cleavage

of pro-MMP-2 The conditioned medium of cells

expressing the pro-MMP-2 P100K mutant showed

highly increased propeptide processing by PCs

(PC5A > PACE4 > furin), whereas the PC-mediated

intracellular cleavage of the mutant was increased

slightly (Fig 8A) Interestingly, the co-culture of

COS-1 cells expressing individual PCs and cells expressing

the mutant showed more robust processing of the

propeptide by extracellular PACE4 and PC5A, but not

by extracellular furin (Fig 8B) These experimental data suggest that Pro100 plays a critical role in regu-lating excessive pro-MMP-2 processing, especially by extracellular PACE4 and PC5A

PC-cleaved MMP-2 is further processed to achieve full activation

Because PCs cleave pro-MMP-2 immediately upstream

of the Cys102 residue that interacts with the catalytic

A

B

D E

C

Fig 6 Cellular location of PC processing of

pro-MMP-2 (A) Protease activities of PCs in

conditioned medium and cell lysates from

COS-1 cells expressing PCs (B) Co-culture

of COS-1 cells expressing pro-MMP-2 or

pro-MMP-2 R101A mutant with cells

expressing PCs or MT1-MMP The

condi-tioned media were analyzed by zymography.

Note that processed MMP-2 is faintly seen

in the conditioned medium of cells

express-ing pro-MMP-2 alone Arrows indicate

pro-, intermediate and processed MMP-2

(MMP-2) (C) Cell surface localization of furin

in the transfected COS-1 cells Flow

cytom-etry and cell surface biotinylation

approaches were used to detect cell

surface furin Arrowhead indicates furin.

(D) Zymographic analysis of cell lysates

from COS-1, HEK293F and MCF-7 cells

co-expressing pro-MMP-2 and PCs Cells

were pretreated with 0.05%

tryp-sin ⁄ 0.53 m M EDTA for 30 min on ice to

remove cell surface proteins (E) Flow

cyto-metric analysis shows the cell surface

locali-zation of MMP-2 in COS-1, HEK293F and

MCF-7 transfected with pro-MMP-2 Cell

surface MMP-2 (dotted line) is absent in the

cells treated with trypsin ⁄ EDTA (T ⁄ E) (full

line) (n = 3 representative experiments).

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domain zinc ion, MMP-2 processed in this manner

may not possess catalytic activity Therefore, we

inves-tigated whether PC-cleaved MMP-2 exhibits enzymatic

activity or whether intermolecular autolytic cleavage at

the Asn109–Tyr peptide bond [36] is required for its

activity after initial processing The degradation of

collagen IV and a fluorescein-conjugated gelatin by

processed MMP-2 from the conditioned medium of HEK293F cells expressing pro-MMP-2, the pro-MMP-2 E404A mutant and the pro-MMP-2 N109I⁄ Y110F mutant in the presence and absence of furin was com-pared Because the catalytic glutamic acid residue within the pro-MMP-2 active site is replaced in the E404A mutant, a proteolytically inactive enzyme is

A

C

B

Fig 7 Intracellular localization of PC-cleaved MMP-2 Cell lysate was obtained from COS-1 cells expressing RKPR(101)-FLAG or pro-MMP-2-RKPA(101)-FLAG with or without furin Western blotting of cell lysate was performed using anti-MMP-2 (A) and anti-FLAG M1 (B) antibody Arrowheads indicate furin-processed MMP-2, and arrow indicates uncleaved pro-MMP-2 (C) Confocal microscope imaging of fixed and

permeabilized COS-1 cells stained with anti-MMP-2 (total MMP-2 staining) or anti-FLAG M1 (MMP-2 or FLAG M1 staining

is green) A negative control in which the primary antibody was omitted showed no signal (data not shown) Scale bar, 20 lm.

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generated Furthermore, the pro-MMP-2 N109I⁄

Y110F mutant showed complete loss of intermolecular

autolytic cleavage following MT1-MMP cleavage

(Fig 4B) Because of concerns about possible

unwanted structural effects of the processed MMP-2

during purification, these experiments were performed

using conditioned medium from cells expressing the

various constructs The concentrations of MMP-2 were

measured by ELISA Substrates were incubated with

an identical amount of MMP-2 and subsequently

ana-lyzed by SDS-PAGE or fluorometry Although the

substrates were degraded proteolytically by MMP-2

that was processed via endogenous routes,

furin-medi-ated cleavage conferred increased proteolytic activity

on MMP-2 (Fig 9) However, the pro-MMP-2

N109I⁄ Y110F mutant showed less proteolytic activity

than the wild-type, even though its enzymatic activity

was also increased by furin-mediated cleavage (Fig 9)

We also obtained similar results with the conditioned

medium from MCF-7 cells expressing the same

constructs (data not shown) However, furin-processed MMP-2 from the conditioned medium of co-transfected COS-1 cells showed much reduced levels of enzymatic activity (e.g 1⁄ 50th to 1 ⁄ 200th of the activity of processed MMP-2 from HEK293F and MCF-7 cells)

by unknown mechanisms (data not shown) Taken together, these data suggest that PC-cleaved MMP-2 is further processed for full enzymatic activity

Discussion

The role of MT1-MMP in pro-MMP-2 activation is well established [7,14], but residual activation of pro-MMP-2 can also be seen in MT1-MMP) ⁄ ) mouse fibroblasts cultured in collagen gel and lung extract [16,17] The residual activation observed might be caused by the presence of other proteases, including metalloproteases (e.g other MT-MMPs) [8–11] and

A

B

Fig 8 Regulation of excessive PC processing of pro-MMP-2 by

Pro100 residue (A) PC processing of pro-MMP-2 and pro-MMP-2

P101K mutant Conditioned medium (CM) and cell lysate from

co-transfected COS-1 cells were analyzed by zymography Data are

the means and standard deviations of n = 3 experiments.

*P < 0.05 versus wild-type (B) Co-culture of COS-1 cells

express-ing the pro-MMP-2 P100K mutant with PC-expressexpress-ing cells The

conditioned medium was analyzed by zymography (n = 3

represen-tative experiments).

A

B

Fig 9 Furin-processed MMP-2 gains its full activity by intermolec-ular autolytic cleavage Digestion assay of collagen IV (A) and a fluo-rescein-conjugated gelatin (B) Conditioned medium was obtained from HEK293F cells expressing pro-MMP-2, pro-MMP-2 E404A mutant and pro-MMP-2 N109I ⁄ Y110F mutant with or without furin The digested substrates were analyzed as described in Materials and methods Zymogram and western blot using anti-MMP-2 show equal amounts of MMP-2 used Arrows indicate pro- and processed MMP-2 (MMP-2) Data are the means and standard deviations of

n = 6 experiments ANOVA test indicates statistically significant dif-ferences in furin versus control and in the N109I ⁄ Y110F mutant versus the wild-type (P < 0.05).

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serine proteases (e.g urokinase⁄ plasmin, thrombin,

chymase, cathepsin G and trypsin-2) [6,12,37,38]

Thus, we examined MT1-MMP-independent

process-ing of pro-MMP-2 usprocess-ing various approaches, all of

which provided evidence for non-MT1-MMP

compo-nents within cells MT-MMPs have been shown to

process pro-MMP-2 through cleavage of pro-MMP-2

at the Asn66–Leu peptide bond by MT1-, MT2-,

MT3- and MT5-MMP, followed by intermolecular

autolytic cleavage at the Asn109–Tyr peptide bond [7–

10], or directly at the Asn109–Tyr peptide bond by

MT6-MMP [11] Moreover, various MT-MMPs are

expressed in the cell types analyzed in this study

How-ever, studies using metalloprotease inhibitors and

pro-MMP-2 mutants incapable of cleavage by MT-MMPs

excluded MT-MMPs as candidates for pro-MMP-2

processing in these cell lines A previous study has also

shown residual MMP-2 activation in fibroblasts treated

with a general metalloprotease inhibitor [16] These

data, taken together with ours, strongly suggest the

existence of non-MT-MMP components for

pro-MMP-2 processing in various cell types

In this study, we found that PCs such as furin, PACE4

and PC5A mediate the MT-MMP-independent

process-ing of MMP-2 Furin-mediated cleavage of

pro-MMP-2 immediately downstream of R(98)KPR(101)

has been reported previously [35], even though it has a

minimal PC recognition motif [18] Moreover,

thrombin-mediated activation of pro-MMP-2 has been shown to

occur in human endothelial cells at a predicted PC

recognition motif for cleavage [12] Because other

serine proteases, including factor Xa and plasmin, have

also been shown to activate pro-MMP-2 [6,39], it

would be interesting to investigate whether these

prote-ases can activate pro-MMP-2 by cleavage at the same

site If this is the case, the PC recognition motif would

be a general cleavage site for pro-MMP-2 activation

Although the conditioned medium of cells expressing

the PC-uncleavable mutant showed a significant

decrease in pro-MMP-2 processing, lower levels of

processed MMP-2 were also seen MT-MMP

expres-sion may contribute to the residual processing of the

mutant in these cells as the mutant can be processed

more fully following MT1-MMP overexpression PCs

are overexpressed in various cancers, including lung,

breast and skin, with a significant role in tumor

progression [40] Moreover, our studies using

metallo-protease and PC inhibitors showed PCs to be major

enzymes for pro-MMP-2 processing in various tumor

cell lines Thus, PC-mediated processing may be a

major mechanism for the activation of pro-MMP-2 in

PC-overexpressing cells (e.g tumor cell lines), whereas

PCs are likely to act alongside MT-MMPs for

pro-MMP-2 activation in cells expressing high levels of MT-MMPs

Furin is localized predominantly in the TGN, but some is present at the plasma membrane [21,22,25] This enzyme is also secreted by cells and may be func-tional in the extracellular space [41,42] However, despite numerous attempts, furin-mediated extracellu-lar processing of pro-MMP-2 could not be detected, leading to the conclusion that furin processing of pro-MMP-2 is exclusively intracellular This finding contra-dicts that of Cao et al [35], who reported that furin processing was both intracellular and extracellular, with intracellular processing as the predominant mech-anism Unlike furin, secreted PACE4 and PC5A are anchored to the cell surface by heparan sulfate proteo-glycan in the extracellular space despite their residence

in the TGN [23] Likewise, MMP-2 has an affinity for binding heparin via its hemopexin-like domain and anchors to heparan sulfate proteoglycans [43,44] Therefore, the binding property of heparan sulfate pro-teoglycans may lead to their co-localization to the cell surface, facilitating the extracellular processing of pro-MMP-2 However, the inability of extracellular furin

to bind heparan sulfate proteoglycans may prevent its co-localization with pro-MMP-2 at the cell surface and its extracellular processing of pro-MMP-2 It is also likely that, once exported from the cell, pro-MMP-2 undergoes a conformational change, thereby hamper-ing furin processhamper-ing Although cells expresshamper-ing PACE4

or PC5A exhibit both intracellular and extracellular processing of pro-MMP-2, intracellular processing

is likely to be predominant because these PCs are concentrated in the TGN to allow more efficient processing of pro-MMP-2

By contrast with previously published data [35], furin-processed MMP-2 showed enzymatic activity However, when furin-processed MMP-2 was obtained from the conditioned medium of COS-1 cells, its enzy-matic activity was much lower than that obtained from HEK293F and MCF-7 cells Several reasons can explain this observation TIMP-2 was highly expressed

in COS-1 cells Furthermore, TIMP-2 is a strong inhibitor of MMP-2 at high concentrations [45], although it activates pro-MMP-2 with MT1-MMP at low concentrations [34] Therefore, we propose that the lack of enzymatic activity is a result of the presence

of a high concentration of TIMP-2 in the conditioned medium of COS-1 cells This was also supported by our observation that autoproteolytic activation of MT1-MMP-processed MMP-2 was detected marginally

in COS-1 cells (Fig 4B) In this study, we found that furin-processed MMP-2 was further processed to its fully activated form, but the detailed mechanism

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