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All MMPs contain an N-terminal signal peptide that directs the enzymes to the secretory pathway, a prodomain with a conserved PRCGXPD sequence that confers the latency of the enzymes and

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Regulation of matrix metalloproteinase activity in health and disease

Elin Hadler-Olsen, Bodil Fadnes, Ingebrigt Sylte, Lars Uhlin-Hansen and Jan-Olof Winberg

Department of Medical Biology, Faculty of Health Sciences, University of Tromsø, Norway

Introduction

Matrix metalloproteinases (MMPs) are a subfamily of

zinc- and calcium-dependent enzymes belonging to the

metzincin superfamily Characteristic for this

super-family is the HEXXHXXGXXH zinc-binding motif

and a conserved methionine located C-terminal to the

zinc-ligands, which forms a Met-turn [1] In humans,

there are 24 MMP genes, but only 23 MMP proteins

because MMP-23 is coded by two identical genes at

chromosome 1 MMPs are built up by various

domains (Fig 1) All MMPs contain an N-terminal

signal peptide that directs the enzymes to the secretory

pathway, a prodomain with a conserved PRCGXPD

sequence that confers the latency of the enzymes and a

catalytic domain with the catalytic zinc localized in the large and relatively shallow active site cleft In addi-tion, all MMPs except the two matrilysins (MMP-7 and -26) and MMP-23 contain a C-terminal

hemopex-in (HPX)-like domahemopex-in that is lhemopex-inked to the catalytic domain through a hinge region In most MMPs, this hinge region consists of 10–30 amino acids, whereas, in MMP-9, this linker contains approximately 64 amino acids and is heavily O-glycosylated [2] In six of the membrane-anchored members of the MMP family, the HPX region ends in either a type I transmembrane domain with a short intracellular sequence or a glycosyl-phosphatidylinositol moiety MMP-23 differs from the

Keywords

activation; compartmentalization;

complexes; exosite; heteromers; inhibition;

matrix metalloproteinases

Correspondence

J.-O Winberg, Department of Medical

Biology, Faculty of Health Sciences,

University of Tromsø, 9037 Tromsø, Norway

Fax: +47 77 64 53 50

Tel: +47 77 64 54 88

E-mail: jan.o.winberg@uit.no

(Received 30 April 2010, revised 4 October

2010, accepted 18 October 2010)

doi:10.1111/j.1742-4658.2010.07920.x

The activity of matrix metalloproteinases (MMPs) is regulated at several levels, including enzyme activation, inhibition, complex formation and compartmentalization Regulation at the transcriptional level is also impor-tant, although this is not a subject of the present minireview Most MMPs are secreted and have their function in the extracellular environment This

is also the case for the membrane-type MMPs (MT-MMPs) MMPs are also found inside cells, both in the nucleus, cytosol and organelles The role

of intracellular located MMPs is still poorly understood, although recent studies have unraveled some of their functions The localization, activation and activity of MMPs are regulated by their interactions with other pro-teins, proteoglycan core proteins and⁄ or their glycosaminoglycan chains, as well as other molecules Complexes formed between MMPs and various molecules may also include interactions with noncatalytic sites Such exo-sites are regions involved in substrate processing, localized outside the active site, and are potential binding sites of specific MMP inhibitors Knowledge about regulation of MMP activity is essential for understanding various physiological processes and pathogenesis of diseases, as well as for the development of new MMP targeting drugs

Abbreviations

APMA, p-aminophenylmercuric acetate; CS, chondroitin sulfate; FnII, fibronectin II; GAG, glycosaminoglycan; GSH, glutathione;

Hp, haptoglobulin; HNL, human neutrophil lipocalin; HPX, hemopexin; MMP, matrix metalloproteinases; MMPI, metalloproteinase inhibitor; MT-MMP, membrane-type matrix metalloproteinase; NuMAP, nuclear MMP-3 associated protein; PG, proteoglycan; SIBLING, small integrin-binding ligand N-linked glycoprotein; TIMP, tissue inhibitor of metalloproteinase; TnI, troponin I.

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other MMPs by lacking the HPX domain, which is

replaced by a C-terminal cystein array region and an

immunoglobulin G-like domain, and, instead of the

N-terminal signal peptide, this enzyme contains an

N-terminal type II transmembrane domain In two of

the secreted MMPs, MMP-2 and MMP-9, the catalytic

domain also contains a module of three fibronectin II

(FnII)-like inserts A recent review described the

molec-ular interactions of the HPX domains of the various

human MMPs [3] The various domains, modules and

motifs in the MMPs are involved in interactions with

other molecules, and hence affect or determine the

activ-ity, substrate specificactiv-ity, and cell and tissue localization,

as well as activation, of MMPs

Activation of proMMPs requires physical

delocaliza-tion of the prodomain from the catalytic site, the

so-called cystein-switch model [4] Two main

mecha-nisms are involved in the activation of MMPs One is

proteolytic cleavage and removal of the prodomain

[5,6] and the other is allosteric activation where the

prodomain is displaced from the catalytic site of

the enzymes without being cleaved (Fig 2) Most of

the MMPs are secreted as proenzymes and their

acti-vation occurs in the pericellular and extracellular

space By contrast, all membrane-type (MT)-MMPs

and three of the secreted MMPs contain a unique sequence (RX[K⁄ R]R) at the C-terminal end of the prodomain (Fig 1) These MMPs can be activated intracellularly by furin, a serine proteinase belonging

to the convertase family, which can cleave the prodo-main at this unique sequence [5,6]

Together, the MMPs are able to degrade most extra-cellular matrix (ECM) proteins In addition, they can process a large number of non-ECM proteins, such as growth factors, cytokines, chemokines, cell receptors, serine proteinase inhibitors and other MMPs, and thereby regulate the activity of these compounds as summarized recently [7] An increasing number of studies have shown that processing of some protein and peptide substrates by MMPs requires that the sub-strates not only interact with the active site, but also regions outside the active site Such regions are referred to as noncatalytic sites or exosites, which can

be motifs localized in the catalytic domain or in one of the other domains An important role of the exosites may be to orient the substrate properly for cleavage and, for some substrates, exosite-binding is an absolute requirement for degradation A recent review [8] focused on current knowledge with respect to struc-tural and functional bases for allosteric control of

Fibronectin II-like domain

MMP-2

MMP-9

Minimal domain

MMP-7, -26

MMP-11, -21, -28

Simple HPX domain

MMP-1, -3, -8, -10, -12, -13, -19, -20, -27

Furin-activated

MMP-23

MT1, -2, -3, -5-MMP MT4, -6-MMP

Zn N C

Zn N

Zn N Zn

N

Zn N

Zn N

Zn N

C C

N Zn

Zn N

Catalytic domain Propeptide domain

Hinge-region

HPX like domain FnII like module RX[K/R]R motif

C Type I transmembrane domain N

C

Type II transmembrane domain GPI-membrane anchor C-terminal Ca-Ig domain Cell membrane

O-glycosylated hinge-region

Fig 1 Domain structure of secreted and membrane-anchored MMPs Most MMPs contain a propeptide domain, a catalytic domain, a linker (hinge-region) and a HPX domain The hinge region in MMP-9 is heavily O-glycosylated The three furin-activated MMPs and all of the mem-brane-anchored MMPs have a basic RX[K ⁄ R]R motif at the C-terminal end of their prodomains This motif can be cleaved inside the cells by furin-like proteinases The two gelatinases (MMP-2 and -9) contain three FnII-like repeats in their catalytic domain, N-terminal to the catalytic Zinc-binding site Four of the six MT-MMPs are anchored to the cell membranes through a type I transmembrane domain and the other two through a glycosylphosphatidylinositol moiety The seventh membrane-anchored MMP, MMP-23, has an N-terminal type II transmembrane domain The two minimal domain MMPs and MMP-23 lack the HPX domain and, in the latter enzyme, this domain is replaced by a C-termi-nal cystein array (Ca) and an immunoglobulin-like (Ig) domain.

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MMP activities Previous reviews have described new

techniques that can be used in the search for exosites

and examples of exosites derived from the use of these

techniques [9,10] Although our knowledge of specific

exosites in the various MMPs is still very limited, these

sites will become of increasing importance as targets

for future drug development Hopefully, future drugs

will not affect all substrate degradation by a given

enzyme, but only the processing of selected substrates

Some of the substrates that MMPs are known to

process are localized intracellularly [7] Although all

MMPs contain a signal peptide that directs them to

the secretory pathway, an increasing number of reports

have found various MMPs localized also inside cells

This may partly explain the ability of some MMPs to

process intracellular proteins and further demonstrates

the complex roles of MMPs under physiological and

pathological conditions Among the earliest

intracellu-lar MMP substrates detected are troponin I (TnI) [11],

aB-crystallin [12] and lens bB1 crystallin [13] In vivo,

MMP cleavage of these substrates was linked to health

and disease MMP-2 degradation of TnI is associated with diminished contractive function of the heart [11], MMP-9 degradation of aB-crystallin with multiple sclerosis [12] and MMP-9 cleavage of lens bB1 crystal-lin with cataract [13]

MMPs interact with various cell surface and pericel-lular molecules that alter the function of the enzyme,

as well as affect cellular behaviour [14] MMP-induced cleavage and degradation of ECM and non-ECM mol-ecules may either prevent or provoke diseases such as cancer [15], as well as cardiovascular, autoimmune, neurodegenerative and various connective tissue dis-eases Knowledge about the regulation of MMP activ-ity is therefore important for understanding various physiological processes, as well as the pathogenesis of

a large number of diseases In addition, such know-ledge is also important for the development of novel treatment strategies A number of excellent reviews on MMPs and their functions are available The present review focuses on the regulation of MMP activity with

an emphasis on post-translational modifications, the

A Proteolytic cleavage of the pro- and HPX-domains B Allosteric activation

Zn N SH

Zn SH

1

Zn

2

Zn

3

Zn

4

Zn SH N

1a

SH Zn

2a Auto-cleavage

Zn

3a Auto-cleavage

Proteases

Mercurials SH-reactive agents Chaotropic agents ROS

Detergents

Zn N SH

Zn

N SH

1

Zn SH N

Zn SH

1a

2a

Zn SH

3a

HgCl 2 / APMA

NGAL (HNL)

Gelatin / Collagen IV / Collagen VI (

α2-chain) / SIBLING

Auto-cleavage

Fig 2 Proteolytic and allosteric activation of MMPs (A) Proteolytic cleavage of the pro- and HPX domain of MMPs by various proteinases, including serine proteases such as trypsin or other MMPs Steps 1–4 represents partly to fully processed propeptide, HPX and hinge regions Processing of the proMMP by another proteinase can be facilitated by the interaction of the target proMMP with other macromole-cules that present the inactive proenzyme to its activator (not shown) Binding of mercurial compounds such as APMA or HgCl 2 , other SH reactive agents, reactive oxygen species (ROS), chaotropic agents and detergents such as SDS results in conformational changes of the pro-enzyme (step 1a) followed by activation through successive autocleavage of the propeptide (steps 2a and 3a) This may also be followed by autoprocessing of the HPX region (not shown) (B) Allosteric activation in which the propeptide remains intact (step 1), as suggested for the binding of proMMP-9 to gelatin or collagen IV, binding of proMMP-2 to collagen VI (a2 chain), as well as binding of individual SIBLINGS to specific MMPs (see text) Binding of HgCl2or APMA to proMMP-9 results in a conformational change (step 1a) followed by autocleavage that did not remove the conserved PRCGV sequence from the enzyme (step 2a) This truncated enzyme had a low specific activity Neutro-phil gelatinase associated lipocalin (NGAL) ⁄ human neutrophil lipocalin (HNL) bound to the new N-terminus without further processing of the enzyme (step 3a), resulting in a fully active enzyme (see text).

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formation of heterodimers and complexes,

compart-mentalization, and the role of exosites in substrate

deg-radation and enzyme inhibition

Activation mechanisms

To induce activation of a proMMP, the prodomain

must be physically delocalized from the catalytic site

(Fig 2) There are various ways to achieve such a

delocalization followed by activation One is through

S-reactive agents, organomercurials and reactive

oxy-gen species, interacting with the conserved cysteine in

the prodomain Another is the induction of

conforma-tional changes through binding of chaotropic agents

and detergents such as SDS In all cases, the

confor-mational changes (Fig 2A, step 1a) are followed by an

autocatalytic stepwise degradation of the prodomain

(Fig 2A, steps 2a and 3a) [5,6] Proteinases can cleave

the prodomain in one or several steps, producing an

active MMP with reduced molecular size A large

number of proteinases such as serine and

metallopro-teinases are involved in the activation of proMMPs In

some cases, one enzyme generate a partly active

enzyme that can be fully activated by a second enzyme

removing one or more amino acids from the

prodo-main, as described for MMP-1 [5,6] Thus, it is not

sufficient to remove the zinc-binding motif in the

prodomain of the MMP to obtain a fully active

enzyme; the catalytic efficiency of the activated MMP

also depends on the cleavage site C-terminal to this

motif

Both MMP-2 and MMP-9 have been shown to be

activated in vivo by serine proteinases such as chymase

and trypsin, suggesting a biological relevance Using

knockout mice, it was also shown that mast cell

chym-ase had a key role in the activation of proMMP-9 and

proMMP-2 [16] In mice with acute pancreatitis,

trypsin induced the activation of proMMP-2 and

proMMP-9 ProMMP-9, when activated by

endoge-nous trypsin, was reported to be a permissive factor

for insulin degradation and diabetes [17] Similarly, a

significant association between high endogen

concen-trations of trypsin and activation of proMMP-9 was

found in ovarian tumor cyst fluids [18] Trypsin has

been shown to be an efficient activator of most

proM-MPs in vitro [6] Instead of activating proMMP-2, it

was reported that trypsin induced degradation of the

enzyme [19] Other studies showed that trypsin could

activate proMMP-2, although less efficiently compared

to compounds such as p-aminophenylmercuric acetate

(APMA) [20–23] There is no contradiction in these

results We have shown that the balance between

acti-vation and degradation is dependent on the actiacti-vation-

activation-temperature as well as trypsin concentration and the two additives, Brij-35 and Ca2+ [22] At 37C, the presence of 0.05% Brij-35 and 10 mm Ca2+ mainly prevented both activation and degradation, whereas a lack of these two compounds resulted in trypsin-induced degradation However, at intermediate concen-trations of Brij-35 and Ca2+, trypsin induced the activation of proMMP-2 Different modes of activa-tion can have implicaactiva-tions for the biochemical proper-ties of the enzymes depending on the cleavage site In the trypsin-activated MMP-2, the N-terminal residue was either Lys87 or Trp90 [22], with the former being identical to the cleavage site generated by human tryp-sin-2 [23] The N-terminal residue was Tyr81 in mem-brane-type1 MMP (MT1-MMP) or APMA-activated enzyme [6] The slightly shorter N-terminus in the trypsin-activated enzyme resulted in reduced catalytic efficiency and weaker tissue inhibitor of metallopro-teinase (TIMP)-1-binding compared to the enzyme activated by MT1-MMP or APMA [22] Docking stud-ies of TIMP-1 revealed that the slightly weaker binding

of the inhibitor to the trypsin-activated MMP-2 could

be attributed to its shorter N-terminus (Lys87⁄ Trp90 versus Tyr81) because Phe83 and Arg86 interacted directly with the inhibitor

Activation through domain specific interactions

A proMMP can be presented to its activator protein-ase by interactions with other proteins or glycosamino-glycans (GAGs) In addition, interactions between a proMMP and other molecules can result in an active MMP without proteolytic processing of the propep-tide, allosteric activation (Fig 2B) It is sufficient that the propeptide is distorted away from the active site, which leaves an open active site that can bind and pro-cess substrates Removal of the binding partner causes

a reversion into an inactive proenzyme Below, we review some of the recent literature that has focused

on the role of various proMMP-binding partners involved in activation

Allosteric activation

Gelatinase interactions with collagen and gelatin Binding of macromolecules or specific thiol-binding reagents to an MMP with an intact or a partially cleaved prodomain can induce enzyme activation despite the presence of the conserved PRCGXPD sequence ProMMP-9 bound to either a gelatin or type

IV collagen-coated surface could cleave a fluorogenic peptide substrate, as well as gelatin, even if the

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prodomain of the enzyme remained intact [24] The

specific activity of the proenzyme bound to the

gelatin-coated surface was approximately 10% of the active

MMP-9 bound to the same surface Furthermore, the

enzymatic activity of both enzyme forms was inhibited

by TIMP-1 with comparable kinetics Similar

observa-tions were made for proMMP-2 The proenzyme could

degrade DQ-gelatin in the presence of low

concentra-tions of the triple-helical domain of the a2 chain of the

microfilamentous collagen VI [25] The above examples

are illustrated in Fig 2B (step 1)

Interactions with small integrin-binding ligand

N-linked glycoprotein (SIBLING)

Individual members of the SIBLING family are known

to bind strongly to both pro- and active forms of

specific MMPs Bone sialoprotein binds MMP-2,

osteopontin binds MMP-3 and dentin matrix protein-1

binds MMP-9, all with a 1 : 1 stoichiometric ratio and

binding constants in the nanomolar range [26] These

SIBLINGs and MMPs are also co-expressed and

colo-calized in salivary glands of humans and mice [27]

The interaction between the SIBLING and its partner

proMMP resulted in an active MMP without

autocata-lytic removal of the propeptide [26] Studies indicated

that binding of a SIBLING to a proMMP induced

large conformational changes in the enzyme,

suggest-ing that the propeptide is physically removed from the

catalytic site, thereby allow substrate binding (Fig 2B,

step 1) Furthermore, the three SIBLINGs have a

ten-to 100-fold higher affinity for the complement

regula-tor facregula-tor H than for their partner MMPs The

proM-MP⁄ SIBLING complex was dissociated in the presence

of factor H and a re-inactivation of the catalytic

activity by the still attached propeptide [26] The same

research group also showed that the amino-terminal

region, especially exon 4, is essential for bone

sialopro-tein-mediated activation of proMMP-2 [28] It appears

that bone sialoprotein also can regulate the activity of

active MMP-2 by modulating the inhibitory effect of

TIMP-2 and synthetic MMP-inhibitors [28,29] The

findings of a recent study challenged the view that

certain SIBLINGs are able to bind and induce

alloste-ric activation of specific MMPs [30]

Interactions between proMMP-9 and neutrophil

gelatinase associated lipocalin

Human neutrophil lipocalin (HNL), also called

neutro-phil gelatinase associated lipocalin, is known to form a

strong reduction sensitive heterodimer with proMMP-9

[31,32] Mercurial compounds such as APMA and

HgCl2 are known to partly activate the 92 kDa proM-MP-9 in several constitutive steps that generate an

83 kDa form of the enzyme with the M75RTPRCGV peptide as the N-terminal sequence [6] Hence, the con-served Cys80 that interacts with the catalytic zinc is not removed (Fig 2B, steps 1a and 2a) Treatment of proMMP-9 with an excess of HNL also induced a partial activation of the proenzyme with an identical N-terminus as the HgCl2 exposed enzyme [33] When the enzyme was activated with a combination of HgCl2 and HNL, this resulted in a fully active enzyme with

an activity comparable to trypsin activated MMP-9 [33] Despite the full activity of the HgCl2 and HNL activated enzyme, this had an N-terminus identical to the HgCl2 activated enzyme (Fig 2B, step 3a) [33], whereas trypsin activation of MMP-9 caused removal

of the entire propeptide, with Phe88 as the N-terminal residue (Fig 2A, steps 1 and 2) [6] Similar results were obtained with isolated proMMP-9 homodimer and proMMP-9⁄ HNL heterodimer when activated with HgCl2 and an excess of HNL By contrast, HNL had

no effect on trypsin-activated MMP-9 Kallikrein is a plasma proteinase that can partially activate

proMMP-9, and the presence of an excess of HNL resulted in a synergistic effect with a 30–50% increase in activity compared to kallikrein activation alone Altogether, this suggested that the N-terminus of the partially acti-vated proenzyme is entrapped in the hydrophobic-binding pocket of HNL and the propeptide–HNL complex is thereby detached from the catalytic site, generating a fully active enzyme without further trun-cation (Fig 2B, step 3a) [33]

Activation by peroxynitrite and glutathione Enzymatic activity of intact proMMPs against physio-logical substrates has also been detected in the pres-ence of peroxynitrite and glutathione (GSH) [34] Examples of this are proMMP-1 and -8 processing of triple helical collagen I, and proMMP-9 processing of gelatin One of the products generated when GSH reacts with peroxynitrite is GSNO2 It was shown that this product most likely activates the proenzymes through S-glutathiolation of the cystein in the con-served PRCGXPD sequence of the propeptide by forming a stable disulfide S-oxide [34] Peroxynitrite can also induce activation of proMMP-2 without loss

of the prodomain This activation appeared to be con-centration-dependent and was attenuated by GSH [35] Other studies have reported activation of proMMP-2

by peroxynitrite, although the activation was followed

by a cleavage of the enzymes prodomain, resulting in

an enzyme with a reduced molecular size [36,37] Thus,

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peroxynitrite as well as GSH along with peroxynitrite

may activate the MMPs by two completely different

mechanisms: one being allosteric and the other

com-prising an autocatalytic removal of the prodomain

Peroxynitrite has also been shown to inactivate

TIMP-1 [38] Thus, it appears that peroxynitrite

poten-tiates MMP activity not only by the direct activation

of proMMPs, but also by preservation of MMP

activity after it is generated There appear to be a

controversy whether GSNO is able to directly induce

activation of MMPs by modulating the conserved Cys

in the enzyme prodomains [39]

Activation through proteolytic removal

of the prodomain

TIMP regulation of MT1-MMP-induced activation

of proMMP-2

MT1-MMP-induced activation of proMMP-2 is a

two-step process involving the MMP inhibitor, TIMP-2,

which has been described in detail in several reviews

Briefly, it has been shown that the TIMP-2 enhancement

of the MT1-MMP-induced activation of proMMP-2 is a

result of the formation of a ternary complex where the

inhibitor acts as a link between the two enzymes In this

complex, the MT1-MMP is inactive as a result of its

interaction with the N-terminal part of TIMP-2,

whereas the C-terminal part of the inhibitor binds to the

HPX domain of proMMP-2 Another MT1-MMP

mol-ecule can now cleave the proMMP-2 in the complex and

generate a 64 kDa inactive intermediate This

intermedi-ate is further autocatalytically processed into the fully

active 62 kDa form of MMP-2 [40,41] The step at

which TIMP-2 is involved when it enhances the

MT1-MMP-induced activation of proMMP-2 has been

questioned because studies have shown that the

inhibi-tor enhances the autoactivation step, but is not

neces-sary for the first cleavage step [42–44] The other

TIMPs, TIMP-1, -3 and -4, can also regulate the

MT1-MMP-induced activation of proMMP-2 [43], where

TIMP-1 only prevents the second step (autoactivation)

and locks the enzyme in an inactive intermediate form

[43,45] These examples demonstrate the complexity of

the MT1-MMP-induced activation of proMMP-2 and

how the activation process can be differently regulated

by various TIMPs

MT-MMP-induced activation of proMMP-2

Other MT-MMPs can also activate proMMP-2,

although this activation does not involve TIMP-2

Both the MT2-MMP and the MT3-MMP-induced

activation of proMMP-2 required a proMMP-2 with

an intact HPX domain [46,47] Both MT3-MMP and proMMP-2 bind to chondroitin sulfate (CS) chains of cell surface proteoglycans (PGs) This interaction enhances the activation of proMMP-2, probably by presenting the gelatinase to its membrane-bound acti-vator [46] Both the catalytic and the hinge region of the MT3-MMP interacted with the CS-chains, whereas proMMP-2 interacted through the HPX domain Furthermore, CS-chains with the sulfate attached to the 4-position of the GAG-chains (C4S) but not to the 6-position (C6S) enhanced the activation in the pres-ence of suboptimal concentrations of MT3-MMP Binding of proMMP-2 to the CS-chains without MT3-MMP did not result in activation The complex interactions of various proteins involved in MT-MMP-induced activation of proMMP-2 are further elucidated

by the involvement of claudins, which are tetraspan membrane proteins MT-MMP mediated proMMP-2 activation was enhanced in the presence of claudin-1, -2, -3 and -5 [48] Claudins not only replaced TIMP-2

in the MT1-MMP-induced activation of proMMP-2, but also enhanced the activation of proMMP-2 by all MT-MMPs Claudin-1 binds to both MT1-MMP and proMMP-2, and this binding appears to involve only the catalytic domains of the two enzymes Another membrane protein shown to enhance MT1-MMP-induced activation of proMMP-2 was avb3 integrin [49–51] MMP-2 binds through its HPX domain to an MT1-MMP-cleaved and activated form of avb3 inte-grin [49–52] This activated inteinte-grin enhanced the sec-ond autocatalytic step of the activation by binding to the 64 kDa intermediate form of MMP-2 [52] Binding and activation of MMP-2 was abrogated in the pres-ence of avb3 integrin-binding macromolecules such as vitronectin and HKa (two-chain high molecular weight kinogen) [50,52,53] Binding of MMP-2 to avb3 inte-grin appears to be controversial because the findings

of another study did not support an interaction between MMP-2⁄ PEX and avb3 integrin [54]

Activation through interactions with elastin, heparin and CD151

ProMMP-2 and active MMP-2 binds to soluble and insoluble elastin through the FnII module of the cata-lytic domain [55] When proMMP-2 binds to insoluble elastin, this induces a fast autoactivation of the proen-zyme followed by inactivation [56] A similar phenom-enon of enhanced autolysis has also been observed when proMMP-2 binds to heparin, although this bind-ing involves the enzymes C-terminal HPX domain [57] These are just two examples of how an interaction of

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the proenzyme with various ECM components

regu-lates the activity of the enzyme

One of the two minimal domain MMPs, proMMP-7,

can also be captured and activated at cell membranes

The proMMP-7 propeptide can interact with the

C-terminal extracellular loop of the transmembrane

protein CD151 [58] The interaction between the

propeptide and CD151 was suggested to induce

confor-mational changes followed by autocatalytic activation

Formation of proMMP-9 dimers affect activation

of the enzyme

MMP-9 is known to form various types of dimers

including homo- and heterodimers that involve the

C-terminal HPX-like domain of the enzyme [31,59–63]

The proMMP-9 monomer is more rapidly activated by

MMP-3 than the homodimer [61] The interaction

between the C-terminal domain of proMMP-9 and a

CSPG core protein has also been shown to affect the

activation of proMMP-9 [64] By contrast to the

9 monomer and homodimer, the

proMMP-9⁄ CSPG complex was not activated by the

organomer-curial compound APMA [64] On the other hand,

Ca2+ which is known to stabilize but not activate

MMPs, induced a concentration independent and

hence intramolecular autoactivation of the proMMP-9

bound to the CSPG The Ca2+-induced activation

resulted in a proteolytic removal of the propeptide

from the complex bound proMMP-9 In the presence

of Ca2+, activated enzyme forms were also released

from the complex This was the result of cleavage of a

part of the PG core protein and at least a part of the

C-terminal HPX domain of proMMP-9, leaving the

hinge region bound to the enzyme [64] A large

reduc-tion of the HPX is likely to alter substrate specificity

because several specific substrate exosites in the HPX

domain may have been removed Only the proMMP-9

in the CSPG complex was activated when Ca2+ was

added to a mixture of purified proMMP-9 and

proM-MP-9⁄ CSPG complex Furthermore, a mixture of

Ca2+ and APMA did not activate the

proMMP-9⁄ CSPG complex [64], although Ca2+ is known to

participate and enhance APMA induced activation of

proMMP-9 [62,65–67]

During hemolysis and⁄ or hemorrhage, Hb is released

into the circulation and⁄ or into surrounding tissues

Heme, the prostetic group of Hb, is released from the

protein and converted to hemin, the Fe3+ oxidation

product of heme During malaria infection, Hb inside

the red blood cells is digested by parasites This results

in the production of the chemically inert crystalline

sub-stance, hemozoin, which is released into the circulation

when the red blood cells burst Hemozoin is indentical

to b-hematin, the synthetic form of hemozoin The HPX domain of proMMP-9 can bind to both hemin and b-hematin, which results in an autocatalytic truncation of parts of the enzyme’s prodomain [68] The truncation in the presence of hemin results in two enzyme forms with Arg17 and Thr64 as N-terminal residues b-hematin induced truncation results in two enzyme forms with Arg42 and Leu54 as new N-terminal residues, with the former identical with the first cleavage

by MMP-1,-2,-3,-7 and -13 [6] These partly truncated forms of MMP-9 are inactive The presence of the hinge region of the enzyme accelerated the truncation process b-hematin, but not hemin, accelerated MMP-3 induced activation to the fully active 82 kDa MMP-9 with Gln89 as N-terminal

Activity regulated through the formation of heterodimers and complexes

Some of the dimers formed with MMP-9 are detected

in SDS⁄ PAGE under nonreducing conditions, but not under reducing conditions Hence, these dimers are reduction sensitive and assumed to be linked through one or several disulphide bridges The formation of different MMP-9 complexes results in altered biochem-ical properties of the enzyme In cells that produce both proMMP-9 and TIMP-1, these two molecules are bound together through their C-terminal domains, and the presence of TIMP-1 affects the activity of the enzyme [69] When proMMP-9 forms a dimer with col-lagenase, binding to TIMP-1 is prevented [70] There are conflicting data concerning whether the proMMP-9 homodimer is able to form a complex with TIMP-1 [59,61,71]

In its heterodimer form with neutrophil gelatinase associated lipocalin, proMMP-9 can bind TIMP-1 and form a ternary complex [72] and the enzyme is pro-tected from degradation [73] Two members of the cystatin family, fetuin-A and cystatin C, bind to MMP-9 and protect the enzyme from autolytic degra-dation [74] The above examples show that there are different ways by which the activity of an MMP can

be regulated and preserved

Both MMP-9 and MMP-2 interact with gelatin as well as collagen through the three FnII-like modules in their catalytic domain [70,75–84] This interaction is important for the ability of these enzymes to degrade these physiological substrates, although it has no effect

on their degradation of several other physiological sub-strates or chromogenic peptide subsub-strates ProMMP-9 forms a complex with one or several CSPG core

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proteins through its HPX domain [64] When

proM-MP-9 is bound to CSPG core proteins, the enzyme

cannot bind gelatin, suggesting that the gelatin-binding

sites in the FnII-like modules of the enzyme are

masked [85] Complex formation involving more than

one domain in the enzyme is likely a result of the high

structural flexibility of the large hinge region The

extreme flexibility of MMP-9 was demonstrated by

atomic force microscopy combined with small-angle

X-ray scattering and analytical ultracentrifugation [86]

The interaction between proMMP-9 and CSPG core

proteins has resulted in changes of several biochemical

properties of the enzyme On this basis, it is tempting

to assume that active MMP-9 still attached to the

CSPG core protein will have altered biochemical

prop-erties compared to unbound active MMP-9 Such

properties may include substrate specificity, catalytic

efficiency and ability to interact with inhibitor

mole-cules, hence giving rise to altered regulation of enzyme

activity

Haptoglobulin (Hp) is a plasma protein mainly

expressed in the liver, and belongs to the family of

acute-phase proteins that is induced during the

inflam-matory process Hp consists of a dimer of ab-chains

covalently linked by disulphide bonds, as well as

oligo-mers [87] Hp have a high affinity for Hb

(Kd= 10)12m), and is considered to be involved in

the clearance of Hb The HPX region of MMP-9 has

been shown to form a strong reduction sensitive

com-plex with Hp [88] Gelatin was reported to bind more

strongly to the proMMP-9⁄ Hp complex than to either

proMMP-9 monomer or homodimer, although the

spe-cific activity against gelatin was similar for the active

MMP-9⁄ Hp complex and the active MMP-9 monomer

Furthermore, binding of proMMP-9 to Hp did not

influence the activation of the enzyme by MMP-3

Binding of MMP-9 to Hp may comprise a method of

regulating MMP-9 activity because Hp is known to

bind cellular receptors followed by internalization and

degradation

Role of exosites in regulation of activity

The complex substrate specificity of individual MMPs

is not only determined by their substrate-binding

sites on each side of the catalytic zinc, but also by

sub-strate-binding to motifs outside this region (exosites)

The role of exosites has been recognized for a long

time for enzymes acting on polymer biomolecules such

as the restriction endonucleases [89], although was not

reported until 1989 for MMPs [90] It was observed

that stored MMP-1 was autocatalytically truncated,

which resulted in a processed enzyme lacking the

C-terminal HPX domain This truncated enzyme was

no longer able to cleave triple helical collagen I, but was able to degrade gelatin (denatured collagen) The HPX region was also found to be necessary for the cleavage

of the triple helical region in interstitial collagen by other collagendegrading MMPs (MMP2, 8, 13 and -14) [91–95] The active site region in the MMPs is too narrow (5 A˚) to allow a triple helical collagen (15 A˚) to enter the active site The HPX region in the collagenases locally unwinds the triple helical collagen, and then a single a-chain can enter the catalytic site and be cleaved [96] In addition, it was shown that a small segment in the catalytic domain, R183WTNNFREY191, is necessary for the enzymes ability to cleave triple helical collagen [96] Production of MMP-3⁄ MMP-1 chimeras revealed that additional unique structural elements in the cata-lytic domain are involved

In the two gelatinases, MMP-2 and MMP-9, the FnII-like repeats in the catalytic site of the enzymes can interact with elastin, type I, III, IV, V, X and XI collagens, as well as gelatins This may facilitate the localization of these enzymes to connective tissue matrices This interaction appears to be of importance for the degradation of macromolecules such as elastin, gelatin and collagens IV, V and XI, but does not influ-ence the degradation of chromogenic substrates or other macromolecules [70,75–84] Hence, the FnII-like module in the gelatinases contains important exosites for the degradation of some substrates

Many potent small molecule MMP inhibitors (MMPIs) have been entered into clinical trials for can-cer treatment, although most of them have been dis-continued as a result of a lack of specificity and selectivity Successful cancer therapy based on MMPIs must not only be selective against MMPs validated as targets, but also spare MMPs validated as antitargets [97,98] To develop new therapeutic MMPIs, it is of pivotal importance to understand the structural basis

of recognition, binding and cleavage of substrates, as well as the recognition and binding of natural inhibi-tors (TIMPs) Recent data indicate that subtype spe-cific inhibitors may also lead to new treatment of acute and chronic inflammatory and vascular diseases [99] Most known MMPIs are targeting the catalytic region and the catalytic zinc, which are very similar between the MMPs Designing specific small molecular MMPIs targeting the catalytic site is therefore prob-lematic [99] MMPIs targeting less conserved binding sites outside the prime subsites of MMPs are consid-ered to be more specific Within the MMP family, dis-tinct preferences for collagen types are seen, which must reflect structural differences in MMP collagen-binding [100] Exosites are considered to be important

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determinants for these differences in specificity by

introducing contact regions between the substrate and

the MMP outside the primary specificity subsites

Exo-sites are regarded as novel binding Exo-sites that represent

unique opportunities for designing subtype selective

inhibitors Efforts have been put into both high

throughput screening [101] and the design of inhibitors

targeting exosites without interfering with the catalytic

zinc [8] Such inhibitors are considered to act

selec-tively against the degradation of a specific substrate,

and represent a novel therapeutic approach with

puta-tive reduced side effects

Binding of the collagen triple helix is necessary for

collagenolysis Some studies have taken advantage of

potential substrate exosites in MMP-2 and MMP-9

collagenolytic behaviour by designing triple helical

substrate and triple helical transition state analogues

One such study indentified inhibitors with high

selec-tivity for the gelatinases (MMP2- and MMP-9)

com-pared to other MMPs [102] Furthermore, the FnII

insert of MMP-9 was suggested to contain exosites

involved in the binding of type V collagen model

sub-strates and inhibitors A triple helical peptide that

incorporates an FnII insert-binding sequence was

con-structed and found to give selective inhibition of

MMP-9 type V collagen-based activity [103]

Exosites related to collagenolysis have also been

iden-tified in the active site cleft [104] and the catalytic

domain [105] of MMP-1, and were also suggested in

analogous regions of MMP-8 and MMP-13 [106]

Recently, a highly selective MMP-13 inhibitor was

reported that did not chelate the catalytic zinc, but

instead bound in the S1¢ pocket [107] This structural

region shows diversity among MMPs A recent study

has further elucidated the role of the specificity loop for

selective MMP-13 inhibition by indentifying the steric

requirements for binding to this region [108] Other

studies have also described selective MMP-13 inhibitors

that do not interfere with the catalytic zinc [101,109]

Regulation of activity through

compartmentalization

Through their motifs and modules, the secreted MMPs

are directed to various compartments in the

extracellu-lar environment as well as to cell membranes Among

their binding partners in these compartments are

colla-gens, laminins, fibronectin, elastin, core proteins and

GAG-chains of PGs This compartmentalization

regu-lates the MMP activity by locating and concentrating

them close to or on potential substrates The

interac-tion with their binding partners varies in strength,

which has implications for the ability to extract a given

enzyme from a tissue Examples are the binding of MMP-1, -2, -7, -8, -9 and -13 to heparin and heparan sulfate [57,72,110–117], where the interaction with hep-arin occurs through the HPX domain of MMP-1, -2 and 9 [110,112,116] MMP-7 lacks the HPX domain and interacts through the catalytic and the prodomain This MMP binds much stronger to the GAG-chains than the other MMPs [117] MMP-7 could be extracted from tissues by heparinase digestion or by using extraction buffer containing heparin, heparan sulfate or protamin [117] Similarily, it was necessary

to use various extraction conditions to quantify the amount of gelatinases in mouse kidneys [118] Binding

of secreted MMPs to cell membranes is another way

of regulating their activity This may lead to the acti-vation of the enzymes, as discussed above, and pro-mote cell migration and cell invasion through basement membranes and tissues Binding of MMPs to cell membranes may also activate intracellular signal-ing cascades, an effect independent of their proteolytic activities [119–123] Cell surface associated enzymes can also be internalized and either directed to the lyso-zymes for destruction or be a source of intracellular activity An emerging concept in MMP regulation is their intra⁄ extracellular location because both secreted and membrane bound MMPs have been found local-ized to various intracellular sites In the following part

of present minireview, we focus on the subcellular location, processing of intracellular substrates and putative physiological relevance of this activity

Nuclear localization MMP-2, -3, -9, -13 and MT1-MMP have been demon-strated in the nucleus of various cell types, including heart myocytes, brain neurons, endothelial cells, fibro-blast and hepatocytes The mechanisms of nuclear translocation of the different MMPs are generally poorly characterized MMP-2 has a typical nuclear localization sequence close to the C-terminus that might be involved in the nuclear localization [124]

A nuclear signaling sequence is also found in the cata-lytic domain of MMP-3, which appeared to be essen-tial for the translocation to the nucleus Full-length MMP-3 was absent from the nucleus, suggesting that processing is required to expose the nuclear localiza-tion signal for nuclear transport [125] For MT1-MMP, a caveolae-mediated endocytosis has been sug-gested as a mechanism of internalization and nuclear translocation as a result of the colocalization of caveo-lin-1 and MT1-MMP in perinuclear regions [126] Nuclear localization of MMPs has been associated with apoptosis in several studies Increased nuclear

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gelatinolytic activity, colocalized with MMP-2, has

been demonstrated in pulmonary endothelial cells

undergoing apoptosis MMP-2 activation in these cells

was suggested to be induced by reactive oxygen and

nitrogen species produced by cigarette smoke [127]

In-tranuclear gelatinolytic activity has also been observed

in rat brain neurons after post-ischemic reperfusion,

and this activity was associated with DNA

fragmenta-tion Furthermore, this gelatinolytic activity colocalized

with MMP-2 and MMP-9, and was reported to be

markedly reduced in the presence of a general MMP

inhibitor or by MMP-2 and MMP-9 antibodies

MT1-MMP as well as furin, a MT1-MT1-MMP activator, was also

found in the nucleus of the ischemic rat brain neurons,

suggesting a possible mechanism for intracellular

acti-vation of MMP-2 by MT1-MMP [128]

In both cardiac myocytes and pulmonary endothelial

cells, as well as in brain neuronal cells, nuclear

gelatin-olytic activity is correlated with the processing of two

important factors in the DNA repair machinery (i.e

the DNA repair enzyme poly-ADP-ribose polymerase

and X-ray cross-complementary factor 1, which protect

cells from apoptosis) These two factors were shown to

be processed by MMP-2 and MMP-9 [124,128] Thus,

nuclear MMP activity may contribute to the apoptotic

process after ischemic injuries by processing

poly-ADP-ribose polymerase and X-ray

cross-complemen-tary factor 1 and hence interfere with the oxidative

DNA repair system [128] In addition to MMP-2 and

MMP-9, expression of active MMP-13 was also

increased in the nucleus of neural cells after cerebral

ischemia in both rats and humans The nuclear

trans-location of MMP-13 was promoted by oxygen and

glucose deprivation in the cells following ischemia,

although the biological relevance of this is not known

[129]

Active MMP-3 in the nuclei of chondrocytic cells in

culture and in nuclei of normal and osteoarthritic

chondrocytes in vivo has been shown to be involved in

transcriptional gene regulation [130] Nuclear MMP-3

bound to a transcription enhancer sequence

(TREN-DIC) in the connective tissue growth factor

(CCN2⁄ CTGF) promoter and activated transcription

of CCN2⁄ CTGF This growth factor promotes

physio-logical chondrocytic proliferation and ECM formation

Pro- and active MMP-3 could activate the

CCN2⁄ CTGF promoter, where various domains of the

MMP participated in the activation Both the HPX

and the Cat-Hinge regions activated the promoter,

whereas the prodomain and the hinge-region alone

had no effect on the activation Compared to the

wild-type MMP-3, lower promoter activation occurred in

the presence of catalytically dead MMP-3 mutants

This suggested that MMP-3 can regulate the CCN2⁄ CTGF promoter activity by two completely dif-ferent mechanisms One involves proteolytic processing

of one or several nuclear proteins, whereas the other is independent of the processing capacity of the protein-ase and involves the HPX domain A DNA-binding domain was found in the HPX domain, as an anti-MMP-3 HPX antibody blocked the protein-DNA interactions The hinge region contains proline-rich sequences found in some transcription factors The properties of MMP-3 as a transcription factor was evaluated by analyzing nuclear MMP-3 associated pro-teins (NuMAPs) Several NuMAPs were detected, such

as heterochromatin proteins, transcription co-activators⁄ corepressors, RNA polymerase II and nucleosome⁄ chromatin assembly protein One of the NuMAPs, HP1c, was demonstrated to interact with MMP-3 and to co-activate the CCN2⁄ CTGF promoter with MMP-3 Another identified NuMAP was the transcription repressor NCoR1, suggesting that MMP-3 might degrade NCoR1 to prevent transcription repression of the CCN2⁄ CTGF promoter [130]

Cytosolic and vesicle localization

A study on dopaminergic neurons suggested a pro-apoptotic role of active intracellular MMP-3 During apoptosis, the proform of MMP-3 was cleaved to a catalytically active form (48 kDa) by a serine protein-ase [131] Lack of intracellular MMP-3 activity pro-tected the dopaminergic cells from apoptosis Inhibition of the MMP-3 activity attenuated the activation of caspase-3, the executioner enzyme in apoptosis

By contrast to the apoptosis-promoting effects of cytosolic MMP-3 and the MMPs localized in the nucleus, perinuclear MMP-1 appeared to prevent apoptosis [132] Intracellular MMP-1 has been demon-strated in various cell types, including glia cells, epithe-lial cells and fibroblasts At an early state of apoptosis, both the pro- (57 kDa) and the active (45 kDa) forms

of MMP-1 colocalized with mitochondria that clus-tered around the nucleus At later stages, it accumu-lated around the nucleus and nuclear fragments, suggesting a possible role in the breakdown of the nuclear envelope Furthermore, the intracellular levels

of MMP-1 varied with cell cycle progression and were highest during the M phase These observations sug-gest that intracellular association of MMP-1 to mito-chondria and nuclei have implications for the control

of cell growth, and may contribute to the well-known association of this enzyme with tumor cell survival and spreading [133,134]

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