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and processing of mast cell secretory granule components Frida Henningsson*, Sonja Hergeth*, Robert Cortelius, Magnus A˚ brink and Gunnar Pejler Swedish University of Agricultural Scienc

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and processing of mast cell secretory granule components Frida Henningsson*, Sonja Hergeth*, Robert Cortelius, Magnus A˚ brink and Gunnar Pejler

Swedish University of Agricultural Sciences, Department of Molecular Biosciences, The Biomedical Center, Uppsala, Sweden

Mast cells (MCs) are characterized by their large

con-tent of electron-dense secretory granules, and these

granules are released following MC activation, a

pro-cess that can be accomplished by various mechanisms,

including antigen-mediated crosslinking of

surface-associated IgE and exposure to neuropeptides,

anaphy-latoxins or calcium ionophores [1,2] The MC granules

contain a broad array of bioactive compounds, with

the exact composition being dependent on the

partic-ular species and subclass of MC [1,3] Histamine is a

major constituent of all types of MC, and it is now

well recognized that MC granules can contain a

num-ber of different cytokines, such as tumor necrosis

factor-a, interleukin (IL)-4, IL-5, IL-13, transforming

growth factor-b and vascular endothelial growth factor

[2] Moreover, the MC granules contain b-hexosamini-dase and a number of MC-specific neutral proteases: chymases, tryptases and carboxypeptidase A (CPA) [4,5] In addition, MC granules contain large amounts

of highly sulfated and thereby negatively charged pro-teoglycans (PGs) of the serglycin (SG) type, and it is these PGs that give the typical metachromatic staining

of MCs with cationic dyes [6] In MCs, SG PGs can accommodate either (or both) chondroitin sulfate or heparin side chains, depending on MC subclass [7] The processes involved in MC degranulation, in par-ticular the signal transduction pathways, have been the subject of intense investigation [8,9] In contrast, strik-ingly little is known regarding the actual formation of

MC secretory granules For example, the factors that

Keywords

mast cells; proteases; proteoglycans;

serglycin; sorting

Correspondence

G Pejler, Swedish University of Agricultural

Sciences, Department of Molecular

Biosciences, The Biomedical Center,

Box 575, 751 23 Uppsala, Sweden

Fax: +46 18 550762

Tel: +46 18 4714090

E-mail: Gunnar.Pejler@bmc.uu.se

*These authors contributed equally to this

work

(Received 28 June 2006, revised 15 August

2006, accepted 4 September 2006)

doi:10.1111/j.1742-4658.2006.05489.x

In the absence of serglycin proteoglycans, connective tissue-type mast cells fail to assemble mature metachromatic secretory granules, and this is accompanied by a markedly reduced ability to store neutral proteases However, the mechanisms behind these phenomena are not known In this study, we addressed these issues by studying the functionality and morphol-ogy of secretory granules as well as the fate of the secretory granule prote-ases in bone marrow-derived mast cells from serglycin+⁄ +and serglycin–⁄ – mice We show that functional secretory vesicles are formed in both the presence and absence of serglycin, but that dense core formation is defect-ive in serglycin–⁄ – mast cell granules The low levels of mast cell proteases present in serglycin–⁄ – cells had a granular location, as judged by immu-nohistochemistry, and were released following exposure to calcium iono-phore, indicating that they were correctly targeted into secretory granules even in the absence of serglycin In the absence of serglycin, the fates of the serglycin-dependent proteases differed, including preferential degrada-tion, exocytosis or defective intracellular processing In contrast, b-hexosa-minidase storage and release was not dependent on serglycin Together, these findings indicate that the reduced amounts of neutral proteases in the absence of serglycin is not caused by missorting into the constitutive path-way of secretion, but rather that serglycin may be involved in the retention

of the proteases after their entry into secretory vesicles

Abbreviations

BMMC, bone marrow-derived mast cell; CPA, carboxypeptidase A; MC, mast cell; mMCP, mouse mast cell protease; PG, proteoglycan;

SG, serglycin; TEM, transmission electron microscopy.

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determine the sorting of granular components are

lar-gely undefined, and the mechanisms that lead to the

assembly of the electron-dense, metachromatically

staining granules seen in mature MCs have been

poorly investigated In a recent study, we generated a

mouse strain in which the SG gene was targeted [10]

We found that, in the absence of SG, mature

metach-romatically staining granules were not observed

Fur-thermore, we noted that storage, but not mRNA

expression, of the various MC proteases was

dramatic-ally defective in SG–⁄ – MCs However, the underlying

mechanisms behind these observations were not

defined The aim of this study was therefore to provide

insights into this issue by determining the fate of

SG-dependent proteases in cells with an inactivated SG

gene Our results are compatible with a model of

secre-tory granule maturation in which SG PG is not

involved in the transport of compounds into secretory

vesicles, but is essential for retention of certain

constit-uents after their entry into the granules

Results

This study was undertaken to resolve the mechanism

behind the previously observed severe granule defects in

SG–⁄ – MCs [10] Given the dramatic effects of the SG

knockout on granular staining properties and storage of

proteases, it was first important to determine whether

the lack of SG affected the actual assembly of granules

and whether secretory granules were also functional in

the absence of SG To this end, bone marrow cells

were recovered from SG+⁄ +and SG–⁄ –mice and were

in vitrodifferentiated into mature bone marrow-derived

MCs (BMMCs) by culturing in medium containing IL-3

[11,12] Cells were recovered at various stages of cellular

differentiation, and their morphology was examined

after staining with May–Gru¨nwald ⁄ Giemsa At day 0,

as expected, no cells with an MC-like appearance were

observed Starting from day 5, cells containing ‘empty’

(May–Gru¨nwald ⁄ Giemsa-negative) vesicles were

observed Such vesicles were seen both in SG+⁄ +and

SG–⁄ – cells, indicating that their formation was not

dependent on SG When the cells were cultured further,

the number of May–Gru¨nwald ⁄ Giemsa-negative

vesi-cles gradually decreased in both SG+⁄ +and SG–⁄ –cells

This was accompanied by the appearance, from about

day 12, of May–Gru¨nwald ⁄ Giemsa-positive granular

structures in SG+⁄ + cells A gradual increase in

May–Gru¨nwald ⁄ Giemsa staining was seen over time in

SG+⁄ +cells In contrast, May–Gru¨nwald ⁄

Giemsa-pos-itive vesicles were not seen in SG–⁄ –cells at any stage of

differentiation (not shown) These results are in

agree-ment with those of a previous study [10]

One potential explanation for the lack of May– Gru¨nwald ⁄ Giemsa-negative vesicles in SG–⁄ – cells at later stages of differentiation could be that immature granules are generated in the absence of SG, but that the lack of SG causes their disruption Alternatively, secretory granules could be present at late stages of maturation also in SG– ⁄ – cells, but not be visible by conventional microscopy To provide further insights into this issue, we examined the cells at the ultrastruc-tural level by transmission electron microscopy (TEM) The TEM analysis indeed revealed the existence of secretory granule-like organelles in SG–⁄ – cells, and these organelles were found in approximately equal numbers as in SG+⁄ + cells (Fig 1; upper panels) However, the morphology of the granules was differ-ent; whereas dense core formation was seen in SG+⁄ + granules, the contents of the SG–⁄ – granule were of more amorphous character, without defined electron-dense cores (Fig 1; lower panels)

To address whether the secretory granules were functional, we measured the ability of the MCs to release b-hexosaminidase, a granule component, upon exposure to calcium ionophore A23187 As shown in Fig 2A, equal amounts of b-hexosaminidase were released by SG+⁄ +and SG–⁄ –cells after calcium iono-phore stimulation, and the kinetics of release were sim-ilar Furthermore, the levels of b-hexosaminidase in conditioned medium from nonstimulated cells were similar in cultures of both genotypes (Fig 2A), indica-ting that the lack of SG PG did not result in increased spontaneous release of b-hexosaminidase These find-ings indicate that the general ability of MCs to degran-ulate is not dependent on SG Experiments were also undertaken to investigate whether the level of stored b-hexosaminidase is influenced by SG Although b-hexosaminidase activity was already detected at day

0, the intracellular content of this enzyme increased markedly after 6 days of culture, and reached a plat-eau from about day 12 (Fig 2B) Both the kinetics of accumulation and the level of maximal storage were virtually identical in SG+⁄ + and SG–⁄ – cells, indica-ting that the storage of b-hexosaminidase is independ-ent of SG

The results above indicate that functional MC secre-tory granules are formed independently of SG PG Hence, the defective storage of MC proteases in the absence of SG [10] is not due to defects in the forma-tion or funcforma-tionality of granular compartments In order to understand the mechanism by which SG PG promotes storage of these compounds, the strategy in the next set of experiments was to follow the fates

of the SG-dependent proteases when SG was absent

To address these issues, we examined the expression,

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cellular storage, processing and secretion of SG and of

various MC proteases at different stages of MC

differ-entiation, as described below

SG core protein transcript was already clearly

detectable at day 0, but the level of transcript appeared

to increase after5 days of culture (Fig 3A) In

con-trast, no detectable mRNA for mouse MC protease 5

(mMCP-5; a chymase), the tryptase mMCP-6 or CPA

was detected at day 0 Starting from day 5, however,

mMCP-6 and CPA transcripts were clearly detected,

and they appeared to increase further after 12 days of

culture The onset of mMCP-5 mRNA expression was

somewhat delayed, with clearly detectable transcript

being seen from day 12 mMCP-5, mMCP-6 and CPA

transcripts were detected in both SG+⁄ + and SG–⁄ –

cells, and the kinetics as regards onset of mRNA

expression were similar in both genotypes, indicating

that the knockout of SG does not affect cellular

differ-entiation into MCs, as judged by the transcription of

the MC protease genes

Further experiments were carried out to examine

how the mRNA expression profiles of SG+⁄ + and

SG–⁄ –cells were reflected at the protein level (Fig 3B) Immunoblot analysis of SG+⁄ + cell extracts showed that neither of the MC proteases were present at day

0 mMCP-5 protein was detected starting from day 12, i.e at the same time as when gene transcription was first seen mMCP-5 protein accumulated over time, with a plateau of maximal storage seen after 26 days

of culture mMCP-6 storage showed similar kinetics as for mMCP-5 In contrast, CPA protein was detected

as early as after 5 days of culture, and a maximal plat-eau of storage was already seen at day 12 Both pro-CPA and mature pro-CPA were detected in SG+⁄ +cells

A dramatically different pattern was seen in SG–⁄ – cells mMCP-5 protein was not detected at any time point, and mMCP-6 protein, although being detect-able, was present at markedly lower levels than in

SG+⁄ + cells Notably, however, mMCP-6 accumula-tion in SG–⁄ – cells showed similar kinetics as in

SG+⁄ + cells In contrast, the total amounts of CPA antigen (pro-CPA + mature CPA) were approximately equal in SG– ⁄ – and SG+ ⁄ + cells An interesting observation was that only the pro-form of CPA was

Fig 1 Transmission electron micrographs The upper panels show representative mature (5 weeks of culture) bone marrow-derived mast cells (BMMCs) from serglycin (SG)+⁄ +and SG–⁄ –mice (original magnification 5000·) The lower panels show enlarged granules (original magnification · 40 000).

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detected in SG–⁄ – cells, indicating that pro-CPA

processing into mature protease is strongly dependent

on SG A plausible explanation for this finding is that

the protease(s) that are responsible for the pro-CPA

processing is dependent on SG In agreement with

such a notion, we showed recently that pro-CPA

processing was defective in cathepsin E–⁄ – MCs and

that the storage of cathepsin E in MCs is dependent

on heparin PG [13] Thus, a likely explanation for the

defective pro-CPA processing in SG–⁄ –MCs is that the

lack of SG also results in defective cathepsin E storage

and that this, in turn, results in defective pro-CPA

processing, leading to an accumulation of pro-CPA

Next, we investigated the possibility that the

pro-teases were constitutively secreted in the absence of

SG PG Conditioned media were collected at different stages of MC differentiation, and were analyzed for the presence of secreted MC proteases As shown in Fig 3C, mMCP-5 protein was present at low levels

in conditioned medium from SG+⁄ + cells after prolonged culture, but was absent in medium from

SG– ⁄ – cells In contrast, mMCP-6 protein was clearly detected, starting from about day 14, in conditioned medium from both SG+⁄ +and SG–⁄ – cells CPA, pre-dominantly in its mature form, was secreted into the medium by SG+⁄ + cells, starting at about day 5 In contrast, only the pro-form of CPA was secreted by

SG–⁄ –cells The total level of secreted CPA (pro-CPA and mature CPA) was somewhat higher in medium from SG–⁄ –than in that from SG+⁄ +MCs, in partic-ular at early time points (Fig 3C) Note that, at early time points, pro-CPA dominated over mature protease, both intracellularly (Fig 3B; day 5) and in conditioned medium from SG+⁄ + cells (Fig 3C; days 6 and 12), indicating that efficient processing of pro-CPA is dependent on the degree of MC maturation In accord-ance with this notion, only the mature form of CPA is detected in fully mature connective tissue-type MCs recovered in vivo [13], and only the pro-form of CPA

is detected in poorly differentiated transformed cell lines of MC origin (M Grujic & G Pejler, unpub-lished results)

The results above indicate that mMCP-6 and pro-CPA are secreted by SG–⁄ – MCs A possible explan-ation for these findings would be that the absence of

SG causes missorting of mMCP-6 and pro-CPA into the constitutive rather than into the regulated pathway

of secretion If indeed this were the case, mMCP-6 and pro-CPA would not be present in the secretory gran-ules, and exposure of SG–⁄ – cells to MC-degranulating agents would not cause increased release of mMCP-6 and pro-CPA If, on the other hand, mMCP-6 and pro-CPA are in fact located in secretory granules also

in SG–⁄ –cells, MC degranulation would be expected to induce their release In order to address these possibil-ities, SG+⁄ +and SG–⁄ –MCs were exposed to the cal-cium ionophore A23187, a compound that is regularly used as an MC secretagogue [14] As shown in Fig 4A, exposure of SG+⁄ + cells to A23187 resulted

in clearly detectable mMCP-6 and CPA in conditioned medium Strikingly, calcium ionophore stimulation also resulted in the release of mMCP-6 and pro-CPA

by SG–⁄ – cells (Fig 4A) The implication of these find-ings is that mMCP-6 and pro-CPA are sorted into releasable secretory vesicles despite the absence of SG

To obtain further evidence for this, SG–⁄ – cells were stained for mMCP-6 antigen, before and after expo-sure to calcium ionophore In resting SG–⁄ – cells,

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+/+ non-stim +/+ A23187 -/- non-stim -/- A23187

A

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Days of culture

+/+

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Fig 2 b-Hexosaminidase content and release (A) Conditioned

media from mature (5 weeks of culture) serglycin (SG)+⁄ + (filled

symbols) and SG – ⁄ – (open symbols) cells were analyzed for

b-hex-osaminidase activity, without stimulation (squares) or after addition

of A23187 (circles) (B) SG+⁄ + (filled squares) and SG–⁄ – (open

squares) cells taken at different stages (days 0–33) of

differenti-ation in interleukin (IL)-3-containing medium were analyzed for total

intracellular b-hexosaminidase activity Results are expressed as

percentages, where the b-hexosaminidase content in SG + ⁄ + cells

at day 33 is set as 100% Results are expressed as means of

tripli-cate determinations ± SD.

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mMCP-6 was found in granule-like compartments

close to the plasma membrane (Fig 4C), indeed

sup-porting the idea that mMCP-6 is transported into

secretory granules even in the absence of SG PG

Fur-thermore, after exposure to A23187, SG–⁄ – cells

showed signs of degranulation and it was also evident

that the released granules stained positively for

mMCP-6 (Fig 4C) Preimmune serum gave only

dif-fuse overall staining of SG–⁄ –cells and a total absence

of granular staining of either unstimulated or

A23187-stimulated cells (Fig 4C)

Next, we investigated the possibility that the MC proteases are subjected to degradation by lysosomal proteases when SG PG is absent For this purpose, cells were incubated with NH4Cl in order to raise the

pH of acidic intracellular compartments, including lysosomes and secretory granules, and thereby inacti-vate lysosomal proteases Incubation of SG–⁄ – MCs with NH4Cl did not affect the level of intracellular mMCP-6, indicating that degradation by lysosomal mechanisms is not a primary fate of mMCP-6 when

SG is absent (Fig 5) In contrast, NH4Cl caused an

SG

mMCP-6 mMCP-5

CPA HPRT

0 5 12 19 26 33 0 5 12 19 26 33

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mMCP-6

mMCP-5

pro-CPA

CPA

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CPA

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Fig 3 mRNA expression and protein analysis (A) Total RNA was prepared from serglycin (SG)+⁄ +and SG–⁄ –bone marrow-derived cells after different durations (days 0–33) of culture in medium containing interleukin (IL)-3 The RNA was used for analysis of the expression of mouse mast cell protease (mMCP)-5, mMCP-6, carboxypeptidase A (CPA) and SG by RT-PCR Expression of hypoxanthine–guanine phopho-ribosyltransferase was used as housekeeping control (B) Cell extracts were prepared from cells taken at various stages (days 0–33) of differ-entiation and were subjected to immunoblot analysis using antisera towards mMCP-5, mMCP-6 and CPA (C) Secretion of MC proteases from SG + ⁄ + and SG – ⁄ – cells Conditioned media were recovered from SG + ⁄ + and SG – ⁄ – cells at various stages (days 0–33) of differentiation

in IL-3-containing medium The media were concentrated and subjected to immunoblot analysis for mMCP-5, mMCP-6 and CPA The results shown are representative of three independent experiments.

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accumulation of mMCP-5 protein in SG–⁄ – cells,

whereas mMCP-5 levels were not affected in SG+⁄ +

MCs (Fig 5; upper panel) This indicates that

mMCP-5, in the absence of SG, is degraded by proteases with

low pH optima, possibly in lysosomal compartments

Interestingly, several ‘lysosomal’ proteases, e.g

cathep-sin C, cathepcathep-sin D and cathepcathep-sin E, have been found

not only in lysosomes but also in MC secretory

gran-ules [13,15,16] Thus, the degradation of mMCP-5 does

not necessarily have to involve transport to lysosomes,

but could in fact occur within the secretory granule

compartment NH4Cl did not cause any noticeable

accumulation of pro-CPA or mature CPA in either

SG+ ⁄ + or SG– ⁄ – MCs However, the NH4Cl

treat-ment resulted in the accumulation of an intermediate

form of CPA, of somewhat lower molecular weight than pro-CPA (Fig 5; lower panel) Most likely, this compound represents an intermediate in processing These findings indicate that the processing of pro-CPA occurs in (at least) two steps, and that the processing

of the intermediate form of CPA to mature protease is dependent on a (lysosomal?) protease with an acidic

pH optimum Control experiments showed that NH4Cl did not affect cellular viability (not shown)

Degradation by the proteasome pathway could con-stitute an alternative degradative pathway in the absence of SG However, incubation of cells with lac-tacystin, an inhibitor of proteasome function, did not cause any accumulation of MC proteases in SG– ⁄ –

MCs (not shown)

C

Fig 4 Protease release after mast cell (MC) degranulation Serglycin (SG)+⁄ +and SG–⁄ – MCs (after 5 weeks of culture) were treated with calcium ionophore A23187 (A) Medium fractions from SG+⁄ +and SG–⁄ –cells were subjected to immunoblot analysis using anti-sera towards carboxypeptidase A (CPA) and mouse mast cell protease (mMCP)-6 Note the increase in extracellular mMCP-6 and CPA antigen, in both SG + ⁄ + and SG – ⁄ – cul-tures, after stimulation with A23187 (B) Cell fractions from SG+⁄ +and SG–⁄ –cells were analyzed for mMCP-6 and CPA by immuno-blotting (C) Cytospin slides were prepared from nontreated and A23187-treated SG–⁄ – cells and were immunohistochemically stained for the presence of mMCP-6 anti-gen Note the granular staining for mMCP-6, both before and after A23187 stimulation The results shown are representative of three independent experiments.

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As shown in Fig 3A, SG core protein mRNA was

already expressed at day 0 However, maximal MC

protease accumulation was not obtained until about

day 26 (Fig 3B), a finding that may appear

contradict-ory, considering the strong dependence of the MC

pro-teases on SG for storage This indicates that the levels

of stored proteases are not directly related to the

amount of SG core protein mRNA being expressed

One potential explanation could be that the amount of

actual sulfated PGs is not directly correlated with the

level of SG mRNA, and it was therefore of interest to

also follow the levels of sulfated PGs during the course

of MC differentiation To this end, SG+⁄ + MCs at

different stages of differentiation were biosynthetically

labeled with 35SO42– 35S-labeled PGs were recovered

both from conditioned medium (secreted PGs) and

from cell extracts, and were quantified As shown in

Fig 6A, the levels of secreted PGs were similar at all

time points tested In contrast, the levels of

intracellu-lar PGs increased markedly over time Notably, the

level of intracellular PGs did not reach a plateau, as

observed for the proteases (Fig 3B) Rather, the level

of cell-associated PGs showed a continuous increase

over time (Fig 6A) Notably, the latter is in good

agreement with the relatively late appearance of May–

Gru¨nwald ⁄ Giemsa-positive granules as compared to

the onset of SG mRNA expression (see above)

Next, the possibility that the different abilities of MCs to store proteases at different stages of differenti-ation could be due to differences in the electrostatic charge of the PGs was addressed For this purpose,

MC PGs recovered at different time points during the course of MC development were examined by anion exchange chromatography At early time points (day 10), there was a distinction between two separate PG populations, one with low anionic charge density [coeluting with standard chondroitin sulphate A (CS-A)] and one population with a markedly higher charge (coeluting with standard pig mucosal heparin) (Fig 6B) Similar elution profiles were seen for PGs recovered from the cell layer and from conditioned medium In contrast, only highly charged PGs were seen at day 23 (Fig 6B) and day 34 (not shown), again with similar charge densities being displayed by cell-associated and extracellular PGs Together, these results indicate that the MC maturation process is associated with both increased total synthesis of sulfated PGs and increased charge density of the synthesized PGs

Discussion

Although the knockout of both SG [10] and N-de-acetylase⁄ N-sulfotransferase-2 [17,18], the latter being

an enzyme involved in the sulfation of heparin chains attached to the SG core protein, has provided strong evidence for a crucial role of PGs in mediating the storage of secretory granule compounds in MCs, the mechanism behind these observations has not been established One potential mechanism would be that

SG is important for the formation of the secretory granule However, we show here that SG–⁄ –MCs also displayed clearly discernible secretory vesicle-like struc-tures By conventional microscopy, such vesicles were May–Gru¨nwald ⁄ Giemsa-negative and, interestingly, May–Gru¨nwald ⁄ Giemsa-negative vesicles were also seen in SG+⁄ + cells at early stages of differentiation Most likely, these structures represent immature secre-tory granules in which the PG content is too low to stain with May–Gru¨nwald ⁄ Giemsa In accordance with this, it was observed that the intracellular content of highly sulfated PGs was relatively low at the corres-ponding (early) time point At later stages of differenti-ation, in contrast, SG+⁄ + MCs showed staining with May–Gru¨nwald ⁄ Giemsa, and this correlated well with

a marked increase in the recovery of highly sulfated intracellular PGs

The presence of secretory vesicle-like structures in

SG–⁄ – cells was also supported at the ultrastructural level TEM analysis showed the presence of highly elec-tron-dense granules in SG+⁄ + cells, but also showed

Fig 5 Inhibition of lysosomal proteases Serglycin (SG)+⁄ + and

SG – ⁄ – cells (after 5 weeks of culture) were incubated for 6 h with

20 m M NH4Cl, or for 20 h with 5 m M NH4Cl Cell extracts were

subsequently subjected to immunoblot analysis using antisera

towards carboxypeptidase A (CPA) and mouse mast cell protease

(mMCP)-6 The arrow indicates a ‘semiprocessed’ form of CPA.

The results shown are representative of three independent

experi-ments.

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an abundance of granule-like organelles in SG–⁄ –cells.

Importantly, however, the granule matrix in SG–⁄ –cells

was more amorphous than in SG+⁄ +cells, and showed

less defined dense core formation Our results also

pro-vide epro-vidence that SG–⁄ – cells retain the full capability

to undergo stimulus-induced degranulation, as

deter-mined by the ability to release b-hexosaminidase in

response to calcium ionophore Together, our data thus

indicate that SG PG is not necessary for the formation

of MC secretory granules, and nor is SG involved in

mechanisms of degranulation

Another possible explanation for the storage defects

seen in SG–⁄ –MCs would be that SG PG is needed for

correct intracellular sorting of the MC proteases into

the secretory granules, the alternative fate being secre-tion by the constitutive pathway If this was the case,

it would be expected that SG-binding compounds such

as the MC proteases would be preferentially released into the extracellular space by SG–⁄ – MCs Such mis-sorting would result in excessive accumulation of granule compounds in conditioned medium from

SG–⁄ –cells We here provide evidence that CPA, in its pro-form, is secreted at higher levels by SG–⁄ – cells than by their SG+⁄ + counterparts, indeed indicating that the lack of SG PG causes increased constitutive release However, rerouting into the constitutive path-way of secretion does not seem to be a general effect

on all MC proteases when SG PG is lacking, as shown

0.0 0.5 1.0 1.5 2.0 2.5

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Fig 6 Analysis of sulfated proteoglycans Serglycin (SG) + ⁄ + bone marrow cells were cultured for different times (10, 23 34 days)

in medium containing interleukin (IL)-3 and were biosynthetically labeled with 35 SO42– (A) Total recovery of 35 S-labeled proteogly-cans per 1 · 10 6

cells into cell (filled bars) and medium (hatched bars) fractions (B) Charge density of sulfated proteoglycans.

35 S-labeled proteoglycans isolated from cell and medium fractions, both derived from

SG + ⁄ + cells, were mixed with internal stand-ards of heparin (hep) and chondroitin sulfate (CS) and were subjected to anion exchange chromatography on a DEAE–Sephacel col-umn The column was eluted with a linear gradient of LiCl Fractions were analyzed for radioactivity (filled symbols) and for uronic acid in order to detect the internal standards (open symbols; A 530 ) The results shown are representative of two independent experi-ments.

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by the fact that mMCP-6 and mMCP-5 were found at

similar or higher levels in medium from SG+⁄ + cells

than in medium from their SG–⁄ – counterparts

More-over, our data provide evidence that the SG-dependent

MC proteases are in fact present in functional

secre-tory granules even in the absence of SG PG This

indi-cates that transport of MC proteases into the secretory

granule compartments can occur independently of

SG PG Hence, SG does not appear to function as

general sorting vehicle for MC proteases

From the data presented here and previously [10], it is

clear that knockout of the SG gene results in a major

reduction of mMCP-5, mMCP-6 and CPA storage

However, the blockade is not complete, indicating that

the proteases can actually be stored to some extent in

MC granules even in the absence of SG PGs to which

they can bind In turn, this may be explained by low

lev-els of granular storage in the absence of any partner PG

An alternative explanation could be that there are low

levels of PGs other than SG in the MC granule, and that

such PG species can provide some compensation for the

lack of SG in terms of promoting MC protease storage

However, the presence of non-SG PG species within

MC granules remains to be demonstrated

So, how does the lack of SG cause such a dramatic

reduction of stored MC proteases? Although general

mechanisms involved in the intracellular sorting of

granule components are still relatively poorly defined,

two major hypotheses have emerged: ‘sorting by entry’

and ‘sorting by retention’ [19] In the sorting by entry

hypothesis (e.g the mannose 6-phosphate system [20]),

each secretory granule compound has a unique sorting

signal that interacts with a cognate receptor on the

luminal side of specific regions in the trans-Golgi

network, leading to budding from the trans-Golgi

network of vesicles containing only molecules with the

corresponding specific sorting signals In the sorting by

retention hypothesis, certain compounds entering the

immature granules may carry sorting motifs that

inter-act with the limiting membrane, but luminal proteins

that are not associated with the trans-Golgi network

membrane may also be included in the budding vesicle

According to this hypothesis, the contents of the

imma-ture granule are subsequently refined, both by

conden-sation of selected compounds and by removal of others

by vesicular transport, e.g to lysosomes for destruction,

or to the extracellular space by ‘constitutive-like’ or

‘piecemeal’ exocytosis [19,21] This process will

eventu-ally result in secretory granule maturation Although

we cannot at this stage with certainty define the role of

SG PG in this process, our results are clearly

compat-ible with a model in which SG organizes secretory

gran-ule maturation according to the sorting by retention

hypothesis In support of this, all of the MC proteases that have been shown to be SG-dependent for storage, i.e mMCP-4, mMCP-5, mMCP-6 and CPA (this study and [10]), display high affinity for sulfated glycosami-noglycans [22–25] It is therefore possible that

mMCP-4, mMCP-5, mMCP-6 and CPA are transported into immature granules independently of SG, but that their retention within the granules is dependent on their tight electrostatic interaction with SG PG However, our data indicate that interaction with SG PG is not an absolute prerequisite for retention of all granule com-pounds within the granule, as shown by the lack of SG dependence for the storage of b-hexosaminidase The sorting for retention model of granule matur-ation implies that compounds not selected for retent-ion are expelled from the maturing granule by vesicular transport In line with this model, our results suggest that mMCP-5 is targeted to degradation if not retained by SG We also see a marked secretion of pro-CPA by SG–⁄ – cells, possibly as a consequence

of defective retention However, there is also secretion

of CPA, albeit in its mature form, from SG+ ⁄ + cells mMCP-6 is also secreted by SG–⁄ – cells, but in con-trast to pro-CPA and mature CPA, mMCP-6 secretion was somewhat higher in SG+⁄ + cells than in their

SG–⁄ – counterparts However, the level of mMCP-6 protein in the conditioned medium from SG–⁄ – cells was considerably higher than the intracellular level, indicating that secretion rather than storage is the dominating pathway for mMCP-6 in the absence of

SG One possible explanation for these findings is that there is continuous low-level release of secretory gran-ule compounds in normal MCs, a process often referred to as ‘piecemeal’ degranulation [21] In the absence of SG as a retention vehicle, this slow release may constitute the dominating pathway

In summary, this study has provided the first insights into the mechanism by which SG PG regulates

MC secretory granule homeostasis

Experimental procedures

Cell culture

experi-ments were approved by the local ethical committee BMMCs were obtained by culturing femural and tibial bone marrow cells in DMEM (SVA, Uppsala, Sweden), supplemented with 10% heat-inactivated fetal bovine serum

2 mm l-glutamine (SVA) and 50% WEHI-3B conditioned medium (which contains IL-3) for 3 weeks The cells were

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kept at a concentration of 500 000 cellsÆmL)1, and the

med-ium was changed every third day

Staining

Three hundred thousand cells were collected on cytospin

slides (700 r.p.m., 5 min) and stained with

3 min, and then stained with May–Gru¨nwald (Merck,

Sol-lentuna, Sweden) for 15 min After being washed with

water, the slides were stained with 5% Giemsa (Merck) in

water for 10 min

TEM

Cells were fixed for 6 h in 2% glutaraldehyde in a 0.1 m

sodium cacodylate buffer supplemented with 0.1 m sucrose,

and this was followed by 1.5 h of postfixation in 1%

osmium tetroxide dissolved in the same cacodylate buffer

After dehydration in ethanol, the cells were embedded in

the epoxy resin Agar 100 (Agar Scientific, Stansted, UK)

Ultrathin sections were placed on copper grids covered with

a film of polyvinyl formal plastic (Formvar; Agar Scientific)

and contrasted with uranyl acetate and lead citrate

Elec-tron micrographs were taken with a Hitachi elecElec-tron

micro-scope (Hitachi Ltd, Tokyo, Japan)

RT-PCR

Total RNA was isolated using the NucleoSpin RNA II kit

(Macherey Nagel, Du¨ren, Germany) Total RNA was used

for first-strand cDNA synthesis using SuperScriptII for

RT-PCR using primers specific for the MC proteases and

SG Hypoxanthine–guanine phosphoribosyltransferase was

used as a positive control for the RT-PCR The PCR

prim-ers used were as specified elsewhere [10]

Immunoblotting

main cultures, centrifuged at 300 g, (Megafuge 1.0R; Heraeus;

equipped with a swing out rotor), resuspended in 1 mL of

serum-free medium (as described above), and further cultured

overnight The cells were thereafter pelleted by centrifugation

at 300 g (10 min, Megafuge 1.0R; Heraeus; equipped with a

swing out rotor), and both the pellet and the medium fraction

analysis, the recovered media were concentrated 50 times

using Amicon Ultra-4 centrifugal filter device (Millipore,

sample buffer containing 5% b-mercaptoethanol Cell pellets

buffer containing 5% b-mercaptoethanol Immunoblotting

was carried out as previously described [10]

Proteoglycan isolation and analysis

) from days 9, 22 and 33 of culture were biosynthetically labeled overnight with 0.32 mCi of

Cells were pelleted by centrifugation for 10 min at 300 g (Megafuge 1.0R; Heraeus; equipped with a swing out

until further analysis For isolation of cell fraction glycos-aminoglycans, cell pellets were solubilized in 500 lL of

Then, the solubilisates were diluted with 9.5 mL of

contain-ing 0.4 mL of DEAE–Sephacel, equilibrated with 50 mm

media were loaded directly onto the columns After

(pH 5.5) Four fractions of 1100 lL each were collected and analyzed for radioactivity by scintillation counting Fractions containing radioactive material were pooled and

anion exchange chromatography on a 5 mL column of DEAE–Sephacel connected to an FPLC system The col-umn was eluted with a gradient of increasing concentra-tions of LiCl, from 0.05 m to 2 m in 50 mm sodium acetate

internal standard, 200 lL of a mixture of unlabeled heparin

Sweden) was added to each sample before anion exchange chromatography analysis Internal standards were detected

by the carbazole method: 25 lL of each fraction was mixed

10 lL of carbazole reagent (0.125% carbazole in 96% eth-anol) The samples were boiled for 10 min and cooled, and the absorbance at 530 nm was measured

Inhibition of proteasome and lysosome function

) were cultured in 5 lm lactacystin (Affiniti Research Products, Exeter, UK) After incubation overnight, cells were pelleted, solubilized and subjected to immunoblotting for mMCP-5, mMCP6 and CPA Lyso-somal function was inhibited by incubation of cells with 5

solubi-lized and subjected to immunoblotting

Degranulation

cells were incubated for 120 min in the presence of 2 lm of the calcium

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