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Our data show that SST-14 was cointernalized with SSTR3, was uncoupled from the receptor, and was sorted into an endocytic degradation pathway, whereas octreotide was recycled as an inta

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somatostatin-receptor 3-mediated endocytosis in rat

insulinoma cells

Dirk Roosterman1, Nicole E I Brune2, Oliver J Kreuzer2, Micha Feld1, Sylvia Pauser1, Kim Zarse2, Martin Steinhoff1and Wolfgang Meyerhof2

1 Department of Dermatology, IZKF Mu¨nster and Ludwig Boltzmann Institute for Cell and Immunobiology of the Skin, Germany

2 Department of Molecular Genetics, German Institute of Human Nutrition Potsdam-Rehbruecke, Nuthetal, Germany

Somatostatin is a cyclic peptide that is widely

expressed throughout the central nervous system,

endocrine tissue, skin and gastrointestinal tract [1]

Somatostatin exerts a wide range of important

biolo-gical effects, including inhibition of secretion of growth

hormone, insulin, glucagon and gastrin as well as other

hormones secreted from the pituitary, skin and

gastro-intestinal tract [2]

Among other actions, somatostatin elicits strong antiproliferative effects in in vivo as well as in vitro models of cancer [3–5] Somatostatin analogs are there-fore being used in the diagnosis and therapy of various tumors, in particular neuroendocrine tumors, which express somatostatin receptors (SSTRs) [3–5] SSTR scintigraphy (SRS), a widely used imaging technique,

is employed to detect and localize such tumors The

Keywords

endocytosis; G-protein-coupled receptor;

neuropeptide; proteolysis; somatostatin

Correspondence

D Roosterman, Department of Dermatology

and IZKF Mu¨nster, Von-Esmarch-Strasse 58,

D-48148 Mu¨nster, Germany

Fax: +49 0251 8357452

Tel: +49 0251 8352932

E-mail: roosterman@gmx.net

(Received 27 March 2008, revised 20 June

2008, accepted 23 July 2008)

doi:10.1111/j.1742-4658.2008.06606.x

Somatostatin receptor (SSTR) endocytosis influences cellular responsiveness

to agonist stimulation and somatostatin receptor scintigraphy, a common diagnostic imaging technique Recently, we have shown that SSTR1 is dif-ferentially regulated in the endocytic and recycling pathway of pancreatic cells after agonist stimulation Additionally, SSTR1 accumulates and releases internalized somatostatin-14 (SST-14) as an intact and biologically active ligand We also demonstrated that SSTR2A was sequestered into early endosomes, whereas internalized SST-14 was degraded by endosomal peptidases and not routed into lysosomal degradation Here, we examined the fate of peptide agonists in rat insulinoma cells expressing SSTR3 by biochemical methods and confocal laser scanning microscopy We found that [125I]Tyr11-SST-14 rapidly accumulated in intracellular vesicles, where

it was degraded in an ammonium chloride-sensitive manner In contrast, [125I]Tyr1-octreotide accumulated and was released as an intact peptide Rhodamine-B-labeled SST-14, however, was rapidly internalized into endo-some-like vesicles, and fluorescence signals colocalized with the lysosomal marker protein cathepsin D Our data show that SST-14 was cointernalized with SSTR3, was uncoupled from the receptor, and was sorted into an endocytic degradation pathway, whereas octreotide was recycled as an intact peptide Chronic stimulation of SSTR3 also induced time-dependent downregulation of the receptor Thus, the intracellular processing of inter-nalized SST-14 and the regulation of SSTR3 markedly differ from the events mediated by the other SSTR subtypes

Abbreviations

EGFP, enhanced green fluorescent protein; FITC, fluorescein isothiocyanate; HSV, herpes simplex virus glycoprotein D; RIN, rat insulinoma; SRS, somatostatin receptor scintigraphy; SST-14, somatostatin-14; SSTR, somatostatin receptor.

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success of SRS is based on specific interactions of

sta-ble radiolabeled somatostatin analogs injected into

patients, causing them to bind to SSTRs expressed by

tumor cells [4,6] These interactions are not restricted

to the binding of the peptide agonist to its cognate

receptor, but also lead to agonists accumulating in the

tumor cell after internalization of the receptor–agonist

complex [7–9] Understanding the internalization of

somatostatin–receptor complexes and their intracellular

fate is therefore of considerable interest in tumor

diag-nostics and therapy as well as neuroinflammation

Somatostatin binds to and activates six different

G-protein-coupled SSTR subtypes: SSTR1, SSTR2A,

SSTR2B, SSTR3, SSTR4 and SSTR5 The various

SSTR subtypes show distinct internalization pathways

[10,11] In human embryonic kidney 293 cells and

neuroendocrine pancreatic b-cells, rat SSTR1,

SSTR2A, SSTR3 and SSTR5 but not SSTR4 were

internalized upon stimulation by somatostatin Further

investigation of SSTR1 and SSTR2A clearly indicated

that the fate of internalized somatostatin-14 (SST-14)

strongly depends on the receptor subtype, although the

particular pathways are not yet fully explored We

recently demonstrated that chronic stimulation of

SSTR1 induced accumulation of SST-14 in cells via a

dynamic process of internalization, recycling and

rein-ternalization of the ligand [11] In contrast, stimulation

of SSTR2A with SST-14 or its stable analog octreotide

induced prolonged sequestration of the receptor–ligand

complex into early endosomes that was dependent on

arrestins [12,13] Subsequently, the endosomal

peptidase endothelin-converting enzyme-1 cleaves

inter-nalized SST-14 between positions Asn5-Phe6 and

Thr10-Phe11, leading to release of internalized SST-14

as SST-14(6–10) (FFWKT) and SST-14(1–5)⁄ (11–14)

(AGCLN⁄ FTSC) [13]

Further analysis of SSTR3, an SSTR subtype of

particular importance in human thymoma [14], shows

that agonist-mediated internalization of SSTR3 is

criti-cally dependent on phosphorylation of the C-terminal

tail [15] As the phosphorylation sites do not

corre-spond to consensus sequences for second

messenger-regulated protein kinases, protein kinase A or protein

kinase C, it was suggested that specific

G-protein-coupled receptor kinases were involved [16] Moreover,

colocalization studies and the use of

dominant-nega-tive mutants of arrestin-2 demonstrated that

internali-zation of SSTR3 involves arrestin-2, the adaptor

protein-2 complex, and proceeds via clathrin-coated

pits and vesicles [16] In contrast to the trafficking

process of the receptor, the fate of the peptide agonist

has not thus far been analyzed after cointernalization

with SSTR3

Therefore, we examined the fate of SST-14 and octreotide cointernalized with SSTR3 in transfected rat insulinoma (RIN) cells by biochemical methods and confocal laser scanning microscopy We show that SST-14 endocytosed with SSTR3, uncoupled from the receptor and proceeded to lysosomal degra-dation, whereas octreotide endocytosed with SSTR3 but was released as an intact peptide from the cells Moreover, chronic stimulation of SSTR3 with

SST-14 induced time-dependent downregulation of the receptor Our results demonstrate that SSTR3 traf-ficking and ligand processing differ markedly from the mechanisms observed for either SSTR1 or SSTR2A

Results

Reduction of cell surface binding sites

To examine the time course of SST-14-induced loss of SSTR3-specified cell surface binding sites, RIN-SSTR3 cells were stimulated with SST-14 for 0–120 min (Fig 1A) Incubation was stopped by placing cells on ice, and surface binding sites were determined Stimu-lation of the SSTR3-expressing cells with SST-14 induced a relatively slow reduction in the number of surface binding sites as compared to SSTR1 [11] Sixty minutes after chronic stimulation with SST-14, the number of binding sites was decreased to  50% of the original density, and it remained at this level for another 60 min

Recovery of cell surface binding sites Next, we determined whether or not cell surface binding recovered following removal of the stimulus RIN-SSTR3 cells were first stimulated with SST-14 for

120 min Cell surface-bound ligand was washed off, and cells were incubated for another 0–120 min The recov-ery of surface binding sites was determined as described above Interestingly, during the first 15 min of incuba-tion, surface binding recovered to 76% However, incu-bation of the cells for a period of up to 120 min did not lead to recovery of surface binding beyond this value (Fig 1B) This result indicates that prolonged incuba-tion of SSTR3-expressing cells with SST-14 induced marked downregulation of the receptor We therefore determined the time dependence of SSTR3 downregula-tion by chronic stimuladownregula-tion Therefore, RIN-SSTR3 cells were stimulated for 0–1300 min with SST-14 at

37C Subsequently, the agonist peptide was washed off, and cells were incubated for recovery of surface binding sites (Fig 1C) Chronic stimulation resulted in

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time-dependent downregulation of the receptor After a

period of 1300 min of stimulation and 120 min of

recov-ery, cell surface binding was reduced to 43 ± 5%

The time-dependent loss of surface binding sites

during stimulation with SST-14 suggests that the

recep-tor was internalized We determined the ratio between

cell surface-located receptors and internalized receptors

after 1 h of incubation with SST-14 (Fig 1D) by

mea-suring cell surface binding and total cellular binding in

the presence of saponin [17] Incubation of untreated

cells with saponin did not significantly change the

number of binding sites After stimulation with SST-14, cell surface binding decreased to 52 ± 3% of that of untreated cells, whereas total binding remained at 91 ± 4% of that of untreated cells Thus, after peptide stimu-lation, approximately 40% of the SSTR3 receptors were localized in intracellular compartments, and the data clearly indicate that SSTR3 was internalized during stimu-lation These data are in line with the fluorescence micros-copy quantification of intracellularly located SSTR3 [18] The loss of cell surface binding sites during chronic stimulation suggests that the receptor is sequestered

Fig 1 Loss and recovery of SST-14 binding sites (A) SST-14-mediated reduction of cell surface binding sites RIN-SSTR3 cells were stimu-lated with SST-14 at 37 C for the indicated times Cells were washed with acidic buffer, and surface binding sites were determined by incu-bation with [ 125 I]SST-14 at 4 C (B) Recovery of cell surface binding sites RIN-SSTR3 cells were stimulated for 120 min with SST-14 at

37 C Cells were washed with acidic buffer and incubated for the indicated times, and cell surface binding sites were determined as described above (C) Downregulation of surface binding sites RIN-SSTR3 cells were stimulated with SST-14 for the indicated times, washed with acidic buffer, and incubated for 120 min at 37 C Surface binding sites were determined as described above (D) Determination of cell surface and total binding after stimulation with SST-14 RIN-SSTR3 cells were stimulated with SST-14 in the absence or presence of sapo-nin Binding was measured as described above The data are expressed at mean ± SEM values from three independent experiments (E, F) Distribution of SSTR3–HSV in control cells and under conditions of receptor downregulation RIN cells expressing SSTR3–HSV were stimulated (F) or not stimulated (E) with SST-14 for 1300 min Then, the peptide was removed and cells were allowed to recover for 90 min Thereafter, the epitope-tagged SSTR3 was visualized by indirect immunfluorescence (F) Localization of SSTR3 after chronic stimulation with SST-14 Chronic stimulation of SSTR3 with SST-14 mediates downregulation of SSTR3 The immunofluorescence signal of SSTR3 is concentrated in one area of the cell and not equally distributed in the cell membrane (arrows).

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within the cells or that it is downregulated by

degrada-tion To distinguish between the two possibilities, we

determined the localization of SSTR3 after 1300 min

of stimulation with SST-14 and 90 min of recovery In

untreated cells, SSTR3 showed a bright

immunofluo-rescence signal at the cell membrane (Fig 1E, arrows)

In cells chronically stimulated with SST-14, the

fluores-cence signal was weaker than the signal seen in

untreated cells Moreover, in all of these cells, the

SSTR3 immunofluorescence signal was locally

concen-trated in only one area of the cell surface and not

evenly distributed over the plasma membrane (Fig 1F,

arrows)

Together, the results indicate that stimulation of SSTR3 with SST-14 induced internalization of the receptor Chronic stimulation with SST-14 mediated downregulation of SSTR3

Uptake of [125I]Tyr11-SST-14 and [125 I]Tyr1-octre-otide in SSTR3-expressing rat insulinoma cells

To examine the fate of SST-14 cointernalized with SSTR3, we measured the uptake of [125

I]Tyr11-SST-14 in RIN-SSTR3 cells in the absence (Fig 2A, diamonds) or presence (Fig 2A, triangles) of ammo-nium chloride Treatment of the cells with

Fig 2 SSTR3-mediated uptake of 125 I-labeled peptides (A) SSTR3-mediated uptake of [ 125 I]Tyr11-SST-14 RIN-SSTR3 cells were incubated with [ 125 I]SST-14 in the presence (triangle) or absence (diamonds) of ammonium chloride Cell surface [ 125 I]Tyr11-SST-14 was washed off, and the amount of cell-associated radioactivity was determined (B) SSTR3-mediated uptake of [ 125 I]Tyr1-octreotide RIN-SSTR3 cells were incubated with [ 125 I]Tyr1-octreotide Cell surface [ 125 I]Tyr1-octreotide was washed off, and the amount of cell-associated radioactivity was determined (C) HPLC separation of cell-associated, agonist-bound internalized radioactivity in the presence of ammonium chloride Cells were pretreated with ammonium chloride, incubated with [ 125 I]Tyr11-SST-14 at 37 C for 30 min in the presence of ammonium chloride, washed with acidic buffer, and analyzed by HPLC (D) HPLC separation of the cell supernatant incubated for 30 min with [ 125 I]Tyr11-SST-14 (E) Time course of SSTR3-mediated uptake of [125I]Tyr11-SST-14 RIN- SSTR3 cells were stimulated for 0–15 min with [125I]Tyr11-SST-14, washed with acidic buffer, and incubated for 0–90 min Cell-associated (triangles) and released (diamonds) radioactivity was determined by HPLC (F) Time course of SSTR3-mediated uptake of [ 125 I]Tyr1-octreotide RIN- SSTR3 cells were incubated for 0–15 min with [ 125 I]Tyr1-octreotide, washed with acidic buffer, and incubated for 0–90 min at 37 C Cell-associated radioactivity and radioactivity from the superna-tants was determined by HPLC The data are expressed as mean ± SEM values from three independent experiments.

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ammonium chloride neutralized acidic cellular

com-partments [19] Within 10–15 min at 37C, the

cellu-lar uptake of [125I]Tyr11-SST-14 reached maximal

levels in the absence of ammonium chloride

corre-sponding to  80% of the amount of the cell

sur-face-bound peptide The amount of intracellular

radioactivity then quickly declined over a period of

 15 min to very low levels corresponding to about

30% of the amount of cell surface-bound peptide

These levels slowly decreased over the next 90 min

to < 20% of the initial value These observations

are best explained by assuming that specific

intracel-lular degradation destroys the radiolabeled peptide,

and the degradation products are then released from

the cells The low level of radioactivity observed to

be cell-associated between 60 and 120 min probably

reflects the steady-state level of [125I]Tyr11-SST-14

determined by receptor-mediated uptake and

degra-dation The receptor population engaged in agonist

uptake appears to be largely diminished at these

times, due to receptor internalization and

desensitiza-tion [20] Notably, the amount of the internalized

peptide corresponds to 80% of the cell surface-bound

peptide, suggesting that most of the agonist-occupied

receptors were engaged in endocytosis in the presence

of subnanomolar concentrations of agonist When the

experiment was carried out in the presence of

ammo-nium chloride (Fig 2A, triangles), radioactivity

accu-mulated with a similar kinetic during the first 10 min of

incubation but reached a plateau corresponding to

almost 100% of cell surface-bound [125I]Tyr11-SST-14

Thus, under conditions in which the vesicular pH is

neutral [19], almost all cell surface-bound radioactivity

accumulated and remained in the cells

Next, we determined the SSTR3-mediated uptake of

[125I]octreotide (Fig 2B) Chronic stimulation of

SSTR3-expressing cells with octreotide induced

contin-uous uptake of the ligand During the first 30 min of

incubation, 118% of surface-bound octreotide was

found to be cell-associated Further incubation induced

a linear accumulation of radioactivity within the cells

After 4 h of incubation, the amount of internalized

radioactivity was equivalent to 256% of cell

surface-bound octreotide

In order to distinguish between radioactivity

corre-sponding to degraded or intact peptide, we examined

the cell-associated radioactivity by HPLC We found

that [125I]Tyr eluted in fractions 1–5, degraded peptide

fragments in fractions 9–11, and intact [125I]SST-14

in fractions 14–17 (Fig 2C,D) Figure 2C shows a

radiogram of the cell-associated radioactivity after

30 min of stimulation with [125I]SST-14 in the presence

of ammonium chloride This treatment blocked the

degradation of [125I]SST-14 For instance, more than 95% of the cell-associated radioactivity eluted as intact [125I]SST-14 in fraction 16 Minor amounts of peptide fragments of [125I]SST-14 were observed in fractions 9–11, suggesting modest degradation of [125I]SST-14 by peptidases The degradation of [125I]SST-14 to [125I]Tyr was completely blocked Together, these results suggest that internalized [125I]Tyr11-SST-14 was targeted in a degradation pathway that is sensitive to ammonium chloride

In contrast, a representative HPLC chromatogram of the supernatant collected 30 min after stimulation of the cells incubated with [125I]Tyr11-SST-14 shows that 97%

of the radioactivity was [125I]Tyr (Fig 2D) [21,22] This result suggests that SST-14 was completely degraded to its amino acids, which were subsequently released into the supernatant Similar HPLC analyses of the radio-active degradation products found in the supernatant of stimulated SSTR1 cells have demonstrated that SST-14

is relatively stable in the supernatant and is only slowly degraded by phosphoamidon-sensitive peptidase [19] Thus, we conclude that [125I]SST-14 is processed to amino acids within the cells

Figure 2E shows the time courses of association of [125I]Tyr11-SST-14 (triangles) with the cells and the accumulation of its degradation product [125I]Tyr (dia-monds) in the extracellular medium, as assayed by HPLC analyses of the fractions During the first 15 min

of stimulation, [125I]Tyr11-SST-14 accumulated within the cells After removal of the peptide agonist by wash-ing and further incubation at 37C, the amount of cell-associated [125I]Tyr11-SST-14 rapidly decreased Ninety minutes after stimulation, the amount of cell-associated [125I]Tyr11-SST-14 was reduced to 6% This decay was paralleled by accumulation of [125I]Tyr (Fig 2E, diamonds) in the medium Thus, all of the internalized peptide was degraded to its amino acids

Next, we analyzed whether or not octreotide was degraded during the internalization process In accor-dance with Fig 2B,F (filled circles) shows that [125I]Tyr1-octreotide was rapidly internalized by RIN-SSTR3 cells during the 15 min stimulation period, i.e as long as the peptide was present However, when the stimulus was removed, the cells released the endocytosed peptide into the supernatatant Inter-estingly, HPLC analysis of the cell lysate demon-strated that octreotide was not degraded (data not shown) Both the radioactivity determined in the supernatant and the cell-associated radioactivity eluted with a retention time identical to that of [125I]Tyr1-octreotide Thus, SSTR3 mediates ligand-specific processing Whereas SST-14 is sorted into an ammonium-sensitive degradation pathway, octreotide

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bypasses degradation, accumulates in the cell and is

released as intact ligand from the cells in the

sur-rounding medium

SSTR3-mediated uptake of fluorescein

isothiocyanate (FITC)–SST-14

To directly visualize the receptor-mediated uptake of

the peptide agonist, internalization of FITC-labeled

SST-14 was examined in RIN-SSTR3 cells by confocal

laser scanning microscopy The fluorescent peptide was

colocalized with herpes simplex virus glycoprotein D

tagged SSTR3 (SSTR3–HSV), as detected by indirect

immunofluorescence Cells were incubated with FITC–

SST-14 at 4C After removal of unbound peptide, a

temperature shift to 37C induced internalization of

cell surface-bound agonist for 2, 30 or 60 min At the

beginning of the observation period at 2 min,

fluores-cence signals of FITC–SST-14 were barely visible

How-ever, a few discrete zones were labeled at the cell surface

(Fig 3A, green arrows, top left) that colocalized with

SSTR3–HSV (Fig 3A, red arrows, top middle panel,

yellow arrows in the overlay) After 30 min, internalized

FITC–SST-14 and SSTR3–HSV frequently colocalized

in intracellular vesicles (Fig 3A, middle panels, yellow

arrows) However, vesicles that appear only in red or

green suggest that some FITC–SST-14 (Fig 3A, green

arrow) dissociated from SSTR3–HSV (Fig 3A, red

arrow) and that SSTR3 and the agonist peptide were

sorted into different cell pathways After 60 min of

stimulation, most of the receptors were recycled to the

plasma membrane (Fig 3A, red arrows, bottom

pan-els), whereas the fluorescence signal of the ligand was

still observed within intracellular vesicular structures

Traces of SSTR3–HSV were also detected within

intra-cellular vesicular compartments, where it colocalized

with SST-14 (Fig 3A, yellow arrowheads)

Agonist-induced mobilization of arrestin-2–

enhanced green fluorescent protein (EGFP)

HPLC analysis of internalized SST-14 and octreotide

demonstrated that SST-14 but not octreotide was

metabolized after internalization We reasoned that the

integrity of the ligand could influence the association

of arrestins with the internalized receptor Therefore,

we analyzed the localization of arrestin-2–EGFP and

SSTR3–HSV after stimulation with 1 lm SST-14 or

octreotide for 15 min (Fig 3B) In unstimulated cells,

arrestin-2–EGFP was diffusely located within the cells

and SSTR3–HSV was primarily located at the plasma

membrane (Fig 3B, top panels) Stimulation with

either of the two agonists induced internalization of

the receptor (Fig 3B, red arrows, middle panel) Accordingly, arrestin-2 was mobilized and transported from the cytosol to the cell membrane (Fig 3B, green arrows, middle panel) Interestingly, 15 min after stim-ulation, arrestin-2 was only partially associated with internalized SSTR3–HSV, indicating that arrestin-2

A

B

Fig 3 Agonist-induced internalization of SSTR3–HSV (A) SSTR3-mediated uptake of FITC–SST-14 RIN-SSTR3 cells were incubated for 60 min with FITC–SST-14 at 0 C Cells were washed and incu-bated for 2, 30 and 60 min at 37 C FITC–SST-14 was detected using the FITC label (shown in green) SSTR3 was detected using antibody directed against the HSV tag (shown in red) (B) Agonist-induced mobilization of arrestin-2–EGFP RIN-SSTR3 cells were transiently transfected with arrestin-2–EGFP Cells were stimulated with SST-14 (1 l M ) or octreotide (1 l M ) for 15 min at 37 C SSTR3–HSV was localized using an antibody against HSV and arres-tin-2-EGFP by EGFP The experiment was performed three times, with similar results.

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dissociated from the internalized receptor at or close

to the plasma membrane Virtually no differences

could be determined in the localization of arrestin-2–

EGFP after stimulation with SST-14 or octreotide

Thus, our data indicate that the stable ligand,

octreo-tide, did not induce stronger association of arrestin-2–

EGFP with the internalized SSTR3 than did SST-14

Internalized SST-14 is transported to lysosomes

The complete intracellular degradation of internalized

SST-14 suggested that the ligand was processed into

the lysosomal degradation pathway in RIN-SSTR3

cells To examine whether fluorescent dye-labeled

SST-14 was sorted to lysosomes, experiments on

colo-calization of rhodamine-B–SST-14 with cathepsin D, a

lysosomal protease [23], were performed (Fig 4)

Therefore, we incubated RIN-SSTR3 cells with

rhoda-mine–SST-14 at 4C Under these conditions, the

fluo-rescence signals of the peptide were predominantly

observed as a punctate pattern at the cell surface,

whereas the fluorescence signals of the lysosomal

pro-tease appeared to be scattered within the cytoplasm

(Fig 4, top panels) Warming the cells to 37C

induced the internalization of rhodamine–SST-14 and

aggregation of lysosomes (Fig 4, middle panels) After

30 min of stimulation, clear colocalization of cathe-psin D and rhodamine-B–SST-14 was observed, indi-cating that the peptide was routed to a lysosomal degradation pathway (Fig 4, middle panel, yellow arrowhead) After 60 min, both fluorescence signals still colocalized within these compartments (Fig 4, middle panel, yellow arrowhead) The observation that endocytosed SST-14 colocalized with cathepsin D agrees with our data obtained using biochemical assays, demonstrating complete degradation of inter-nalized SST-14 in RIN-SSTR3 cells

Discussion

Recent studies provided clear evidence that the SSTR subtypes (SSTR1, SSTR2, SSTR3 and SSTR5) inter-nalize to similar extents after stimulation with SST-14, somatostatin-28, and synthetic agonists [16,18,20, 24,25] However, detailed analyses of the endocytic processes and the pathways of trafficking of the SSTR subtypes revealed explicit differences

For example, SSTR1 did not mobilize arrestin-2 during internalization, whereas SSTR3 interacted tran-siently with arrestin-2, and internalized SSTR2A formed a stable complex with arrestin-2 [11,16,25] The differences between the receptor subtypes in their inter-action with arrestins indicate the existence of internali-zation and trafficking pathways that are specific for the SSTR subtypes

Determining the fate of the internalized ligand revealed three different pathways of receptor traffic-king and agonist processing SSTR1 mediates accumu-lation and release of intact SST-14 This phenomenon was accomplished by a dynamic process of internaliza-tion, recycling and reinternalization of the peptide, a pathway consistent with the role of SSTR1 as an auto-receptor [11] In contrast, SSTR2A induced sequestra-tion of the receptor–ligand complex within early endosomes SSTR2A did not recycle within a period of

2 h after agonist stimulation SST-14, endocytosed with SSTR2A, was degraded by endothelin-converting enzyme-1 and other peptidases and was not routed into lysosomal degradation This strong association of arrestins with the internalized receptor and the seques-tration of the receptor in early endosomes is indicative

of a class B receptor [13,26] Stimulation of SSTR2A with octreotide induced long-lasting sequestration of the intact ligand into early endosomes

Here, we investigated the intracellular trafficking of SSTR3 and the processing of internalized [125 I]Tyr11-SST-14 and [125I]Tyr1-octreotide Our data show that SSTR3 transiently interacts with arrestins and

Fig 4 Rhodamine-B–SST-14 is transported to lysosomes

RIN-SSTR3 cells were incubated for 2 h with rhodamine-B–SST-14 at

4 C, washed, and incubated for 0, 30 and 60 min at 37 C

Rhoda-mine-B–SST-14 (red) was detected using rhodamine-B

fluores-cence; lysosomes (green) were detected using an antibody against

cathepsin D The experiment was performed three times, with

sim-ilar results.

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directs SST-14 to lysosomal degradation This

transient interaction of the receptor with arrestins is

indicative of a class A receptor, and our data are in

line with data in [16] and [25]

When we analyzed the fate of the ligand, we

demon-strated that SSTR3 routed internalized SST-14 towards

a lysosomal degradation pathway Internalized

[125I]Tyr11-SST-14 was rapidly degraded, and [125I]Tyr

was released into the cell supernatant Confocal laser

scanning microscopic analyses of internalized

fluores-cent dye-labeled SST-14 showed strong colocalization of

the fluorescence signal with cathepsin D, a specific

mar-ker protein for lysosomes The persistence of the

fluores-cence signal within lysosomes as compared to the rapid

degradation of the radioligand within 30 min most

likely reflects the stability of the fluorophore and not

that of the peptide moiety It is known that internalized

ligands that are routed to lysosomes are degraded by

acidic proteases [27] To address the question of whether

somatostatin is also degraded by acidic proteases, we

interfered with the acidification of endocytic vesicles by

incubating the cells in the presence of ammonium

chlo-ride [19] Under these conditions, the degradation of the

internalized radioligand and the continued endocytosis

of the peptide ligand were markedly blocked, suggesting

that receptor trafficking proceeds via acidic vesicles and

that the degradation of somatostatin is accomplished by

acidic proteases when endocytosed with SSTR3

Inter-estingly, the endosomal degradation of internalized

SST-14, observed after internalization through

SSTR2A, was partially inhibited by neutralization of

acidic cell compartments [13], suggesting that different

peptidases are involved in the degradation process of

SST-14, depending on the coendocytosed SSTR

sub-type, i.e either SSTR2A or SSTR3

We also analyzed the intracellular processing of

octreotide in SSTR3-expressing cells Octreotide is a

synthetic SST-14 analog that binds to SSTR2A as well

as SSTR3 Octreotide is resistant to degradation by

endosomal peptidases [13] Interestingly, octreotide

was also stable when it was internalized via SSTR3,

suggesting that the synthetic agonist is also resistant to

lysosomal degradation or, alternatively, that it was not

routed to the lysosomes Chronic stimulation of the

cells with octreotide induced continuous accumulation

of the intact peptide within these cells After 4 h of

chronic stimulation, 256% of surface-bound octreotide

was observed to be cell-associated, indicating that

SSTR3 was continuously recycled to the cell

mem-brane and reinternalized during chronic stimulation,

thereby mediating the accumulation of octreotide in

the cells A similar observation was described for the

SSTR1-mediated accumulation of SST-14 [11]

Interestingly, chronic stimulation of SSTR3 with SST-14 induced time-dependent downregulation of SSTR3 One hundred and twenty minutes after stimu-lation, SSTR3 was recycled up to 75%, whereas it was recycled up to only 43% after 1300 min In contrast, SSTR1, which does not direct SST-14 to lysosomal degradation, recovered up to 100% under the same conditions [11,20] This observation underlines our finding that SSTR3 continuously recycles and is re-endocytosed under chronic stimulation One hour after stimulation of the cells with SST-14, immunofluo-rescence signals of SSTR3–HSV still colocalized with the fluorescence signal of the internalized ligand At this time point, the ligand was simultaneously detected within lysosomes in SSTR3-expressing cells The data suggest that lysosomal targeting of SSTR3 is responsi-ble for the downregulation of the receptor

Taken together, our results show that: (a) SSTR3 continuously internalizes, recycles and reinternalizes under chronic agonist stimulation; (b) the internalized SST-14 is routed to lysosomal degradation, where internalized [125I]Tyr11-SST-14 is degraded to [125I]Tyr; (c) internalized octreotide is resistant to deg-radation, but is accumulated within cells as an intact ligand; and (d) chronic stimulation of SSTR3 with SST-14 induces time-dependent downregulation of the receptor, probably through lysosomal degradation of SSTR3

At least two conclusions may be drawn from these observations First, agonist-induced SSTR internaliza-tion is a complex process depending on the receptor subtype and the nature of the stimulating agonist Besides the above-described differences in the regula-tion of receptor internalizaregula-tion, trafficking and recy-cling, further functional differences among SSTR subtypes may be postulated through interactions with distinct SSTR-binding proteins In fact, such binding proteins that specifically associate with SSTR subtypes have been recently identified [28,29]

Radiolabeled or fluorescent dye-labeled somatostatin analogs accumulating in certain cancer cells are used with the diagnostic method SRS, and conjugates of stable somatostatin analogs with toxic compounds or radioisotopes have been used for chemotherapy in certain tumors [30] Therefore, detailed knowledge of the mechanisms underlying agonist-induced endocyto-sis and trafficking of the SSTR subtypes is of great clinical importance, and cancer patients may benefit from it in the future

Our results indicate that future drugs should be tested for all known aspects of agonist-induced traf-ficking They also indicate that the considerable knowl-edge about the interaction of octreotide with SSTR2A

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cannot be generalized to other SSTR subtypes and

ligands without experimental proof The receptor

subtype-specific transport of SSTR2A and the

ligand-specific processing of octreotide go well with the use of

octreotide in SSTR2A scintigraphy [13] On the other

hand, these advantages adversely affect the use of

octreotide in tumor treatment, because this peptide

leads to extensive sequestration of SSTR2A and

desen-sitization of the targeted tumor cells for prolonged

periods [13] Our results also show that octreotide

recycled during the SSTR3-mediated transport

Because it did not remain sequestered in the cell when

internalized with SSTR3, labeled octreotide appears

not to be suitable for detecting SSTR3 in receptor

scintigraphy

Experimental procedures

Materials

SST-14 and octreotide were obtained from Bachem (Weil

am Rhein, Germany), [125I]Tyr11-SST-14 (2000 CiÆmmol)1)

was from Amersham (Braunschweig, Germany), and

[125I]Tyr1-octreotide was from Anawa (Wangen,

Switzer-land) FITC–SST-14 was from Advanced Bioconcept

(Derry, NH, USA) FITC-conjugated anti-rabbit IgG,

Texas Red-conjugated anti-mouse IgG, paraformaldehyde,

glycerol⁄ gelatin solution and BSA (fraction IV) were

pur-chased from Sigma (Taufkirchen, Germany) The

poly-clonal antiserum against cathepsin D was a generous gift

from A Hille-Rehfeld (Goettingen, Germany), and has

been described in detail elsewhere [23]

Generation of cDNA constructs and cell line

The construct with arrestin-2 tagged with EGFP has been

described previously [31] Generation of the neuroendocrine

RIN 1046-38 cell line stably expressing the C-terminal HSV

epitope-tagged rat SSTR3 tagged with the HSV

glycopro-tein D epitope at the C-terminus (SSTR3–HSV) has been

described previously, and it has been demonstrated to

possess a maximal binding capacity of 1660 (± 350) fmol

per 2· 104cells for [125I]Tyr11-SST-14 [20]

Synthesis of rhodamine-B-labeled SST-14

SST-14 was generated on a LIPS vario multiple peptide

synthesizer using the robot’s standard protocol following

the Fmoc strategy (peptides&elephants, Potsdam, Germany)

The rhodamine-B label was attached by deprotection of the

N-terminal a-amino function The rhodamine-B was

acti-vated using ByBop (Novabiochem, Darmstadt, Germany)

and N-methylmorpholine as a base Rhodamine-B was

added in a four-fold surplus to the a-amino function

The rhodamine⁄ ByBop ⁄ N-methylmorpholine ratio was

1 : 0.9 : 2 in 1 mL of dimethylformamide The coupling reaction was performed two times for 3 h The resin was washed with dimethylformamide until the washing solution was colorless After this, the resin was washed with dichloromethane and dried overnight The next day, the peptide was cleaved and deprotected using reagent K [tri-isopropylsilan (5%), water (2.5%), trifluoroacetic acid (92.5%)] The cleavage was performed for 2.5 h at room temperature After this, the peptide was precipitated with diethyl ether and washed three times with ice-cold diethyl ether Cyclization was performed following the protocol of Bodansky and Bodansky [32]

The peptide was further purified by HPLC, and the identity was confirmed by MALDI-TOF MS Rhodamine-B–SST-14 has a 10-fold lower affinity for SSTR3 than unlabeled SST-14 [24]

Reduction of cell surface binding Cells grown in 24-well dishes were stimulated with 1 lm SST-14 in RPMI-1640 (0.1% BSA) for 0–120 min at 37C Cells were placed on ice, washed three times with chilled acidic buffer, and incubated with 100 000 c.p.m per 0.3 mL of [125I]Tyr11-SST-14, 0.01 nm SST-14, and 0.1% BSA in RPMI-1640, at 4C for 90 min Bound [125

I]Tyr11-SST-14 was collected after lysing of the cells in 1 mL of

1 m NaOH and determined in a c-counter (Canberra Pack-ard, Dreieich, Germany) Calculations and graphical presentations were carried out using ms-excel and adobe photoshop Unspecific binding was determined in the presence of 0.1 mm SST-14 [20]

Recovery of cell surface binding Cells grown in 24-well dishes were stimulated with SST-14 (1 lm) in RPMI-1640 (0.1% BSA) for 120 min at 37C Surface-bound SST-14 was removed by three acidic washes with Hank’s buffered saline (HBS) (acetic acid, pH 4.8) and incubated for the indicated times in RPMI-1640 (0.1% BSA) The cells were placed on ice and incubated with

100 000 c.p.m per 0.3 mL of [125I]Tyr11-SST-14, 0.01 nm SST-14, and 0.1% BSA in RPMI-1640, at 4C for 90 min Bound [125I]Tyr11-SST-14 was collected after lysing of the cells in 1 mL of 1 m NaOH and determined in a c-counter (Canberra Packard) [20]

Determination of cell surface and total binding RIN-SSTR3 cells grown in 24-well dishes were stimulated with SST-14 (1 lm) in RPMI-1640 (0.1% BSA) at 37C for 60 min Cells were washed three times with HBS (acetic acid, pH 4.8) in the presence or absence of 0.1% saponin The cells were washed with RPMI-1640 to adjust the pH

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Surface binding sites were determined by incubation with

100 000 c.p.m per 0.3 mL of [125I]Tyr11-SST-14, 0.01 nm

SST-14, and 0.1% BSA in RPMI-1640, at 4C for 90 min

Total binding was determined by incubation with

100 000 c.p.m per 0.3 mL of [125I]Tyr11-SST-14, 0.01 nm

SST-14, 0.1% BSA and 0.1% saponin in RPMI-1640, at

4C for 90 min Bound [125I]Tyr11-SST-14 was collected

after lysing of the cells in 1 mL of 1 m NaOH and

deter-mined in a c-counter (Canberra Packard) [20]

Downregulation of cell surface binding sites

RIN-SSTR3 cells grown in 24-well dishes were stimulated

with SST-14 (1 lm) in RPMI-1640 (0.1% BSA) for the

indicated times at 37C Surface-bound SST-14 was

removed by three acidic washes with HBS (acetic acid,

pH 4.8) and incubated for 120 min in RPMI-1640 (0.1%

BSA) The cells were placed on ice and incubated with

100 000 c.p.m per 0.3 mL of [125I]Tyr11-SST-14, 0.01 nm

SST-14, and 0.1% BSA in RPMI-1640, at 4C for 90 min

Bound [125I]Tyr11-SST-14 was collected after lysing of the

cells in 1 mL of 1 m NaOH and determined in a c-counter

(Canberra Packard) [20]

Uptake of [125I]Tyr-labeled ligand

RIN 1046-38 cells transfected with SSTR3–HSV cDNA

were seeded in 24-well microplates and grown to 75%

con-fluence The culture medium was replaced by serum-free

medium containing [125I]Tyr11-SST-14 or [125

I]Tyr1-octreo-tide (100 000 c.p.m., 2000 CiÆmmol)1) and 0.1% BSA

pre-warmed to 37C, and incubated at this temperature for the

indicated times Cells were then washed at acidic pH to

remove all cell surface-bound peptide [33], and

cell-associ-ated radioactivity was determined in a c-counter (LKB

Wallac, Ontario, Canada) following lysis of the cells in 1 m

NaOH In parallel experiments, cell surface binding was

determined at 0C [20] Cell-associated radioactivity was

expressed as percentage of total cell surface-bound

radio-activity In addition, the experiment was carried out in the

presence of 40 mm NH4Cl [11]

HPLC analysis of internalized and released

[125I]Tyr-labeled ligand

RIN-SSTR3 cells grown in 24-well dishes were stimulated

for 0–30 min with [125I]Tyr11-SST-14 or [125

I]Tyr1-octreo-tide (100 000 c.p.m.) in RPMI-1640 (0.1% BSA) in the

presence or absence of 40 mm NH4Cl The cells were

washed in acidic buffer and incubated for 0–90 min in

RPMI-1640 (0.1% BSA) The supernatants were collected,

and acidified by adding 10 lL of trifluoroacetic acid The

supernatants were centrifuged (5 min, 13 000 g) and

sub-jected to HPLC separation Cell-associated radioactivity

was determined by adding 0.5 mL of HPLC buffer A Lysed cells were centrifuged (5 min, 13 000 g) and subjected

to HPLC separation HPLC was performed on a reverse-phase C-18 column (2· 25 mm) A separating gradient of 0–40% acetonitrile⁄ 0.08% trifluoroacetic acid for 25 min at

a flow rate of 1 mLÆmin)1 was used with an HPLC-Akta (General Healthcare, Munich, Germany) The HPLC gradient was fractionated every minute, and the eluted radioactivity was determined in a c-counter (LKB Wallac) The radioactivity of each fraction was divided by the initial amount of cell-associated radioactivity determined after

15 min of incubation with 100 000 c.p.m.ÆmL)1 radioacti-vity [11]

Microscopy and immunofluorescence Cells were incubated with SST-14 (1 lm) for 1300 min, washed, and incubated for 90 min at 37C The cells were fixed with paraformaldehyde 4%, washed, and incubated for

30 min in NaCl⁄ Pi(0.05% saponin, 5% normal goat serum) SSTR3–HSV was detected using mouse antibody against glycoprotein D (1 : 10 000) and Texas Red-conjugated anti-mouse IgG (1 : 200) In other experiments, cells were incu-bated with FITC–SST-14 or rhodamime-B–SST-14 on ice in RPMI-1640 and 0.1% BSA Unbound ligand was washed off, and the cells were incubated for the indicated times at

37C, washed with HBS ⁄ acetic acid (pH 4.75) at 4 C, fixed, and permeabilized for 30 min in HBS, 5% normal goat serum, and 0.05% saponin SST-14 was detected using the fluorescence dye, cathepsin D was detected using polyclonal antiserum against cathepsin D, and SSTR3–HSV was detected by using mouse antibody against glycoprotein D (1 : 10 000, overnight incubation at 4C) FITC-conjugated

or Texas Red-conjugated goat anti-(mouse IgG) or goat anti-(rabbit IgG) were used as secondary antibodies (1 : 200,

1 h, room temperature) Cells were embedded in Vectashield mounting medium (Vector, Burlingame, CA, USA) and observed with confocal microscopy [20,32]

Acknowledgements

This work was supported by grants from IZKF (STEI2⁄ 076 ⁄ 06), SFB 293 (A14), SFB 492 (B13), DFG STE 1014⁄ 2-2 (to M Steinhoff), the Rosacea Foundation (to M Steinhoff and D Roosterman) and IMF Mu¨nster (RO 120611) (to D Roosterman)

References

1 Olias G, Viollet C, Kusserow H, Epelbaum J & Meyer-hof W (2004) Regulation and function of somatostatin receptors J Neurochem 89, 1057–1091

2 Csaba Z & Dournaud P (2001) Cellular biology of somatostatin receptors Neuropeptides 35, 1–23

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