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Tiêu đề Loss-of-function variants of the human melanocortin-1 receptor gene in melanoma cells define structural determinants of receptor function
Tác giả Jesús Sánchez Más, Concepción Olivares Sánchez, Ghanem Ghanem, John Haycock, José Antonio Lozano Teruel, José Carlos Garcı́a-Borrón, Celia Jiménez-Cervantes
Trường học University of Murcia
Chuyên ngành Biochemistry and Molecular Biology
Thể loại journal article
Năm xuất bản 2002
Thành phố Murcia
Định dạng
Số trang 9
Dung lượng 336,63 KB

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Loss-of-function variants of the human melanocortin-1 receptorgene in melanoma cells define structural determinants of receptor function Jesu´s Sa´nchez Ma´s1, Concepcio´n Olivares Sa´nc

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Loss-of-function variants of the human melanocortin-1 receptor

gene in melanoma cells define structural determinants

of receptor function

Jesu´s Sa´nchez Ma´s1, Concepcio´n Olivares Sa´nchez1, Ghanem Ghanem2, John Haycock3,

Jose´ Antonio Lozano Teruel1, Jose´ Carlos Garcı´a-Borro´n1and Celia Jime´nez-Cervantes1

1

Department of Biochemistry and Molecular Biology, School of Medicine, University of Murcia, Spain;2LOCE,

Free University of Brussels, Brussels, Belgium;3Department of Engineering Materials, University of Sheffield, Sheffield, UK

The a-melanocyte-stimulating hormone (aMSH) receptor

(MC1R) is a major determinant of mammalian skin and hair

pigmentation Binding of aMSH to MC1R in human

mel-anocytes stimulates cell proliferation and synthesis of

pho-toprotective eumelanin pigments Certain MC1R alleles

have been associated with increased riskof melanoma This

can be theoretically considered on two grounds First,

gain-of-function mutations may stimulate proliferation, thus

promoting dysplastic lesions Second, and opposite,

loss-of-function mutations may decrease eumelanin contents, and

impair protection against the carcinogenic effects of UV

light, thus predisposing to skin cancers To test these

possi-bilities, we sequenced the MC1R gene from seven human

melanoma cell (HMC) lines and three giant congenital nevus

cell (GCNC) cultures Four HMC lines and two GCNC

cultures contained MC1R allelic variants These were the

known loss-of-function Arg142His and Arg151Cys alleles

and a new variant, Leu93Arg Moreover, impaired response

to a superpotent aMSH analog was demonstrated for the cell line carrying the Leu93Arg allele and for a HMC line homozygous for wild-type MC1R Functional analysis in heterologous cells stably or transiently expressing this vari-ant demonstrated that Leu93Arg is a loss-of-function mutation abolishing agonist binding These results, together with site-directed mutagenesis of the vicinal Glu94, demon-strate that the MC1R second transmembrane fragment is critical for agonist binding and maintenance of a resting conformation, whereas the second intracellular loop is essential for coupling to the cAMP system Therefore, loss-of-function, but not activating MC1R mutations are com-mon in HMC Their study provides important clues to understand MC1R structure-function relationships Keywords: melanocortin 1 receptor; melanoma; loss-of-function mutations; loss-of-functional coupling; structure-loss-of-function relationships

G protein-coupled receptors (GPCRs) constitute the largest

family of cell surface receptors involved in signal

transduc-tion, with over 1% of the human genome encoding for more

than 1000 proteins of this type [1] The structural hallmarks

of GPCRs are an heptahelical transmembrane structure,

with an N-terminal extension of variable length facing the extracellular side of the cell membrane, and an intracellular C-terminus, which is often post-translationally modified by acylation of conserved Cys residues [2] Recent evidence supports a role of GPCRs in the control of normal and aberrant cell growth Indeed, many potent mitogens stimu-late cell proliferation upon binding to their cognate GPCRs [3–5], and the mas oncogene belongs to this superfamily [6] Moreover, activating mutations of members of the GPCR family cause several dysplatic syndromes such as hyper-functioning thyroid adenoma [7], familial male precocious puberty [8], and Jansen-type metaphyseal chondrodysplasia [9]

The melanocortin 1 receptor (MC1R) is a GPCR involved in the regulation of key aspects of mammalian skin biology, which belongs to a subfamily of the GPCRs comprising five members designated MC1 to MC5 [10] The genes encoding for the mouse and human MC1R were cloned in 1992 [11] The human MC1R gene maps to chromosome 16q2 and contains an open reading frame of

954 base pairs corresponding to a 317 amino acids protein

It is highly polymorphic [12], and specific variants have been found associated with red hair and fair skin [13–15] The preferential natural agonists of MC1R are aMSH and adrenocorticotropic hormone Both proopiomelano-cortin-derived peptides bind to the MC1R with the same

Correspondence to C Jime´nez-Cervantes, Department of Biochemistry

and Molecular Biology, School of Medicine, University of Murcia,

Apto 4021 Campus de Espinardo, 30100 Murcia, Spain.

Fax: + 34 68 830950, Tel.: + 34 68 364676,

E-mail: celiajim@um.es

Abbreviations: FSK, forskolin; GPCR, G protein coupled receptor;

GCNC, giant congenital nevus cells; HMC, human melanoma cells;

MC1R, human melanocortin 1 receptor; mc1r, mouse melanocortin 1

receptor; aMSH, a-melanocyte stimulating hormone; NDP-MSH,

[Nle4,D-Phe7]-a-melanocyte stimulating hormone; TM,

transmembrane.

Note: The research group web site is available at http://www.um.es/

bbmbi/melanocitos.htm

Note: Nucleotide sequence data are available at the DDBJ/EMBL/

GenBankdatabases under the accession numbers AF326275

(con-sensus wild-type MC1R sequence), and AF529884 (Leu93Arg MC1R

variant) The SWISS-PROT entry for human MC1R is Q01726.

(Received 20 August 2002, revised 14 October 2002,

accepted 23 October 2002)

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affinity and, upon binding to the receptor, trigger the

cAMP cascade, thus activating a variety of intracellular

signaling pathways [16] As a result of MC1R activation,

the activity of the rate-limiting enzyme in melanin

synthe-sis, tyrosinase, is increased and skin pigmentation is

promoted Melanin pigments are complex heteropolymers,

which can be classified into two main groups: the brown to

blackeumelanins, and the reddish to yellow,

sulfur-containing phaeomelanins [17] Although both types of

melanins are found in different relative proportions in all

skin types, the phaeomelanin/eumelanin ratio is higher in

individuals with red hair and fair skin [18] Activation of

MC1R by its agonists promotes the switch from phaeo- to

eumelanogenesis, and increases the

eumelanin/phaeomela-nin ratio [10] Eumelaeumelanin/phaeomela-nins are photoprotective pigments,

and UV irradiation is considered the main ethiologic factor

for skin cancers Thus, it can be hypothesized that an

impairment of the normal function of the aMSH/MC1R

system as a result of loss-of-function mutations in the

MC1Rgene, might lead to an increased riskof melanoma

In keeping with this view, an association of several MC1R

allelic variants with increased melanoma and

nonmel-anoma skin cancer risk has been demonstrated [19–21]

These variants were subsequently shown to be

loss-of-function mutations [22]

In addition to its effect on melanocyte differentiation, it is

well established that aMSH stimulates normal melanocyte

proliferation [23] Because of this mitogenic activity, it could

also be thought that hyperactivity of the aMSH/MC1R

system might promote abnormal melanocyte growth, thus

contributing to premalignant or malignant phenotypes In

agreement with this, growth of normal melanocytes and

nevus cells in culture, but not of melanoma cells, is

dependent on aMSH and/or other stimulators of the cAMP

cascade [24]

Most studies on the possible involvement of MC1R

gene variants in melanoma reported thus far are

case-control studies where MC1R was sequenced from

peripheral blood of melanoma patients or healthy

indi-viduals These studies have established an increased risk

of melanoma associated with MC1R loss-of-function

variants leading to light skin phototypes, and hence to

increased UV sensitivity However, they might have failed

to detect somatic gain-of-function mutations of the

MC1R gene within melanocytes, leading to increased,

aMSH-independent proliferation In order to establish

whether or not activating mutations are present in

malignant or premalignant melanocytes, we have

sequenced the entire open reading frame of the MC1R

gene from cultured HMC and GCNC The functional

properties of the allelic variants found have been

analyzed Moreover, we have compared the

aMSH-triggered responses in heterologous cells expressing the

receptor variants under study, and the ones of malignant

melanocytes of defined MC1R genotype Our results

show that loss-of-function, but not gain-of-function,

mutations of MC1R are indeed frequent in HMC lines,

and that impairment of signaling through the cAMP

cascade occurs in these cells even in the absence of

mutations in the coding region of the gene Finally, our

study of the natural MC1R variants highlights several

aspects of the structure–function relationships in the

MC1R protein, such as the critical importance of the

TM2 fragment and the second cytosolic loop, and can target the design of site-directed mutagenesis studies

M A T E R I A L S A N D M E T H O D S

Cell culture Seven HMC lines were used HBL and LND1 cell lines were established at the LOCE, Brussels, Belgium DOR, IC8 and T1C3 cells were a gift from J F Dore´, INSERM, Lyon, France The IC8 and T1C3 cells are clones of the same melanoma line and were isolated based on their different metastatic potential A375-SM cells were a gift from I J Fidler (University of Texas M D., Houston, TX, USA), and C8161 a gift from Prof Meyskens (University of California, Irvine, CA, USA) All HMC lines were cultured

as previously described [25] in HAM-F10 medium supple-mented with 5% fetal bovine serum, 5% newborn calf serum, 2 mM glutamine, 100 UÆmL)1 penicillin, 0.1 mgÆmL)1streptomycin sulfate and 0.1 mgÆmL)1 kana-mycin sulfate (all from Gibco, Paisley, UK) Three primary cultures of GCNC were also analyzed Isolation and culture

of GCNC was performed as described [26] Briefly, the tissue was incubated overnight in HAM-F10 medium containing 0.6 UÆmL)1dispase and 0.05 UÆmL)1 collage-nase, supplemented with 200 UÆmL)1 penicillin G, 0.2 mgÆmL)1streptomycin sulfate, 0.2 mgÆmL)1kanamycin sulfate and 25 lgÆmL)1gentamycin The detached cells were washed, seeded in culture flasks at the density of

105cellsÆmL)1 and incubated for 48 h with 0.1 mgÆmL)1 geneticin in the culture medium described, supplemented with 2% Ultroser-G, 16 nM phorbol 12-myristate 13-acetate, and 0.1 mMisobutyl methylxanthine GCNC were cultured for a maximum of 15 passages

DNA extraction, amplification of theMC1R gene and sequencing

Genomic DNA was extracted from cultured cells with the Wizard kit (Promega, Madison, WI) The complete MC1R coding sequence was amplified by PCR, with the forward

ACA (called universal MC1R forward primer), and the

TGCACCGC These primers match nucleotides 435–456 and 1418–1439, respectively, according to the sequence reported in [11], and yield a 1023-bp fragment that can be cloned by means of added HindIII and EcoRI restriction sites (underlined) Thirty PCR rounds (denaturation for

1 min at 95C, annealing for 2 min at 68 C and extension for 3 min at 72C, followed by a final 10 min extension at

72C) were performed using 1 lg of genomic DNA, 0.5 lg

of each primer, 200 lM each dNTP and 2.5 U of the proofreading Pfu polymerase The PCR products were purified by agarose gel electrophoresis and completely sequenced in both strands using internal primers, at the DNA sequencing facility of the Centro de Investigaciones Biolo´gicas, Madrid, Spain When necessary for functional studies, the amplification product was cloned in the expression vector pcDNA3 (Invitrogen, Carlsbad, CA, USA), using the added restriction sites, following standard procedures [27] The identity of the clones was ascertained

by complete resequencing of the cloned inserts

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Transient expression of MC1R

HEK 293T cells were grown in six-well plates with RPMI

1640, 10% fetal bovine serum, 100 UÆmL)1penicillin and

0.1 mgÆmL)1 streptomycin Transfection was carried out

with the Superfect reagent (Qiagen, Paisley, UK), as per

instructions, with 1.5 lg plasmid DNA per well Three

hours after adding the transfection mix, the medium was

removed Cells were gently washed with 500 lL NaCl/Pi

and 1 mL of fresh medium was added After 24 h, cells were

completely serum-deprived for an additional 24 h before

binding or coupling assays

Radioligand binding assay

Transfected cells were incubated (1 h, 37C) with

increas-ing concentrations of [Nle4,D-Phe7]-aMSH (NDP-MSH,

Sigma, Saint Louis, MO, USA), ranging from 10)12 to

10)6M and a fixed amount of 125I-labelled-NDP-MSH

(Amersham Pharmacia Biotech, Little Chalfont,

Bucking-hamshire, UK), corresponding to 10)10Mand 0.1 lCi per

well, in a final volume of 500 lL RPMI Cells were then

washed twice with RPMI for 5 min at room temperature,

and trypsinized The cell suspension was pipetted into

plastic tubes and the associated radioactivity was measured

Non-specific binding was estimated from the radioactivity

bound in the presence of 10)6M NDP-MSH or to cells

transfected with empty vector and incubated with 125

I-labelled-NDP-MSH alone, with similar results

Determination of agonist-induced cAMP increases

Cells were serum-deprived for 24 h and then incubated

with 10-13)10-7

M NDP-MSH, for 20 min The medium

was aspirated, cells quickly washed with 1 mL ice-cold

NaCl/Pi, lysed with 350 lL preheated 0.1M HCl (70C),

and carefully scrapped The resulting mix was freeze-dried

for 90 min, washed with 100 lL H2O, and freeze-dried for

another 20 min Dried samples were dissolved in suitable

volumes of 50 mMTris, 4 mMEDTA, pH 7.5, from 65 to

300 lL, depending on the expected cAMP content cAMP

was measured by radioimmunoassay (Amersham

Phar-macia Biotech), as per instructions Parallel dishes for

protein determination were included Cells were dissolved

in 10 mM phosphate buffer pH 7, 1% Igepal CA-640,

containing 0.1 mM EDTA, and 0.1 mM

phenyl-methanesulfonyl fluoride The protein concentration in

these lysates was determined by the bicinchoninic acid

method

Construction and cloning of a MC1R tagged-sequence

The wild-type and Leu93Arg variant sequences of MC1R

were tagged by adding a (HA)2His6tag to the C-terminus

of the protein This tag corresponds to the sequence

immediately after the C-terminal W317 residue of

MC1R It contains two consecutive influenza virus

hemagglutinin epitopes (HA) and a terminal hexahistidine

sequence (His6) In order to prepare the constructs, we

amplified the tag sequence from the pREP1-cdc2Ha6His

vector (a kind gift from Prof Jose´ Cansado, Department

of Genetics and Microbiology, University of Murcia,

Spain) by using the primers CGCGAATTCTACCCA TACGAT (forward) and AGCTCTAGATTAGTGGT GATG (reverse), containing EcoRI and XbaI sites (underlined) We also amplified the complete coding sequence of the wild-type and Leu93Arg variant of MC1R with the universal MC1R forward primer and

CAG reverse primer This primer contains an EcoRI restriction site before a stop codon (shown in bold) and a XbaI site immediately after it PCR amplification reactions were performed with 30 ng of template DNA, 0.5 lg of each corresponding primer, 200 lMeach dNTP and 2.5 U

of the proofreading Pfu polymerase Thirty rounds of amplification were carried out (denaturation 1 min at

95C, annealing 2 min at 48 C and extension for 3 min

at 72C) The MC1R amplicons were cloned into pcDNA3 by means of the HindIII and XbaI restriction sites The tag sequence was then cloned into the MC1R-pcDNA3 constructs, with the added EcoRI and XbaI sites The identity of the products was verified by complete sequencing

Construction of the Glu94Lys MC1R variant The Glu94Lys variant was generated in two PCR steps First, we used the universal MC1R forward primer and the reverse primer GACGGCCGTCTTCAGCACGTTGCT, which introduces the desired amino acid change (variant base shown in bold), to yield a 328-bp fragment This amplicon was then used as a forward primer with the rev-erseCTGGAATTCACACTTAAAGCGCGTGCACCGC (stop codon in bold, EcoRI site underlined) The resulting cDNA was cloned into pcDNA3 The sequence of this artificial variant was ascertained by double strand DNA sequencing

Western blot and related procedures Cells were solubilized in 50 mM Tris/HCl, pH 8.8, 1 mM EDTA, 1% Igepal CA-630 and 10 mM iodoacetamide, and then centrifuged at 105 000 g, for 30 min in a table-top Beckman TL-100 ultracentrifuge Electrophoresis was performed in 10% acrylamide gels, under reducing conditions For immunochemical detection of the tagged MC1R constructs in extracts from transfected cells, 10 lg

of protein from each sample were mixed in a 2 : 1 ratio with sample buffer (0.18M Tris/HCl, pH 6.8, 15% glycerol, 0.075% bromophenol blue, 9% SDS, and 3M

2 mercaptoethanol) For deglycosylation studies, the extracts were heated at 95C for 5 min prior to incuba-tion at 37C for 4 h in the presence of 5 U of N-glycosidase F (from Roche, Mannheim, Germany) in

a 50-mM phosphate buffer, pH 7.0, containing 10 mM EDTA and 0.1% SDS Control samples were treated under identical conditions, except for the omission of the glycosidase These samples were processed as previously described for electrophoresis Gels were transferred to poly(vinylidene difluoride) (PVDF) membranes, blocked with 5% nonfat dry milkand incubated overnight at 4C with a monoclonal anti-HA Ig (Sigma) as per instructions Staining of immunoreactive bands was performed with a chemiluminescent substrate (Amersham Pharmacia Bio-tech), after incubation with a peroxidase-labeled secondary

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antibody Comparable loading and transfer were

ascer-tained by cutting the lower portion of the membrane

before blocking and staining for total protein with Amido

Black

R E S U L T S A N D D I S C U S S I O N

Seven HMC lines and three GCNC cultures were selected

for genotyping and functional studies, based mostly on

previous observations of high MC1R gene expression at the

mRNA level [28] Sequencing of the complete coding region

of MC1R after amplification of genomic DNA with suitable

primers [29,30] showed that four HMC, and two GCNC

cultures harbored MC1R variants (Table 1) The variants

found were the well-known Arg151Cys and Arg142His

alleles and a new variant not reported so far, to the best of

our knowledge, the Leu93Arg allele That this variant was

indeed present in the sample and was not the result of a

PCR artifact was ascertained by repeated amplification and

sequencing reactions, and by the observation that the same

allele was found in the IC8 and T1C3 cell lines, which both

come from the same parental cell line and correspond to two

clones isolated on the basis of their different metastatic

potential (J F Dore´, personal communication) The

posi-tions within the MC1R molecule of the substituposi-tions found

in our study are shown in Fig 1, where several other

functionally relevant residues are also highlighted

The Arg151Cys and Arg142His alleles are two

well-documented loss-of-function MC1R variants [22,34] The

Arg151Cys allele is strongly associated with red hair

[14,15,22,35], and its functional impairment might be related

to deficient coupling to the cAMP signaling pathway, as it

has been reported that the binding properties of the mutant

receptor are very similar, if not identical, to wild-type

[22,34] The Arg142His substitution has a similar functional

effect, with conserved binding properties but strongly

impaired coupling to the cAMP generation system [22]

Interestingly, both substitutions are located in the second

intracellular loop of the receptor protein, thus highlighting

the contribution of this region to efficient coupling to GS

Moreover, Arg142 is part of a DRY sequence conserved in

most if not all GPCRs, and particularly in all members of the melanocortin receptors subfamily

We next tried to correlate the MC1R genotype of several

of the HMC lines with their degree of responsiveness to agonists, by studying their cAMP levels after treatment with the superpotent melanocortin analog NDP-MSH (Fig 2) LND1 and HBL cells, homozygous for the wild-type allele, both responded with strong and concentration-dependent increases in cAMP, although the maximal levels of the second messenger were higher for the former Surprisingly, both DOR cells, homozygous for wild-type MC1R, and IC8 cells, carrying one variant Leu93Arg allele, failed to increase their cAMP intracellular levels in response to the superpotent agonist That this failure is not due to a defective adenylyl cyclase was shown by a strong stimulation of the enzyme activity in cells treated with the specific activator forskolin (Fig 2, B) Conversely, DOR and IC8 cells also failed to respond to the natural agonists aMSH and adrenocortico-tropic hormone, employed at a saturating concentration of

10)7M(not shown) It is worth noting that the unrespon-siveness of DOR cells is also unrelated to a lackof MC1R gene expression, as we have previously found that the mRNA levels for MC1R are comparable in DOR, LND1 and HBL cells, and higher in these HMC than in normal human melanocyte cultures [28] Moreover, both DOR and IC8 cells display a significant number of specific binding sites,

in the range of 2500 ± 500 sites per cell This is approxi-mately 50% as compared to the responsive HBL cells The lackof functional coupling of these cell lines, particularly of DOR cells homozygous for the wild-type MC1R, is therefore perplexing and will be the subject of further studies

On the other hand, as opposed to the well-known Arg142His and Arg151Cys variants, no functional data are available for the new Leu93Arg allele Although the unresponsiveness of the IC8 HMC line suggested that it may correspond to a loss-of-function mutation, no clear conclusion could be drawn at this stage, as DOR cells, homozygous for wild-type MC1R, were also defective in signaling through cAMP Therefore, we performed a func-tional analysis of the Leu93Arg MC1R For comparison,

Table 1 Occurrence of MC1R variant alleles in human melanoma and

GCN cells.

a

0, homozygous wild-type; 1, variant heterozygous; 2, variant

compound heterozygous; 3, variant homozygous b The IC8 and

T1C3 cells lines derive from the same patient, and correspond to

two different clones selected on the basis of their different

meta-static potential.

Fig 1 Structure of MC1R The topology of the TM fragments is depicted according to the model proposed in [31], and the length of the signal peptide (hatched first 22 amino-terminal residues) was estimated according to [32] The allelic variants found in this study, as well as other natural loss-of-function mutations described in the literature (reviewed in [33]) are specified (gray circles) and highlighted by an arrow.

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the Arg151Cys receptor was also included in the study.

Figure 3 shows the coupling properties of the wild-type and

mutant receptors, as analyzed in clones of stably transfected

CHO cells As expected, Arg151Cys clones failed to respond

to saturating concentrations of NDP-MSH with increases in

their intracellular cAMP levels, thus confirming results by

others [22,34] A complete lackof functional coupling was

also observed for the Leu93Arg receptor Next, the binding

properties of both variants were compared to wild-type, in

order to determine whether lackof agonist-induced cAMP

generation was related to impaired binding or coupling

properties Clones stably transfected with the Leu93Arg

form were unable to specifically bind significant levels of

radiolabeled agonist (Fig 4) However, and as previously

reported by others [22], the affinity for NDP-MSH was

identical, within experimental error, for the wild-type and

the Arg151Cys receptors (not shown)

This result was in keeping with the lack of hormone-induced cAMP generation, and suggested that the func-tional impairment was mostly explained by the inability of the mutant receptor to bind melanocortins However, the possibility still existed that the unresponsiveness of the clones stably transfected with the Leu93Arg variant could

be related to other causes, such as low expression or aberrant processing of receptor molecules To checkthese possibilities, we performed transient expression experiments using HEK 293T cells Previous studies have shown that, in

Fig 2 Functional coupling of several HMC lines of defined MC1R

genotype (A) Dose–response curves for intracellular cAMP levels in

different HMC lines treated with increasing concentrations of

NDP-MSH Results are shown as mean ± SD (n ‡ 3) (B) Levels of cAMP

in human melanoma cell lines treated with a saturating concentration

of NDP-MSH (10)7M ), or with the adenylyl cyclase stimulator

forskolin (FSK, 10)5M ), for 20 min Results are the mean ± SD of

two independent experiments, each performed in triplicate dishes.

Fig 3 Lack of functional coupling of the Arg151Cys and Leu93Arg MC1R in stably transfected CHO cells CHO cells from clones stably transfected with the variants indicated, and selected on the basis of high MC1R expression at the mRNA level, were seeded in six-well plates, grown to semiconfluence and serum-deprived for 24 h Then, the cells were challenged with vehicle or with 100 n M NDP-MSH for

20 min, before cell lysis and determination of the cAMP contents in the lysates For each clone, parallel dishes were solubilized for protein determination Results are the mean ± SD of two independent experiments, each performed in triplicate dishes (n ¼ 6) Similar results were obtained with two independent clones for each variant.

Fig 4 Inability of the Leu93Arg MC1R variant to bind NDP-MSH Clones of CHO cells stably transfected with the variant or wild-type receptor were seeded in six-well plates, and incubated with a fixed amount of125I-labelled-NDP-MSH in 500 lL of serum-free medium

in the presence of increasing concentrations of unlabeled agonist After washing and harvesting as described in Materials and methods, the radioactivity associated with the cell pellets was counted Results are the mean ± SD of two independent experiments, each performed in triplicate dishes (n ¼ 6).

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this system, the expression of MC1R binding sites is high,

with Bmaxvalues ranging from 2 to 8 pmolesÆmg protein)1,

depending on the construct under study [30] Figure 5

shows that the Leu93Arg mutant was also unable to

mediate cAMP increases (A) or bind significant levels of

radiolabeled agonist (B), under conditions of strong

over-expression in transiently transfected HEK 293T cells Under

identical conditions, the wild-type construct, which was

expressed at a density of 2.2 ± 0.25 pmoles binding sites per mg protein, was highly efficient in eliciting a cAMP response in cells challenged with NDP-MSH Moreover, MC1RmRNA levels for the wild-type and Leu93Arg alleles were very similar in transiently transfected cells (C) This was expected, as the two constructs are identical except for the single base substitution in codon 93 determining the Arg

to Leu mutation On the other hand, in order to detect

Fig 5 The Leu93Arg MC1R variant is adequately expressed in transiently transfected HEK 293T cells, but fails to bind agonists or elicit agonist-induced cAMP increases (A) Functional coupling to cAMP production in cells transfected with empty vector (pcDNA), wild-type receptor or the Leu93Arg variant Cells were serum deprived 24 h before the measurement of cAMP under basal conditions (empty bars), or after stimulation with NDP-MSH (10)7M , closed bars) Results are the mean ± SD of quadruplicate independent dishes (B) Equilibrium binding of125 I-labelled-NDP-MSH to the transiently expressed wild-type and Leu93Arg variants Transiently transfected cells seeded in six-well dishes were incubated for 1 h in the presence of 10)10M125I-labelled-NDP-MSH, corresponding to 0.1 lCi per well Data are given as specifically bound c.p.m., after subtraction of the radioactivity bound to cells treated under identical conditions but in the presence of 10)6M unlabeled NDP-MSH Results are the mean ± SD

of quadruplicate independent dishes (C) Comparable levels of MC1R mRNA in cells transfected with the wild-type or Leu93Arg constructs Cells were seeded in 25 cm 2 flasks and transfected with empty vector (–), or the wild-type (WT) or Leu93Arg (L93R) receptors, under conditions comparable to the transfections for functional studies Total RNA was extracted and analyzed for MC1R mRNA abundance by Northern blot (upper), as previously described [28] Comparable loading was ascertained by probing the membranes with a GAPDH probe (lower) Specific signals were detected in a GS-525 phosphorimager from Bio-Rad (Hercules, CA) (D) Upper: Western blot detection of epitope-tagged Leu93Arg (Arg93-T) and wild-type (WT-T) receptors The electrophoretic mobility of molecular weight markers is shown on the left, and the molecular weight

of the specific bands is shown on the right (expressed in kDa) The specificity of the bands is clearly demonstrated by their absence in the lane corresponding to cells transfected with empty vector (–) Lower: effect of treatment with N-glycosidase F on the electrophoretic mobility of the tagged receptor protein Control and glycosidase F-treated (EndoF) extracts from cells transfected with the WT-T construct were analyzed by Western blot using the anti-HA monoclonal antibody Upon treatment with the glycosidase, the band of higher molecular size was transformed into

a band comigrating with the lower molecular weight form.

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possible effects on protein stability and/or processing, two

constructs were prepared, where an epitope-containing tag

was included at the C-terminus of the wild-type and Arg93

proteins, so as to enable the detection of the transiently

expressed proteins by Western blots These constructs,

termed WT-T and Arg93-T were identical to the ones used

in functional studies, except for the presence of an in frame

C-terminal extension coding for 27 amino acids, with two

HA and an His6 epitope

The protein levels of the tagged Arg93 protein were easily

detectable by Western blot By means of an

antihemagglu-tinin antibody, an identical electrophoretic pattern, with two

bands corresponding to apparent molecular weights of 34

and 38.7 kDa were detected for the WT-T and Arg93-T

receptors (D) The relationship of these bands was studied

by deglycosylation of the samples followed by Western

blotting In samples deglycosylated with N-glycosidase F,

only the higher mobility band was observed, thus showing

that this band does not correspond to a degradation

product of the higher molecular weight protein Rather, the

faster band is very likely the de novo form of the tagged

MC1R, which, upon glycosylation and post-translational

processing, gives raise to the lower mobility band In any

case, the slightly lower levels of the Arg93-T protein, as

compared to the wild-type, do not seem to be sufficient to

account for the complete loss of functional response in

terms of agonist binding or coupling to adenylyl cyclase,

specially considering the high overexpression obtained

under our experimental conditions Moreover, the identical

electrophoretic pattern strongly suggests that the Leu93Arg

mutation has no effect on the processing of the receptor

molecule, at least as studied with the tagged forms of the

protein Taken together, these results show that the

efficiency of expression of wild-type and Leu93Arg MC1R

is similar at the mRNA and protein levels, yet neither

agonist binding or functional coupling can be demonstrated

for the Leu93Arg mutant

Therefore, the lackof specific binding of melanocortins to

the Leu93Arg receptor most likely reflects an actual

impair-ment of the receptor binding properties Consistent with this

hypothesis, a pocket located between TM domains 2, 3 and 6

or 7 is probably responsible for the docking of agonists

[32,36,37] Within this pocket, acidic residues Glu94 in TM2

and Asp117 or Asp121 in TM3 have been shown to be

critical for ligand–receptor interactions [37] These negatively

charged residues are presumably spatially adjacent and

would provide a hydrophilic binding pocket interacting with

the positively charged Arg8 of theD-Phe7-Arg8-Trp9 core

sequence of NDP-MSH [37] Within this context, it appears

likely that the introduction of a positively charged residue at

position 93 might either interfere with the positively charged

Arg8 residue of the agonist, or alternatively, counteract a

negative charge in the receptor protein important for

electrostatic interaction with the agonist It is worth noting

that a constitutively active variant of the mouse Mc1r, the

naturally occurring somber Eso)3J allele is also associated

with a substitution of a charged residue in TM2, namely

Glu92Lys, and that Glu92 in Mc1r is equivalent to Glu94 in

human MC1R Interestingly, the constitutively active

som-ber Mc1r might also display a reduced binding affinity [38]

Therefore, the functional properties of the naturally

occurring Leu93Arg variant, along with site-directed

muta-genesis studies reported by others [37], strongly suggest that

the TM2 fragment of human MC1R plays a pivotal role in agonist binding, and might also be an important determi-nant of the receptor coupling properties To further explore this possibility, we generated an artificial construct homo-logous to the mouse somber Eso)3Jallele, namely Glu94Lys, and analyzed its functional properties in transiently trans-fected HEK 293T cells The coupling behaviour of the MC1R mutant was highly reminiscent of the one reported

by Robbins et al [38] for the mouse somber allele (Fig 6A) After transfection in HEK 293T cells, human Glu94Lys MC1R displayed a noticeable agonist-independent consti-tutive activity, as shown by the induction of high levels of cAMP These levels corresponded to approximately 50% of the maximal stimulations achieved, and were approximately twice as high as those found in cells transfected with the wild-type receptor Also in keeping with results reported for the mouse Eso)3J allele, higher stimulations of adenylyl cyclase were only obtained at high agonist doses (Fig 6A), consistent with a loss of binding affinity observed in radioligand binding assays (Fig 6B) This reduced affinity for NDP-MSH of the Glu94Arg variant was evident by a

Fig 6 Functional analysis of an artificial MC1R homologue of the mouse somber Eso)3J constitutively active allele (A) Functional coupling to the cAMP production system (B) Displacement curves of

125 I-labelled-NDP-MSH (10)10M in the incubation medium) by the indicated concentrations of unlabeled ligand The radioactivity bound

by the Glu94Lys variant in the absence of competing ligand was approximately four times lower than for the wild-type receptor.

Trang 8

two logs rightwards shift of the displacement curve and by

the lower amount of radioactivity bound in the absence of

competitor (in spite of the lackof statistically significant

differences in the number of binding sites, Bmax)

In summary, our results show that impaired signaling

through the MSH/MC1R pathway is common in HMC

lines, consistent with previous reports of increased

melan-oma riskin individuals carrying germline mutations of the

MC1R gene [19–21], and with the notion that

loss-of-function mutations in the MC1R gene sensitize human

melanocytes to the DNA damaging action of UV light [39]

Moreover, functional analysis of naturally occurring

vari-ants highlights important features of structure-function

relationships within the receptor protein, and points to the

extracellular side of TM2 as a major determinant of agonist

binding Within this region, results by others have shown

that removal of the negative charge at position 94 strongly

diminishes agonist binding affinity [37], without yielding a

constitutively active receptor We have shown here that the

change of a neutral side chain for a positively charged amino

acid at position 93 completely abolishes agonist binding

Moreover, the nonconservative substitution of Glu94 for a

positively charged Lys residue not only decreases binding

affinity by two logs, but also confers constitutive activity to

the mutant receptor Therefore, the balance of electric

charges in the external side of TM2 (and, most likely, their

interactions with adjacent negative charges in TM3) not

only determines the ability of the receptor protein to bind

ligands with high affinity, but also the prevalence of a

resting, uncoupled conformation as opposed to an active

conformation able to couple to Gs in an

agonist-independ-ent fashion Again consistagonist-independ-ent with the crucial role of charge

interactions between the external side of TM2 and TM3, the

Cys125Arg mutation confers constitutive activity to the fox

receptor, and the homologous Cys123Arg mutation in the

mouse receptor displays a similar pharmacology, highly

reminiscent of the one observed for the mouse Glu92Lys

and the human Glu94Lys variants [10, this study] On the

other hand, residues present in the second intracellular loop

appear critical for interaction with G proteins Several

naturally occurring mutations in, or near this region, such as

the Arg142His, Arg151Cys and Arg160Trp and Arg162Pro

variants found by us and others abolish efficient coupling

without major effects on binding [22,29,34, this study]

Notably, with the possible exception of the Arg142His

allele, all these mutations abolish completely a positive

charge in the relatively short second intracellular loop It is

tempting to speculate that the overall positive charge of this

loop could be important for binding a negatively charged

surface of the Gs protein In many GPCRs, the third

intracellular loop and the cytoplasmic C-terminal extension

are the main regions involved in coupling to the G proteins

[2] It is clear that in the case of the MC1R, the contribution

on the second intracellular loop is also relevant

A C K N O W L E D G E M E N T S

This workhas been supported by grants PM1999-0138, from the DGI,

Ministry of Science and Technology, Spain and PTR1995-0582-OP.

Jesu´s Sa´nchez Ma´s is recipient of a fellowship from the Fundacio´n

Se´neca, Comunidad Auto´noma de la Regio´n de Murcia, and

Concepcio´n Olivares Sa´nchez of a FPI fellowship from the Ministry

of Education, Spain.

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