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Báo cáo khoa học: Secondary structure assignment of mouse SOCS3 by NMR defines the domain boundaries and identifies an unstructured insertion in the SH2 domain pdf

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SOCS3 consists of a short N-terminal sequence followed by a kinase inhibitory region, an extended SH2 domain and a C-terminal suppressor of cytokine signalling SOCS box.. SOCS3 and the r

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defines the domain boundaries and identifies an

unstructured insertion in the SH2 domain

Jeffrey J Babon1, Shenggen Yao1, David P DeSouza1,*, Christopher F Harrison1,*, Louis J Fabri2, Edvards Liepinsh3, Sergio D Scrofani2, Manuel Baca1,† and Raymond S Norton1

1 Walter and Eliza Hall Institute, Parkville, Victoria, Australia

2 Amrad Corporation Ltd, Richmond, Victoria, Australia

3 Department of Medical Biochemistry and Biophysics, Karolinska Institute, Stockholm, Sweden

Cytokine signalling acts through membrane-bound,

multisubunit receptor complexes that are

phosphoryl-ated by activphosphoryl-ated Janus kinases (JAKs), leading to

sub-sequent activation and phosphorylation of members of

the signal transduction and activators of transcription

(STAT) family The duration of the signalling response

is moderated by a classic negative feedback control

mechanism involving members of the suppressors of

cytokine signalling (SOCS) family (SOCS1–7) and cytokine-inducible SH2-containing protein (CIS) The SOCS family members share similar architecture, inclu-ding an N-terminal region of varying size, a central SH2 domain and a C-terminal SOCS box [1] (Fig 1) The SOCS SH2 domains are responsible for binding

to phosphorylated tyrosine residues on intracellular domains of the cytokine receptors and⁄ or the JAKs

Keywords

cytokine signalling; NMR; PEST sequence;

SOCS

Correspondence

J J Babon, Walter and Eliza Hall Institute,

1G Royal Parade, Parkville 3050, Victoria,

Australia

Fax: +61 3 93470852

Tel: +61 3 93452451

E-mail: babon@wehi.edu.au

Present addresses

*School of Biochemistry, University of

Melbourne, Parkville 3050, Australia;

†Amrad Corporation Ltd, 576 Swan Street,

Richmond 3121, Victoria, Australia

(Received 31 July 2005, revised 22

September 2005, accepted 10 October 2005)

doi:10.1111/j.1742-4658.2005.05010.x

SOCS3 is a negative regulator of cytokine signalling that inhibits Janus kinase-signal transduction and activator of transcription (JAK-STAT) mediated signal tranduction by binding to phosphorylated tyrosine residues

on intracellular subunits of various cytokine receptors, as well as possibly the JAK proteins SOCS3 consists of a short N-terminal sequence followed

by a kinase inhibitory region, an extended SH2 domain and a C-terminal suppressor of cytokine signalling (SOCS) box SOCS3 and the related pro-tein, cytokine-inducible SH2-containing propro-tein, are unique among the SOCS family of proteins in containing a region of mostly low complexity sequence, between the SH2 domain and the C-terminal SOCS box Using NMR, we assigned and determined the secondary structure of a murine SOCS3 construct The SH2 domain, unusually, consists of 140 residues, including an unstructured insertion of 35 residues This insertion fits the criteria for a PEST sequence and is not required for phosphotyrosine bind-ing, as shown by isothermal titration calorimetry Instead, we propose that the PEST sequence has a functional role unrelated to phosphotyrosine binding, possibly mediating efficient proteolytic degradation of the protein The latter half of the kinase inhibitory region and the entire extended SH2 subdomain form a single a-helix The mapping of the true SH2 domain, and the location of its C terminus more than 50 residues further down-stream than predicted by sequence homology, explains a number of previ-ously unexpected results that have shown the importance of residues close

to the SOCS box for phosphotyrosine binding

Abbreviations

CIS, cytokine-inducible SH2-containing protein; ESS, extended SH2 subdomain; IPTG, isopropyl thio-b- D -galactoside; ITC, isothermal titration calorimetry; JAK, Janus kinase; KIR, kinase inhibitory region; PtdIns, phosphatidylinositol; SOCS, suppressor of cytokine signalling; STAT, signal transduction and activator of transcription.

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themselves [2] They act therefore by directly blocking

signal transduction or by interfering with STAT access

to the phosphorylated receptor subunits

SOCS3, in particular, has a 22-residue N-terminal

segment, followed by a 12-residue kinase inhibitory

region (KIR) Mutation of essential residues in the

KIR, or its deletion, affects kinase inhibition without

affecting phosphotyrosine binding [3,4] One model

proposed to explain the KIR action is that it can

mimic the activation loop found in kinases such as

JAK2 and FGF receptor kinase [5] and prevent

sub-strate access to the catalytic groove of the kinase [6]

In support of this, the sequences of the SOCS3 and

SOCS1 KIRs share some homology with that of the

JAK1 and JAK2 activation loops [6] There is no

structural information available for the KIR, but if

this mechanism operates it implies that the KIR is an

extended loop or unstructured

Immediately following the KIR in SOCS3 is the

extended SH2 subdomain (ESS), an 11-residue segment

preceding the true SH2 domain, which can affect

phos-photyrosine binding via an unknown mechanism [3]

There is no direct structural information available for

the ESS, but sequence analysis, modelling [7] and the

slight homology shared between the ESS and similar

regions on Stat1 [8] and Stat3b [9] suggest that it may

consist of one or two a-helices

The SH2 domain of SOCS3 is immediately

down-stream from the ESS The SH2 domain is a common

motif, present in proteins capable of binding to

phos-photyrosine residues It typically contains around 100 residues, and adopts a fold consisting of a central b-sheet flanked on each face with an a-helix The SH2 domain of murine SOCS3 has been mapped previously

by sequence comparison to residues 46–142 [10], but mutagenesis experiments have shown that residues as far away as Leu182 are important for phosphotyro-sine–peptide binding [3] There is therefore some uncer-tainty about the extent of the SH2 domain, depending

on whether it is predicted by sequence homology or functional analysis

In addition to their role in blocking the activation

of downstream signalling intermediates, the SOCS pro-teins may also act by directing the degradation of bound signalling molecules [11] As the C-terminal SOCS box is capable of interacting with an E3–ubiqu-itin ligase complex by binding directly to elongins B and C [12], SOCS proteins can recruit bound signal transduction proteins, such as activated kinases or the cytokine receptors themselves, for proteasome-medi-ated degradation [11,13,14] Although there is no struc-tural information on the SOCS box, sequence and functional homologies suggest that it will adopt a sim-ilar structure to the corresponding region in the VHL protein [15], which is also responsible for binding to elonginB⁄ C Reports differ as to whether the interac-tion between elonginB⁄ C and SOCS stabilizes [16,17]

or destabilizes [12,18] the SOCS proteins themselves Unambiguous secondary structure assignment, whe-ther by NMR or owhe-ther spectroscopic techniques, can

socs1 socs2 socs3

socs4 socs5 socs6 socs7

CIS

N-terminal SH2 SOCS

box

P

P

P P

P P

Fig 1 The suppressor of cytokine signalling (SOCS) family of proteins The eight members of the SOCS family [SOCS1–7 and cytokine-indu-cible SH2-containing protein (CIS)] are shown schematically All eight members of the SOCS family contain a C-terminal SOCS box (black), a central SH2 domain (dark grey) and an N-terminal domain of varying lengths (light grey) CIS also contains a small insertion of  60 residues between the SH2 domain and the SOCS box (light grey) The SH2 domain boundaries shown for SOCS3 are as identified in this study The position of potential PEST motifs in the SOCS family, as suggested by this work, are indicated by a boxed ‘P’; note that they are not shown

to scale SOCS4–7 have much longer N-terminal domains than the other SOCS family members (300–400 residues), the dotted lines indicate that these regions are not drawn to scale The residue numbering refers to SOCS3 only.

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be a powerful tool in determining domain architecture.

In this study we show that the N-terminal portion of

the KIR of murine SOCS3 is unstructured, but the

C-terminal half of the KIR and the entire ESS form

one single a-helix In addition, we show that the SH2

domain is a 140-residue domain that contains a

35-residue unstructured PEST motif insertion which is

not required for phosphotyrosine binding but may

have an important functional role

Results

SOCS3 phosphotyrosine peptide complex

Two initial constructs of mouse SOCS3 [SOCS3(22–

225) and SOCS3(22–185)] were cloned and expressed

in Escherichia coli Both contain the KIR and the

extended SH2 domain, but SOCS3(22–185) lacks the

C-terminal SOCS box Both constructs expressed in

inclusion bodies in E coli and required refolding A

phosphotyrosine peptide from gp130

(STASTV-EpYSTVVHSG) has been shown previously to bind

with high affinity to mouse SOCS3 [19,20] The

addi-tion of a molar excess of peptide significantly increased

the solubility in NaCl⁄ Pi from << 1 mgÆmL)1 to

 1 mgÆmL)1 for SOCS3(22–225) and to 3 mgÆmL)1

for SOCS3(22–185)

As SOCS3(22–185) in the presence of the

tyrosine-phosphorylated peptide could not be concentrated

beyond  0.2 mm, seven constructs of shorter length

were expressed in E coli and their solubility examined

All constructs contained the SH2 domain, as defined by

sequence homology [10], but included differing lengths

of sequence outside this region All seven constructs

(22–142, 22–128, 22–126, 44–185, 44–142, 44–128 and

44–126), and the control 22–185 and 22–225 fragments,

were expressed in inclusion bodies in E coli and

required refolding The construct showing the highest

solubility was SOCS3(22–185) Constructs shorter than

this at the C-terminal end did not bind tightly to the

gp130 peptide (data not shown) All of the other

con-structs had equal or lower solubility, even in the

pres-ence of the tyrosine-phosphorylated peptide, including

the predicted SH2 domain alone (44–142) This implied

that the SH2 domain itself was a cause of poor

solubil-ity, as was the SOCS box The sequences of the SOCS3

SH2 domain and the phosphatidylinositol (PtdIns)

3-kinase (N-terminal) SH2 domain (the SH2 domain

with the highest sequence identity in the PDB) were

therefore aligned and hydrophobic residue substitutions

in SOCS3 that were surface-exposed in the PtdIns

3-kin-ase structure were considered as candidates for point

mutagenesis Six residues that were solvent-exposed and

hydrophilic in PtdIns 3-kinase but not in SOCS3 were identified and mutated to match the PtdIns 3-kinase residue The six mutants (A50D, G53R, L58E, A62E, A65E, G99D) were all cloned and expressed in E coli as part of a 22–185 construct All six constructs again expressed in inclusion bodies and required refolding The maximum concentration obtained by any of the six point mutants was  3 mgÆmL)1, in the presence of peptide, no higher than the wild-type SOCS3(22–185) construct As SOCS3(22–225) was too poorly soluble

to obtain any meaningful structural data, the wild-type SOCS3(22–185) construct was pursued

NMR assignments for murine SOCS3(22–185) After buffer optimization, SOCS3(22–185) was soluble

to  0.5 mm, but UV-visible spectra of the protein showed that significant aggregation was occurring at this concentration, indicated by a high apparent absorp-tion at 320 nm as a result of scattering Many NMR experiments required for full protein assignment there-fore did not yield acceptable results, in particular HNCACB, HCCH-TOCSY and 13C-NOESY-HSQC Nevertheless, near-complete backbone resonance assign-ments were made for SOCS3(22–185) Apart from five missing spin systems (Ser25–Ser28 and Gly170), 100%

of 1HN, 100% of 15N (excluding 18 proline residues), 96% of13Ca, 84% of13Cb, 87% of13C¢ and 84% of1Ha were assigned unambiguously (Fig 2) HNCO experi-ments were used to obtain13C¢ resonances and therefore all 13C¢ N-terminal to proline residues remain unas-signed The majority of side-chain assignments were determined, but because of the poor spectral quality of HCCH-TOCSY and 13C NOESY-HSQC experiments,

no hydrophilic or polar c, d or e carbon assignments were made Secondary structure elements were deter-mined by analysis of backbone and13Cbchemical shifts (supplementary figure Fig S1), from characteristic NOE patterns in the15N-edited NOESY-HSQC and by using talos [21] Assignments revealed that SOCS3 had

an aabbbbbabbb topology, with the ESS and the C-ter-minal end of KIR forming the first a-helix (Fig 2) Sig-nificantly, there was a large unstructured region between Met128 and Arg163 that contained a high proportion of proline residues (12 out of 35) The chemical shifts of mouse SOCS3 have been deposited in BioMagRes-Bank (http://www.bmrb.wisc.edu) with accession number 6580

Murine SOCS3 contains a PEST region The sequence of the unstructured region of murine SOCS3 is highly conserved in mammalian SOCS3, as

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shown in Fig 3 This region displays all of the com-mon features of PEST sequences [22], namely a high proportion of Pro, Glu, Ser and Thr residues, the absence of Lys, His and Arg except at the termini, and the fact that it is completely unstructured based on the absence of medium- and long-range NOEs and the observation of intense backbone amide peaks (Fig S1) The primary sequence of SOCS3 was analysed for the presence of a PEST sequence by using the pestfind program (http://www.at.embnet.org/embnet/tools/bio/ PESTfind) [23] This analysis identified the likely pres-ence (PESTfind score +11.11 [23]) of a single PEST sequence in SOCS3 spanning residues His126–Lys162 The unstructured region of SOCS3 spans Met128– Arg163 and therefore matches almost exactly the pre-dicted PEST region Residues from Met128–Arg163 showed no inter-residue NOEs other than sequential connectivities, did not have restrained /⁄ w angles according to TALOS, had amide resonances in the random coil region of the 15N-HSQC spectrum and showed significantly narrower line-widths than any other residues in the protein This indicates that the PEST sequence is an unstructured, highly mobile region within SOCS3

The PEST sequence is an insertion in the SH2 domain

Analysis of the secondary structure of SOCS3, and sequence alignments with SH2 domains, reveal that the PEST sequence begins immediately after the last residue

of helix B in the SH2 domain However, most SH2 domains do not end with this helix, but contain further structural elements at their C termini, including the ‘BG loop’ and the ‘G’-strand (Fig 2) [24] Hortner et al [25] have modelled the structure of the SOCS3 SH2 domain and suggest that the BG loop and bG strand are formed from residues Gly132–Val148, which we have shown to

be unstructured and part of the PEST region We exam-ined the sequence of the 19 structured residues immedi-ately downstream of the PEST region and found a high likelihood that they constitute the BG loop and bG strand of the SH2 domain of SOCS3 (supplementary figure Fig S2) In particular, Leu176–Leu182 aligned well with the seven C-terminal residues of a number of SH2 domains, supporting this hypothesis In agreement with this scenario, deletion of residues 182–185 had been shown previously to affect phosphotyrosine pep-tide binding [3] Although the sequence between Tyr165 and Pro175, which would form the ‘BG loop’, was not significantly similar to other SH2 domains, the SHP-2 [26], grb7 [27] and, in particular, STAT3b [9] SH2 domains contain extended loops in this region that

A

B

Fig 2 15N- 1 H HSQC spectrum and secondary structure

assign-ment of SOCS3(22–185) (A) The 15 N- 1 H HSQC spectrum is shown

of 0.1 m M SOCS3 at 500 MHz and 298 K in 50 m M

sodium-phos-phate buffer (pH 6.7) containing 2 m M dithiothreitol The assigned

residues are labelled with their residue number in the HSQC; some

assignment labels are omitted for clarity (B) The secondary

struc-ture of SOCS3 was assigned by examining NOE patterns, analyses

of backbone and 13 Cbchemical shifts, and TALOS predictions [26],

and is shown schematically with residue numbers marking the

boundaries of each motif The PEST motif is shown as a thick black

line The relevant secondary structure motifs are indicated at the

top of the figure with the nomenclature used by Grucza et al [30].

The topology of the b-sheet and two b-hairpins was determined by

examining long-range backbone–backbone NOEs (supplementary

table Table S1) ESS, extended SH2 subdomain; PEST, PEST motif.

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structurally resemble a b-hairpin Analysis of the

secon-dary structure of SOCS3 shows that it forms a b-hairpin

in this region Thus, it appears that the PEST sequence

constitutes an insertion in the true SOCS3 SH2 domain

Murine SOCS3(D129–163) binds to a

phosphotyrosine peptide from gp130

In order to determine whether deleting the PEST

region would have an impact on the function of the

SH2 domain, binding studies and isothermal titration

calorimetry (ITC) were performed using a 22–185

con-struct lacking the PEST region [SOCS3(22–185)(D129–

163)] and the tyrosine phosphorylated peptide from

gp130 SOCS3(D129–163) was constructed by replacing

Pro129–Arg163 inclusive, with an eight residue [(Gly–

Ser)· 4] linker in the 22–185 construct As shown in

Fig 4, the construct lacking the PEST region binds to

the gp130 peptide ITC analyses showed that the

titra-tion curve could be fitted using a single binding site

mode with a Kd of 74 ± 7 nm The Kd of wild-type

SOCS3(22–185) binding was 152 ± 25 nm

PEST sequences in other SOCS family proteins

In order to determine whether other members of the

SOCS family contained PEST motifs, their sequences

were analysed using the PESTfind algorithm [23]

Of the eight members of the murine SOCS family,

SOCS1, -3, -5 and -7, and CIS, show a probable

PEST motif with a PESTfind score of > 5 (Table 1)

CIS and SOCS3 have the PEST motif within the

SH2 domain, while SOCS1, -5 and -7 contain PEST

motifs in the N-terminal domain The PEST sequence

in the CIS SH2 domain is located eight residues

downstream from the terminus of the predicted aB

helix Whether those eight residues are also

unstruc-tured, thus placing the unstructured insertion at an

identical position to the PEST sequence in SOCS3,

could not be determined Secondary structure

predic-tion by sequence analysis gives no predicpredic-tion for

those eight residues

The KIR⁄ ESS consists of a single a-helix Based on observed NOEs, chemical shift deviations and TALOS predictions, residues Glu29–Ser44 form a sin-gle a-helix, whilst residues 22–28 are unstructured The helix encompasses the entire ESS and the four residues

at the C terminus of the KIR The remaining residues that comprise the KIR appear to be unstructured

Discussion

In this study we defined the secondary structure ele-ments of the SOCS3 protein, apart from the first 21 residues and the SOCS box The true SH2 domain boundaries were also defined for the first time, and an unstructured insertion therein was identified Residues 29–128 and 164–185 of SOCS3 are structured, but the N-terminal half of the KIR, and 35 residues in the SH2 domain, were shown by NMR to be unstruc-tured This was evinced by the lack of any nonadja-cent inter-residue NOEs in those regions, as well as the significantly sharper line-widths, characteristic of mobile, unstructured sections of polypeptide That the KIR is mostly unstructured when SOCS3 is in isola-tion is perhaps not surprising in view of the hypothesis for its mechanism proposed by Yasukawa et al [6] This requires the KIR to structurally mimic the activa-tion loop of JAK2, so that in the absence of JAK2 the KIR would consist of an extended loop struc-ture or be completely unstrucstruc-tured and separate from the globular core of the protein, so it can access, and block, the catalytic groove of the JAK2 kinase domain

Mutagenesis studies have shown that a number of residues [3,4,25,28], important in binding phosphotyro-sine-containing peptides or proteins, lie outside the SH2 domain predicted by sequence homology This led

to the 12 residues immediately upstream of the SH2 domain being designated the ESS Our secondary structure assignment of SOCS3 shows that the entire ESS forms a single a-helix Giordanetto & Kroemer [7] modelled the structures of the ESS and KIR of

Fig 3 PEST sequence conservation in SOCS3 Sequence alignment of the region of SOCS3 containing the PEST motif for a number of mammalian species is shown, with conserved residues in the unstructured PEST motif shown hatched in grey The numbering refers to mouse SOCS3 The unstructured residues defined by this study are shown in bold.

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SOCS1, based on the similarity of the ESS sequence to

a similar region in Stat1 [8] and Stat3b [9], and

sugges-ted that the ESS and KIR form two short orthogonal

helices This differs from the single a-helix found in

SOCS3, but a comparison of the ESS sequences from

SOCS1 and SOCS3 shows that there are several

diver-gent residues in this region, including a leucine (Leu32)

in SOCS3 in place of an arginine (Arg67) in SOCS1,

predicted in their model to make a critical ion pair

with Asp76

The identification, by deletion mutagenesis, of

resi-dues affecting phosphotyrosine binding but located

> 50 residues downstream of the predicted C terminus

of the SH2 domain suggested that the functional SH2

domain was longer than originally suggested by

sequence comparison [3] However, subsequent

attempts to determine key residues important for the

binding specificity of SOCS3 by structural modelling

were hampered by the logical, yet incorrect,

assump-tion that the SH2 domain consisted of c 100

contigu-ous residues In this report we have shown that the

true SH2 domain is disrupted in murine SOCS3 by a

35-residue unstructured insertion that is predicted to

form a PEST motif [22] This results in residues 164–

185 forming the BG loop and bG strand of a classic

SH2 domain [24], rather than residues 129–147, as

commonly assumed [25] This information is crucial

for future attempts to alter the specificity of the

SOCS3 SH2 domain by point mutation

The PEST sequence identified in SOCS3 does not

occur, according to sequence analysis, in the same

location in any other members of the SOCS family,

apart from CIS Analysis of the sequence of CIS using

the PESTfind algorithm [23] shows a probable PEST sequence in residues 172–187, a region suggested by sequence homology to be located in a similar site in the SH2 domain as in SOCS3 Other members of the SOCS family contain putative PEST sequences, but these are all located in the N-terminal region, upstream

of the SH2 domain The conservation of the PEST motif of SOCS3 in mammals (Fig 3), and the presence

of probable PEST regions in most SOCS family mem-bers, suggests that it has an important functional role The appropriate duration of the cellular response to cytokine signalling will be determined, in large part, by the rate of turnover of the SOCS proteins Expression

of the SOCS proteins is induced directly by STAT binding to the appropriate promoters Rapid destruc-tion of the SOCS protein is also necessary, once signal-ling has ceased, to allow for subsequent cytokine stimulation The level of SOCS1 and SOCS3 protein

in vivo appears to be strongly regulated by protein de-gradation, and the short half-life of SOCS proteins intracellularly appears to be the result primarily of proteolytic degradation [28,29] This may be important mechanistically, as the efficient turnover of SOCS pro-teins, and their induction of degradation of associated signalling molecules via the SOCS box, allows cells to respond to cytokine stimulation, quickly inhibit any prolonged activation and rapidly return to basal SOCS levels, ready for another round of stimulation There appear to be a number of features important for effect-ive degradation of SOCS proteins, even apart from any role the SOCS box may play in this process Sasaki

et al [28] have shown that a naturally occurring alternative transcript of SOCS3, lacking the first 11

Fig 4 SOCS3 lacking the PEST motif binds

a gp130 peptide with high affinity (A)

Titra-tion of 80 l M gp130 peptide into 10 l M

SOCS3(D101–133) The integrated heats

from which the heat of dilution has been

subtracted are shown, as well as the fit to a

single site binding isotherm that yielded Kd

78 n M and DH )6.4 kcal mol )1 (B) Titration

of 160 l M gp130 peptide into 13 l M wild

type SOCS3 The fit to a single site binding

isotherm is shown, yielding a K d of 168 n M

and a DH of )6.2 kcalÆmol )1 Both the

wild-type and (D101-133) proteins used spanned

residues 22–185 and not 22–225 because of

the higher solubility of the former.

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residues, has a prolonged half-life in Ba⁄ F3

haemopoi-etic cells owing to the absence of Lys6, a major

ubiqui-tination site of SOCS3 Chen et al [18] found that the

N-terminal region of SOCS 1 (upstream of the SH2

domain) contained a site for pim-1 kinase

phosphory-lation that significantly increased SOCS1 stability

SOCS3 has also been shown to interact, and be

phos-phorylated by, pim-1 kinase, at an unknown site,

which also confers stability [30]

Proteasome-induced proteolysis is catalysed by the

presence of regions of unstructured sequence in a

pro-tein [31] The PEST sequence is one such sequence

commonly found in intracellular proteins of extremely

short half-life [22,32] PEST sequences are hydrophilic,

contain a high proportion of proline, glutamic acid,

serine and threonine residues, and do not contain

lysine, arginine or histidine The X-ray structures of

several proteins containing PEST sequences have been

determined, but in each case the electron density of the

PEST sequence is missing (e.g NF-jb [33] and

ornith-ine decarboxylase [34]), presumably because this region

is unstructured and mobile They can act in a modular

manner, as transplanting PEST sequences from

unsta-ble proteins into staunsta-ble proteins has been shown to

reduce the half-life of the resulting chimaeras

[32,35,36] The presence of a PEST sequence has been

shown to be important in the proteolysis⁄ degradation

of a number of proteins with diverse functions, such as

the glutamate receptor [37], proto-Dbl [38], and c-Fos

[39] Biophysical characterization of the NF-jb PEST

sequence [40] has shown it to be solvent-exposed and

probably unstructured

The PEST sequence in SOCS3 is located between

two secondary structural elements, namely the aB

helix and the BG loop In all SH2 domains these are

located on the opposite face of the protein to the

phosphotyrosine-binding site, so the PEST sequence is

not expected to interfere with phosphotyrosine binding

by the SH2 domain Indeed, replacing the entire 35-residue PEST sequence with GSGSGSGS had little effect upon binding a phosphorylated gp130 peptide,

as shown by ITC In fact, the construct lacking the PEST motif bound slightly more tightly to the phos-photyrosine containing gp130 peptide than did wild-type SOCS3(22–185) Whether the twofold change in

Kd is significant is difficult to determine as the con-struct lacking the PEST motif shows significantly less aggregation than wild-type SOCS3, which could alter the binding kinetics without representing a truly enhanced Kd The similarity of the two Kd values implies that the PEST sequence does not significantly affect phosphotyrosine binding Structurally, the PEST sequence is a benign insertion that may nevertheless play a critical functional role in regulating cellular SOCS3 levels

Our identification of the secondary structure and cor-rect domain boundaries of SOCS3 will enable manipu-lation of SOCS3 function by rational mutagenesis This includes mutagenesis of the PEST motif, either by com-plete removal or by point mutagenesis, to determine the effect it has on the biological function of SOCS3

in vivo, as well as mutagenesis of the SH2 domain to alter substrate specificity These approaches will allow

a more thorough dissection of SOCS3 activity

Experimental procedures

Cloning and expression Fragments of mouse SOCS3 were subcloned by PCR into a ligation-independent cloning vector constructed by one of

us (JJB) The vector encodes constructs with the leader sequence MASYHHHHHHDYDIPTTENLYFQGAHDGS, which consists primarily of a His6-tag and a TEV protease

Table 1 Predicted PEST motifs in suppressor of cytokine signalling (SOCS) family proteins Sequences of predicted PEST motifs in the SOCS family members are shown with their PESTfind score [29] and domain location NA indicates, for SOCS-2, -4 and -6, that no PEST motif was predicted for these proteins.

Protein

PESTfind

SOCS7 11.9 74 KTAGGGCCP CPCPPQPPPPQPPPPAAAPQAGEDPTETSDALLVLEGLESEAESLETNSCSEEELSSPGR 142 N terminus

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cleavage site For unlabelled protein, expression was

per-formed in baffled flasks, with cells grown to an attenuance

(D) at 600 nm of 0.6 in superbroth containing 50 lgÆmL)1

kanamycin Expression was induced with 1 mm isopropyl

thio-b-d-galactoside (IPTG) Cells were harvested, 3 h after

induction, by centrifugation (6200 g, 4C, 30 min) For

15

N labelling, cells were grown to a D at 600 nm of 0.6 in

Neidhardt’s medium [41] containing 1.0 gÆL)1 15NH4Cl as

the sole nitrogen source For 15N⁄13

C-labelled samples, 1.0 gÆL)1 15NH4Cl and 2 gÆL)1 13C glucose were the sole

sources of nitrogen and carbon, respectively Cells were

harvested 8 h after IPTG induction by centrifugation

(6200 g, 4C, 30 min) All SOCS3 clones express as

insol-uble inclusion bodies

Protein purification and buffer screening

Inclusion bodies were prepared via cell homogenization and

centrifugation at 20 000 g, and solubilized using 6 m

guani-dine hydrochloride The soluble inclusion body preparation

was then purified using Ni-nitrilotriacetic acid resin

(Qiagen, Valencia, CA, USA) Protein binding was

per-formed at pH 8.0, washing at pH 6.3, and elution at

pH 4.5 The eluted protein was quantified by absorbance at

280 nm, diluted to 0.1 mgÆmL)1, then refolded by extensive

dialysis against 25 mm sodium phosphate, 50 mm sodium

chloride, 5 mm 2-mercaptoethanol, pH 6.7 The refolded

protein was tested for correct conformation by binding an

aliquot to a column with immobilized phosphorylated

gp130 peptide (STASTVEpYSTVVHSG; pY¼

phospho-tyrosine [19,20]) The refolded protein was limited in its

solubility, but addition of a 1.5· molar excess of the

gp130-derived phosphopeptide increased the solubility to

c 3 mgÆmL)1 As this concentration was still too low for

structure determination by high-resolution NMR, a

thor-ough screen of buffer conditions was undertaken in an

attempt to improve the maximum solubility obtainable for

SOCS3(22–185) The buffer screen was performed in

micro-drop format [42] and studied the pH range from 4 to 9 in

0.5 unit intervals, the salt concentration from 0 to 500 mm

in 50 mm intervals, and temperatures of 4, 25 and 37C

Both constructs of SOCS3 showed highest solubility in

buffers of low salt and high pH, and at low temperature

The buffer conditions chosen for further additive screening

were 20 mm Tris, pH 8.5, 20 mm NaCl, at 25C This

starting condition was used to test the effect of 14 different

additives, most at several concentrations The additive

screen yielded promising results, and SOCS3 was shown to

be soluble to 10 mgÆmL)1 ( 0.5 mm) in buffers

contain-ing > 10% glycerol, > 0.5 m non detergent sulfobetaine

(NDSB), > 0.5 m trehalose or 50 mm arginine plus 50 mm

glutamate [43] However, initial NMR analysis showed that

under these conditions, many amide cross-peaks were

missing from 15N HSQC spectra As the high pH was

judged to be the cause of this, the most promising additives

were screened again at pH 6.7 At this pH only the presence of 50 mm arginine plus 50 mm glutamate [43] yielded an increase in protein solubility, from 3 to

10 mgÆmL)1, although UV-visible spectroscopy suggested that there was significant aggregation at that concentration SDS⁄ PAGE analysis of the protein after storage revealed that disulphide bond-linked multimers formed slowly over time in the absence of a reducing agent In the presence of dithiothreitol and EDTA, the protein was stable at 4C for

at least 2 months The final buffer conditions chosen for SOCS3 were therefore: 20 mm sodium phosphate, 20 mm NaCl, 50 mm arginine, 50 mm glutamate, 2 mm dithio-threitol, 1 mm EDTA, pH 6.5 Concentration to

10 mgÆmL)1 was performed using centrifugal concentration devices (Amicon Inc., Beverly, MA, USA)

NMR spectroscopy Spectra were recorded at 298 K on a Bruker Avance 500 (using a cryoprobe), DRX-600, DMX-600 (using a cryo-probe) and Varian Unity INOVA 800 spectrometers Con-ventional 2D TOCSY and NOESY spectra were obtained using 2048 complex data points in the directly detected dimension and typically 200–400 t1 increments A TOCSY spin-lock time of 60 ms and a NOESY mixing time of

120 ms were used Spectra were processed using xwinnmr (Bruker AG, Karlsruhe, Germany) or nmr-pipe [44], and were analysed using xeasy (version 1.3.13) [45] or nmrdraw [44] Spectra were referenced to the H2O signal

at 4.77 p.p.m (298 K) or a small impurity at 0.15 p.p.m

Ca, Cb, Ha, C¢, and N chemical shifts were used in the program TALOS [21] to obtain backbone torsion angle pre-dictions Sequence-specific resonance assignments for the backbone were accomplished using HNCA, HN(CO)CA, CBCA(CO)NH, HN(CA)CO and HNCO experiments [46] Side-chain assignments were accomplished by combining the data from the following experiments: 15N-edited TOCSY-HSQC and NOESY-HSQC, HCCH-TOCSY and HCCH-COSY [46]

ITC Isothermal calorimetric titrations were performed using a Microcal omega VP-ITC (MicroCal Inc., Northampton,

MA, USA) SOCS3(22–185) was dialysed against buffer (50 mm NaCl, 50 mm arginine, 50 mm glutamate, 5 mm 2-mercaptoethanol, pH 6.7) and the dialysis buffer was used to dissolve the tyrosine-phosphorylated gp130 peptide Experiments were performed at 298 K Solutions of 10–

25 lm SOCS3 in the cell were titrated by injection of a total of 290 lL of 80–200 lm of the gp130 peptide The heat of dilution of the gp130 peptide into buffer was deter-mined in control experiments and subtracted from the raw data of the binding experiment The data were analysed using the evaluation software, Microcal Origin, version

Trang 9

5.0, provided by the manufacturer The binding curve fitted

a single-site binding mode in all cases, and Kd values were

determined from experiments repeated at least twice

Acknowledgements

We thank Gottfried Otting for generously recording

NMR spectra on SOCS3 We thank the Knut and

Alice Wallenberg Foundation for the cryoprobe used

to record NMR spectra at 600 MHz and access to the

800 MHz NMR spectrometer at Biovitrum AB

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