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Structural characterization of the human Nogo-A functional domainsSolution structure of Nogo-40, a Nogo-66 receptor antagonist enhancing injured spinal cord regeneration Minfen Li1, Jiah

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Structural characterization of the human Nogo-A functional domains

Solution structure of Nogo-40, a Nogo-66 receptor antagonist enhancing injured spinal cord regeneration

Minfen Li1, Jiahai Shi1, Zheng Wei1, Felicia Y H Teng2, Bor Luen Tang2and Jianxing Song1,2

1 Department of Biological Sciences and 2 Department of Biochemistry, National University of Singapore, Singapore

The recent discovery of the Nogo family of myelin inhibitors

and the Nogo-66 receptor opens up a very promising avenue

for the development of therapeutic agents for treating spinal

cord injury Nogo-A, the largest member of the Nogo

fam-ily, is a multidomain protein containing at least two regions

responsible for inhibiting central nervous system (CNS)

regeneration So far, no structural information is available

for Nogo-A or any of its structural domains We have

sub-cloned and expressed two Nogo-A fragments, namely the

182 residue Nogo-A(567–748) and the 66 residue Nogo-66 in

Escherichia coli CD and NMR characterization indicated

that Nogo-A(567–748) was only partially structured while

Nogo-66 was highly insoluble Nogo-40, a truncated form

of Nogo-66, has been previously shown to be a Nogo-66

receptor antagonist that is able to enhance CNS neuronal

regeneration Detailed NMR examinations revealed that a Nogo-40 peptide had intrinsic helix-forming propensity, even in an aqueous environment The NMR structure of Nogo-40 was therefore determined in the presence of the helix-stabilizing solvent trifluoroethanol The solution structure of Nogo-40 revealed two well-defined helices linked

by an unstructured loop, representing the first structure of Nogo-66 receptor binding ligands Our results provide the first structural insights into Nogo-A functional domains and may have implications in further designs of peptide mimetics that would enhance CNS neuronal regeneration

Keywords: CNS neuronal regeneration; NMR spectroscopy; Nogo-40; NogoA; spinal cord injury

Survivors of severe central nervous system (CNS) injury

often suffer from permanent disability Previously, it was

thought that the inability of CNS neurons to regenerate was

due to the absence of growth-promoting factors in CNS

neurons However, recent discoveries challenge this dogma

It has been shown that the failure of CNS neuronal

regeneration results to a large extent from the existence of

inhibitory molecules of axon outgrowth in adult CNS

myelin [1] So far, three proteins have been identified that

cause inhibitory effects on CNS neuronal regeneration,

namely Nogo [2–4], myelin-associated glycoprotein [5] and

oligodendrocyte myelin glycoprotein [6] All three molecules

appear to exert their inhibitory action through the initial

binding of the Nogo-66 receptor (NgR) [3], first identified as

a high affinity neuronal receptor for Nogo-A [7] NgR

binding leads to subsequent activation of signaling

path-ways that possibly involve Rho activation, and the

induc-tion of growth cone collapse [8] These discoveries raise a

promising possibility to enhance axonal growth by

disrupt-ing the interaction between NgR and its ligands

Of the three myelin-associated molecules above, the CNS-enriched Nogo belonging to the reticulon protein family has received intense attention recently Nogo has several splicing variants, among which Nogo-A is the largest, composed of 1192 amino acids (Fig 1) Recent studies have demonstrated that NogoA is a multidomain protein containing several discrete regions with growth inhibitory functions [4,9–11] Two major inhibitory regions have been identified The first is a stretch in the middle of the Nogo-A molecule (residues 544–725 for mouse and residues 567–748 for human Nogo-A proteins) that restricts neurite outgrowth and cell spreading and induces growth cone collapse The second is the extracellular 66 amino acid loop called Nogo-66 that is also capable of inhibiting neurite growth and inducing growth cone collapse [4,9–11] The Nogo-66 domain has been shown

to be anchored on the oligodendrocyte surface and binds

to the neuronal glycophosphatidylinositol-linked NgR, via its leucine-rich repeat containing domain The binding of Nogo-66 to NgR is competitively inhibited by a peptide consisting of the N-terminal 40 residues of Nogo-66, named Nogo-40 [12,13] This Nogo-40 peptide has been experimentally demonstrated to be a strikingly effective NgR antagonist capable of enhancing recovery from spinal cord injury [13]

In contrast to the extensive functional studies on

Nogo-A, thus far no structural information has been available for any region of the Nogo-A protein In the present study, we cloned and expressed the two functional regions of human Nogo-A and performed structural characterization by CD

Correspondence to J Song, Department of Biochemistry, National

University of Singapore; 10 Kent Ridge Crescent, Singapore 119260.

Fax: +65 6779 2486, Tel.: +65 6874 1013,

E-mail: bchsj@nus.edu.sg

Abbreviations: CNS, central nervous system; IPTG, isopropyl

thio-b- D -galactoside; NgR, Nogo-66 receptor; rmsd, root mean square

deviation; TFE, trifluoroethanol.

(Received 10 June 2004, revised 6 July 2004, accepted 12 July 2004)

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and NMR spectroscopy While Nogo-66 is highly insoluble,

the 182 residue fragment was found to be partially

structured and could be further induced to form a helical

structure with the introduction of 4 mM Zn2+ We

conducted further NMR studies on two truncated forms

of Nogo-66: Nogo-40 and Nogo-24 Although Nogo-40

and Nogo-24 appeared to be unstructured in aqueous

buffer, a detailed NMR analysis revealed that these have intrinsic helix-forming propensity This observation, together with results from secondary structure predictions, offered the rationale to study the structure of Nogo-40 after its intrinsic helix-forming propensity is stabilized by the introduction of the helix-stabilizing solvent trifluoroethanol

We report here the structure of Nogo-40, a Nogo-66

Fig 1 Schematic representation of the domain organization of the human Nogo-A protein (A) The domain organization of human Nogo-A showing the N-terminal stretch region Nogo-A(567–748) and the extracellular 66 amino acid loop Nogo-66 with growth cone collapsing functions The black boxes indicate transmembrane domains (B) The amino acid sequence of Nogo-40, a Nogo-66 receptor antagonist that has been demonstrated to enhance CNS neuronal regeneration (C) The amino acid sequence of the N-terminal 24 residues of Nogo-40.

Fig 2 Expression and purification of Nogo-A(567–748) and Nogo-66 (A) Coomasie Brilliant Blue stained SDS/PAGE gel showing the expression and affinity-purification of the human Nogo-A(567–748) protein Lane 1, total cell extract before isopropyl thio-b- D -galactoside (IPTG) induction; lane 2, total cell extract after 0.5 m M IPTG induction at 20 C overnight; lane 3, supernatant of the cell lysate after high speed centrifugation; lane 4, pellet of the cell lysate after high speed centrifugation; lane 5, Ni-agarose beads with bound Nogo-A(567–748); lane 6, protein molecular mass markers; lane 7, affinity-purified Nogo-A(567–748) protein; lane 8, protein molecular mass markers (B) Coomasie Brilliant Blue stained SDS/ PAGE gel showing the expression and affinity-purification of the Nogo-66 protein under denaturing conditions Lane 1, total cell extract before IPTG induction; lane 2, total cell extract after 0.5 m M IPTG induction at 20 C overnight; lane 3, Ni-agarose beads with bound Nogo-66; lane 4, elution 1 under denaturing conditions (in the presence of 8 M urea); lane 5, elution 2 under denaturing conditions (in the presence of 8 M urea); lane

6, elution 3 under denaturing conditions (in the presence of 8 M urea); lane 7, elution 4 under denaturing conditions (in the presence of 8 M urea); lane 8, protein molecular mass markers.

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receptor antagonist, determined by NMR spectroscopy.

The obtained results may contribute to further

understand-ing of Nogo-A function and aidunderstand-ing in future designs of

NgR antagonists

Experimental procedures

Cloning and expression of the Nogo-A fragments

The Nogo-A cDNA (designated KIAA 0886) was obtained

from the Kazusa DNA Research Institute

(Kazusa-Kamatari, Kisarazu, Chiba, Japan) A DNA fragment

encoding a 182 residue Nogo-A fragment from residues

567–748 (designated as Nogo-A(567–748); Fig 1) was

generated by PCR with a pair of primers: 5¢-CG

CGCGCGCGGATCCACTGGTACAAAGATTGCT-3¢

(forward) and 5¢-CGCGCGCGCCTCGAGCTAAAAT

AAGTCAACTGGTTC-3¢ (reverse) A DNA fragment

encoding human Nogo-66 corresponding to residues

1055–1120 of Nogo-A (Fig 1) was likewise obtained by

PCR The PCR fragment encoding Nogo-A(567–748) was

subsequently cloned into BamHI/XhoI restriction sites of

the expression vector pET32a (Novagen) The fragment

encoding Nogo-66 was cloned into the NdeI/BamHI

restriction sites of pET-15b (Novagen) The DNA sequences were confirmed by automated DNA sequencing The recombinant His-tagged A(567–748) and

Nogo-66 were expressed in Escherichia coli BL21 cells Briefly, the cells were cultured at 37C until D ¼ 0.6 Isopropyl thio-b-D-galactoside was then added at a final concentration of 0.5 mM to induce the recombinant protein expression overnight at 20C The Nogo-A(567–748) protein was purified by Ni2+-affinity chromatography under native conditions, while the Nogo-66 protein was purified under denaturing conditions because Nogo-66 was found in the inclusion body

For heteronuclear NMR experiments the Nogo-A(567– 748) and Nogo-66 proteins were prepared in15N-labeled form using a similar expression protocol except that E coli BL21 cells were grown in minimal M9 media instead of rich (2YT) media, with the addition of [15NH4]2SO4 for

15N-labeling

Peptide synthesis and purification Nogo-40 peptide with a sequence of RIYKGVIQAIQ KSDEGHPFRAYLESEVAISEELVQKYSNS(1–40) and the Nogo-24 peptide consisting of the N-terminal 24

Fig 3 CD and NMR characterization of Nogo-A(567–748) (A) Far-UV CD spectra of Nogo-A(567–748) collected at 20 C in a phosphate buffer

at pH 6.5 (black line) and in a Tris/HCl buffer at pH 6.5 containing 4 m M zinc ion (grey line) (B) The 1 H- 15 N HSQC spectrum of Nogo-A(567– 748) collected at 20 C in a phosphate buffer at pH 6.5.

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residues of Nogo-40 were chemically synthesized using the

standard Fmoc method The peptides were purified by

HPLC on a reverse-phase C18 column (Vydac), and its

identity was verified by MALDI-TOF mass spectrometry

and NMR resonance assignments

Circular dichroism spectroscopy

CD experiments were performed on a Jasco J-810

spectro-polarimeter equipped with a thermal controller The far-UV

CD spectra of Nogo-A(567–748), Nogo-40 and Nogo-24

were collected at 20C at peptide concentrations of

10–50 lM using 1 mm path length cuvettes with a 0.1 nm

spectral resolution Data from five independent scans were

added and averaged

NMR experiments and structure calculation

NMR samples in aqueous buffer were prepared by

dissol-ving the Nogo-40 and Nogo-24 synthetic peptides in 50 mM

phosphate buffer (pH 6.5) to a final concentration of

1 mM NMR samples for structure determination contained

1 mM Nogo-40 in either (50 : 50, v/v) trifluoroethanol

(TFE)-d3/H2O or TFE-d3/D2O in the presence of 50 mM

phosphate (final pH or pD  6.5) The deuterium lock

signal for the NMR spectrometers was provided by the

addition of 50 lL D2O

NMR experiments including two-dimensional NOESY

[14], TOCSY [15], DQF-COSY and 1H-15N HSQC [16]

were performed on a Bruker Avance-500 spectrometer equipped with an actively shielded cryoprobe and pulse field gradient units A mixing time of 250 ms was used for NOESY and 65 ms for TOCSY experiments Spectral processing and analysis were carried out usingXWINNMR

(Bruker), NMRPIPE [17] and NMRVIEW [18] software Sequence-specific assignments for Nogo-40 were achieved through identification of spin systems in the TOCSY spectra combined with sequential NOE connectivities in the NOESY spectra [19]

For structural calculations, NOE connectivities were collected from NOESY spectra of Nogo-40 in TFE/H2O

or TFE/D2O mixtures All NOE data were grouped into four categories: strong, medium, weak and very weak, corresponding to upper bound interproton distance restraints of 3.0, 4.0, 5.0 and 6.0 A˚, respectively The sum of the Van der Waals radii of 1.8 A˚ was set to be the lower distance bound Due to resonance line broadening, overlap or small 3JHNHa, or all three, the measurement of 3JHNHa based on a DQF-COSY spec-trum was on the whole unsuccessful Therefore, the backbone dihedral angles were set to center at )60 degrees for residues having both aN(i+3) NOEs and large helical conformational shifts The solution structure of Nogo-40 was calculated on a Linux-based

PC station using the simulated annealing protocol [20] in the CRYSTALLOGRAPHY and NMR system [21] The struc-tures were analyzed by INSIGHTII AND MOLMOL graphic softwares [22]

Fig 4 NMR characterization of Nogo-24 NH-NH region of a NOESY spectrum of Nogo-24 (mixing time of 250 ms) acquired in an aqueous buffer (50 m phosphate buffer at pH of 6.5) The observed sequential NH-NH NOEs are labeled.

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Expression and structural characterization of

Nogo-A(567–748) and Nogo-66

Nogo-A(567–748) and Nogo-66 were successfully cloned

and expressed as His-tagged proteins As shown in Fig 2,

both recombinant proteins could be affinity-purified by

affinity columns either under native condition for Nogo-A(567–748) or under denaturing condition for Nogo-66 Attempts to refold Nogo-66 by dialysis and fast dilution were unsuccessful, indicating that Nogo-66 is highly insol-uble On the other hand, the 182 residue Nogo-A(567–748) was soluble and its molecular mass as determined by MALDI-TOF MS matched that predicted from the amino acid sequence Interestingly the apparent molecular mass of

Fig 5 CD and NMR characterization of Nogo-40 (A) Far-UV CD spectra of Nogo-40 collected at 20 C in the presence of methanol at different concentrations Black, 50 m M phosphate buffer (pH 6.5); pink, 20% TFE; green, 36%; cyan, 49%; dark violet, 60%; brown, 68%; dark green, 74% and blue, 80% (B) Far-UV CD spectra of Nogo-40 collected at 20 C in the presence of TFE at different concentrations black: 50 m M phosphate buffer (pH 6.5); pink, 20% TFE solution; green, 36%; cyan, 49% and red, 60% (C) NH-aliphatic region of a NOESY spectrum (mixing time of

250 ms) of Nogo-40 acquired in a 50 m M phosphate buffer (pH 6.5) at 15 C (D) NH-aliphatic region of a NOESY spectrum of Nogo-40 (mixing time of 250 ms) acquired in a 50 : 50 (v/v) TFE/H 2 O mixture at 35 C.

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Nogo-A(567–748) estimated by SDS/PAGE (Fig 2A) was

about 37 kDa, much larger than that expected for a 182

residue protein This anomalous behavior on SDS/PAGE

has been previously observed for cloned Nogo-A fragments

and was attributed to the existence of a high number of

charged residues in Nogo-A [4,10]

The structural properties of Nogo-A(567–748) were first

investigated by CD spectroscopy As shown in Fig 3A, the

CD spectrum of Nogo-A(567–748) in aqueous buffer had a

maximal negative peak at 202 nm and had no significant

positive signal at 198 nm, indicating that the polypeptide

was not fully structured [23] However, the existence of the

maximal negative signal at around 202 nm, rather than

198 nm, together with the negative shoulder signal at

 225 nm, indicated that the polypeptide was also not

assuming a random coil structure To explore whether

Nogo-A(567–748) had any specific interaction with metal

ions, we utilized CD measurements to monitor

conforma-tional changes induced by the addition of metal ions,

including Ca2+, Mg2+, Cu2+, Ni2+and Zn2+ Only Zn2+

was able to induce a significant conformational change in

the polypeptide As shown in Fig 3A, the CD spectrum of

Nogo-A(567–748) with dual negative signals at 206 and

221 nm in the presence of 4 mMZn2+resembles that for a

typical helical protein The results indicate that Zn2+could

specifically induce, to a significant degree, the polypeptide to assume a helical conformation

The structural properties of the Nogo-A(567–748) were further assessed by the NMR HSQC experiment, which is very sensitive to both secondary structures and tertiary packings As shown in Fig 3B, the poor chemical disper-sions of the spectrum at both 1H and 15N dimensions indicated that Nogo-A(567–748) did not have a tight side-chain packing In particular, the number of observed NMR cross peaks was only about 35, much less than expected for

a 182 residue protein, thus indicating that slow conform-ational exchanges existed over most regions of the protein Usually, slow conformational exchange would result in significant line-broadening for HSQC peaks and make these peaks undetectable The manifested HSQC peaks in Fig 3B most likely resulted from the unstructured and flexible regions of the Nogo-A(567–748), while the peaks for the regions undergoing slow conformational changes were undetectable The results above indicated that Nogo-A(567–748) was partially structured, probably with some properties characteristic of molten globule states [24–27] Interestingly, upon addition of 4 mMZn2+, no new HSQC peaks appeared but the intensities of the existing peaks became stronger (spectrum not shown) This observation suggests that although the introduction of Zn2+was able to

Fig 6 NMR spectral assignment of Nogo-40 The NH-aH region of a NOESY spectrum of Nogo-40 (mixing time of 250 ms) acquired in a 50 : 50 (v/v) TFE/H 2 O mixture at 35 C with sequential assignments indicated Several medium-range NOEs defining helical structures are labeled.

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significantly enhance the helical structure of Nogo-A(567–

748) as detected by CD, it was not sufficient to make the

tertiary packing as tight as those found in a well-structured

protein

CD and NMR characterization of Nogo-24 and Nogo-40

The purified Nogo-66 was found to be highly insoluble in

both aqueous buffer and a TFE/H2O mixture An attempt

to acquire a 1H-15N HSQC spectrum of Nogo-66 was

unsuccessful We therefore focused our NMR structure

determination on Nogo-40, which has been shown

previ-ously to be an excellent NgR antagonist by virtue of its

ability to interact with NgR without eliciting downstream

inhibitory signaling [10,11]

Secondary structure prediction suggested that Nogo-40 had a strong propensity to form a helical structure (data not shown) However, the preliminary CD and NMR study indicated that Nogo-40 was largely unstructured in aqueous buffers As a result, it was not possible to assign the NMR spectra of Nogo-40 under these conditions due to the severe peak overlap To gain insight into the intrinsic secondary structure preference of Nogo-40 experimentally, we dissec-ted Nogo-40 into two fragments, namely the N- and C-terminal parts While several attempts to synthesize the C-terminal part of Nogo-40 failed, the peptide Nogo-24, comprising the N-terminal 24 residues of Nogo-66, was successfully produced The sequential assignment of

Nogo-24 was successfully achieved and the chemical shifts determined (data not shown) The NOE assignment shown

Fig 7 The secondary structures of Nogo-24 and Nogo-40 (A) Ca proton conformational shifts of Nogo-24 (grey) and Nogo-40 (black) (B) The NOE patterns of Nogo-40 used to define its secondary structure.

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in Fig 4 clearly indicates that sequential NH-NH NOE

connectivities exist over many residues of Nogo-24, strongly

indicating intrinsic helix-forming propensity in the Nogo-24

peptide, even in aqueous buffer This observation, together

with the secondary structure predictions for Nogo-40,

prompted us to conduct further NMR studies of Nogo-40

in the presence of TFE and methanol, which is well-known

for its ability to stabilize intrinsic helixes

Figure 5A shows the CD spectra of Nogo-40 in aqueous

buffer and methanol/H2O mixtures The CD spectrum of

Nogo-40 in the aqueous buffer has a negative peak at

 198 nm, indicating that Nogo-40 had no stable

confor-mation in aqueous buffer [23] Interestingly, with the

introduction of methanol, the CD spectra of Nogo-40

undergo dramatic changes The CD spectra of Nogo-40 in

the presence of methanol at a concentration of 74% or

above show one positive peak at  198 nm and two

negative peaks at  208 and 222 nm, respectively This

observation clearly indicates that Nogo-40 adopts a

well-formed helical conformation in the presence of 74% or

higher percentages of methanol Similarly, as shown in

Fig 5B, TFE is also able to stabilize the helical

conforma-tion of Nogo-40 It appears that 50% TFE is sufficient to

stabilize a full helical conformation for the peptide

NMR spectroscopy was further utilized to explore the

structural properties of Nogo-40 The very narrow

reson-ance dispersion of amide protons ( 0.7 p.p.m) and the lack

of side-chain packing with aromatic ring protons in aqueous

buffer (Fig 5C) demonstrate that Nogo-40 in aqueous

buffer had no stable structure, which is consistent with the

CD results above In contrast, the same NOESY region of

Nogo-40 in the 50 : 50 (v/v) TFE/H2O mixture (Fig 5D)

shows a dramatically increased dispersion of amide protons

( 1.5 p.p.m) and extensive side-chain packing with

aro-matic ring protons, indicating that Nogo-40 adopts a

well-formed helical structure in the presence of 50% TFE

NMR structure determination of Nogo-40

Based on the observations above, the structure

determin-ation of Nogo-40 by NMR spectroscopy was thus carried

out in a 50 : 50 (v/v) TFE/H2O mixture Figure 6

presents a NH-aH region of NOESY spectrum of

Nogo-40 with sequential assignments labeled The aH

conformational shifts (Fig 7A) suggest that Nogo-40

contains two helical fragments, one at the N-terminal part

and the other over the C-terminus The medium-range

NOE connectivities such as daN(i, i+2), daN(i, i+3),

daN(i, i+4) and dab(i, i+3) used for identification of

secondary structures, again support the observation that

two helical segments exist in Nogo-40 (Fig 7B) It is also

noteworthy that the helical conformational shifts already

existed for Nogo-24 in aqueous buffer (Fig 7A), although

were less pronounced than those for Nogo-40 in 50%

TFE

Fifty Nogo-40 structures were calculated from the NMR

restraints detailed in Table 1 with a simulated annealing

protocol implemented by the Crystallography and NMR

system Out of these, the 10 lowest-energy structures with a

distance violation of less than 0.3 A˚ and a dihedral angle

violation of less than 5 were selected for further analysis

The structural statistics for the 10 selected structures are also

included in Table 1 The low values of distance and dihedral angle energies indicate that all selected structures satisfy the experimental NMR constraints Moreover, the covalent geometry is well-respected as demonstrated by the low root mean square deviation (rmsd) values for the bond lengths (0.0019 A˚) and the valence angles (0.4)

All 10 structures of Nogo-40 contain two helices, one over residues 7–12 and another over residues 26–37 Superimposition of the 10 structures over either helix (Fig 8A,B) gives low rmsd values (Table 1), indicating that both helices are well defined However, due to the absence of NOEs between N- and C-terminal helices, their relative orientation cannot be determined A more detailed exam-ination of the 10 selected structures shows that there are two populations among the 10 structures Five of these struc-tures, as represented in Fig 8C, contain only two helices (one from residues 7 to 12 and another from 26 to 37) However, another set of five structures, as represented in Fig 3D, has an additional helix over residues 20–24 Indeed, conformational shifts shown in Fig 7A and medium-range NOEs in Fig 7B indicate a helical confor-mation over residues 20–24 Possibly due to the existence of side-chain–side-chain NOEs among residues His17, Phe19, Tyr22 and Leu23, the helix over residue 20–25 is distorted to some extent and consequently became undetectable in five

of the 10 selected structures Figure 8E shows a represen-tation of the electrostatic potential associated with the contact surface of the Nogo-40 structure The most interesting observation here is that the N- and C-terminal parts of Nogo-40 have opposite electrostatic potential surfaces More specifically, the N-terminal nine residues of

Table 1 NMR restraints used for structure calculation and structural statistics for the 10 selected lowest-energy structures.

Restraints for structure determination NOE distance constraints 198

Medium range (|i-j| £ 4) 76 Statistics for structure calculation

Final energies (kcalÆmol)1)

E(Van der Waals) 21.0 ± 2.5

Root mean square deviations from idealized geometry

Angle (degree) 0.400 ± 0.0135 Improper (degree) 0.285 ± 0.0350

Average RMSD (A˚) from the lowest-energy structure for backbone/heavy atoms

N-terminal helix (7–12) 0.22/1.11 C-terminal helix (26–37) 0.61/1.58 Additional helix (20–24) 0.78/1.69

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Nogo-40 constitute a large positive surface (blue) while the

C-terminal residues make up a large negative surface (red)

Discussion

The discovery that the molecular interaction between

Nogo-66 and NgR poses inhibitory effects on the CNS neuronal

regeneration makes the Nogo-66–NgR interface an

extre-mely promising target for design of molecules to treat CNS

injuries However, it has been extensively speculated that in

addition to the Nogo-66 loop, other regions of Nogo-A

might also play critical roles in inhibiting CNS neuronal

regeneration [7–11] Indeed, a recent study showed that

Nogo-A, the longest member of the Nogo transcripts

encoding for more than 1000 amino acid residues, has at least two discrete regions with neuronal growth inhibitory effects [4,11] As no previous structural study has been reported for Nogo-A, we carried out a detailed CD and NMR investigation in an attempt to gain structural insights into these two functional regions Our results revealed that although Nogo-A(567–748) is functionally active, it is only partially structured either due to the loss of the stabilizing contacts provided by other parts of the Nogo-A protein or is

a member of so called natively unstructured proteins, which only become well-structured upon binding to their inter-acting partners or cognate receptors [28,29], or even both Interestingly, the observation that the Zn2+ was able to specifically induce the formation of helical structures in

Fig 8 Solution structure of Nogo-40 (A) The 10 lowest-energy structures superimposed over the N-terminal helix over residues 7–12 (B) The same

10 lowest-energy structures superimposed over the C-terminal helix over residues 26–37 (C) Ribbon representation of one conformational ensemble

of Nogo-40 structure with only two helices formed (D) Ribbon representation of another conformational ensemble of Nogo-40 structure with an additional helix over residues 20–24 (E) Representation of the electrostatic potential associated with the contact surface of the Nogo-40 solution structure Two distinctive surfaces are observed: the N-terminal surface is largely positive (blue) while the C-terminal part is negative (red).

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Nogo-A(567–748) might constitute an interesting clue for

future functional studies of Nogo-A

On the other hand, the recent identification of Nogo-40

as a potent NgR antagonist suggests a promising starting

point for the design of potential therapeutic agents to

enhance CNS neuronal regeneration Knowledge of the

three-dimensional structure of Nogo-40 is necessary for

both understanding the endogenous Nogo-66–NgR

inter-action and for the rational design of other NgR-binding

antagonists Although Nogo-40 is highly disordered in

aqueous buffer, close NMR examination indicates that it

has an intrinsic propensity to assume helical conformations

This provides a key rationale for the use of TFE, which

represents a common practice in stabilizing the structure of

a polypeptide with intrinsic helical propensity to enable their

further analysis [29]

The NMR structure of Nogo-40 reveals that the N- and

C-terminal segments of Nogo-40 have opposite

electro-static potential surfaces, thus providing an important

clue for understanding the Nogo-40–NgR interaction

Recently, the determination of the crystallographic

struc-ture of the NgR ectodomain led to the speculation that

one potential Nogo-66 binding site on NgR has

charac-teristics of a negative cavity, consisting of residues Asp111,

Asp114, Ser113 and Asp138 [30,31] As shown in Fig 8E,

the C-terminal part of Nogo-40 is highly negatively

charged, making it unlikely as a candidate for binding to

this acidic NgR cavity On the other hand, it is highly

probable that the N-terminal positive part is responsible

for its binding to the NgR negative cavity This is in

complete agreement with previous findings that deletion of

the first five residues at the N-terminal end of Nogo-66

greatly diminished NgR binding, and deletion of the first

10 residues abolished NgR binding [10] It has also been

shown that residues 30–33 of Nogo-66 (containing residues

Glu31 and Glu32) are important for NgR binding Given

the fact that both N- and C-terminal residues of Nogo-40

were required for NgR binding, it would be logical to

speculate that the C-terminal part of Nogo-40 may bind to

a positively charged surface on NgR, which is not revealed

by the current NgR structure Alternatively, it is also

possible that this part of Nogo-40 may even bind to other

molecules such as the recently identified NgR coreceptor

p75NTRin the formation of a multicomponent complex

In summary, our study represents the first structural

insights into the two functional regions of Nogo-A

critical for inhibiting CNS neuronal regeneration The

results showed that the region consisting of Nogo-A(567–

748) is only partially structured but can be induced to

form a helical structure via interaction with Zn2+

Furthermore, the determination of the Nogo-40 solution

structure offers a starting point for further understanding

the interaction between NgR and Nogo-40, and for

future designs of molecules to enhance CNS neuronal

regeneration using NMR methodology as demonstrated

previously [32–35]

Acknowledgements

This work is supported by the NMRC grant R183-000-092-214, the

BMRC grant R-183-000-097-305 and the BMRC Young Investigator

Award R-154-000-217-305 to J Song and BMRC grant

R-183-000-098-305 to B.L Tang The authors acknowledge J Lefebvre for peptide synthesis, H Zhang, Y.H Han for accessing NMR spectrometer and X.H Wu at the Protein and Proteomics Center (PPC), National University of Singapore for MALDI-TOF mass spectrometric analysis.

References

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