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However, PrP113 – 231 lacked any toxicity suggesting the normal N-terminus of the C-terminal metabolic cleavage product of the prion protein suppressed toxicity.. PrP peptides and protei

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Toxicity of novel C-terminal prion protein fragments and peptides harbouring disease-related C-terminal mutations

Maki Daniels1, Grazia Maria Cereghetti2and David R Brown1

1 Department of Biochemistry, Cambridge University, UK;2Institute of Molecular Biology and Biophysics, ETH-Hoeneggerberg, Zu¨rich, Switzerland

Mice expressing a C-terminal fragment of the prion protein

instead of wild-type prion protein die from massive neuronal

degeneration within weeks of birth The C-terminal region

of PrPc (PrP121 – 231) expressed in these mice has an

intrinsic neurotoxicity to cultured neurones Unlike PrPSc,

which is not neurotoxic to neurones lacking PrPcexpression,

PrP121 – 231 was more neurotoxic to PrPc-deficient cells

Human mutations E200K and F198S were found to enhance

toxicity of PrP121 – 231 to PrP-knockout neurones and

E200K enhanced toxicity to wild-type neurones The normal

metabolic cleavage point of PrPcis approximately

amino-acid residue 113 A fragment of PrPccorresponding to the

whole C-terminus of PrPc (PrP113 – 231), which is eight

amino acids longer than PrP121 – 231, lacked any toxicity This suggests the first eight amino residues of PrP113 – 121 suppress toxicity of the toxic domain in PrP121 – 231 Addition to cultures of a peptide (PrP112 – 125) correspond-ing to this region, in parallel with PrP121 – 231, suppressed the toxicity of PrP121 – 231 These results suggest that the prion protein contains two domains that are toxic on their own but which neutralize each other’s toxicity in the intact protein Point mutations in the inherited forms of disease might have their effects by diminishing this inhibition Keywords: prion; neurotoxicity; circular dichroism; neuro-degeneration

PrPcis a normal cell surface glycoprotein expressed by many

cells including neurones and astrocytes [1– 3], microglia [4],

oligodendroglia [2], leukocytes [5] and muscle cells [6]

PrPc is attached to the cell membrane via a GPI

(glyco-phosphoinositol) anchor [7] Predominantly expressed at

synapses [8], it has been suggested that PrPcis important for

neuronal activity [9] More recently it has been shown that

PrPcbinds copper via an octameric repeat region [10] PrPc

has been shown to bind significant amounts of copper in

vivo and this copper binding may be necessary for its

normal form [11] Recent work has suggested two functions

for the protein PrPc influences uptake of copper into

neurones [12] where it can be utilized for synaptic release

[12] or incorporation into enzymes such as Cu/Zn

super-oxide dismutase [13] Other data suggest that once PrPchas

bound copper, the protein can act as a superoxide dismutase

or superoxide scavenger [14]

During normal metabolism of PrPc, cleavage occurs in a

region around amino-acid residues 112 – 114 The metabolic

C-terminal fragment of this protein can be detected

nor-mally in brain [15] and the N-terminal fragment, retaining

the copper binding region can be purified by metal affinity

chromatography from brain [16] The rate of cleavage is

regulated by protein kinase C [17] and cleavage has been

suggested to be brought about by the metalloprotease

disintegrins ADAM10 and ADAM17 [18] However, the

cellular fate or function of these fragments after cleavage remains unknown Conformational change in PrPcstructure results in a higher percentage of b sheet structure and increased protease resistance, suggesting that the protein can

no longer be cleaved at this point

Prion diseases are fatal neurodegenerative diseases In these diseases, PrPcis converted to a protease resistant form (PrPSc)that cannot be cleaved at the normal cleavage site PrPScrepresents an altered isoform that differs markedly in conformation and accumulates to high levels in nervous tissue [19] PrPScis either a major part or the sole constituent

of the infectious agent of prion disease [20] and is also neurotoxic when applied to cultured cells [21] PrPSc is evidently the cause of neurodegeneration in vivo However, induction of neuronal loss both in vivo and in vitro requires the expression of PrPc[21,22] Mice lacking expression of PrPc are resistant to both the toxicity of PrPSc and its neurodegenerative effects [22,23]

Attempts to understand the mechanism of PrPSc neuro-toxicity have focussed on a single peptide known as PrP106 – 126 [24,25] This peptide corresponds to the region

of the human protein that is normally cleaved during cellular processing of PrPc but which becomes protease resistant when PrPc is converted to PrPSc This peptide has many features of PrPSc including protease resistance, ability to form fibrils and high b sheet content The mechanism of the action of this peptide has been studied in detail in culture by many groups [24,26,27,28,29,30,31] including our own [25,32,33,34,35,36,37] and has also been shown to be toxic

in vivo [38] The basic mechanism by which PrP106 – 126 kills neurones in cerebellar cell cultures has been shown

to be the same as that by which PrPScacts Both require neuronal expression of PrPc[21,25,32] and the involvement

of a stress event such as superoxide production by activated microglia [21,25] PrP106 – 126 kills the neurones, probably

Correspondence to D R Brown, Department of Biology and

Biochemistry, University of Bath, Bath BA2 7AY, UK.

Fax: 1 44 1225 826 779, Tel.: 1 44 1225 323 133,

E-mail: bssdrb@bath.ac.uk

(Received 14 September 2001, accepted 1 October 2001)

Abbreviations: MTT,

3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl-tetrazolium bromide.

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as a result of reduction in neuronal resistance to oxidative

stress [33] Apoptosis induced by the peptide follows as a

result of increased calcium influx throughL-type channels

and NMDA receptors [34] Attempts to define the toxic

region of the protein further have identified the region

AGAAAAGA as being necessary for both fibril formation

and PrPSc-like toxicity [36] The maximum toxicity was

found for a peptide corresponding to amino-acid residues

113 – 126 of the human sequence containing this palindrome

[36]

Mice have been generated that express truncated versions

of PrPc In particular, a mouse expressing a prion protein of

106 amino acids [39] has been used to identify those parts of

the protein necessary for both infection and

neurodegenera-tion in prion disease The truncated version of PrPccan be

converted into a truncated PrPSc capable of infecting the

same transgenic mice and inducing neurodegeneration The

106 amino acids comprise the amino-acid residues 89 – 140

and from 177 to the C-terminus

Although some mice expressing truncated forms of PrPc

do not develop spontaneous disease [39,40] others do [41,42]

Of particular interest are mice with N-terminal deletions

lacking amino-acid residues up to 121 or 134 of the mouse

sequence These mice express truncated protein at the cell

surface and develop degeneration in the cerebellum shortly

after birth This disease is not prion disease but represents a

novel form of cerebellum-specific degeneration Some mice

that have genetic ablations to prevent expression of all PrPc

overexpress the prion protein homologue, Doppel [43] Such

mice show Purkinje cell degeneration Doppel is

homo-logous to the N-terminally truncated PrP that induces

cerebellar cell loss Co-expression of full length PrPcwith

either the N-terminally truncated PrPcin mice [42] or

re-introduced into the Doppel expressing PrPc-knockout mice

[44] prevents neurodegeneration Therefore expression of

Doppel or a C-terminal region of PrPc(PrP121 – 231) in the

absence of the full length prion protein leads to

neurodegeneration The mechanism of this is unknown

The present investigation was carried out to determine if

the C-terminal region of PrPc(PrP121 – 231) has intrinsic

neurotoxicity and whether PrPchas an intrinsic mechanism

to inhibit this Unlike PrPScPrP121 – 231 is more neurotoxic

to PrPc-deficient cells Mutants of PrP121 – 231 carrying

known human mutations in the C-terminal region (E200K,

D178N and F198S) were also investigated In particular,

E200K and F198S were also found to enhance toxicity

However, PrP113 – 231 lacked any toxicity suggesting the

normal N-terminus of the C-terminal metabolic cleavage

product of the prion protein suppressed toxicity

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

Unless stated, pharmacological agents were purchased from

Sigma

Animals

Prion protein knockout mice (Npu-Prnp8/8) used in this study

were those described by Manson et al [45] or for some

experiments a different strain was used (Zrk-Prnp8/8) and

these were as described by Bu¨eler et al [46] The wild-type

mice used were either 129Ola mice (as control for

Npu-Prnp8/8) or descendants of an F1 generation mouse produced

by interbreeding the original parental strains (C57BL/6 J and 129/Sv(ev) mice) used to generate Zrk-Prnp8/8 mice originally

Neuronal cell culture Preparation of cerebellar cells from 6-day-old mice (P6) or cortical cells from newborn mice (P0) was as previously described [25,36] Briefly, the cerebella were dissociated

in Hank’s Solution (Gibco) containing 0.5% trypsin (Sigma) and plated at 1– 2  106cells:cm22in 24-well trays (Falcon) coated with poly D-lysine (50 mg:mL21, Sigma) Cultures were maintained in Dulbecco’s minimal essential medium (Gibco) supplemented with 10% fetal bovine serum, 2 mM glutamine and 1% antibiotics (penicillin, streptomycin, fungizone; Gibco) Cultures were maintained at 37 8C with 5% CO2for 10 days The neuronal nature of these cultures was confirmed by immunostaining of parallell wells with neurofilament as previously described [3]

Peptides or proteins were added to cultures initially and on the third day Cell survival was determined on day

5 or 7 3-(4,5-Dimethylthiazol-2-yl)-2,5-diphenyl-tetrazo-lium bromide (MTT; Sigma) was diluted to 200 mM in Hanks’ solution (Gibco) and added to cultures for 1 h at

37 8C The MTT formazan product was released from cells

by addition of dimethylsulfoxide (Sigma) and measured at

570 nm in a Unicam Helios spectrophotometer (ATI Unicam) Relative survival in comparison to untreated control cultures could then be determined

For coculture experiments, cerebellar cells were plated as normal in 24-well trays Microglia were plated at 10 000 cells per well in Falcon insets with 0.4-mm pore diameter Peptides could then be applied directly to the lower wells and to the insert After peptide treatments, the inserts were removed and MTT assays carried out on the cerebellar cells

as before

Glia cell culture Microglia were isolated as described previously [25] Briefly, cortices from newborn mice were dissociated with trypsin and seeded into tissue culture flasks (Falcon) When cultures were confluent, microglia were isolated by rapid shaking for 2 hours Microglia were isolated by shaking mixed glial cultures for 2 h The floating cells were collected and plated for 30 min The nonadhering cells were discarded The adhering cells were identified as pure cultures of micro-glia by immunostaining for ferritin as previously described [25]

PrP peptides and protein Mouse prion protein peptides (PrP121 – 231), both wild-type and those carrying human mutations, were generated as previously described [47] The wild-type peptide (PrP121 – 231) was mutated to carry amino-acid substitutions equivalent to the human mutations E200K, D178N and F198S as previously described [47] The numbering refers to the human sequence but the equivalent amino-acid residue

of the mouse sequence was altered (one codon proximal in each case)

Purification of these mutants from inclusion bodies was as previously described [47] except that the bacteria were

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grown at 26 8C to avoid major degradation of the protein and

no gradient was applied to the DE52/CM52 column during

purification Full length protein (PrP23 – 231) and other

recombinant proteins equivalent to the complete metabolic

C-terminal cleavage product of PrP (PrP113 – 231) or

dele-tion mutants, PrP23 – 112, PrP79 – 231 and PrP105 – 231,

were also purified and refolded as previously described [14]

PrP23 – 112, PrP113 – 231, PrP105 – 231 and PrP79 – 231

were generated by PCR-based mutagenesis using splint

oligonucleotides to introduce a restriction site before codon

113, 105 or 79 or after codon 112 Following digestion of the

pET-PrP construct with Nde I the N-terminus encoding

region was removed and religation of the vector lead to a

pET-PrP construct expressing the complete metabolic

C-terminal fragment of PrP as determined by sequencing

The N-terminal fragment was prepared by digestion of the

mutated plasmid with Xho I, removing the C-terminal

encoding fragment and religating the plasmid Fidelity of

the N-terminus of these deletion mutants was determined by

mass spectroscopy analysis

Shorter peptides were synthesized in house by the PNAC

facility These peptides based on the mouse prion protein

sequence with corresponding amino-acid residues were

PrP112 – 125(AGAAAAGAVVGGLG), 121 – 146(AVVGG

LGYMLGSAMSRPIIHFGSDYED), PrP147 – 171(RYYRE

NMYRYPNQVYYRPVDQYSNQ), PrP163 – 184(RPVDQ

YSNQNNFVHDCVNITIK), PrP180 – 198(NITIKQHTVTT

KGENFT) and PrP196 – 220(NFTETDVKMMERVVRQM

CVTQYQKE)

CD spectroscopy and analysis

CD spectra were recorded for prion proteins and peptides

using a CD6 spectropolarimeter (Jobin Yvon, Division

d’Instrumente S.A.) or a Jasco J-810 spectropolarimeter,

calibrated with ammonium (1)-camphor-10-sulfonate by a

method similar to that described previously [36] Peptide

samples were diluted from high concentration

dimethylsulf-oxide stocks to a concentration of 2 mg:mL21 in 10 mM

sodium phosphate (pH 7.4) These samples were measured

in cuvettes of 1 mm or 0.5 mm pathlength (Hellma) The

spectrum from 190 nm to 250 nm was analysed with step

resolution of 0.5 nm at a temperature of 23 8C Five scans

were averaged and the background from buffer was

subtracted Spectra are presented as molar ellipticity (u)

R E S U L T S

PrP121 – 231 is toxic to neurones

Prion proteins of different lengths were tested for toxicity by

application to cultures of cerebellar neurones Cerebellar

cultures were prepared from 6-day-old mice The proteins

were applied to the cultures and the cultures were

maintained in serum-free medium for 7-days The medium

was changed every 3 days and replenished with prion

proteins At the end of that time, survival was determined

using an MTT assay Full length recombinant PrPc, PrP79 –

231, PrP105 – 231 and PrP113 – 231 showed no toxicity to

wild-type cultures of cerebellar cells (Fig 1A) However,

PrP121 – 231 was toxic to these cells in a dose-dependent

manner The proteins were also applied to cultures of

Npu-Prnp8/8 cerebellar cells and the same results were obtained

(Fig 1B) However, PrP121 – 231 was more toxic to Prnp8/8 cerebellar cells than to wild-type cells (Student’s t-test,

P , 0.05) Additionally, PrP121 – 231 was more toxic to Zrk-Prnp8/8 cerebellar cells than wild-type cerebellar cells

Fig 1 Toxicity of prion proteins Cerebellar cell cultures from wild-type (A) and Npu-Prnp8/8 (B) cerebellar cells were grown in serum-free medium and treated with prion proteins at different concentrations for

7 days After that time the survival of the cultures was measured with an MTT assay The values were compared to those for untreated cultures as

a percentage Shown are PrP23 – 231 (W) PrP79– 231 (O), PrP105–231 (A), PrP113–231 (K) and PrP121–231 (X) Bovine serum albumin (B) was used as a negative control (C) Wild-type and Zrk Prnp8/8 cerebellar cells were either treated with L -leucine methyl ester (grey bars) or cocultured with additional microglia (black bars) Cerebellar cells were treated with 1 mg:mL21PrP23– 231 or PrP121 – 231 for 7 days After this time, the survival was measured using an MTT assay and comparing values to those of untreated cultures (open bars) Shown are the mean ^ SEM of four experiments (different cultures) with three determinations (separate wells) each.

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(Fig 1C) This confirms that the increased toxicity to

Prnp8/8 cerebellar cells is a result of the lack of PrPc

expression and not the genetic background of the mice

These results suggest that the toxicity of PrP121 – 231 does

not require the expression of native PrPc

Previously, it has been shown that the synthetic peptide

fragment PrP106 – 126 is toxic and that this toxicity requires

microglia L-Leucine methyl ester selectively destroys

microglia [25] Cultures of wild-type and Zrk- Prnp8/8

cerebellar cells were treated with 50 mM L-leucine methyl

ester for 2 h before application of PrP121 – 231 or were

cocultured continuously with wild-type microglia during

application of PrP121 – 231 for 7 days At the end of this

time an MTT assay was carried out Treatment with

L-leucine methyl ester had only a minor effect on the

toxicity of the protein Addition of microglia had no

signifi-cant effect on the toxicity of PrP121 – 231 These results

suggest that the toxicity of PrP121 – 231 does not require

involvement of microglia

In order to verify that PrP121 – 231 is toxic to neurones,

staining with Hoechst 33342 reagent was carried out during

treatment of cerebellar cell cultures Dying neurones could

be determined by the presence of condensed and/or

frag-mented nuclei (Fig 2) Treatment with PrP121 – 231 caused

a great increase in the number of fragmented nuclei present

after 4 days of treatment as compared to treatment with full

length protein (PrP23 – 231) The quantitation of this is

shown in Fig 2C

Peptide dissection of PrP121 – 231 toxicity

Five synthetic peptides corresponding to the majority of

PrP121 – 231 were synthesized These peptides were

PrP121 – 146, PrP147 – 171, PrP163 – 184, PrP180 – 198 and

PrP196 – 220 Initially we attempted to synthesize a set of

four nonoverlapping peptides However, one of these

peptides self terminated during synthesis Therefore two

overlapping peptides were produced to cover the region

172 – 180 As for the recombinant proteins, the toxicity of

these peptides was tested on cultures of wild-type and

Npu-Prnp8/8 cerebellar cells (Fig 3) Peptides PrP121 – 146,

PrP147 – 171 and PrP180 – 198 showed little or no toxicity to

wild-type cells whereas PrP196 – 220 and PrP163 – 184 were

both toxic to wild-type cerebellar cells (Fig 3A) However,

when applied to Npu-Prnp8/8 cerebellar cells PrP147 – 171

showed toxicity This suggests that this peptide is toxic in

the absence of PrPcexpression PrP163– 184 showed reduced

toxicity However, PrP196 – 220 also remained similarly

toxic (Fig 3B) These results suggest that the toxicity of the

C-terminal domain of PrPcin particular is associated with

amino-acid residues 163 – 184 but that amino-acid residues

further N-terminal to this may also participate in the toxicity

to PrPcdeficient cells Additionally residues of PrP196 – 220

might also participate in this toxicity

The peptides used in this analysis were studied using

the CD spectroscopic technique The analysis of the

struc-tural content was determined by the curve fitting program

CNNR The CD spectra of the five peptides appears in Fig 4

The analysis of the structural content of the peptides appears

in Table 1 As can be seen in Fig 4, PrP180 – 198 has a

noticeably different spectrum with an unusual minimum at

230 nm It is currently unclear what this minimum

represents PrP196 – 200 has a high percentage of b sheet

structure This peptide readily forms fibrils (data not shown)

Mutants of PrP121 – 231 Further recombinant mouse proteins based on PrP121 – 231 were analysed for toxicity These new proteins contained the equivalent of one of three human point mutations associated with human prion disease The mutations analysed were E200K, D178N and F198S For simplicity the mutants of PrP121 – 231 shall be referred to by these mutation assign-ments even though in the mouse sequence the location of the residue is numerically one place closer to the N-terminus in the sequence (e.g E200K in human but in mouse the E is at 199) PrP121 – 231 will be referred to as wild-type protein Wild-type cerebellar cells were treated with the four

Fig 2 PrP121–231 causes apoptotic cell death Cerebellar cells from wild-type mice were exposed to PrP23 – 231 (A) or PrP121 – 231 (B) for 2 days The cells were then stained with the Hoechst reagent to detect fragment or condensed nuclei An increase in aberrant nuclei (bright condensed, fragmented) was only detected in cultures treated with PrP121 – 231 Scale bar, 50 m M (C) Quantitation of aberrant nuclei

in culture treated with either PrP23 – 231, PrP121 – 231 or the control Ten fields were counted on three coverslips for four separate experiments Shown and mean and SEM.

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different proteins for 7 days, after which time an MTT assay

was used to quantitate survival The E200K mutation was

the only mutation to increase the toxicity of PrP121 – 231

significantly above that of the wild-type protein (P , 0.05)

(Fig 5A) Zrk-Prnp8/8 cerebellar cells were also treated with

the proteins and assayed for survival in the same manner

(Fig 5B) Both E200k and F198S showed significantly

(P , 0.05) more toxicity to Zrk-Prnp8/8 cerebellar cells than

the wild-type PrP121 – 231 The implication of these results

is that the mutations in the region of amino-acid residues

198 – 200 enhance the toxicity of the peptide PrP121 – 231

Peptide inhibition of PrP121 – 231 toxicity

In the paper by Shmerling et al [42] it was suggested that

the in vivo toxicity of PrP121 – 231 was inhibited by the

coexpression of full length PrPc(PrP23 – 231) Therefore we tested whether PrP23 – 231, PrP23 – 112, PrP105 – 231 or PrP113 – 231 would inhibit the toxicity of PrP121 – 231 to Npu-Prnp8/8 cerebellar cells Of these proteins only PrP23 –

231 inhibited toxicity completely as determined by MTT assay (Fig 5C) However, PrP105 – 231 showed a low level

of inhibition This result suggests that PrP23 – 231 contains a domain inhibitory to the toxicity of PrP121 – 231, but this domain does not lie in the unstructured N-terminus; possibly

it lies in the hydrophobic domain of PrPc

A recent study on optimization of the neurotoxicity of the well characterized prion protein peptide PrP106 – 126 [36] indicated that optimal toxicity of this region is located in amino-acid residues 113 – 126 of the human sequence This region is identical to amino-acid residues 112 – 125 of the

Fig 4 Circular dichroism study of peptides Peptides were freshly prepared in 10 m M phosphate buffer pH 7.4 at 2 mg:mL21 The peptides shown are PrP112 – 125, PrP121 – 146, PrP147 – 171, PrP163 –

184, PrP180 – 198 and PrP196– 220 Five sweeps were collected at 0.5-nm intervals Spectra are presented as molar ellipticity (u).

Fig 3 Toxicity of peptides to cerebellar neurones Cerebellar cell

cultures from wild-type (A) and Npu-Prnp8 / 8 (B) cerebellar cells were

grown in serum free medium and treated with prion protein peptides at

different concentrations for 5 days After that time the survival of the

cultures was measured with an MTT assay The values were compared

to those for untreated cultures as a percentage Shown are PrP121 – 146

(W) PrP147–171 (X), PrP163–184 (A), PrP180–198 (K) and PrP196–

220 (O) Shown are the mean ^ SEM of four experiments with three

determinations each.

Table 1 Analysis of CD of peptides Values determined using the

CNNR program Analysis based on the spectra between 190 and 250 nm.

Helix b Sheet b Turn Random coil

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mouse sequence This peptide is highly toxic to wild-type

cerebellar cells but is not at all toxic to Zrk-Prnp8/8

cerebellar cells [37] The ability of this peptide to inhibit

the toxicity of PrP121 – 231 was analysed Increasing

amounts of PrP112 – 125 were mixed with fixed amounts

of E200K, D178N, F198S and wild-type PrP121 – 231 and

applied to Npu-Prnp8/8 cerebellar cells for 5 days After

this time, an MTT assay was used to measure survival

(Fig 5D) PrP112 – 125 suppressed the toxicity of

wild-type PrP in a dose-dependent manner reaching saturation

above a 1 : 1 molar ratio PrP112 – 125 was not able to

completely suppress the toxicity of the mutant proteins

There was no further effect of toxicity above a 1: 1 molar

ratio The relative order of effective suppression was

wild-type F198S E200K D178N Indeed, for

D178N there was no significant inhibition of toxicity

(P 0.05)

CD analysis of peptide – protein interaction

The CD spectra of PrP121 – 231 and its mutants (in the

presence or absence of an equimolar amount of PrP112 –

125) were measured (Fig 6) In general, and as previously

described [47], the three point mutations did not alter the CD

spectra markedly (Fig 6A) PrP112 – 125 has previously been shown to have a predominantly random coiled structure with some amount of b sheet (Fig 4) The mixture of wild-type PrP121 – 231 and PrP112 – 125 resulted

in a unique CD spectrum that did not resemble that of PrP121 – 231, PrP112 – 125 or an arithmetic sum of the two

Fig 5 Toxicity of PrP121 – 231 mutants Cerebellar cell cultures

from wild-type (A) and Zrk-Prnp8/8 (B) cerebellar cells were grown in

serum free medium and treated with mutants of PrP121 – 231 at

different concentrations for 7 days After that time the survival of the

cultures was measured with an MTT assay The values were compared

to those for untreated cultures as a percentage Shown are wild-type (W)

D178N (K), F198S (O) and E200K (X) (C) Npu-Prnp8/8 cerebellar

cells were either treated with 50 m M of PrP121 – 231 and with

increasing concentrations of PrP23 – 231 (X), PrP23–112 (W), PrP105–

231 (K) or PrP112–231 (O) After 5 days treatment the survival was

measured using an MTT assay and comparing values to those of

untreated cultures Shown are the mean ^ SEM of four experiments

with three determinations each (D) Npu-Prnp8 / 8 cerebellar cells were

either treated with PrP112 – 125 at varying concentrations alone (B) or

with the addition of 50 m M of PrP121 – 231 (W) or PrP121–231

mutants, D178N (K), F198S (O) or E200K (X) After 5 days treatment

the survival was measured using an MTT assay and comparing values to

those of untreated cultures Shown are the mean ^ SEM of four

experiments with three determinations each.

Fig 6 Circular dichroism study of prion proteins Proteins were freshly prepared in 10 m M phosphate buffer pH 7.4 at 0.1 mg:mL21 Wild-type PrP121– 231 (WT) and three mutants (E200K, F198S, D178N) were measured either on their own (compared in A) or mixed with an equimolar amount of PrP112 – 125 (B – E) The spectra of the wild-type form of PrP121 – 231 and the mutants on their own (thin line) are compared to spectra of the same proteins mixed with PrP112 – 125 (thick line) In addition the spectra for PrP105 – 231 (F) and PrP113 –

231 (G) were also determine on their own (thin line) or mixed with PrP112 – 125 (thick line) The increased levels of structural elements were determined by a CD spectra analysis program Five sweeps were collected at 0.5-nm intervals Spectra are presented as molar ellipticity [u] The increased helical content in all the proteins induced by PrP112 – 125 was determined and plotted in (H).

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PrP112 – 125 had similar but lesser effect on the mutant

proteins E200K and F198S There was little effect on the

spectrum of D178N In particular, the mixtures showed

relative increases in helical content (Fig 6H) This change

in spectrum possibly represents a change in the structure of

the protein as a result of an interaction between the protein

and the peptide

In order to determine if the structure produced by the

interaction of PrP112 – 125 and PrP121 – 231 represents a

‘true’ PrP structure, the CD spectra of PrP105 – 231 and

PrP113 – 231 was determined (Fig 6) The CD spectra of

both proteins appear similar but dissimilar to the mixtures

between PrP121 – 231 and PrP112 – 125 The spectra of

PrP113 – 231 and PrP105 – 231 were similar to that of

PrP121 – 231 However, both spectra show a loss of a strong

minima at 222 nm and an increase at 230 nm However,

mixing these proteins with PrP112 – 125 did not cause any

change in the spectrum except a slight increase at 230 nm

There was no increase in helical content (Fig 6H)

D I S C U S S I O N

The precise mechanism of neurodegeneration in prion

disease is unknown Much research has concentrated on a

peptide PrP106 – 126 to understand neuronal death in

models of these diseases Until this report there has been

no complete investigation of the prion protein for toxic

domains It has been known for some time that the

N-terminus (amino-acid residues 23 – 90) is not associated

with disease We aimed to investigate whether the

C-terminal domain has inherent toxicity to neurones

because a recent publication by Shmerling et al [42] has

shown that mice expressing a C-terminal fragment of PrPc

(either deletion of amino-acid residues 32 – 121 or 32 – 134)

die within several weeks of birth due to massive

neuro-degeneration in the granule cell layer of the cerebellum A

different C-terminal fragment of PrPc (PrP112 – 231) is

generated by normal cleavage of the protein [15] It has been

suggested that this fragment can be cycled back to the

cell surface where it may have a function independent of the

full length molecule [48] We found that the fragment

PrP121 – 231 was highly neurotoxic This seemed to us to be

paradoxical as one would not expect a normal cleavage

product to be potently neurotoxic However, slightly longer

peptides (PrP105 – 231 and PrP113 – 231) showed no

toxicity The region of the mouse protein containing

amino-acid residues 105 – 125 is almost identical to the

sequence of human PrP, which is known as PrP106 – 126, the

neurotoxic peptide used by many laboratories as a model of

the neurotoxicity of PrPSc However, this region of the

protein, as part of a C-terminal fragment of PrPc, has no

demonstrable toxicity Furthermore, addition of a peptide

with amino-acid residues 112 – 125 of the mouse PrPc

sequence to cerebellar cultures in parallel with PrP121 – 231

neutralized the toxicity of PrP121 – 231 The same result

was obtained with mouse PrP121 – 231 and the human

PrP106 – 126 (data not shown) Under these conditions, the

PrP106 – 126 toxicity was fully inhibited Additionally we

also showed that PrP23 – 231 inhibits toxicity but that

neither the N-terminal fragment (PrP23 – 112) nor the full

C-terminal fragment (PrP113 – 231) inhibit the toxicity

Studies of the N-terminus have shown that it is unstructured

and therefore it is unlikely to undergo a conformational

change when PrP23 – 231 is cleaved However, PrP113 – 231 contains a very hydrophobic N-terminus (amino-acid residues 113 – 135) and it is quite possible that this region would be masked if it interacted with other hydrophobic residues in the rest of the protein

The normal cleavage product of PrPc metabolism is a protein cleaved at around amino-residue 112 – 114 and not

121 – 122 [15,17,18] Therefore separation of the hydro-phobic, palindromic region of 112 – 120 from the rest of the C-terminus is artefactual Such a fragment of the protein has never been shown to exist in vivo Furthermore, the paper by Shmerling et al [42] demonstrates that expression of a fuller C-terminal cleavage product with a deletion only of residues

32 – 106 does not develop pathology The toxicity of the C-terminal part of PrPchas never been apparent before the publication by Shmerling et al [42] and most interest has focussed on the known neurotoxic region PrP106 – 126 whose toxicity came to attention because of study of the toxicity of PrPSc[24] If deletion of PrPcup to residue 121 creates a toxic protein then one would expect that deletion of the C-terminus of the protein should similarly cause prob-lems Muramato et al [41] showed that deletion of amino-acid residues 177 – 200 or 201 – 217 results in neurodegen-erative disease in mice expressing such modified PrPs However, the disease was not as severe as that described by Shmerling et al [42] and the cell death does not appear to be due to the toxicity of the hydrophobic domain (amino-acid residues 112 – 135) Our findings regarding PrP121 – 231 mediated neurotoxicity might explain the cerebellar degeneration described by Shmerling et al [42] However, although our results suggest that the neurodegeneration in this model could be the result of direct neurotoxic effects of PrP121 – 231, the full mechanism of this effect needs to be elucidated

The neurodegeneration seen in the 32 – 121 deleted mice [42] was prevented by the presence of coexpressed full-length PrPc The previous interpretation of this result was that PrPchas a ligand that interacts with it at two domains When the protein only interacts with PrPcat the C-terminal domain, the resulting signal transduction leads to death However, the problem with this model is that the metabolic C-terminal domain of PrPc(PrP112 – 231) exists in neurones all the time Even if it has a much lower affinity for the

‘ligand’ than full length PrPcthen one would nevertheless be causing the death of cerebellar granular cells A better hypothesis according to our data is that the C-terminal domain (PrP121 – 231) as expressed by Shmerling et al [42] can interact with full length PrPc This interaction via binding to the hydrophobic domain of PrPcthen inhibits the toxicity of the C-terminus

The normal N-terminal domain of the C-terminal cleavage product of PrPcis conserved so highly as to be unchanged from reptile to man [49,50] This is very unusual, especially for a region of the protein associated with neurotoxicity Therefore it is clearly essential to the normal metabolism of PrPc We have shown previously [11,37] that this region of the protein is the site of interaction between PrPc with PrPSc Therefore it is possible, under normal metabolic conditions, that the hydrophobic-palindromic region of PrPcinteracts directly with the globular domain of the C-terminus of another molecule of PrPc However, we consider it more likely that each molecule folds in such a way that the very N-terminus of PrP’s C-terminal cleavage

Trang 8

product folds into the globular domain Due to the very

hydrophobic nature of this region, this may occurs directly

after cleavage of the protein

Our studies of toxicity used wild-type neurones and

neurones deficient in PrPc expression in parallel This

allowed us to distinguish fragments or peptides that were

toxic in absence of PrPc This also allowed us to demonstrate

that the toxicity of PrP121 – 231 is different to that of PrPSc,

as PrPScis nontoxic to cells lacking PrPcexpression [21] but

the toxicity of PrP121 – 231 is increased to Prnp8/8 cerebellar

cells In particular, the region of amino-acids 147 – 171

shows toxicity only to Prnp8/8 cerebellar cells and might

explain the increased toxicity of PrP121 – 231 to Prnp8/8

cerebellar cells PrP peptides based on the hydrophobic

domain of PrPchave also been suggest to have effects not

mediated directly through PrPc[28,30] but this is the first

time the peptides based other regions of PrP have been

shown to be toxic to Prnp8/8 neurones

Of importance are the studies with peptides that highlight

the region of the C-terminus involved in the toxicity of

PrP121 – 231 to cerebellar neurones Two peptides, PrP163 –

184 and PrP196 – 220, appeared to be the most toxic This is

of considerable interest as the majority of point mutations

associated within inherited human prion disease are found

within these regions (e.g D178N, V180I, T183A, F198S,

E200K, R208H, V201I, Q217R) Indeed, the two point

mutations studied in this paper, E200K and F198S, both map

to PrP196 – 220 and both enhanced the toxicity of PrP121 –

231 It is quite possible that these point mutations alter the

ability of the globular domain to interact with the conserved

hydrophobic region This was demonstrated here by a

decreased ability of PrP112 – 125 to inhibit the toxicity of

the PrP121 – 231 mutants

Many of these point mutations lie along a hydrophobic

cleft in the protein [47,51] It is quite possible that the

N-terminal domain of the C-terminal cleavage product will

fold into this cleft However, this report does not give any

information on this aspect of the structure of the protein

Previously, NMR studies of PrPchave used either PrP121 –

231 or PrP23 – 231 as the protein for analysis [47,52 – 55]

The general finding of these reports was that the C-terminal

of the protein contains three helices that fold together to

make a globular domain while the N-terminus has little

structure For both the full length protein and the C-terminal

fragment the globular domain was very similar However,

the protein PrP121 – 231 does not represent the true

C-terminal fragment of PrP as it does not include the

perfectly conserved amino-acid residues 112 – 120 which

constitute the true N-terminus Therefore it is probably of

vital importance that the C-terminal fragment containing

these additional amino acids be studied further, as the true

C-terminal fragment of PrPcmay form a novel conformation

as yet unknown Support for this comes from the analysis by

CD of two proteins PrP105 – 231 and PrP113 – 231 that have

moderately different spectra to that of PrP121 – 231 It has

previously been suggested that such proteins prepared

from bacteria are sensitive to protease digestion and the

amino-acid residues up to 121 are cleaved off [53] We took

particular care to ensure that our proteins were not degraded

in this way

Analysis of the effect of point mutations on the structure

of PrPchave focussed on their effect on the protein PrP121 –

231 We have observed that two mutations alter the toxicity

of this protein but this is not likely to have direct relevance

to prion disease as the protein PrP121 – 231 does not normally exist However, if the amino-acid residues where these mutations occur are central to refolding of the protein after cleavage then it is possible that C-terminus could be toxic in the inherited prion diseases Alternatively, or in addition, a misfolded C-terminal protein could somehow influence formation of PrPSc Another alternative is that interaction between the globular domain and the hydro-phobic-palindromic region influences cleavage of the protein Then, a large amount of uncleaved mutant PrPc might remain and be sufficient to eventually aggregate and begin conversion to PrPSc

In summary, we have shown that a C-terminal fragment of PrPccommonly used in the investigation of PrPcstructure and known to induce neurodegeneration in mice lacking expression of the full length PrPcis neurotoxic This neuro-toxicity does not require expression of PrPc The neuro-toxicity can be inhibited by the presence of the hydrophobic-palindromic region (amino-acid residues 112 – 125) of the protein either applied as a separate peptide or attached to the protein Known human point mutations enhance the toxicity

of this PrPc fragment However, PrP121 – 231 might not represent the true C-terminal cleavage produce of PrPc metabolism and re-investigation of the biology of the C-terminus of PrPcis necessary

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

The authors than Charles Weissmann for the Zrk1 prion protein knockout mice and Jean Manson for the Npu prion protein knockout mice Thanks also to Rudi Glockshuber for PrP121 – 231 mutant proteins In addition we thank Bill Broadhurst and Tim Daffron for help with the CD analysis.

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