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In gel mobility shift assays, in vitro translated LdEcR alone bound weakly to the pal1 ecdysone response ele-ment, although LdUSP alone did not, and this binding was dramatically enhance

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confirmation of ecdysone receptor and ultraspiracle from the Colorado potato beetle Leptinotarsa decemlineata

Takehiko Ogura1, Chieka Minakuchi1,*, Yoshiaki Nakagawa1, Guy Smagghe2and

Hisashi Miyagawa1

1 Division of Applied Life Sciences, Graduate School of Agriculture, Kyoto University, Japan

2 Laboratory of Agrozoology, Department of Crop Protection, Faculty of Bioscience Engineering, Ghent University, Belgium

The growth of insects progresses via unique

physiologi-cal events such as molting and metamorphosis Those

processes are strictly regulated by two peripheral

hor-mones, molting hormone (20-hydroxyecdysone; 20E)

and juvenile hormone (JH) 20E controls transcription

of target genes by interacting with molting hormone

receptor proteins, which bind to ecdysone response

ele-ments (EcREs) located upstream of the target genes

The transcriptional activation by 20E triggers signal

cascades, and the development is accomplished via

complex regulatory mechanisms [1] The heterodimer

of two nuclear receptors, ecdysone receptor (EcR) and ultraspiracle (USP), functions as a molting hormone receptor, and 20E is known to be a ligand for EcR USP is the homologue of vertebrate RXR [2,3] Amino-acid sequences of EcR and USP were first determined in the dipteran fruit fly Drosophila melano-gaster [4–6], and subsequently determined in other insects [7–25], as well as a crustacean [26] and a tick [27,28] These receptor proteins consist of regions

Keywords

ecdysone receptor (EcR); Leptinotarsa

decemlineata; ponasterone A; ultraspiracle

(USP); 20-Hydroxyecdysone

Correspondence

Y Nakagawa, Division of Applied Life

Sciences, Graduate School of Agriculture,

Kyoto University, Kyoto 606–8502, Japan

Fax: +81 75 7536123

Tel: +81 75 7536117

E-mail: naka@kais.kyoto-u.ac.jp

Present address

*Department of Biology, University of

Washington, Seattle WA 98195–1800, USA

(Received 27 April 2005, revised 13 June

2005, accepted 16 June 2005)

doi:10.1111/j.1742-4658.2005.04823.x

cDNA cloning of ecdysone receptor (EcR) and ultraspiracle (USP) of the coleopteran Colorado potato beetle Leptinotarsa decemlineata (LdEcR and LdUSP) was conducted Amino-acid sequences of the proteins deduced from cDNA sequences showed striking homology to those of other insects, especially the coleopteran yellow mealworm Tenebrio molitor Northern hybridization analysis showed a 12.4-kb message for the LdEcR A-isoform,

a 10.5-kb message for the LdEcR B1-isoform and a 5.7-kb message for the LdUSP, in fat body, gut, integument, testis and ovaries In developmental profile studies, expression of both the LdEcR and LdUSP transcript in integument changed dramatically In gel mobility shift assays, in vitro translated LdEcR alone bound weakly to the pal1 ecdysone response ele-ment, although LdUSP alone did not, and this binding was dramatically enhanced by the addition of LdUSP LdEcR⁄ LdUSP complex also showed significant binding to an ecdysone agonist, ponasterone A (KD¼ 2.8 nm), while LdEcR alone showed only weak binding (KD¼ 73.4 nm), and LdUSP alone did not show any binding The receptor-binding affinity of various ecdysone agonists to LdEcR⁄ LdUSP was not correlated to their larvicidal activity to L decemlineata From these results, it was suggested that multiple factors including the receptor binding affinity are related to the determination of the larvicidal activity of nonsteroidal ecdysone agon-ists in L decemlineata

Abbreviations

ANS-118, chromafenozide; DBH, dibenzoylhydrazine; EcR, ecdysone receptor; EcRE, ecdysone response element; 20E, 20-hydroxyecdysone; pIC50, reciprocal logarithmic value of IC50; PonA, ponasterone A; RH-0345, halofenozide; RH-2485, methoxyfenozide; RH-5849, N-tert-butyl-N,N¢-dibenzoylhydrazine; RH-5992, tebufenozide; RXR, retinoid X receptor; THR, thyroid hormone receptor; USP, ultraspiracle.

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referred to as A⁄ B, C (DNA binding), D, E (ligand

binding) and F, which is consistent to other members

of the nuclear receptor superfamily Molecular

regula-tory mechanisms of transcriptional activation by 20E

were studied intensively in D melanogaster [29–33],

and were also reported for a dipteran, the yellow fever

mosquitoe Aedes aegypti [34], and lepidopterans, the

tobacco hornworm Manduca sexta [35–37] and the

silkworm Bombyx mori [38,39] On the other hand,

the natural ligand of USP is unknown, although recent

in vitro experiments indicated that JH binds to USP

and regulates transcriptional events [40–42]

Although 20E is a steroidal compound, some

syn-thetic ecdysone agonists which have no steroid

struc-ture are known Interestingly, it has been noted that,

while the binding affinity of ecdysteroids such as 20E

and its agonist, ponasterone A (PonA), is comparable

among insect species, that of nonsteroidal ecdysone

agonists, dibenzoylhydrazines (DBHs), are different

among insect orders [43] Recently, the X-ray crystal

structure of the ligand binding domain of EcR was

solved for the lepidopteran tobacco budworm

Helio-this virescens [44] Superimposition of PonA and a

DBH type compound, BYI06830, as bound to EcR

ligand binding domain, suggested that an aromatic

ring moiety of BYI06830 occupies a binding pocket

which is not fully shared with PonA Thus, there is a

possibility that the difference of binding affinity of

DBHs to receptors among insect species is due to the

difference of structures of the ligand binding pocket

In the other study, we demonstrated that the molting

hormone activities of ecdysone agonists measured in

cultured integument system of the lepidopteran rice

stem borer Chilo suppressalis are correlated to and

ruled by their respective receptor binding affinity to

in vitrotranslated EcR and USP proteins of C

suppres-salis[45] These recent results indicate that the

import-ance to investigate ligand–receptor interactions and

compare structures of molting hormone receptors

among insects is increasing for a better understanding

of the function of molting hormone in insect growth

and development

Previously, we performed structure–activity

relation-ship (SAR) studies of ecdysone agonists using C

sup-pressalis, the lepidopteran Spodoptera exigua and a

coleopteran field pest, the Colorado potato beetle

Leptinotarsa decemlineata[46–57] In those studies, the

larvicidal activity of DBHs against C suppressalis was

correlated with those against S exigua but not

correla-ted with those against L decemlineata, suggesting that

the receptor-binding of DBHs in L decemlineata is

dif-ferent to those in C suppressalis and S exigua The

aim of this study is to examine the SAR of ecdysone

agonists for the molecular interaction with the molting hormone receptor Here, we report (a) the determin-ation of primary amino acid structures of EcR and USP from L decemlineata (b) the analysis of mRNA expression profile of L decemlineata, EcR and USP, and (c) the measurement of the binding affinity of steroidal and nonsteroidal ecdysone agonists to the

in vitro translated receptor proteins Comparison of the receptor-binding affinity between various insects is expected to lead molecular bases for the divergence of the toxicity of ecdysone agonists

Results

cDNA cloning of LdEcR and LdUSP

A 379-bp fragment was amplified by RT-PCR using degenerate primers, and its sequence was determined A deduced amino acid sequence of the PCR product was homologous to a corresponding part of EcRs of other insects Then we subsequently conducted 5¢-RACE and 3¢-RACE, and sequences of 1337-bp and 998-bp frag-ments were determined, respectively Combining these sequences of PCR fragments, we deduced the whole cDNA sequence of LdEcR to be 2714-bp long The lon-gest open reading frame (ORF), which is followed by an in-frame termination codon, encodes a 565 amino acid peptide (Fig 1A) The deduced amino acid sequence has a structure typical for the nuclear receptor super-family We also amplified an 833-bp fragment by 5¢-RACE to determine a 2165-bp sequence A 488 amino acid sequence was deduced from this 2165-bp cDNA sequence, which was different to the 565 amino acid sequence only in a part of A⁄ B region (Fig 1B) A database search was conducted using the blast program (http://www.ncbi.nlm.nih.gov/BLAST/) and the longer sequence (565 amino acids) was found to be highly homologous to previously reported EcR A-isoform of other insects Thus we concluded that the longer cDNA encodes L decemlineata EcR A-isoform (LdEcR-A)

On the other hand, the shorter sequence (488 amino acids) was determined to be an EcR B1-isoform of

L decemlineata(LdEcR-B1)

In the same way, we determined a 1699-bp sequence

by combining sequences of 157-bp, 690-bp and 994-bp

of RT-PCR, 5¢-RACE and 3¢-RACE fragments A 384 amino acid sequence (Fig 1C) encoded by the longest ORF of the cDNA sequence has a structure typical for the nuclear receptor superfamily A database search with the blast program showed that this deduced sequence is highly homologous to other USPs Thus

we determined this sequence as L decemlineata USP (LdUSP)

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LdEcR-A and LdUSP amino acid sequences were

compared with EcR and USP sequences of other

insects, respectively (Table 1) The C region of

LdEcR shares a very high amino acid identity with

that of other EcR sequences (91–94%) The E region

of LdEcR is also highly homologous to those of

other EcRs (> 60%), especially to EcR-A from

coleopteran Tenebrio molitor (TmEcR-A, 91%) and

orthopteran Locusta migratoria (LmEcR, 89%) The

D region is homologous to those of T molitor and

L migratoria (78% and 70%, respectively), but less

homologous to those of others (< 38%) The A⁄ B

regions are rather diverse among all sequences

(< 52%) Similarly, the amino acid identity of the

C region of LdUSP is also very high among all

sequences (89–95%) Both D and E⁄ F regions are

also highly homologous to those of T molitor and

L migratoria (96% and 75%, 88% and 69%,

respec-tively), although they are less homologous to other

USPs A⁄ B regions of USPs are highly diverse (6–

45%), as observed for EcRs

mRNA expression profiles The spatial expression pattern of EcR mRNA was analyzed using total RNA prepared from the fat body, gut, integument and whole body of L decemlineata larvae at day 4 of the last (4th) instar A 12.4-kb mes-sage was detected by the LdEcR common probe in the integument and whole body, and slightly in the gut The mRNA of EcR was not detectable in the fat body (Fig 2A) We also demonstrated the temporal expres-sion pattern of LdEcR in the integument of 4th instar larvae As shown in Fig 2A, the EcR message steeply increased at day 4, then remained at the high expres-sion level until day 8 Total RNAs from the whole body of male and female adult, testis and ovaries as well as from L decemlineata cells were subjected to northern hybridization analysis Although the EcR message was detected in all tissues, the message was weak in adult males Expression of mRNA of LdEcR seems to be much higher in adult female than in adult male The EcR transcript abounds in L decemlineata

Fig 1 The deduced amino acid sequence of L decemlineata molting hormone receptor (A) The deduced amino acid sequence of LdEcR-A The DNA binding domain (DBD, C-region) is underlined The ligand binding domain (LBD, E-region) is underlined with dashes The junction of LdEcR-A and LdEcR-B1 is shown by an arrow head Gly164 and the downstream sequences are common between LdEcR-A and LdEcR-B1 The five amino acids encoded a 15-bp sequence that is absent in some cDNAs is boxed (B) The deduced amino acid sequence of the iso-form-specific region of LdEcR-B1 This sequence connects to Gly164 in (A) (C) The deduced amino acid sequence of LdUSP The DNA bind-ing domain (DBD, C-region) is underlined The ligand bindbind-ing domain (LBD, E ⁄ F-region) is underlined with dashes The sequence data of LdEcR-A, LdEcR-B1 and LdUSP have been submitted to the DDBJ ⁄ EMBL ⁄ GenBank nucleotide sequence database under the accession number AB211191, AB211192 and AB211193, respectively.

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cells A 10.5-kb transcript was also detected in all

tis-sues and developmental stages, although the signals

were very weak (Fig 2A) Northern hybridization

ana-lysis using LdEcR-A and LdEcR-B1 probes indicated

that the 12.4-kbp signal is mRNA of LdEcR-A, and

the 10.5-kbp transcript is LdEcR-B1 mRNA (Fig 2B)

We used LdEcR-A in the following experiments of our

study because the expression of LdEcR-A is much

higher than LdEcR-B1

Northern hybridization analysis was also conducted

with the probe for USP using the same series of total

RNA The expression pattern of LdUSP, as 5.7-kb

message, was similar to that of LdEcR-A over the dif-ferent tissues and developmental stages The very high expression was observed in the whole body of female adults (Fig 2A)

SDS/PAGE and gel mobility shift assay of

in vitro translated proteins LdEcR-A and LdUSP proteins were prepared by

in vitro transcription⁄ translation with [35S]methionine and subjected to SDS⁄ PAGE analysis (Fig 3) Molecular mass for LdEcR-A and LdUSP was

A

B

Fig 2 mRNA expression profiles of LdEcR

and LdUSP (A) LdEcR mRNA and LdUSP

mRNA expression in the fat body (FB), gut

(GUT), integument (INT) and whole body

(WB) at day 4 in the last larval instar, in the

INT at day 0, 2, 4, 6 and 8 in the last larval

instar, and in the adult male WB (#), female

WB ($), testis TES and ovary (OVA), and

L decemlineata cells BCIRL-Lepd-SL1

(CELL) For detecting LdEcR transcripts,

LdEcR common probe was used Ethidium

bromide staining of rRNA is shown as a

control for equal loading (B) The expression

of LdEcR-A and LdEcR-B1 mRNA in

integument of last instar larvae Temporal

expression profiles were studied using

isoform-specific probes.

Table 1 Comparison of sequences Sequence comparison between (A) L decemlineata EcR A-isoform (LdEcR-A) and other EcR-A’s (B) LdUSP and other USPs Amino-acid identity against LdEcR-A and LdUSP is expressed as percentage in each region We could not com-pare F regions because their sequences are too short TmEcR-A: Tenebrio molitor EcR-A (GenBank accession number Y11533 [22]), LmEcR: Locusta migratoria EcR (AF049136), DmEcR-A: Drosophila melanogaster EcR-A (M74078, S63761), CsEcR-A: Chilo suppressalis EcR-A (AB067811), AamEcR-A2: Amblyomma americanum (AF020188), UpEcR: Uca pugilator EcR-A2 (AF034086), TmUSP: T molitor USP (AJ251542), LmUSP: L migratoria USP (AF136372), DmUSP: D melanogaster USP (X53417), CsUSP: C suppressalis USP (AB081840), UpUSP: U pugilator USP (AF032983).

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estimated to be 64 kDa and 49 kDa, respectively, from

the mobility in the gel The 64 kDa LdEcR-A protein

was consistent with the predicted size from the

deduced amino acid sequence (63.4 kDa) In the lane

of translation products of LdEcR-A, extra bands with

lower molecular weight were observed They were

probably degradation products of the full length

64 kDa protein Similar results were obtained for the

in vitro translation of USP of C suppressalis [13]

Otherwise, they might be products of internal initiation

or premature termination of translation The 49 kDa

LdUSP protein was slightly larger than the size

predic-ted from deduced amino acid sequence (43.1 kDa)

This might be the result of post-translational

modifica-tions

A gel mobility shift assay was conducted using

in vitro translated LdEcR-A and LdUSP proteins

(Fig 4) The mixture of LdEcR-A and LdUSP clearly

bound to the pal1 EcRE probe [58] Interestingly, a

weak signal was also detected for LdEcR-A alone

When a 100-fold excess of unlabeled competitor was

added, the band shift observed for the mixture of

LdEcR-A and LdUSP disappeared Drosophila hsp27

EcRE [59] probe gave the same results as pal1 (data

not shown) These results indicate that LdEcR-A and

LdUSP form the complex (LdEcR-A⁄ LdUSP) and

bind to the EcRE Addition of 20E to the reaction

mixture enhanced the probe-binding (data not shown)

as observed in D melanogaster [3], B mori [60],

Choris-toneura fumiferana [15] and Chironomus tentans [17],

although EcR alone did not show binding to EcRE in those studies

Ligand binding assay The specific binding of in vitro translated proteins to PonA was calculated by the difference between total binding and nonspecific binding as we previously reported [45] The dissociation equilibrium constant,

KD, of PonA was calculated from the saturation curve

of the specific binding and the Scatchard plot (Fig 5) The KDvalues of LdEcR-A and LdEcR-A⁄ LdUSP cal-culated from saturation curves were 72.6 and 2.8 nm, respectively

Receptor-binding affinity of ecdysone agonists to LdEcR-A⁄ LdUSP is shown in Table 2 The binding affinity of DBHs tested in this study was relatively low (< 6.00 in terms of pIC50) compared to that against

C suppressalis The SARs for binding affinities of

Fig 3 SDS ⁄ PAGE of in vitro translated LdEcR-A and LdUSP

pro-teins pET-23a (+) vector (lane 1), in vitro translated LdEcR-A (lane

2), LdUSP (lane 3) and LdEcR-A ⁄ LdUSP translated simultaneously

in the same tube (lane 4) with [ 35 S]methionine were separated on

10% SDS ⁄ PAGE gel.

Fig 4 Binding of LdEcR-A ⁄ LdUSP complex to the ecdysone response element (EcRE) In vitro translated LdEcR-A and ⁄ or LdUSP protein were incubated with 32 P-labeled pal1 EcRE and then applied for nondenaturing polyacrylamide gel electrophoresis Water (lane 1), a reaction mixture using pET-23a(+) vector substitute to LdEcR-A or LdUSP construct (negative control, lane 2), LdEcR-A (lane 3), LdUSP (lane 4) and LdEcR-A and LdUSP translated simulta-neously in the same tube (lane 5 and 6) were mixed with probes and loaded In the lane 6, 100-fold excess of the same EcRE oligo-nucleotide was added for competition experiment.

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ecdysteroids were linearly correlated between L

decem-lineataand C suppressalis, whereas those of DBHs were

not (Fig 6A) No positive correlation was observed

between receptor-binding and larvicidal activity against

L decemlineatawith respect to DBHs (Fig 6B) [52,55]

Discussion

The comparison of EcRs and USPs

Three cDNAs encoding LdEcR-A, LdEcR-B1 and

LdUSP were obtained, and they had high amino acid

identity with EcR-A, EcR-B1 and USP of other

insects, respectively It is known that many insect

spe-cies have two or three EcR isoforms (EcR-A, EcR-B1

and EcR-B2), and their functions are different depend-ing on tissues, developmental stages and species [5,12,14,22,61,62] In D melanogaster, it was reported that EcR-B1 is predominantly expressed in larval tissues, and expression of EcR-A is predominant in imaginal discs [5] In B mori, C fumiferana, C sup-pressalis and M sexta, EcR-B1 was observed as the major isoform in larval stage, although expression pat-terns of EcR isoforms appeared to be diverse among these lepidopteran insects [12,14,61,62] Thus, functions

of EcR isoforms in larval stage might be different between lepidopteran and dipteran insects In this study, we showed that L decemlineata also possesses two isoforms, and the expression of LdEcR-A was much stronger than LdEcR-B1 (Fig 2A) Expression

of EcR-A was also predominant in larval tissue of coleopteran T molitor [22] These facts also indicate that the dominant isoform of EcR in larval develop-ment is different depending on tissues and insect orders Furthermore, LdEcR-A transcripts in the integument increased steeply at day 4 of 4th instar lar-vae (Fig 2A) We previously reported that the molting hormone titer in the hemolymph during 4th instar development of L decemlineata was constant until day

6 except for a small peak at day 4, and rapidly increased to the major peak between day 8 and day 9 [63] Thus, EcR-A transcripts in integument are pro-bably induced by the small peak of ecdysteroid on day

4, prior to the major hemolymph ecdysteroid peak The strong expression of EcR transcripts prior to the peak of ecdysteroid titer in hemolymph was also repor-ted in various insects such as D melanogaster and

M sexta [5,10,12,14,22,61] Therefore, expression of EcR mRNA could be up-regulated by the rising of ecdysteroid titer in hemolymph to secure sufficient responsibility to the peak of ecdysteroid titer Further studies for the mechanism of their transcriptional regu-lation would support the elucidation of different roles

of EcR isoforms in Coleoptera

Although we have obtained only one isoform from

L decemlineata, two USP isoforms, MsUSP-1 and MsUSP-2, were cloned from lepidopteran M sexta, and their different role on MHR3 promoter activation was shown [21,64] Dipteran Aedes aegypti and C ten-tans also possess two USP isoforms (A and USP-B) [17,65] Therefore, other USP isoforms might exist and contribute to the development of L decemlineata LdUSP showed higher conservation with two USP isoforms of the tick Amblyomma americanum (AamUSP-1 and AamUSP-2 [28]) than USPs of

A aegypti, C tentans and D melanogaster, but no significant difference was observed between homologies

to two USP isoforms LdUSP as well as T molitor

Fig 5 The binding affinity of ponasterone A (PonA) to in vitro

translated proteins In vitro translated LdEcR-A or LdEcR-A ⁄ LdUSP

were incubated with various concentration of [3H]-labeled PonA, in

the presence or absence of excess PonA Saturation

radioligand-binding curves and Scatchard plots are shown.

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and L migratoria USP showed higher homology to

RXR of human and mouse than USP isoforms of

dip-teran and lepidopdip-teran insects Thus, the functions of

USP of L decemlineata, T molitor and L migratoria

might have the similar function to RXR, being

differ-ent from those of Diptera and Lepidoptera The

LdUSP transcript showed similar developmental and

spatial expression profiles as LdEcR-A USP

tran-scripts also changed with the hemolymph ecdysteroid

titer in T molitor, C fumiferana and M sexta,

although their expression profiles were different from

the case of L decemlineata [15,21,23] On the contrary,

USP mRNA expression in the epidermis of C

suppres-salis and B mori was ubiquitous throughout the last

larval instar [13,66] Such a difference suggests that

hormonal regulatory mechanisms of USP transcription

are different among insect species

Previously, it was pointed out that there is a

con-served motif (motif-1) between T molitor EcR-A (amino

acids 29–39) and D melanogaster EcR-A (143–153)

The presence of conserved motif-2 between M sexta

EcR-A (60–79) and D melanogaster EcR-A (177–196)

was also pointed out in A⁄ B region of EcRs [22] The

sequence of amino acids 108–118 of LdEcR-A is

homo-logous to the motif-1, and this was also the case for EcR-A of coleopteran T molitor Interestingly, the sequence of amino acids 143–162 of LdEcR-A also has

a striking homology with the motif-2 It is different from

T molitor EcR-A, but consistent to EcR-A of lepidop-teran M sexta and C suppressalis EcR-A sequences of lepidopteran insects showed relatively lower homology

to LdEcR-A in comparison with EcR-A homologies between insects of other orders and coleopteran L de-cemlineata Thus, each of these two conserved motifs in

Table 2 Binding affinity of ecdysone agonists Binding affinity

(pIC50: M) of steroidal and nonsteroidal ecdysone agonists to the

receptor of L decemlineata (LdEcR-A ⁄ LdUSP) is shown

Com-pound 9: RH-5849, 10: halofenozide (RH-0345), 11: tebufenozide

(RH-5992), 12: methoxyfenozide (RH-2485), 13: chromafenozide

(ANS-118).

No.

N N H O

O Xn

Yn

Binding affinity

L decemlineata

12 3,5-(CH3)2 2-CH3-3-OCH3 5.94

13 3,5-(CH 3 ) 2 2-CH 3 -3,4-(CH 2 ) 3 O- 5.77

A

B

Fig 6 Relationships among biological activities (A) Receptor-bind-ing affinity (pIC50: M) of ecdysone agonists against the receptor of

L decemlineata is compared to that of C suppressalis Triangles: ecdysteroids Circles: DBHs (B) Receptor-binding affinity (pIC 50 : M) and larvicidal activity (pLD50: m M ⁄ insect) of DBHs against

L decemlineata [52,55] were compared.

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A⁄ B region might play different roles and be important

for determining the function of the EcR-A, which is

dif-ferent among insect species

The functional analysis of LdEcR-A and LdUSP

The gel mobility shift assay showed that the complex

of in vitro translated LdEcR-A and LdUSP proteins

bound to EcREs, indicating that cDNAs cloned in this

study encode functional EcR and USP LdEcR-A

alone also bound to EcREs, although the binding was

much weaker than that of LdEcR-A⁄ LdUSP The

binding experiment of EcR and USP proteins to

EcREs was also conducted in dipteran D melanogaster

[2], A aegypti [65] and C tentans [17], and lepidopteran

B mori [60], C suppressalis [13] and C fumiferana

[15] In those experiments, EcR alone did not bind to

EcRE, which is different from the result of this study

The degree of mobility shift of a band which is caused

by monomeric binding of LdEcR-A alone should be

much smaller than that by LdEcR-A⁄ LdUSP

How-ever, the degree of band retardation by addition of

A alone was a little larger than that of

LdEcR-A⁄ LdUSP Therefore LdEcR-A alone appeared to

bind to EcREs as a homodimer Homodimeric binding

to DNA sequences is reported for vertebrate THR,

which shows similar characteristics to EcR [67,68]

Furthermore, it is concerned that the determinant of

the binding type of nuclear receptors to its response

element, namely monomer, homodimer and

heterodi-mer, is the nucleic acid sequence of the hormone

response element [69] Thus, perhaps pal1 and hsp27

probes, which are not intrinsic EcREs of L

decemlin-eata, enable LdEcR-A to form a homodimer

From the ligand binding assays using [3H]PonA, the

KD value of ponA for LdEcR-A⁄ LdUSP is 2.8 nm

The KDvalue was close to that for CsEcR-B1⁄ CsUSP

(C suppressalis) and DmEcR⁄ DmUSP (D

melanogas-ter), which have been reported to be about 1.0 nm

[3,45] Thus, it was shown that in vitro translated

LdEcR-A⁄ LdUSP heterodimers are capable of

inter-acting with ligands with high affinity, and possess a

required ability for a receptor

The ligand binding affinity of LdEcR-A/LdUSP

As shown in Fig 6A, receptor-binding affinities of

ecdysteroids were well correlated between

LdEcR-A⁄ LdUSP and CsEcR ⁄ CsUSP, whereas this is not

the case for DBHs As shown in Table 1, sequence

homology of ligand binding domains between

LdEcR-A and lepidopteran CsEcR-A is considerably

lower than those between LdEcR-A and coleopteran

TmEcR-A Therefore, the difference between struc-tures of ligand binding domain is most likely respon-sible for the difference in receptor-binding affinities

of DBHs among different insect orders On the other hand, the ligand binding domain should have a sub-stantial conservation in the structure which is neces-sary for ecdysteroid binding regardless of insect orders, because 20E is believed to be the most active form of molting hormone in all insects The crystal structure analysis of EcR of lepidopteran H virescens indicated the amino acid residues which are import-ant for the binding with PonA and a DBH analog BYI06830 [44] We examined the conservation of these amino acid residues among several insects by comparing the sequences of the ligand binding domain of EcRs (Fig 7) As expected, amino acids which have been shown to be important for ecdyster-oids-binding are highly conserved among all insects Thus, probably the structure of EcR ligand binding domain is also conserved among insects for arran-ging these amino acid residues in proper location to accommodate an ecdysteroid molecule However, amino acids which have been shown to be important for binding with BYI06830 are also well conserved among EcRs The difference in receptor-binding affinity of DBHs among insect orders might rather

be attributed to the amino acid residues which are considered to be involved in binding to both types

of ligands Amino acids which are corresponding to Met429 and Thr451 of LdEcR-A represent the pos-sibility, as they are different between EcR-As of lepi-dopteran and other insects Further studies such as point mutation and X-ray crystal structure analysis

of various EcRs will elucidate the factors responsible for difference of the binding of DBHs to EcRs among insects

We previously reported that larvicidal activity and receptor-binding of DBHs are correlated very well in C suppressalis, suggesting that receptor-binding affinity of DBHs is concerned to rule the strength of their

larvicid-al activity [45] Among DBHs, it was reported that hlarvicid-alo- halo-fenozide (RH-0345) has a high insecticidal activity against coleopteran field pests such as Popillia japonica and L decemlineata, but tebufenozide (RH-5992), meth-oxyfenozide (RH-2485) and chromafenozide (ANS-118) were not so potent against these insects [43] Thus, based

on the case of DBHs in C suppressalis, the receptor-binding affinity of RH-0345 was expected to be high in

L decemlineata However, the receptor-binding affinity

of RH-0345 and the other three DBHs to

LdEcR-A⁄ LdUSP was low (Table 2) Furthermore, the binding affinity of RH-2485 and ANS-118 was higher than that

of RH-0345 This means that the receptor-binding

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affinity of DBHs is not a major factor to determine the

larvicidal activity in L decemlineata To make this

point clear, we tested the receptor-binding affinity of

other DBHs against LdEcR-A⁄ LdUSP (Table 2) The

measured binding affinity of 12 DBHs (1–12; Table 2)

did not show any correlation to the larvicidal activity

(Fig 6B) Furthermore, our previous SAR study

demonstrated that hydrophobicity of compounds is

important to larvicidal activity of DBHs against C

sup-pressalis; thus the hydrophobicity is important for

receptor-binding affinity However, the hydrophobicity

of DBHs was not correlated to their receptor-binding

activity to LdEcR-A⁄ LdUSP, although existence of

optimal hydrophobicity for larvicidal activity of DBHs

against L decemlineata was shown in our previous

study [52,55] Therefore, other factors such as

absorp-tion through the membrane and metabolism in the

insect body might play a very important role Otherwise,

although DBHs are considered to show potency as

agonists of 20E in C suppressalis by binding to

EcR⁄ USP, there is a possibility that different

mecha-nisms, such as neurotoxicity and the existence of other

receptors, give influence on the larvicidal activity of

DBHs in L decemlineata Further study such as X-ray

crystal structure analyses of EcR⁄ USP and metabolic

analyses of DBHs in various insects would confer new

knowledge of the mode of action of DBHs

A recent study of phylogenic analysis suggests that

EcR and USP have coevolved during diversification

of insects [70], which is supported by the result of this study (Table 1) It was also suggested that EcRs and USPs of lepidopteran and dipteran insects are under a strong acceleration of evolutionary rate in comparison with those of insects in other orders This raises a possibility that the results of studies for EcRs and USPs of lepidopteran and dipteran insects are not necessary applicable for those of insects in other orders Therefore, although a number of stud-ies has been conducted in lepidopteran and dipteran insects, more detailed studies on EcR and USP of insects in other orders and other ecdysozoan are necessary for precise understanding of their physiology

In conclusion, we successfully performed cDNA cloning of EcR and USP of L decemlineata, and

in vitro translation of corresponding receptor proteins The translated proteins could bind to EcREs and ecdysone agonists as heterodimers, indicating that they are functional molting hormone receptors of

L decemlineata As L decemlineata is a major pest in agriculture world-wide, the receptor proteins isolated

in this study can be very helpful to develop effective compounds in high throughput assays and SAR stud-ies Furthermore, although EcR and USP proteins have been isolated from various insects, the down-stream of the ecdysone signaling pathway which is triggered by their activation function of transcription still remains to be elucidated The isolated genes and

Fig 7 Comparison of the ligand binding domain sequence of EcRs Amino-acid sequences are compared for ligand binding domain of EcRs LdEcR: L decemlineata EcR, TmEcR: T molitor EcR, LmEcR: L migratoria EcR, D melanogaster EcR, CcEcR: Ceratitis capitata EcR (Gen-Bank accession number AJ224341), AaeEcR: A aegypti EcR (P49880), CtEcR: Chironomus tentans EcR (P49882), CsEcR: C suppressalis EcR, CfEcR: C fumiferana EcR (U29531), HvEcR: H virescens EcR (O18473), BmEcR: B mori EcR (P49881) Sequences are separated in three groups according to insect orders The upper three sequences are EcRs of insects belonging to orders other than Diptera and Lepidop-tera The middle four (shaded with light gray) are EcRs of dipteran insects, and the lower four are that of lepidopteran insects Amino-acid residues which are important for the binding with PonA are shaded with dark gray, and that of BYI06830 are boxed [47] The position of LdEcR-A Met429 and Thr451 are shown by arrow heads Activation function 2 (AF-2) is indicated with dots Amino acids which correspond

to a-helical structures are also indicated.

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proteins will also be available to study

protein–pro-tein interactions in such hormonal regulatory

path-ways, and be helpful to understand the complicated

physiology of insects

Experimental procedures

Chemicals

Ecdysone and 20E were purchased from Sigma Chemical

Co (St Louis, MO, USA) and PonA was from Invitrogen

Corp (Carlsbad, CA, USA) Tritiated ponasterone A

([3H]PonA, 150 CiÆmm)1) was purchased from American

Radiolabeled Chemicals Inc (St Louis, MO, USA)

Ecdy-steroids (cyasterone and makisterone A) and all DBHs were

from our stock samples [52,55]

Isolation of RNA from L decemlineata

Larvae and adults of L decemlineata were reared as

des-cribed previously [63] A L decemlineata cell line

(BCIRL-Lepd-SL1), which was established from female pupae, was

routinely maintained as described previously [71] Total

RNA was isolated from the whole bodies and tissues of last

instar (4th) larvae and adults using TRIzol (Gibco BRL,

Grand Island, NY, USA) as described previously [13]

BCIRL-Lepd-SL1 was also used for isolation of total

RNA Poly (A)-rich RNA was purified from the total RNA

using mRNA Purification Kit (Amersham Bioscience Corp.,

Piscataway, NJ, USA)

RT-PCR

Reverse-transcription was conducted using ReadyÆToÆ

GoTM T-Primed First-Strand Kit (Amersham Bioscience

Corp.) for total RNA isolated from the fat body and integument of last instar larvae Three forward and reverse degenerate primers were designed for EcR based

on amino acid sequences conserved in C-E regions of other EcRs (Table 3) In the same way, two forward and one reverse degenerate primers were designed for USP using the homology in C region of other USPs (Table 3) The first PCR for EcR was conducted using LdEcR-F1 and LdEcR-R1 primers (annealing temperature: 48C) Subsequently, the second and the third nested PCR were performed with LdEcR-F2 and LdEcR-R2 primers (52C) and with LdEcR-F3 and LdEcR-R3 primers (46C), respectively The first PCR with LdUSP-F1 and LdUSP-R1 primers and the second nested PCR with LdUSP-F2 and LdUSP-R1 primers were conducted for USP Annealing was performed at 48C and 46 C, respectively

Rapid amplification of cDNA ends Poly (A)-rich RNA extracted from L decemlineata cells was subjected to the 5¢- and 3¢- rapid amplification of cDNA ends (RACE) with SMARTTM RACE cDNA amplification kit (Clontech, Palo Alto, CA, USA) For both of EcR and USP, two reverse primers for 5¢-RACE and two forward primers for 3¢-RACE were designed (Table 3) 5¢-RACE for EcR was executed by PCR with primer LdEcR-RR1, and 3¢-RACE for EcR was per-formed with LdEcR-RF1, respectively, according to manu-facturer’s instructions 5¢-RACE and 3¢-RACE were followed by nested PCR using LdEcR-RR2 (annealing temperature: 66C), LdEcR-RF2 (66 C), respectively In the same way, 5¢-RACE for USP was executed with LdUSP-RR1, and 3¢-RACE for USP with LdUSP-RF1 Each RACE reactions were followed by nested PCR

Table 3 Primers used in this study Degenerate primers and 5¢- and 3¢-RACE primers are shown The term N means a mixture of A, T, G and C In the same way, D (A, G, T), H (A, C, T), K (G, T), M (A, C), R (A, G), S (C, G), W (A, T) and Y (C, T) means a mixture of deoxynucleo-side.

Degenerate primers

5¢-RACE

3¢-RACE

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