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In developed countries, more than 80% of children under the age of 3 years will be diagnosed at least once Keywords lipooligosaccharide; moiety; Moraxella catarrhalis; outer membrane; ro

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molecule in biological activities of the Moraxella

catarrhalis outer membrane

Daxin Peng1,*, Wei-Gang Hu1,†, Biswa P Choudhury2, Artur Muszyn´ski2, Russell W Carlson2 and Xin-Xing Gu1

1 Vaccine Research Section, National Institute on Deafness and Other Communication Disorders, National Institutes of Health, Rockville,

MD, USA

2 Complex Carbohydrate Research Center, University of Georgia, Athens, GA, USA

Moraxella catarrhalis, once considered a

nonpatho-genic bacteria to humans, is now one of the leading

causes of bacterial otitis media in children, after

Strep-tococcus pneumoniae and Haemophilus influenzae [1–3]

In developed countries, more than 80% of children under the age of 3 years will be diagnosed at least once

Keywords

lipooligosaccharide; moiety; Moraxella

catarrhalis; outer membrane; role

Correspondence

Xin-Xing Gu, 5 Research Court,

Room 2A31, Rockville,

MD 20850, USA

Fax: +1 301 435 4040

Tel: +1 301 402 2456

E-mail: guxx@nidcd.nih.gov

Present addresses

*School of Veterinary Medicine,

Yangzhou University, Yangzhou,

Jiangsu, China

†Defence Research and Development

Canada-Suffield, Medicine Hat, Alberta,

Canada

Database

The nucleotide sequence of lgt3 gene in

Moraxella catarrhalis strain O35E has been

submitted to the GenBank database under

the accession number DQ208195

(Received 19 June 2007, revised 30 July

2007, accepted 21 August 2007)

doi:10.1111/j.1742-4658.2007.06060.x

Lipooligosaccharide (LOS), a major component of the outer membrane of Moraxella catarrhalis, consists of two major moieties: a lipid A and a core oligosaccharide (OS) The core OS can be dissected into a linker and three

OS chains To gain an insight into the biological activities of the LOS molecules of M catarrhalis, we used a random transposon mutagenesis approach with an LOS specific monoclonal antibody to construct a sero-type A O35Elgt3 LOS mutant MALDI-TOF-MS of de-O-acylated LOS from the mutant and glycosyl composition, linkage, and NMR analysis of its OS indicated that the LOS contained a truncated core OS and consisted

of a Glc-Kdo2 (linker)-lipid A structure Phenotypic analysis revealed that the mutant was similar to the wild-type strain in its growth rate, toxicity and susceptibility to hydrophobic reagents However, the mutant was sensi-tive to bactericidal activity of normal human serum and had a reduced adherence to human epithelial cells These data, combined with our previ-ous data obtained from mutants which contained only lipid A or lacked LOS, suggest that the complete OS chain moiety of the LOS is important for serum resistance and adherence to epithelial cells, whereas the linker moiety is critical for maintenance of the outer membrane integrity and sta-bility to preserve normal cell growth Both the lipid A and linker moieties contribute to the LOS toxicity

Abbreviations

BHI, brain-heart infusion; CFU, colony forming units; COPD, chronic obstructive pulmonary disease; DPBSG, Dulbecco’s phosphate-buffered saline containing 0.05% gelatin; EU, endotoxin units; Kdo, 3-deoxy- D -manno-2-octulosonic acid; kds, 3-deoxy- D -manno-2-octulosonic acid transferase; LOS, lipooligosaccharide; lpxA, UDP-N-acetylglucosamine acyltransferase; OMPs, outer membrane proteins; OMVs, outer membrane vesicles; OS, oligosaccharide.

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with otitis media, and M catarrhalis is responsible for

15–25% of those cases [4,5] M catarrhalis is also a

common cause of lower respiratory tract infections in

adults with chronic obstructive pulmonary disease

(COPD), the fourth leading cause of death in the

Uni-ted States [6,7] Lower respiratory tract infections have

been shown to contribute to the progression of the

COPD Approximately 20 million cases of such

exacer-bations are reported each year in the United States, up

to 35% of them resulting from M catarrhalis

infec-tions

The pathogenesis of M catarrhalis infection is not

well understood As a gram-negative bacterium,

M catarrhalis without capsular polysaccharides is

surrounded by an outer membrane, consisting of

lipo-oligosaccharide (LOS), outer membrane proteins

(OMPs) and pili outside phospholipids [2] The outer

membrane of gram-negative bacteria was initially

con-sidered to protect the bacteria from several antibiotics,

dyes, and detergents (hydrophobic compounds) which

would normally damage the cell wall However, more

outer membrane biological activities have become

apparent over years of extensive research and there is

indication today that the outer membrane of

gram-negative bacteria has some other biological activities,

such as adherence and invasion in vitro, colonization

in vivo, maintenance of cell surface charge and serum

bactericidal resistance [8–13]

Which component on the outer membrane of

M catarrhaliscontributes to the above-mentioned

bio-logical activities? Several OMPs of M catarrhalis were

identified, but their functions were mainly reported as

potential vaccine antigens, although some of them

were indicated to be adhesins [5,14–17] Pili were

con-sidered to be associated with bacterial attachment, but

both piliated and nonpiliated M catarrhalis strains

could adhere to human mucosal cells in vitro [18] LOS

has mostly been investigated for these biological

activi-ties of the M catarrhalis outer membrane [19–24]

M catarrhalis LOS is a major component of the bacterial outer membrane with three main serotypes A,

B and C, of which serotype A is the major type [25,26] Quite a few studies have demonstrated that such an LOS molecule is an important virulence factor for some other respiratory tract pathogens, such as Neisseria meningitidis, Neisseria gonorrhoeae, and

H influenza [27–29] Studies have also implicated the

M catarrhalis LOS as important in the pathogenesis

of the M catarrhalis infection [13,21,23,24] We recently reported that a mutant which lacked LOS showed decreased toxicity, reduced resistance to nor-mal human serum killing, and reduced adherence to human epithelial cells in vitro and in vivo, while show-ing hypersensitivity to hydrophobic compounds, indi-cating that LOS contributes to most biological activities of the M catarrhalis outer membrane [24] The molecular structure of the M catarrhalis LOS is smaller than its lipopolysaccharide counterparts in gram-negative pathogens like Escherichia coli and Sal-monella typhimurium and does not have the O-anti-genic side chain of the repeating units characteristic of classical lipopolysaccharide As showed in Fig 1, the LOS consists of lipid A and a core oligosaccharide (OS) The latter can be further dissected into three OS chains and a linker composed of a central Glc and two 3-deoxy-d-manno-2-octulosonic acids (Kdo) How do the three moieties play their roles in biological activi-ties of the outer membrane? Biosynthesis of LOSs in

M catarrhalis is complex and strictly sequential, requiring many enzymes such as UDP-glucose-4-epi-merase, Kdo-8-phosphate synthase, Kdo transferase (kdt), glycosyltransferase enzymes, and UDP-N-acetyl-glucosamine acyltransferase (lpxA) Recently, several genes encoding these enzymes have been reported [20,22–24,26,30–32] A series of stepwise-truncated LOS mutants can therefore be established by knocking out some of the genes and then the biological activities

of the different truncated LOS mutants can be

Fig 1 Schematic structure of M catarrhalis

LOS [8] Lipooligosaccharide (LOS) consists

of two major moieties: lipid A and a core

oligosaccharide (OS) The core OS can

further be dissected into three OS chains

and a linker (boxed) composed of a Glc and

two Kdo p, pyranose.

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compared to decipher potential roles of each moiety of

the LOS Previously, we identified an lpxA gene

encod-ing UDP-N-acetylglucosamine acyltransferase and a

kdtAgene encoding Kdo transferase [23,24] The lpxA

or the kdtA mutant contained no LOS or lipid A-only

structure Both mutants showed a variety of changes

of biological activities in vitro as well as in vivo In this

study, we further found an lgt3 gene by a random

transposon mutagenesis approach followed with a

screen by an LOS-specific mAb A subsequently

iso-genic lgt3 mutant contained a truncated core OS and

consisted of a linker (Glc-Kdo2)-lipid A structure The

phenotype of this mutant was examined to investigate

the roles of different moieties of the LOS molecule in

biological activities of the M catarrhalis outer

mem-brane

Results

Construction of M catarrhalis O35Elgt3 mutant

M catarrhalis O35E mutants were constructed by

in vitrotransposon mutagenesis The resulting

kanamy-cin-resistant colonies were screened for loss of

reactiv-ity to a specific anti-LOS mAb 8E7 Two clones were

selected and the EZ:TN transposon was found to be

inserted at position 901 and 1203 of an open reading

frame (ORF) of 1605 bp, respectively (Fig 2) BLAST

searches at GenBank with the deduced polypeptide

sequence of the ORF revealed 99.6% and 100%

iden-tity with a recently identified lgt3 gene encoding b(1–4)

glucosyltransferase of M catarrhalis serotype B strain

7169 [30] and a putative lgt3 gene from a serotype A

strain 25238 [26], respectively

An lgt3 knockout mutant of M catarrhalis O35E

was constructed by allelic exchange with an insertion

of a kanamycin-resistant cassette and deletion of an

822 bp fragment between two HindIII sites of the lgt3

(Fig 2)

Silver staining revealed that the mutant LOS mole-cule migrated more rapidly and showed less density than those of the wild-type, indicating a truncated LOS molecule resulting from the mutant (Fig 3A) Western blot analysis demonstrated that the LOS from O35Elgt3 lost the binding activity to the mAb 8E7 when compared with the wild-type strain (Fig 3B) Purified LOSs from both strains also showed similar results to those described above (data not shown) To further compare LOS expression levels between the wild-type and mutant strains, the amounts of Kdo from both strains were determined as an indicator They were 73 ng and 70 ng per 80 lg of outer mem-brane vesicles (OMVs) for the wide type and mutant strains, respectively, indicating the LOS expressions in both strains were similar

Composition analysis by GC-MS showed that the carbohydrates derived from the wild-type O35E strain consisted of Glc, Gal, GlcNAc and Kdo, whereas the carbohydrates derived from the mutant O35Elgt3 con-sisted exclusively of Glc and Kdo The glycosyl linkage analysis by GC-MS showed that the OSs from the wild-type strain consisted of terminal-, 2-, 4-, and 3,4,6-linked glucosyl residues, terminal- and 4-linked galactosyl residues, and a terminal-linked N-acetylglu-cosaminosyl residue These linkage results were consis-tent with the structure of the LOS reported for serotype A strain 25238 [33] The only hexosyl residue

in the mutant LOS structure was terminally linked Glc

Fig 2 Strategy for construction of the lgt3 mutant in M catarrhalis

O35E Large arrows represent the direction of transcription; the

site of the transposon insertion identified in the O35E is denoted

as EN:TN, and the location of the deletion replaced by the

kanamy-cin-resistant gene (kanR) is between two HindIII cleavage sites.

The sites of primers used are indicated as small arrows (25, 26,

and 40 of Table 1).

Fig 3 LOS patterns of SDS ⁄ PAGE followed by silver staining (A)

or western blotting (B) of M catarrhalis wild-type strain O35E (lane 1) and mutant O35Elgt3 (lane 2) Each lane represents extracts from proteinase K-treated whole cell lysates from 1.9 lg

of each bacterial suspension An anti-LOS MAb 8E7 was used at

1 : 100 dilution (B) Molecular markers (Mark 12; Invitrogen) are indicated on the left.

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The de-O-acylated LOSs from the wild-type O35E

and the mutant O35Elgt3 were further analyzed by

MALDI-TOF MS (Fig 4) The mass spectral data of

de-O-acylated LOS from O35E was consistent with the

reported structure of serogroup A LOS Among

the major ions m⁄ z 2672.8(M-H)– corresponds to the

molecular mass of the de-O-Ac LOS containing five

Glc, two Gal, one GlcNAc, two Kdo and

O-acyl-ated lipid-A bearing two phosphate moieties The

de-O-acylated lipid-A unit consists of two GlcNAc and

two 3-OH C12:0 groups Among the other ions m⁄ z of

2654.8, 2694.8 and 2717.4 indicates the presence of the

anhydro form and mono- and di-sodiated form of the

molecular ion 2672.8 (Fig 4A) Among other

charac-teristic ions, 1558.2 and 1778.4 represent the mass of

intact OS with one and two Kdo residues, respectively

The low molecular mass with m⁄ z of 895.4 is from the Y-type fragment ion from the de-O-acylated lipid-A portion (as observed in the negative mode) The ions with m⁄ z of 917.4 and 877.4 (unmarked) are mono-sodiated and anhydro forms of 895.4 ion, respectively The ion with m⁄ z of 797.4 was from the anhydro frag-ment ion of de-O-acylated lipid-A bearing only one phosphate group (Fig 4A)

The MALDI-TOF mass spectral data of de-O-acyl-ated LOS for the mutant O35Elgt3 showed the pres-ence of ions with m⁄ z of 1479.6, 1497.6, 1519.6 and 1541.6, respectively The ion at m⁄ z 1497.6 (M-H)– corresponds to the deprotonated molecular mass, con-taining one Glc, two Kdo, de-O-acylated lipid-A and two phosphate moieties The ions with m⁄ z of 1519.6 and 1541.6 are mono- and di-sodiated forms of the de-O-acylated LOS and the ion with m⁄ z of 1479.6 is the anhydrous form of the de-O-acylated LOS The ion 1277.6 is the de-protonated molecular ion from de-O-acylated LOS containing only one Kdo residue (Fig 4B) The low molecular ions with m⁄ z of 917.4 and 877.4 are from the mono-sodiated and anhydro forms of the Y-type fragment ion 895.4 arising from the de-O-acylated lipid-A

Finally, proton NMR spectra of carbohydrates from both wild and mutant strains showed that the spec-trum for the O35E carbohydrates was identical to that published from strain 25238 LOS (Fig 5) [33] The mutant carbohydrate spectrum showed only one ano-meric resonance, a result consistent with a single termi-nal-linked glucosyl residue in the above GC-MS analysis

Taken together, the O35Elgt3 mutant contained only

a linker-lipid A (Glc-Kdo2-lipid A) structure without

OS chains (Fig 1)

Morphology, growth rate, and OMV⁄ OMP profiles of M catarrhalis O35Elgt3 mutant There were no significant differences in morphology, growth rate, or OMV⁄ OMP profiles between the wild-type and the lgt3 mutant (data not shown) The yields

of OMVs from both strains were similar (data not shown)

Susceptibility of M catarrhalis O35Elgt3 mutant

A broad range of hydrophobic agents and a hydrophilic glycopeptide were used to determine the susceptibility of the mutant O35Elgt3 O35Elgt3 showed similar resis-tance or intermediate susceptibility to hydrophobic anti-biotics, reagents [azithromycin (15 lg), deoxycholate (100 mgÆmL)1), fusidic acid (10 mgÆmL)1), novobiocin

A

B

Fig 4 MALDI-TOF MS spectrum (negative mode) of the

de-O-acyl-ated LOS from M catarrhalis wild-type strain O35E (A) and the

mutant O35Elgt3 (B) This analysis was done in the negative mode,

and all ions represented as deprotonated [M-H]–ions The source

of the ions was as indicated in the structure shown in the inset.

The m ⁄ z 917.4 and 797.4 are due to sodiated and dehydrated

forms, respectively, of the m ⁄ z 895.4 fragment ion.

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(5 lg), polymycin B (300 international units), rifampin

(5 lg), Triton X-100 (5%, w⁄ v), Tween 20 (5%, v ⁄ v)]

and a hydrophilic glycopeptide, vancomycin (5 lg), as

the wild-type strain (data not shown)

Biological activity of M catarrhalis O35Elgt3

mutant

The mutant was tested for LOS-associated biological

activity In a Limulus amebocyte lysate assay, whole

cell suspensions (D620¼ 0.1) gave 3.7 · 103 endotoxin

units (EU) mL)1 for O35E and 2.0· 103 EUÆmL)1 for

the O35Elgt3 mutant In a bactericidal assay with

normal human serum, strain O35E survived at 25% normal human serum However, 75% of the mutant cells died at 25% normal human serum (P < 0.05, Fig 6) indicating a reduced resistance from the mutant

To test the adherence of the O35Elgt3 mutant to human epithelial cells, Chang and HeLa cell lines were used The adherence percentage of O35Elgt3 to Chang and HeLa epithelia were 19.1 ± 4.6 and 27.3 ± 8.4, respectively, whereas those of the wild-type were 41.7 ± 9.1 and 47.0 ± 4.1 (P < 0.01)

To investigate the effect on survival of the O35Elgt3 mutant in a murine model of nasopharyngeal clear-ance, mice were challenged with the wild-type or mutant strains by aerosolization (Fig 7) Mutant

A

B

Fig 5 Proton NMR spectra of LOS derived from M catarrhalis

O35E (A) and the mutant O35Elgt3 (B) For the O35E strain, the

assignments were made based on the identity of this spectrum

with that of the published structure for the LOS from type A

M catarrhalis The spectrum for the mutant lgt3 disaccharide

shows numerous resonances for the H3 protons of Kdo due to the

fact that a 5-linked Kdo residue can, on mild acid hydrolysis, form

4,8-anhydroKdo, 4,7-anhydroKdo, and 2,7-anhydroKdo; all of which

have different H3 resonances.

5.5 6 6.5 7

Normal human Serum (%)

*

Fig 6 Bactericidal activity of normal human serum against

M catarrhalis wild-type strain O35E (black bar) and the mutant O35Elgt3 (gray bar) ‘HI’ represents the group of 25% heat-inactivated normal human serum The data represent the average

of three independent assays An asterisk represents statistical sig-nificance between the wild-type and mutant strains.

0 1 2 3 4 5

0

Nasal wash

*

*

Time post challenge (h)

Bacterial recovery (log CFU/mouse)

Fig 7 Time courses of bacterial recovery in mouse nasal washes after an aerosol challenge with M catarrhalis wild-type strain O35E (r) and the mutant O35Elgt3 (h) Each time point represents a geometric mean of six mice Asterisks represent statistical signifi-cance between the wild-type and mutant strains.

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O35Elgt3 present in the nasopharynx showed an

accel-erated clearance at 3 h (85.5% versus 60.2%,

P< 0.01) or 6 h (98.0% versus 86.8%, P < 0.01)

compared to the wild-type

Discussion

In this study, an lgt3 gene was found and its products

confirmed from a M catarrhalis serotype A strain

O35E through an isogenic O35Elgt3 mutant Structural

analysis revealed that the O35Elgt3 mutant contained

a truncated core OS and consisted of a linker

(Glc-Kdo2)-lipid A structure, similar to that reported

previ-ously [30,34] The O35Elgt3 mutant demonstrated no

significant difference in its growth rate, LOS

expres-sion level and susceptibility to the hydrophobic

com-pounds compared with the wild-type strain However,

our previous mutants which lacked LOS [24] or

con-tained only lipid-A structure [23] showed reduced

growth rate and hypersusceptibility to the hydrophobic

compounds It implies that the linker moiety of the

LOS might be critical for maintenance of outer

mem-brane integrity, stability or flexibility by resistance to

foreign hydrophobic compounds to preserve normal

cell growth In addition, the O35Elgt3 mutant was

sen-sitive to the bactericidal activity of normal human

serum at 25% as compared with the wild-type strain,

but less sensitive than that of the mutant with lipid

A-only structure [23] It indicates that the linker moiety

(Glc-Kdo2) might also contribute to the serum

bacteri-cidal resistance However, another possibility also

exists As the susceptibility of the lipid A-only mutant

to hydrophobic compounds was higher than that of

the O35Elgt3 mutant, the permeability barrier of the

outer membrane might significantly contribute to the

bactericidal activity of normal human serum, and

might cause a much more sensitive phenotype of the

lipid A-only mutant than that of the O35Elgt3 mutant

Nevertheless, as the O35Elgt3 mutant did not change

its susceptibility to hydrophobic compounds but was

shown to be more sensitive to the bactericidal activity

of the human serum as compared with the wild-type

strain, it suggests that a complete OS chain moiety

contributes to the serum bactericidal resistance

LOS toxicity was assumed to be associated only with

the lipid A moiety By using Limulus amebocyte lysate

assay, we found that the O35Elgt3 mutant did not

show significant changes of the toxicity, whereas the

lipid A-only mutant [23] showed decreased toxicity

(6· 102EU Æ mL)1) six-fold as compared with the

wild-type strain (3.7· 103EU Æ mL)1), suggesting that

the LOS toxicity is attributable not only to the lipid A

moiety but also to the linker moiety (Glc-Kdo2)

Bacterial adherence to the surface of epithelial cells plays a critical role in colonization and is believed to

be the first step in the pathogenesis of microbial infec-tions It has been reported that several LOSs from respiratory tract bacteria are associated with bacterial adherence [29,35,36] Consistent with our previous results from the lipid A-only mutant, the O35Elgt3 mutant showed more than a 50% reduction in attach-ment to Chang or HeLa cells and enhanced clearance from the mouse nasopharynx after an aerosol chal-lenge when compared to the wild-type strain [23] Our data suggest that the M catarrhalis adherence to epi-thelial cells may not be associated with the linker and lipid A moieties, but with the OS chain moiety

In summary, we constructed a serotype A

M catarrhalisO35Elgt3 mutant that produced a linker (Glc-Kdo2)-lipid A structure The mutant showed sig-nificant changes in its biological activities in vitro and

in vivo These data, combined with our previous data from mutants which lacked LOS or contained only lipid A structure, suggest that a complete OS chain moiety of the M catarrhalis LOS is important in bio-logical activities such as serum resistance and adher-ence of epithelial cells, the linker moiety is critical for maintenance of outer membrane integrity and stability

to preserve normal cell growth, and both lipid A and linker moieties contribute to the LOS toxicity

Experimental procedures

Strains, plasmids, and growth conditions Bacterial strains, plasmids and primers are given in Table 1

M catarrhalis strains were cultured on chocolate agar plates (Remel, Lenexa, KS), or brain-heart infusion (BHI) (Difco, Detroit, MI) agar plates at 37C in 5% CO2 Mutant strains were selected on BHI agar supplemented with kanamycin at 20 lgÆmL)1 Growth rates of wild-type and mutant were measured as follows: an overnight culture was inoculated in 10 mL of BHI media (adjusted D600¼ 0.05) and shaken at 37C at 250 r.p.m The bacterial cultures were monitored spectrophotometrically at D600 Escherichia coli was grown on Luria-Bertani agar plates or broth with appropriate antibiotic supplementation The antibiotic concentrations used for E coli were as follows: kanamycin, 30 lgÆmL)1; and ampicillin, 50 lgÆmL)1

General DNA methods DNA restriction endonucleases, T4 DNA ligase, E coli DNA polymerase I Klenow fragment, and Taq DNA poly-merase were purchased from Fermentas (Hanover, MD) Preparation of plasmids, purification of PCR products and

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DNA fragments were performed using kits manufactured

by Qiagen (Santa Clarita, CA) Bacterial chromosomal

DNA was isolated using a genomic DNA purification kit

(Promega, Madison, WI) DNA nucleotide sequences were

obtained via 3070xl DNA analyzer (Applied Biosystems,

Foster City, CA) and analyzed with dnastar software

(DNASTAR Inc., Madison, WI)

Transposon mutagenesis and identification

of lgt3 gene

In vitro transposon mutagenesis of M catarrhalis was

per-formed as described previously [23] The resulting

kana-mycin-resistant colonies were screened by colony blot

assay and further identified by whole cell enzyme-linked

immunosorbent assay (ELISA) for loss of binding

reactiv-ity to an anti-LOS MAb (8E7) generated by serotype A

strain O35E [21] The transformants without the 8E7

binding activity were subsequently evaluated by

examin-ing the LOS profiles from proteinase-K-treated whole cell

lysates [37] on sodium dodecyl sulfate-polyacrylamide gel

electrophoresis (SDS⁄ PAGE) and LOS silver staining [38]

The clones with different LOS bands from the wild-type

LOS were selected for isolation of chromosomal DNA

The DNA fragment with the transposon insertion was

subsequently sequenced and the lgt3 homologue from

strain O35E identified by BLAST searches at GenBank of

the National Center for Biotechnology Information,

Bethesda, MD

Cloning of lgt3 homologue and construction

of the knockout mutants The entire lgt3 was amplified from the chromosomal DNA

of M catarrhalis strain O35E using primers 25 and 26 (Table 1, Fig 2) The PCR product was cloned into pCR2.1 using a TOPO TA cloning kit (Invitrogen, Carls-bad, CA) to obtain pCRlgt3 The insert was released by EcoR I-SalI digestion and then subcloned into an EcoRI-SalI site of pBluescript SK(+) to form pSlgt3 The kana-mycin-resistant gene from pUC4K was digested with EcoRI and subsequently inserted into the lgt3 gene using the HindIII site to form pSlgt3K

After verification by sequence analysis, the mutagenic lgt3 gene with the inserted kanamycin-resistant gene in pSlgt3K was amplified by PCR and purified for electropo-ration to O35E-competent cells After 24 h incubation, the resulting kanamycin-resistant colonies were selected for PCR analysis of chromosomal DNA using primers 40 and

26 (Table 1, Fig 2) An inactivated lgt3 mutant was verified

by sequence analysis and named as O35Elgt3

LOS determination

A crude LOS extraction was performed from both the wild-type strain O35E and the mutant O35Elgt3 using the proteinase-K-treated whole cell lysate method [37] The resulting extracts from each bacterial suspension (1.9 lg of protein amount) were resolved by 15% SDS⁄ PAGE and

Table 1 Strains, plasmids, and primers used in this study.

Plasmids

inserted into blunted HindIII site of pSlgt3 with internal deletion

This study

Primers

lgt3 sense, SalI site underlined

lgt3 antisense, EcoRI site underlined

5¢ flanking DNA of lgt3 sense

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visualized by silver staining [38] Western blot using MAb

8E7 was performed [21]

To further quantify LOSs expressed on both the

wild-type and mutant strains, a Kdo assay was applied [39] with

OMVs prepared using an EDTA-heat induced method [40]

as whole cells were not applicable for the Kdo assay The

amount of Kdo was determined by using 80 lg of OMVs

as samples and Kdo ammonium salt (Sigma, St Louis,

MO) as a standard

Structural analysis of LOS

For the composition analysis, 30–35 g of wet cells from

O35E and O35Elgt3 were prepared for LOS purification by

phenol–water extraction [41] The purified LOSs were

washed with a 9 : 1 ethanol⁄ water (v ⁄ v) mixture to remove

phospholipids The OSs were prepared by mild acid

hydro-lysis of LOSs in 1% aqueous acetic acid (v⁄ v) for 2.5 h at

100C and gel-filtration chromatography using Bio-Gel P-2

with deionized water as the eluent The glycosyl

composi-tions of OSs in O35E and O35Elgt3 were determined by the

preparation and GC-MS analysis of trimethylsilyl

methyl-glycosides The glycosyl linkages were determined by the

preparation and GC-MS analysis of partially methylated

aldiol acetates Analysis of GC-MS was performed on an

HP)5890 GC interfaced to a mass selective detector

5970 MSD using a Supelco DB1 fused silica capillary

col-umn (30 m· 0.25 mm Internal diameter, J & W Scientific,

Folsom, California) For MS analysis, the LOS was

O-deacylated by treatment with anhydrous hydrazine for

20 min at 37C [42] The de-O-acylated LOS samples were

dissolved in deionized water at 1 lgÆlL)1concentration and

mixed with equal volumes of 0.5 m 2,5-dihydroxy benzoic

acid (matrix) in methanol and spotted with 1 lL on a

100-well stainless steel MALDI plate The mass spectra were

col-lected on a MALDI-TOF instrument (Applied Biosystems)

in the negative reflectron mode NMR was performed on

the OSs by lyophilizing each sample from D2O (99.999 atom

percentage D, Sigma) twice, dissolved in D2O (100 atom

percentage D), and acquiring spectra using a Varian

Ino-va 500 or 600 MHz spectrometer (Varian, Palo Alto, CA)

Limulus amebocyte lysate assay

The chromogenic Limulus amebocyte lysate assay for

endotoxin activity was performed using the QCL-1000 kit

(Bio-Whittaker Inc., Walkersville, MD) Overnight cultures

from chocolate agar plates were suspended in BHI broth to

D620of 0.1 and serial dilutions of these stocks were tested

Susceptibility determination

The sensitivity of strains to a panel of hydrophobic agents

or a hydrophilic glycopeptide was performed using

standard disk-diffusion assays [43] Bacteria were cultured

in BHI to a D600of 0.2 and 100 lL portions of the bacte-rial suspension were spread onto chocolate agar plates Antibiotic disks or sterile blank paper disks (6 mm, Becton Dickinson, Cockeysville, MD) saturated with the various agents were plated on the lawn in triplicate at 37C for

18 h Sensitivity was assessed by measuring the diameter of the zone of growth inhibition in two axes and the mean value was calculated

Bactericidal assay to normal human serum

A complement-sufficient normal human serum was pre-pared and pooled from eight healthy adult donors A bacte-ricidal assay was performed in a 96-well plate [23] Normal human serum was diluted to 0.5, 2.5, 5.0, 12.5, and 25% in

pH 7.4 Dulbecco’s phosphate-buffered saline (NaCl⁄ Pi) containing 0.05% gelatin (DPBSG) Bacteria (10 lL of 106

colony forming units, CFU) were inoculated into 190 lL reaction wells containing the diluted normal human serum, 25% of heat-inactivated normal human serum, or DPBSG alone and incubated at 37C for 30 min Serial dilutions (1 : 10) of each well were plated onto chocolate agar plates The resulting colonies were counted after 24 h of incuba-tion

Adherence assay Chang (conjunctival; CCL20.2) and HeLa (cervix; CCL-2) human epithelial lines were cultured in Eagle’s minimal essential medium (ATCC, Manassas, VA) supplemented with 10% heat-inactivated fetal bovine serum in an atmo-sphere of 5% CO2at 37C A quantitative adherence assay was performed on a 24-well tissue culture plate (Corning Incorporated, Corning, NY) [34] Adherence was expressed

as the percentage of bacteria attached to the human cells relative to the original bacteria added to the well The data represent the average of three independent assays

Nasopharyngeal clearance pattern in animal model

Female BALB⁄ c mice (6–8 weeks of age) were obtained from Taconic Farms Inc (Germantown, NY) The mice were housed in an animal facility in accordance with National Institutes of Health guidelines under animal study protocol 1158–04 Bacterial aerosol challenges were carried out in mice using the same D540value for wild-type strain O35E (1.24· 109 CFUÆmL)1) or mutant O35Elgt3 (8.2· 108 CFUÆmL)1) in a 10 mL DPBSG [44] The num-bers of bacteria present in nasal washes were measured at various time points postchallenge The minimum detectable number of viable bacteria was 4 CFU per nasal washing Clearance of M catarrhalis was expressed as the percentage

Trang 9

of bacterial CFU at each time point compared with the

number deposited at time zero

Statistical analysis

The adherence and clearance percentages were analyzed by

a Chi-square test

Acknowledgements

We thank Eric J Hansen for providing strain O35E,

Wenzhou Hong for assisting in the animal challenge,

and Robert Morell and Yandan Yang for helping in

DNA sequencing This research was supported by the

Intramural Research Program of the NIH, NIDCD

The analytical work was supported in part by the

Department of Energy-funded (DE-FG09–93ER20097)

Center for Plant and Microbial Complex

Carbohy-drates

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