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Of these four families, only members of the MATE family have been shown to function mechanistically as secondary carriers, and no member of the MVF family has been shown to function as a

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R E V I E W A R T I C L E

The multidrug/oligosaccharidyl-lipid/polysaccharide (MOP)

exporter superfamily

Rikki N Hvorup, Brit Winnen, Abraham B Chang, Yong Jiang, Xiao-Feng Zhou and Milton H Saier Jr Division of Biological Sciences, University of California at San Diego, USA

The multidrug/oligosaccharidyl-lipid/polysaccharide (MOP)

exporter superfamily (TC #2.A.66)consists of four

previ-ously recognized families: (a)the ubiquitous multi-drug and

toxin extrusion (MATE)family; (b)the prokaryotic

poly-saccharide transporter (PST)family; (c)the eukaryotic

oligosaccharidyl-lipid flippase (OLF)family and (d)the

bacterial mouse virulence factor family (MVF) Of these

four families, only members of the MATE family have been

shown to function mechanistically as secondary carriers,

and no member of the MVF family has been shown to

function as a transporter Establishment of a common

ori-gin for the MATE, PST, OLF and MVF families suggests a

common mechanism of action as secondary carriers

cata-lyzing substrate/cation antiport Most protein members of

these four families exhibit 12 putative transmembrane

a-helical segments (TMSs), and several have been shown to

have arisen by an internal gene duplication event;

topo-logical variation is observed for some members of the

superfamily The PST family is more closely related to the

MATE, OLF and MVF families than any of these latter

three families are related to each other This fact leads to the

suggestion that primordial proteins most closely related to

the PST family were the evolutionary precursors of all members of the MOP superfamily Here, phylogenetic trees and average hydropathy, similarity and amphipathicity plots for members of the four families are derived and provide detailed evolutionary and structural information about these proteins We show that each family exhibits unique characteristics For example, the MATE and PST families are characterized by numerous paralogues within a single organism (58 paralogues of the MATE family are present in Arabidopsis thaliana), while the OLF family consists exclusively of orthologues, and the MVF family consists primarily of orthologues Only in the PST family has extensive lateral transfer of the encoding genes occurred, and in this family as well as the MVF family, topological variation is a characteristic feature The results serve to define a large superfamily of transporters that we predict function to export substrates using a monovalent cation antiport mechanism

Keywords: transport; membranes; proton motive force; superfamily; phylogeny; drug resistance; polysaccharides; lipid-linked oligosaccharides

Major families of drug efflux pumps

Bacterial species that have developed clinical resistance to

antimicrobial agents are increasing in numbers and have

become a serious problem in hospitals [1] One of the major

mechanisms of drug resistance in both prokaryotes and

eukaryotes involves drug efflux from cells There are many

drug efflux systems known in bacteria [2–5], and these

belong to five ubiquitous transporter (super)families [6,7]

Four of them (RND, DMT, MFS and MATE; see below)

one, the ATP-binding cassette (ABC), uses ATP hydrolysis Most characterized members of the resistance/nodula-tion/division (RND)superfamily [8] function as drug or heavy metal efflux pumps in Gram-negative bacteria Homologues in Gram-positive bacteria serve as lipid exporters [9] Small multidrug resistance (SMR)family pumps within the drug/metabolite transporter (DMT) superfamily [10] consist of homodimeric or heterodimeric structures with only four TMSs per subunit [11] They export cationic drugs using a simple cation antiport mechanism involving a conserved glutamyl residue [12] Drug exporters of the major facilitator superfamily (MFS)are found within six families, each known to transport a broad range of structurally distinct drugs [13,14]

The ABC superfamily of ATP-driven transporters includes many families that are potentially active in the uptake or efflux of metabolite analogues and other drugs For instance, the oligopeptide uptake transporter of

antibio-tics such as kanamycin and neomycin (reviewed in [7]) Uptake systems segregate from the efflux systems phylo-genetically [15] Members of this superfamily can also act on

Correspondence to: M Saier, Division of Biological Sciences,

University of California at San Diego, La Jolla, CA 92093 0116,

USA Fax: 001 858 534 7108, Tel.: 001 858 534 4084,

E-mail: msaier@ucsd.edu

Abbreviations: ABC, ATP-binding cassette; MATE, multi-drug and

toxin extrusion; MOP,

multidrug/oligosaccharidyl-lipid/polysaccha-ride; MPA, membrane-periplasmic auxiliary; MVF, mouse virulence

factor; OLF, oligosaccharidyl-lipid flippase; PST, prokaryotic

polysaccharide transporter; TMS, transmembrane segment.

(Received 23 July 2002, revised 14 November 2002,

accepted 9 December 2002)

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many types of macromolecules, a unique characteristic of

the ABC superfamily [16]

The MATE family of drug exporters (TC #2.A.66.1)

Only a few members of the multidrug and toxin extrusion

(MATE)family [3] are characterized functionally (Table 1)

These proteins include: (a)NorM and (b)VmrA in

Vibrio parahaemolyticus, a halophilic marine bacterium

that is one of the major causes of food poisoning in Japan

[17–19]; (c)YdhE from Escherichia coli, a close homologue

of NorM [20]; (d)Alf5 from the plant, A thaliana [21];

(e)VcmA from Vibrio cholerae non-O1, a nonhalophilic

protein, elevates resistance to the methionine analogue,

ethionine [24]

NorM, VmrA and VcmA have been shown to function

antiporters Several members are annotated as DinF

proteins The functions of the DinF proteins are unknown,

but expression of some of these proteins has been shown to

be induced by DNA damage [25,26] A function related to

the export of nucleotides excised from damaged DNA

during photorepair can be postulated

The polysaccharide transporter (PST) family

(TC #2.A.66.2)

Characterized protein members of the PST family are

generally of 400–500 amino acid residues in size and traverse

the membrane 12 times as putative a-helical TMSs

Analyses conducted in 1997 [27] showed that members of

the PST family formed two major clusters, one of which was

concerned putatively with lipopolysaccharide O-antigen

repeat unit export (flipping)in Gram-negative bacteria, the other which was concerned with exopolysaccharide or capsular polysaccharide export in both Gram-negative and Gram-positive bacteria However, numerous archaeal homologues are now recognized, and bacteria use PST systems to export other complex carbohydrates such as teichuronic acids [28] The mechanism of energy coupling for PST exporters is not established

PST transporters may function together with auxiliary proteins that regulate transport and allow passage of complex carbohydrates across both membranes of the negative bacterial envelope [29] Thus, each Gram-negative bacterial PST system specific for an exo- or capsular polysaccharide functions in conjunction with

a cytoplasmic membrane-periplasmic auxiliary (MPA) protein with a cytoplasmic ATP-binding domain (MPA1-C; TC #8.A.3)as well as an outer membrane auxiliary protein (OMA; TC #1.B.18)[27] Each Gram-positive bacterial PST system functions in conjunction with a homologous MPA1 + C pair of proteins (TC #8.A.3) equivalent to an MPA1-C protein of Gram-negative bacteria The C-domain has been shown to possess tyrosine protein kinase activity, suggesting that it functions

in a regulatory capacity [30] The lipopolysaccharide exporters may function specifically in the translocation of the lipid-linked O-antigen side chain precursor from the inner leaflet of the cytoplasmic membrane to the outer leaflet, but this possibility has not been established experimentally

The oligosaccharidyl-lipid flippase (OLF) family (TC #2.A.66.3)

N-Linked glycosylation in eukaryotic cells follows a conserved pathway in which a tetradecasaccharide

Table 1 Functionally characterized members of the multidrug and toxin extrusion (MATE)family.

Gene name

Arabidopsis thaliana Ath57 Alf5 (BAB02774)Tetramethylammonium, PVP (polyvinylpyrrolidone)

pyrrolidinone

[21] Escherichia coli Eco2 NorM (YdhE)

(P37340)

Ciprofloxacin a , berberine, kanamycin b , streptomycin b , acriflavine, tetraphenylphosphonium ion (TPP) chloramphenicol e , norfloxacin a , enoxacin a , fosfomycin, doxorubicin c , trimethoprim d , ethidium bromide, benzalkonium, deoxycholate

[1,25]

Bacteroides

thetaiotaomicron

Bth1 BexA (BAB64566)Norfloxacin1, ciprofloxacina, ethidium bromide [19] Vibrio cholerae Vch1 NorM (VcmA)

(Q9KRU4)

Norfloxacin1, ciprofloxacina, ofloxacin1, daunomycinc, doxorubicinc, streptomycinb, kanamycinbethidium bromide, 4¢6¢-diamidino-2-phenylindole dihydro-chloride (DAPI), Hoechst33342, acriflavine

[10]

Vibrio parahaemolyticus Vpa1 NorM (O82855)Norfloxacin1; ethidium bromide; kanamycinb;

ciprofloxacin1, streptomycin b

[25] Vpa3 VmrA (BAB68204)4¢6¢-diamidino-2-phenylindole (DAPI), (TPP),

acriflavine, ethidium bromide

[17]

a

Quinolones and fluoroquinolones;baminoglycosides;c anthracyclines such as adriamycin hydrochloride;d trimethoprim-sulfamethox-azole;emiscellaneous antibiotics.

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endoplasmic reticular (ER)membrane as a

dolichylpyro-phosphate (Dol-PP)-linked intermediate before being

trans-ferred to an asparaginyl-residue in a lumenal protein An

cyto-plasmic side of the membrane and translocated across the

membrane so that the oligosaccharide chain faces the ER

lumen where biosynthesis continues to completion [31] The

exporter in Saccharomyces cerevisiae that catalyzes the

translocation step is the 574 amino acid nuclear division

Rft1 protein with 12 putative TMSs [31] Homologues are

found in plants, animals and fungi

The mouse virulence factor (MVF) family (TC #2.A.66.4)

A single member of the MVF family, MviN of

Salmo-nella typhimurium, has been shown to be an important

virulence factor for this organism when infecting the mouse

[32] In several bacteria, genes encoding MviN homologues

occur in operons that also encode the uridylyl transferase,

GlnD, that functions in the regulation of nitrogen

meta-bolism [33] Nothing more is known about the function of

MviN or any other member of the MVF family However,

as will be shown below, these proteins are related to

members of the PST and MATE families with greatest

sequence similarity to members of the PST family It is

therefore possible that MVF family members are related

functionally to PST family members exporting complex

carbohydrates or related substances

The MOP superfamily

In this paper, we show that the MATE family of drug

exporters, the PST family of polysaccharide exporters, the

OLF family of lipid-linked oligosaccharide exporters and the

MVF family of mouse virulence-related proteins are all

homologous and are, therefore, related by common descent

We designate the superfamily that includes these four related

families the MOP (MATE/MVF-OLF-PST)superfamily

Currently sequenced members of these families are identified,

and the distribution of their members in the living world is

determined While MATE family members are found in all

domains of life (bacteria, archaea and eukaryotes), PST

family members are restricted to prokaryotes (both archaea

and bacteria), OLF family members are restricted to

eukaryotes and MVF family members are restricted to

bacteria In contrast to the MATE and PST families that

exhibit multiple paralogues in any one organism, the

eukaryotic OLF family is currently very small, consisting

of only eight sequenced orthologous members with no more

than one homologue per organism, and the MVF family,

while much larger, probably also consists primarily of

orthologues Because at least some members of the

pro-karyotic-specific PST family can flip lipid-linked

oligosac-charides (i.e O-antigen precursors of lipopolysacoligosac-charides in

Gram-negative bacteria), members of this family may serve

as the functional counterpart of the oligosaccharidyl lipid

exporters of eukaryotes The reported sequence analyses lead

us to suggest that prokaryotic oligosaccharidyl-lipid

export-ers were the primordial systems that gave rise to all membexport-ers

of the MOP superfamily We tabulate these proteins

according to family and derive reliable multiple alignments

website:http://www.biology.ucsd.edu/msaier/align.html/)

We also derive average hydropathy, similarity and amphi-pathicity plots which allow us to make transmembrane topological predictions, and these in turn lead to predictions regarding the evolutionary origins of protein topological types found within the MOP superfamily Most importantly, our results allow us to propose that all members of the MOP superfamily function as secondary efflux carriers using a solute/cation antiport mechanism

Computer methods Sequences of the proteins that comprise the MATE, PST, OLF and MVF families were obtained separately by initial

PSI-BLAST searches [10] using the SCREENTRANSPORTER

program without iterations [35] Recognizable members

June 2002

Multiple sequence alignments were constructed using the

CLUSTAL Xprogram [39] The gap penalty and gap extension

respectively, although other combinations were tried Average hydropathy, similarity and amphipathicity plots

program [40] Phylogenetic trees were derived by the neighbor-joining method from alignments generated with the CLUSTAL X program using the BLOSUM62 scoring

Charge bias analyses of membrane protein topology were

andTOPPRED2 [45] programs Motif searches were

of intrafamilial and interfamilial protein sequence similari-ties (i.e between members within each of the four families of the MOP superfamily as well as between members of the

BLOSUM62 scoring matrix, a gap opening penalty of )8,

BLAST2 program [50] was used additionally for comparison

analyses of internally duplicated intraprotein segments Binary comparison scores are expressed in standard devi-ations (SD)[51] A value of 9 SD is deemed sufficient to

to position TMSs in one protein relative to its homologues Thus, the positions of the extra TMSs in 14 TMS proteins relative to their 12 TMS homologues could be determined using this program

The four tables of family members (Tables S1–S4)and the multiple alignments from which the results reported in this paper were derived (Figs S1–S4), as well as additional

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supplementary supporting data can be found on our

ALIGN website

Results

The four families of the MOP superfamily

The general characteristics of the four currently recognized

families within the MOP superfamily are summarized in

Table 2 Columns 1 and 2 present the family abbreviations

and the TC # while column 3 gives the number of family

members identified The MATE family is the largest with

203 members while the PST, MVF and OLF families are of

decreasing sizes in that order (155, 45 and 8 recognized

members, respectively) As shown by the results presented in

column 4 of Table 2, most of the members of these four

families fall within the same size range However, a few of

the homologues were much larger (Table 2) Thus, in the

MATE family, two plant proteins, Ath10 and Ath8, have

1094 and 746 amino acid residues, respectively The

extended hydrophilic regions in these two proteins did not

show sequence similarity with anything else in the

data-bases Of greater interest were four large MVF family

homologues, all from high G + C Gram-positive bacteria

These four proteins were Mle of Mycobacterium leprae

(1206 amino acid residues), Mtu of M tuberculosis (1184

amino acid residues), Cgl of Corynebacterium glutamicum

(1083 amino acid residues)and Sco of Streptomyces

homologous to regions of eukaryotic-type serine/threonine

kinases Presumably, these C-terminal domains function in

a regulatory capacity, possibly to control the activities of the

N-terminal transporter protein domains

Column 5 in Table 2 summarizes the topological types

identified within each of the four families of the MOP

superfamily MATE and OLF family permeases may all

have 12 (or possibly 13)TMSs, but about one-third of all

PST family members are predicted to have 14 TMSs, and

MVF family members have 10, 12, 13, 14 or 15 putative

TMSs These will be analyzed in greater detail below

Finally, as summarized in column 6 of Table 2, each of

the four families within the MOP superfamily has

a distinctive organismal distribution While the MATE

family is present in all three domains of living organisms (archaea, bacteria and eukaryotes), the PST family is found both in archaea and bacteria but not in eukaryotes, while the OLF and MVF family members are restricted to eukaryotes and bacteria, respectively

The MATE family Our searches revealed that the MATE family contains 203 currently sequenced proteins, including representatives from all three domains of life (Table S1) In this sense, the family

is ubiquitous The family could be divided into 15 subfamilies (see phylogenetic tree displayed in Fig 1) Most

of the members are of about 450–550 amino acid residues in length and possess 12 putative TMSs The yeast proteins are larger (up to about 700 residues)whereas the archaeal proteins are generally smaller Large transporter size is

a characteristic of the eukaryotic domain while small size is

a characteristic of the archaeal domain [11]

Table S1 presents a summary of the 15 subfamilies (phylogenetic clusters)of the MATE family The sub-families, some of which include sequence divergent proteins, are as presented in the phylogenetic tree shown in Fig 1 The subfamily numbers as well as the names, organismal sources and abbreviations of the members of the MATE family are presented in columns 1–4 of Table S1 A short description of the proteins (column 5), the gene names,

TREMBLandSWISS-PROT)(columns 6–8)are also provided Finally, columns 9–10, respectively, present the protein sizes

in numbers of amino acid residues and the numbers of putative transmembrane a-helical TMSs per polypeptide chain, based on hydropathy plots The same format of presentation is used for tabulation of the proteins of the PST, OLF and MVF families (see Tables S2–S4)

The functionally characterized members of the family are found in subfamilies 1 (Sce3), 3 (Ath57), 4 (Eco2, Vch1, Vpa1), 7 (Vpa3) and 9 (Bth1) Subfamily 1 consists exclusively of yeast proteins; subfamily 2 includes only mammalian proteins, and subfamily 3 contains only plant proteins, mostly from A thaliana Most of the other subfamilies consist exclusively of bacterial and/or archaeal proteins Of them, only subfamilies 6, 7 and 10 include proteins from both of these prokaryotic domains In

Table 2 Characteristics of the families of the MOP superfamily For the MATE family, two larger homologues were found in Arabidopsis thaliana: Ath10, 1094 aas, and Ath8, 746 aas (see web table S1, Results section) No sequence similarity was observed for the extra portions of these proteins For the OLF family, two homologues in Kluyveromyces lactis, Kla, 417 aas, and A thaliana, Ath, 401 aas (see web table S3, Results section)are believed to be fragments For the MVF family, four larger homologues, all from high G + C Gram-positive bacteria, were found in Mycobac-terium leprae, Mle, 1206 aas, MycobacMycobac-terium tuberculosis, Mtu, 1184 aas, CorynebacMycobac-terium glutamicum, Cgl, 1083 aas and Streptomyces coelicolor, Sco, 811 aas Mle, Mtu and Cgl all include C-terminal domains (residues 720–950)that are homologous to each other and to domains in eukaryotic-type serine/threonine protein kinases A, archaea; B, bacteria; E, eukaryotes; aas, amino acid residues per polypeptide chain; TMSs, transmembrane a-helical segments.

Number

of members

Size range (number aas)

Number TMSs

Distribution among organisms

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subfamily 14, plant and bacterial proteins cluster very

loosely together Thus, seven subfamilies are bacterial

specific, three include both archaeal and bacterial proteins,

one is archaeal specific, one includes bacterial and plant

proteins, and three are eukaryotic specific The three

eukaryotic subfamilies consist of yeast, animal and plant

proteins, respectively (Fig 1)

Many organisms exhibit multiple MATE family

para-logues For example, among the bacteria, E coli and

and L monocytogenes each have six and Clostridium

both S cerevisiae and S pombe have three paralogues, but

these are not all orthologous to each other Most

impres-sively, A thaliana has 58 MATE family paralogues No

archaeon has more than four MATE family paralogues

Individual paralogues from a single species may either be

closely related, presumably arising from a recent gene

duplication event, or distantly related, arising from an earlier gene duplication event Extensive phylogenetic studies of more than 70 transporter families have shown that substrate specificity typically correlates with phylogeny [54–56] although exceptions have been reported [57] This fact allows functional predictions for many uncharacterized transporters

In Subfamily 7, the Thermotoga maritima homologue clusters loosely together with three archaeal proteins

small-subunit ribosomal RNA phylogeny has suggested that this bacterium is one of the deepest and most slowly evolving bacterial lineages [58] By using whole-genome similarity comparisons, T maritima appears to be the most archaeal-like of all sequenced bacteria It has been suggested that much of the similarity between T maritima and the archaea

is due to a shared ancestry of portions of their genomes as

a result of lateral gene transfer [59] In subfamilies 6 and 10,

Fig 1 Phylogenetic tree for the multidrug and toxin extrusion (MATE)family The tree was derived using the CLUSTAL X program The 15 subfamilies are labeled 1–15 together with the class of organisms from which the included proteins were derived; B, bacteria; Ar, archaea;

An, animals; Y, yeast; Pl, plants The arrow indicates the probable root of the tree as determined with outlying sequences.

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the archaeal proteins are so distant from the bacterial

homologues that the results are probably consistent with

vertical transmission from a common ancestor without

lateral transfer

Drug resistances demonstrated for characterized MATE

proteins mediate resistance to a wide range of cationic dyes,

fluoroquinolones, aminoglycosides and other structurally

diverse antibiotics and drugs It is interesting to note that

while cationic dyes are generally amphipathic and positively

charged, aminoglycosides are strongly hydrophilic, and

norfloxacin is amphiphilic Thus, MATE family transporter

substrates are diverse in nature

Average hydropathy and similarity plots for the MATE

family are shown in Fig 2A All 12 peaks of hydrophobicity

are well conserved Two additional peaks that are very

poorly conserved are found just preceding and following

conserved peak 12 The peak of hydrophobicity preceding

TMS 12 is due to an inserted sequence in just one protein,

C-terminal peak following putative TMS 12 is due to

extension of the animal homologues These few proteins

may have 13 rather than the usual 12 TMSs that

charac-terize the MATE family The extra regions in these few

proteins are presumably nonessential for transport function

Figure 3 shows an alignment of the first half of a MATE

family protein with the second half of the same protein

(PAB0243 from Pyrococcus abyssi) The two halves exhibit

40–50% similarity, 30% identity and a comparison score of 14.5 SD These values are sufficient to establish homology [52] Homology between the two halves of members of the PST and MVF families could also be established but not for the two halves of members of the OLF family

The PST family The sequenced proteins of the PST family are tabulated in Table S2 These proteins are derived exclusively from bacteria and archaea However, many diverse groups of these organisms are represented The transport functions of these systems are indicated when gene position or bio-chemical evidence allows postulation of their substrates The format of presentation for Table S2 (as well as Tables S3 and S4)is as for Table S1 Interestingly, and in contrast

to MATE family members, many PST family members are predicted to exhibit 14 rather than 12 TMSs However, few proteins are predicted to have odd numbers of TMSs (11 or 13) As will be shown below, the extra two TMSs in the 14 TMS PST family proteins are localized to the C-termini of these proteins

A dendrogram for the PST family is shown in Fig 4 Of the 12 clusters shown, only clusters 1, 2, 6 and 12 are restricted to the bacterial domain All other clusters include both archaeal and bacterial proteins This surprising observation shows that protein phylogeny does not corre-late with organism phylogeny In contrast to most families

Fig 2 Average hydropathy plots (top)and average similarity plots (bottom)for the MATE (A), PST(B), OLF(C) and MVF (D) families The

A VE H AS Program [40] was used to generate the plots with a window size of 19 Alignment position is indicated at the bottom of the figures The numbers above the hydropathy plots indicate the numbers of the putative TMSs In A and B, but not C and D, nonhomologous hydrophilic extensions were removed prior to graph generation.

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of transporters, including the MATE family of the MOP

superfamily, extensive horizontal transfer may have

occurred during the evolution of the PST family

In some cases we were able to provide convincing

evidence that horizontal transfer had in fact occurred For

example, in subfamily 5, Mth3, from the archaeon

Meth-anobacterium thermoautotrophicum, and Cac1, from the

encoding the Clostridium acetobutylicum protein (but not

that encoding the Methanobacterium thermoautotrophicum

homologue)showed a G + C content that differed

sub-stantially from that of the DNA of this organism overall

(0.31 for the genome and 0.24 for the gene) These results

taken together provide strong evidence for lateral transfer of

PST family genes across the bacterial–archaeal boundary It

should be noted that evidence for lateral transfer of genes

encoding cell surface bacterial polysaccharide biosynthetic

enzymes is extensive [60–62]

Figure 2B shows the average hydropathy (top)and

similarity (bottom)plots for PST family members Fourteen

peaks of hydropathy are evident, and for each of the first 12

such peaks, there is a corresponding peak of average

similarity However, the last two peaks of hydropathy are

not well conserved These two peaks represent the extra

peaks present in a minority of PST family members The

identities of the proteins exhibiting 14 rather than 12

putative TMSs is possible by examining the data presented

in Table S2

About one-third of the PST family members were

predicted to exhibit 14 TMSs Surprisingly, these proteins

were found in most subfamilies although only in subfamily 8

did the 14 TMS homologues predominate In some cases,

fairly close homologues were predicted to differ in topology

For example, Axy1 of Acetobacter xylinum (14 TMSs)and

Pae6 of Pseudomonas aeruginosa (12 TMSs)in cluster 1 had

essentially identical topologies except that Axy1 had

a C-terminal extension including the extra two TMSs that were lacking in Pae6 In fact, all 14 TMS proteins that were checked carefully were homologous throughout their first

12 TMSs to the 12 TMSs of their shorter homologues but had an extra C-terminal 2 TMS segment It was therefore concluded that the 14 TMS topological types arose from the

12 TMS proteins by addition of two TMSs at the C-termini The phylogenetic analyses suggest that this event has occurred repeatedly throughout the evolutionary history

of the PST family

The OLF family The proteins of the OLF family are presented in Table S3 and the corresponding phylogenetic tree is shown in Fig 5 All eukaryotic organisms with a fully sequenced genome have one and only one OLF family member with the notable exception of Plasmodium falciparum, a eukaryotic parasite that lacks N-glycoproteins [63] and also lacks an OLF family homologue These proteins are of 401–547 residues in length and display variable numbers of putative TMSs, from eight to 14 The two proteins with only eight putative TMSs, from Kluyveromyces lactis and A thaliana, may be incomplete sequences, due to incomplete sequencing and to nonrecognition of exons, respectively The other proteins are predicted to have 11–14 TMSs, and this prediction is dependent on the TMS prediction program used The actual numbers of TMSs may be 12 as suggested

by Helenius et al 2002 [31] The phylogeny of these proteins follows that of the organisms with the fungal, plant and animal proteins segregating as expected This fact suggests orthologous relationships for all family members and therefore suggests a common function (Fig 5)

The average hydropathy and average similarity plots for the six full length members of the OLF family are shown in Fig 2C We interpret the results in terms of a 12 TMS topology, the same as the major topological type observed

Fig 3 Binary alignment of the first half of a MATE family protein with its second half This protein is one of the three paralogues from Pyrococcus abyssi (PAB0243) The two halves were aligned using the GAP program with 500 random shuffles using the BLOSUM 62 program as the scoring matrix, a gap opening penalty of )8 and a gap extension penalty of )2 The two halves have a similarity of 40.5%, an identity of 29.8% and a comparison score of 14.5 SD |, an identity; :, a close conservative substitution; Æ, a more distant conservative substitution.

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Fig 4 Phylogenetic dendrogram for the polysaccharide transporter (PST)family The dendrogram was derived essentially as described in the legend

to Fig 1 The 12 subfamilies are labeled 1–12 together with the class of organisms from which the included proteins were derived; B, bacteria;

A, archaea.

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for the MATE and PST families However, the first two

putative TMSs are not strongly hydrophobic, and it is

therefore possible that these are localized to the cytoplasmic

side of the membrane as has been shown for members of

the chromate-resistance (CHR)family of transporters

(TC #2.A.51)[64] Although the proteins of the OLF

family can be hypothesized to exhibit a 6 + 6 TMS

topology with a large, well-conserved cytoplasmic loop

between putative TMSs 6 and 7 (Fig 2C), homology

between the two halves of these proteins could not be

demonstrated

As noted above, the first two putative TMSs displayed in

Fig 2C are quite hydrophilic, and they were therefore

examined in greater detail When putative TMSs 1 of the

full-length OLF family members were drawn in an a-helical

wheel, the helices (which lack prolyl and glycyl residues)

proved to be strongly amphipathic with three fully

con-served hydrophilic residues (helix residues Q4, R8 and N15)

tightly clustered on one side of the helix All other residues,

hydrophobic or slightly semipolar (data not shown)

Putative helix 2 was similarly amphipathic with four

well-conserved hydrophilic or semipolar residues (S5, E9, Q12

and S13)localized to one side of the helix These two helices

could provide a partially hydrophilic transmembrane

path-way for passage of lipid-linked oligosaccharides through the

membrane Alternatively, these two putative helices may be

localized to the cytoplasmic surface of the membrane The

remarkable conservation of Q4, R8 and N15 in helix 1

suggests an important function for these residues

The MVF family

The phylogenetic tree for the MVF family is shown in

Fig 6 Only two organisms, Pseudomonas aeruginosa and

Streptomyces coelicolor, both large genome organisms, have

more than a single MVF family member encoded within

their genomes, and they have only two MVF family

paralogues Except for the two extra paralogues, Pae2

and Sco2 (subfamily 8), all a-, b-, c- and d-proteobacterial proteins (23 proteins)are found in the lower half of the tree These fall into three primary clusters: cluster 1 includes only a-proteobacterial homologues, cluster 2 includes only b- and c-proteobacterial homologues, and cluster 3 includes the one d-proteobacterial homologue Within cluster 1, the phylogenies of all a-proteobacterial homologues follow the phylogenies of the 16S rRNAs [65], suggesting that they are orthologues Within cluster 2, the phylogenies of most b- and c-proteobacterial homologues are in accordance with those of the 16S rRNAs except for Vch which clusters with Pmu and Hin but should be between Ype and Pae, and Bap which should be close to Eco [65] Finally, the separate clustering of the d-proteobacterial protein, Bba, distant from all other homologues, is as expected

The upper part of the tree shows sequence divergent proteins from sequence divergent bacteria Only a few clusters are noteworthy Thus, cluster 5 includes all four high G + C Gram-positive bacterial homologues, cluster 6 includes the two cyanobacterial homologues, cluster 8 includes the two low G + C Gram-positive bacterial proteins, cluster 11 includes the two e-proteobacterial proteins, and cluster 15 includes the chlamydial orthologues Thus, with the exception of just four proteins (Bap, Vch, Pae2 and Sco2)the protein phylogenies follow the organi-smal (16S rRNA)phylogenies within experimental error This fact suggests that most of these bacterial proteins are orthologues, possibly serving a single function

The G + C contents and codon usage frequencies for the four anomalous genes were compared with the correspond-ing values for the protein-encodcorrespond-ing regions of the genomes

of the same organisms For Bap, the G + C content was 26% for both the gene and the organism For Vch, both values were 48%; for Sco2, the values were 76% for the gene and 72% for the genome; and for Pae2, the values were 72% for the gene and 67% for the genome In no case was the codon usage frequency for the gene significantly different from that for the organism as a whole These approaches therefore failed to provide further evidence for recent horizontal gene transfer of genes encoding MVF homo-logues

All MVF family proteins fell within the size range 480–

555 amino acid residues except for the high G + C Gram-positive bacterial homologues which were large (811–1184 amino acid residues)exhibiting 15 putative TMSs Three of these four proteins exhibit soluble protein kinase-like domains of about 250 residues in their C-terminal regions Most of the proteobacterial homologues appear to have 13

Fig 2D) Thus, there is probably some topological hetero-geneity in the MVF family

Establishment of homology for the four families

of the MOP superfamily The superfamily principle states that if A is homologous to

B, and B is homologous to C, then A is homologous to C [52] We have previously published the criteria used to establish homology, namely a comparison score in excess of

9 SD for two protein sequences of greater than 60 amino acid residues in length [52] Nine SD corresponds to a

Fig 5 Phylogenetic tree for oligosaccharidyl-lipid flippase (OLF)

family proteins See the legend to Fig 1 for format of presentation.

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arose by chance [51] In order to establish homology

between two coherent families, it is only necessary to

establish homology between one member of each of these

families Two such representative examples for each

inter-familial comparison are presented in Table 3 although

many more with comparison scores in excess of 9 SD could

have been selected When an equivalent number of

non-homologous proteins are compared (i.e comparing proteins

of the MOP superfamily with proteins of the major

facilitator superfamily (MFS; TC #2.A.1), values never

exceeded 7 SD

Figure S5 shows a binary alignment of an established

MATE family member with an established PST family

member The two proteins exhibit 38% similarity and 22%

identity with a comparison score of 28 SD The

corres-ponding alignment for interconnecting the OLF and PST

families is presented in Fig S6 The two proteins are 37%

similar and 25% identical with a comparison score of

13 SD The corresponding alignment for interconnecting

the MVF and PST families is shown in Fig S7 The two

proteins are 36% similar and 26% identical, yielding a

comparison score of 19 SD These comparisons and at least

one additional representative interfamilial comparison, giving values in excess of 9 SD, are summarized in Table 3 Many other binary comparisons gave comparison scores of greater than 9 SD However, the values reported in Table 3 are more than sufficient to establish homology

No member of the OLF family gave a comparison score

in excess of 6 SD with a member of the MATE or MVF family, and no member of the MVF family gave a score with

a MATE family member as high as the values obtained with PST family members The values recorded in Table 3 suggest a relative degree of relatedness of the four families as indicated in Fig 7 It is clear that the PST family is more closely related to the other three families than any two of the latter are related to each other

Identification of interfamilial conserved motifs

motifs in families of proteins, and these can be used to identify regions of sequence similarity between families [66] We therefore applied this program and selected two interfamilial regions of conservation for the pairs of

Fig 6 Phylogenetic tree for mouse virulence factor (MVF)family proteins See the legend to Fig 1 for format of presentation The 15 subfamilies are indicated 1–15.

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