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Structure, regulation and evolution of Nox-family NADPH oxidases that produce reactive oxygen speciesHideki Sumimoto Medical Institute of Bioregulation, Kyushu University, Fukuoka CREST,

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Structure, regulation and evolution of Nox-family NADPH oxidases that produce reactive oxygen species

Hideki Sumimoto

Medical Institute of Bioregulation, Kyushu University, Fukuoka

CREST, Japan Science and Technology Agency, Tokyo, Japan

Keywords

Duox; Nox; Noxa1; Noxo1; p22phox; p40phox;

p47 phox ; p67 phox ; Rac; Rboh

Correspondence

H Sumimoto, Medical Institute of

Bioregulation, Kyushu University, 3-1-1

Maidashi, Higashi-ku, Fukuoka 812-8582,

to four Ca2+-binding EF-hand motifs are present at the N-termini inseveral subfamilies, such as the respiratory burst oxidase homolog (Rboh)subfamily in land plants (the supergroup Plantae), the NoxC subfamily insocial amoebae (the Amoebozoa), and the Nox5 and dual oxidase (Duox)subfamilies in animals (the Opisthokonta), whereas an SH3 domain isinserted into the ferredoxin–NADP+reductase region of two Nox enzymes

in Naegleria gruberi, a unicellular organism that belongs to the supergroupExcavata Members of the Nox1–4 subfamily in animals form a stable hete-rodimer with the membrane protein p22phox, which functions as a dockingsite for the SH3 domain-containing regulatory proteins p47phox, p67phox,and p40phox; the small GTPase Rac binds to p67phox (or its homologousprotein), which serves as a switch for Nox activation Similarly, Rac acti-vates the fungal NoxA via binding to the p67phox-like protein Nox regula-tor (NoxR) In plants, on the other hand, this GTPase directly interactswith the N-terminus of Rboh, leading to superoxide production Here Idescribe the regulation of Nox-family oxidases on the basis of three-dimen-sional structures and evolutionary conservation

Abbreviations

AIR, autoinhibitory region; Duox, dual oxidase; FNR, ferredoxin–NADP+reductase; Fre, ferric reductase; FRO, ferric-chelate reductase; Noxa1, Nox activator 1; Noxo1, Nox organizer 1; NoxR, Nox regulator; PI3K, phosphatidylinositol-3-kinase; PKC, protein kinase C; PMA, 4b-phorbol 12-myristate 13-acetate; PPII, polyproline II; PRR, proline-rich region; PtdIns(3)P, phosphatidylinositol 3-phosphate; PtdIns(3,4)P2,phosphatidylinositol 3,4-bisphosphate; PX domain, phagocyte oxidase domain; Rboh, respiratory burst oxidase homolog; ROS, reactive oxygen species; TPR, tetratricopeptide repeat.

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Reactive oxygen species (ROS) are conventionally

regarded as inevitable deleterious byproducts of

aero-bic metabolism On the other hand, there exist

enzymes dedicated to ROS production The first

exam-ple of such enzymes is an NADPH oxidase expressed

in mammalian professional phagocytes [1–10] During

engulfment of invading microbes, the phagocyte

NADPH oxidase becomes activated to reduce

molecu-lar oxygen to superoxide anion (O2)), a precursor of

microbicidal ROS, in conjunction with oxidation of

NADPH As the rapid increase in oxygen consumption

during phagocytosis is known as the respiratory burst,

this enzyme is also called respiratory burst oxidase

The significance of the phagocyte oxidase in host

defense is exemplified by recurrent and life-threatening

infections that occur in patients with chronic

granu-lomatous disease, whose phagocytes genetically lack

the superoxide-producing activity [11,12]

The catalytic core of the phagocyte NADPH oxidase

(phox) is gp91phox, a membrane-integrated glycoprotein

with an apparent molecular mass of about 91 kDa

gp91phox contains two hemes in the N-terminal membrane region, and NADPH-binding and FAD-binding domains in the C-terminal cytoplasmic region(Fig 1A), forming a complete apparatus that trans-ports electrons from NADPH via FAD and two hemes

trans-to molecular oxygen In the mid-1990s, homologs ofthe flavocytochrome gp91phox were discovered in landplants; these have been designated respiratory burstoxidase homolog (Rboh) [13–15] Subsequent searches

in genome databases led to the identification of novelhomologs of gp91phox in animals, which are presentlyknown as Nox (NADPH oxidase) or Duox (dual oxi-dase) [1–10] The human genome contains seven genesencoding gp91phox homologs: Nox1–Nox5, wheregp91phox is renamed Nox2, and the distantly relatedoxidases Duox1 and Duox2 It is currently known that

a wide variety of eukaryotes express ducing NADPH oxidases that harbor a gp91phox-likeelectron-transferring system; the enzymes constitute theNox family Recent studies on Nox-family enzymeshave increasingly clarified the importance of deliberateROS production in various biological events, includingsignal transduction, development, and hormone bio-synthesis, in addition to well-established roles in hostdefense [1–10] It is likely that individual Nox enzymeshave developed regulatory systems, according to theirrespective special functions, during the course ofeukaryote evolution by inserting a regulatory domain(or motif) into their own sequences or by obtaining atightly associated protein as a regulatory subunit Reg-ulation by these proteins includes multiple protein–protein and protein–lipid interactions In this review, Idescribe post-translational regulation of Nox-familyenzymes on the basis of three-dimensional structuresand evolutionary conservation

superoxide-pro-Structure of Nox-family enzymes

The phagocyte NADPH oxidase gp91phox⁄ Nox2 (570amino acid residues) exists in not only the plasmamembrane but also the membrane of the specific gran-ule in neutrophils: the latter contains a higher amount

of Nox2 [1–10] Although the phagosomal membrane

is considered to primarily derive from the plasmamembrane, the specific granule is fused to the phago-some during phagocytosis, and thus gp91phox⁄ Nox2 isfurther enriched in the phagosomal membrane Forkilling engulfed microbes, superoxide (and microbicidalROS derived from superoxide) must be produced frommolecular oxygen within the phagosome The intra-phagosomal production requires electrons to be trans-ported from the cytoplasmic NADPH across themembrane into the interior of the phagosome Such

Fig 1 (A) A model for the structure of gp91 phox Cylinders

repre-sent six transmembrane a-helices (B) Bis-heme ligation in

gp91phox Heme-coordnating His residues are numbered according

to their localization in gp91 phox (C) Intramembrane bis-heme motifs

in various cytochromes The numbers of intervening amino acids

that separate a pair of His residues in a transmembrane segment

are indicated.

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transmembrane electron transport very often involves

di-heme membrane proteins

gp91phox⁄ Nox2 can be divided into two parts of

sim-ilar size (Fig 1A) The C-terminal half is a cytoplasmic

domain homologous to ferredoxin–NADP+ reductase

(FNR), bearing the NADPH-binding and

FAD-bind-ing sites [16,17], whereas the N-terminal moiety

com-prises six predicted a-helical transmembrane segments

(Fig 1A) The bipartite structure is common not only

to all the Nox-family enzymes but also to the family

of fungal ferric reductases (Fre) [18] Fre enzymes,

which are expressed in the plasma membrane, reduce

Fe3+ and Cu2+ for iron and copper uptake, but fail

to use molecular oxygen as a substrate [19,20]

Among the conserved transmembrane segments of

gp91phox⁄ Nox2, the third and fifth helices each contain

two invariant His residues, which are considered to

provide the axial and distal ligands for binding to the

irons of two nonidentical hemes, thereby placing one

heme towards the cytoplasmic face and the other

towards the outer face (Fig 1B) As the hemes are

ori-ented perpendicular to the surface of the membrane,

electrons are transferred from the cytosolic NADPH,

through FAD, and across the membrane via the hemes

to molecular oxygen, leading to superoxide production

Thus, transmembrane electron transport in gp91phox⁄

Nox2 is considered to occur in the N-terminal

bis-heme-containing region [18,21]

This model was initially proposed on the basis of a

similar motif consisting of two pairs of spaced His

resi-dues that was predicted to be linked to heme

coordina-tion in a class of organelle and bacterial b-type

cytochromes, such as the bis-heme cytochrome b of the

mitochondrial cytochrome bc1 complex (complex III)

and cytochrome b6 of the chloroplast cytochrome b6f

complex [22–24] (Fig 1C) The model for two

bis-hist-idyl heme ligation was subsequently verified by

determi-nation of crystal structures of protein complexes

containing these cytochromes [25–28] In cytochrome b

of the cytochrome bc1complex, containing eight

a-heli-cal transmembrane segments, the two b-type hemes are

bound within a four helix bundle formed by the first

four segments: His residues ligated to both hemes are

located in the second and fourth helices [25,26,29], and a

pair of the His residues in each helix are separated by 13

intervening amino acids (Fig 1C) A similar

coordina-tion occurs in cytochrome b6 of the cytochrome b6f

complex in cyanobacteria and chloroplasts [27,28]:

cyto-chrome b6 comprises four a-helical transmembrane

segments [30,31], and the two hemes are

bis-His-coordi-nated by imidazole side chains separated by 13 and 14

residues in the second and fourth helices, respectively

(Fig 1C) In the fungal Fre-family enzymes, both His

pairs are separated by 13 amino acids, as in chrome b of the cytochrome bc1complex (Fig 1C).Although gp91phox⁄ Nox2, as well as other Nox-familyenzymes, contains a pair of His residues in the thirdtransmembrane a-helix with 13 intervening amino acids(His101 and His115 in human gp91phox⁄ Nox2), the otherpair in the fifth helix (His209 and His222 in humangp91phox⁄ Nox2) are separated by 12 amino acids(Fig 1) It should be noted that the imidazoles sepa-rated by 12–14 amino acids are likely to face the sameside of the helix Substitution of any of these four Hisresidues results in disrupted insertion of hemes intogp91phox⁄ Nox2 [32], supporting the view that the twobis-histidyl heme ligation also occurs in gp91phox⁄ Nox2.Reduction of molecular oxygen to superoxide ingp91phox⁄ Nox2 requires both heme groups to be in thelow-spin (hexacoordinate) state, which implies thatelectron transfer to oxygen occurs via the outer heme

cyto-in a pocket near the heme edge, rather than throughdirect coordination of oxygen to the heme iron [33,34].This outer sphere (or peripheral) mechanism is consis-tent with the ‘two bis-histidyl heme ligation’ structure,and explains well why gp91phox⁄ Nox2-catalyzed super-oxide production is not inhibited by cyanide or carbonmonoxide Taken together, electron transfer fromNADPH to molecular oxygen occurs in a module des-ignated the Nox superdomain The Nox superdomaincomprises two moieties, the N-terminal bis-heme cyto-chrome b, composed of six a-helical transmembranesegments, and the C-terminal FNR, which containsFAD-binding and NADPH-binding domains Thus,gp91phox⁄ Nox2 and its relatives (the Nox family) areflavocytochromes [16,17,35]

It is known that members of the Duox subfamily inanimals, in contrast to oxidases of the other subfa-milies, release H2O2 without forming detectableamounts of superoxide [36] However, they are alsoexpected to produce superoxide as an initial product,

as Duox has the superoxide-producing Nox domain that comprises the bis-heme-containing trans-membrane region and the FNR-like moiety Indeed, ithas been reported that Duox in an immature form iscapable of producing superoxide [37] In mature Duox,superoxide produced by the Nox superdomain may berapidly converted to H2O2 via intramolecular dismuta-tion, possibly by a peroxidase-like ectodomain; thismodule is located on the outer surface of the mem-brane, where superoxide is expected to be released

super-In addition to the Nox and Fre families, both thebis-heme transmembrane segment and FNR-relatedmoiety are present in ferric-chelate reductase (FRO) ofland plants [38] To acquire iron from soils of low ironavailability, land plants such as Arabidopsis thaliana

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reduce Fe3+ to Fe2+ by FRO in the plasma

mem-brane of root epithelial cells Four His residues in

FRO that lie on two predicted, similarly orientated,

transmembrane a-helices are in equivalent locations to

the His residues in Nox enzymes that coordinate the

two hemes: the 13 and 12 amino acids separating

heme-liganding His residues exist in the helices

(Fig 1C) The FRO-family enzymes contain eight or

10 transmembrane segments, which is different from

the situation in members of the Nox and Fre families;

the precise membrane topology of FRO enzymes

remains controversial [39,40]

Origin of Nox-family enzymes

There is no evidence for the presence of Nox, Fre or

FRO in prokaryotes: a superfamily of

flavocyto-chromes that transport electrons across membranes On

the other hand, members of this superfamily are

pres-ent in a variety of eukaryotes The shared bis-heme

binding motif raises the possibility of an evolutionary

and functional relationship between the eukaryotic cell

surface membrane proteins Nox, Fre and FRO and the

prokaryotic (or organelle) b-type cytochromes On the

other hand, the C-terminal moiety of the

flavocyto-chrome superfamily is homologous to FNR, a

prokary-otic (organelle) protein that is made up of two

structural domains, each containing about 150 amino

acids: the C-terminal region includes most of the

resi-dues involved in NADPH binding, whereas the large

cleft between the two domains accommodates the FAD

group [41,42] It is tempting to postulate that a gene

encoding a protein containing two di-heme

transmem-brane helices was fused to an FNR gene in eukaryote

evolution, leading to a common ancestor of the Nox

and Fre families (Fig 2) In this context, it seems

inter-esting that FNR directly interacts with the chrome b6f complex of plant chloroplasts, albeit in anoncovalent manner, and participates in electron trans-fer [43]; cytochrome b6 in the complex has two b-typehemes across the membrane, as expected for Nox

cyto-A similar fusion of the FNR gene with a geneencoding an electron-transporting protein is also con-sidered to have occurred during evolution: eukaryoticdiflavin reductases such as NADPH–cytochrome P450reductase (CPR or P450R), methionine synthase reduc-tase and novel reductase 1 probably arose from thefusion of the ancestral genes for FNR and flavodoxin,

a prokaryotic FMN-containing protein that transferselectrons in a variety of photosynthetic and nonphoto-synthetic reactions in prokaryotes [43–48] (Fig 2) Inturn, a diflavin reductase is likely to be the precursor

of further fusion products such as nitric oxide tase, which consists of a C-terminal CPR-like domainand an N-terminal, heme-containing oxygenase domain[48,49]

reduc-Distribution of Nox-family enzymes

in eukaryotes

In contrast to the absence of Nox in prokaryotes,genes encoding Nox-family enzymes are found in awide variety of eukaryotes Eukaryotes can be dividedinto several major supergroups, including the Opi-sthokonta, the Amoebozoa, the Plantae, the Excavata,the Rhizaria, and the Chromalveolata (the Hetero-konta plus the Alveolata): animals and fungi belong tothe Opisthokonta; the social amoeba Dictyostelium dis-coideum is a member of the Amoebozoa; land plantsand red algae belong to the Plantae; and diatoms andoomycetes are members of the Heterokonta, a groupthat belongs to the Chromalveolata (Fig 3) [50–52]

Fig 2 A putative common ancestor of the Nox family CPR, NADPH–cytochrome P450 reductase.

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The relationships between these supergroups, however,

remain to be determined, and thus the root of

eukary-otes is presently uncertain [53,54]

Recent expansion of information available in

gen-ome databases has revealed that Nox-family enzymes

are present in all the eukaryotic supergroups except

the Rhizaria (Fig 3) This suggests that a common

ancestor of Nox genes emerged at an early stage in the

evolution of eukaryotes; it diverged well in some

lin-eages (e.g in the Opisthokonta and Plantae), whereas

it was often lost in some other lineages The loss of

Nox genes appears to have occurred at multiple stages

in eukaryote evolution For example, in the

super-group Amoebozoa, the social amoeba Di discoideum

contains three Nox genes [55], whereas they are absent

in Entamoeba histolytica [56] In the supergroup

Excav-ata, the heterolobosa Naegleria gruberi has at least two

Nox genes, as found by the present search using the

database of the DOE’s Joint Genome Institute (http://

genome.jgi/psf.org/euk_home.html) (Fig 3); on the

other hand, no Nox gene has been found in the

kineto-plastid Leishmania major or Trypanosoma brunei, or

the diplomonad Giardia lamblia [56] In the

Chromal-veolata, Nox genes are present in genomes of the

oomycete Phytophthora sojae [56,57] and the diatom

Thalassiosira pseudonana [58], although they have not

been found in the genomes of Plasmodium falciparum

and Theileria parva, both of which belong to the same

supergroup [56] Even in the Opisthokonta, Nox genes

have been lost independently in several fungal lineages;

for example, a Nox gene is absent in budding andfission yeasts [56,57,59]

Regulation of Nox-family enzymes

by Ca2+

Superoxide production by Nox is regulated by variousmechanisms Several subfamilies of Nox enzymesappear to be directly regulated by Ca2+ It is wellestablished that mammalian thyroid oxidase and seaurchin NADPH oxidase, both of which belong to theDuox subfamily, are reversibly activated by Ca2+ Inaddition to the Nox superdomain comprising the bis-heme-containing transmembrane region and the FNR-homologous moiety, Duox-subfamily oxidases feature

an N-terminal peroxidase-like ectodomain that is rated from two EF-hands by an additional transmem-brane segment (Fig 4) Biosynthesis of thyroidhormones in humans requires Duox2, which is highlyexpressed in the thyroid gland: mutations in Duox2are associated with a loss of thyroid hormone synthesisand can lead to permanent and severe congenital hypo-thyroidism [60] With the H2O2 produced by Doux2,thyroid peroxidase catalyzes conjugation of iodide ions

sepa-to Tyr residues on thyroglobulin in the thyroid cles, an essential step for the synthesis of the activehormone [61] On the other hand, during fertilization

folli-of sea urchins, a rapid increase in H2O2 generationoccurs, which is catalyzed by the sea urchin Duoxhomolog Udx1, leading to formation of the fertiliza-

Fig 3 Distribution of Nox-family enzymes

in eukaryotes and animals Upper panel:

eukaryotes can be divided into six major

supergroups, including the Opisthokonta,

the Amoebozoa, the Plantae, the Excavata,

the Rhizaria, and the Chromalveolata All the

supergroups except the Rhizaria are known

to contain Nox genes Lower panel: M b.,

Mo brevicollis; N v., Ne vectensis; L g.,

Lot gigantea; C sp I, Capitella sp I; C e.,

Ca elegans; D m., Dr melanogaster; S p.,

S purpuratus; B f., B floridae; C i., Ci.

intestinalis; D r., Da rerio; X t., X

tropical-is; G g., Ga gallus; H s., Homo sapiens.

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tion envelope as the physical block to polyspermy [62].

It is also known that Duox1 of Caenorhabditis elegans

in the phylum Nematoda is involved in cross-linking

of Tyr residues of extracellular matrix proteins,

thereby facilitating cuticle formation [63], and that

Duox plays a critical role in innate immunity in the

gut of the fruit fly Drosophila melanogaster in the

phylum Arthropoda [64]

Regulation of Duox by Ca2+probably occurs via its

paired EF-hand motif It has been reported that

lim-ited proteolysis with a-chymotrypsin renders thyroid

NADPH oxidase fully and irreversibly active

indepen-dently of Ca2+ [65] This implies that the Ca2+

-bind-ing EF-hands of Duox serve as an autoinhibitory

domain, whereas those of Nox5 function as an

activa-tion domain [66] The inhibiactiva-tion of Duox by the

EF-hands might be released reversibly by physiological

Ca2+-induced conformational change and irreversibly

by proteolytic removal of the autoinhibitory domain

[37] A recent study has shown that ectopically

expressed Duox produces ROS without cell stimulants,

and the production is enhanced two-fold by the

addi-tion of ionomycin [67], suggesting that elevaaddi-tion of

cytoplasmic concentrations of Ca2+ is dispensable

Besides direct regulation by Ca2+, protein kinase C

(PKC) may modulate Duox in a Ca2+-independent

manner, as ROS production in thyrocytes is triggered

by 4b-phorbol 12-myristate 13-acetate (PMA), an

agent that activates PKC without elevating the

cyto-plasmic concentration of Ca2+[68] A PKC-dependent

pathway may also function in H2O2 generation atfertilization in the sea urchin [62]

In addition to the animal Duox subfamily, oxidases

of other two subfamilies have been shown to bedirectly regulated by elevations in cytoplasmic Ca2+concentrations: the Nox5 subfamily in animals[66,69,70], and the Rboh subfamily in land plants[71,72] (Fig 4) The regulation by Ca2+ appears to beconsistent with the presence of the Ca2+-bindingEF-hand motif in the cytoplasmic region N-terminal tothe Nox superdomain (Fig 4)

Human Nox5 is abundantly expressed in T and

B cells of spleen and lymph nodes, and also in the spermprecursors of testis [69] Although the role for mamma-lian Nox5 remains unknown, Drosophila Nox5 has beenreported to mediate smooth muscle contraction [70].Oxidases of this subfamily build on the basic structure

of the Nox prototype, adding an N-terminal extensionthat contains four EF-hands: three canonical motifsand one noncanonical motif [63] (Fig 4) Biochemicalanalysis has shown that activation of Nox5 is directlyregulated by Ca2+: superoxide production by Nox5-containing membrane fractions is dependent on thepresence of Ca2+ [66]; and cells ectopically expressingNox5 produce superoxide in response to the Ca2+iono-phore ionomycin [69] The Ca2+-binding domain ofNox5, in contrast to that of Duox, may function as anactivator module: the binding of Ca2+causes a confor-mational change, which leads to intramolecular interac-tion of the N-terminal Ca2+-binding domain with the

Fig 4 Models for structures of various types of Nox-family enzymes Cylinders rep- resent six transmembrane a-helices EF,

sub-Ca 2+ -binding EF-hand motif.

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C-terminal Nox superdomain, culminating in Nox5

acti-vation [66] On the other hand, the EC50for calcium of

about 1 lm, determined in a cell-free activation system

for Nox5 [66], is relatively high and unlikely to be

achieved in most cells treated with physiological

stimu-lants Two mechanisms for the elevation of the Ca2+

sensitivity have recently been proposed [73,74] First,

PKC phosphorylates Ser⁄ Thr residues in the

FAD-bind-ing domain of Nox5, which increases the Ca2+

sensitiv-ity of the Nox5 activsensitiv-ity regulated by the N-terminal

Ca2+-binding domain [73] Second, a consensus

calmod-ulin-binding site is present in the NADPH-binding

domain of Nox5; calmodulin interacts with the site at a

lower concentration of Ca2+, thereby elevating the

Ca2+sensitivity for Nox5 activation [74]

The Rboh subfamily of NADPH oxidases is

respon-sible for ROS formation associated with plant defense

responses, and also plays a crucial role in plant

devel-opment [13,14,75] Ten and nine members are present

in A thaliana [14] and the rice Oryza sativa [76],

respectively The Rboh-subfamily enzymes carry an

N-terminal extension with two EF-hand motifs

(Fig 4) It has been reported that only about a

two-fold to three-two-fold increase in superoxide production

occurs in the membrane fraction of tobacco and

tomato upon addition of Ca2+; in addition, the effect

requires high concentrations of Ca2+ (approximately

millimolar) [71] This observation suggests that the

direct effect of Ca2+may not contribute to Rboh

acti-vation to a large extent A recent study has shown that

elicitor-responsive phosphorylation of the N-terminal

region of Rboh is involved in superoxide production

[77,78], which is mediated by Ca2+-dependent protein

kinases [77] Activation of Rboh is also regulated by

plant homologs of the Rho-family small GTPase Rac

(also known as Rop for Rho-like protein) [79–81]; Rac

in the GTP-bound form functions by directly binding

to the N-terminal region of Rboh, and this is probably

inhibited by Ca2+ [76] Thus, regulation of Rboh is

more complicated than previously expected, as

described in detail in a later section

As in plant Rboh, two copies of EF-hands are

pres-ent in the N-terminal cytoplasmic region of the

NoxC-subfamily members in the Amoebozoa and Nox

enzymes in oomycetes of the eukaryotic supergroup

Chromalveolata [57], whereas enzymes in the fungal

NoxC subfamily contain a single EF-hand in the

N-terminal cytoplasmic region [56,57,59] These

sub-families of Nox enzymes may be regulated by Ca2+;

however, no experimental evidence for Ca2+-mediated

regulation has been obtained

It is presently unknown whether the

EF-hand-con-taining Nox subfamilies originated from a common

ancestor gene It seems rather likely that EF-handmotifs have been obtained independently several timesduring evolution The genomes of Monosiga brevicollis

in the choanoflagellates (a sister group of animals) andNematostella vectensis in the cnidarians (a basal group

of animals) contain solely Nox2-like enzymes, and notEF-hand-containing oxidases such as Nox5 and Duox,although these two families are found in a variety ofspecies of protostomes and deuterostomes (Fig 3).Thus, Nox5 and Duox may have evolved from Nox2-like prototype oxidases Similarly, in fungi, the NoxCsubfamily containing an EF-hand is found solely inmore evolved groups, including the Sordariomycetesand Dothideomycetes, whereas the Nox2-likeEF-hand-free subfamilies NoxA and NoxB are presentalso in relatively basal groups such as the Chytridi-omyceta and Basidiomycota [57] These features sug-gest that the NoxC subfamily emerged at a later stage

of fungal evolution Thus, the classification of the Noxfamily in eukaryotes into the two major groups,depending on the presence or absence of the EF-handmotif, does not seem to reflect molecular evolution

Regulation of Nox-family enzymes by protein–protein interactions

The genome of Na gruberi (http://genome.jgi/psf.org/euk_home.html), a member of the eukaryotic super-family Excavata, contains two genes encoding Nox-family enzymes of 627 and 630 amino acids, both ofwhich have an SH3 domain and thus are tentativelydesignated as NoxSH3 (Fig 5) The SH3 domain isinserted into a loop region in the NADPH-bindingdomain of the C-terminal FNR-homologous region(Fig 5) It is tempting to postulate that the NoxSH3enzymes in Naegleria are regulated by a protein har-boring a proline-rich region (PRR); SH3 domains aregenerally known as modules that recognize a PRR tomediate protein–protein interactions [82,83] Identifica-tion of a NoxSH3-binding protein will shed light onour understanding of Nox regulation

Nox1–Nox4 in animals form a heterodimer with thenonglycosylated integral membrane protein p22phox,which contains two (or possibly four) putative trans-membrane segments (Fig 4) The complex ofgp91phox⁄ Nox2 with p22phoxin phagocytes is known asflavocytochrome b558 In the C-terminal cytoplasmicregion of p22phox, there exists a PRR, which serves as

an anchoring site, thereby juxtaposing the catalyticcenter gp91phox and the SH3 domain-containing regu-latory proteins p47phox, p67phox, and p40phox; on theother hand, the small GTPase Rac functions in Noxactivation by interacting with p67phox or its homolo-

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gous proteins Detailed mechanisms for regulation by

these proteins will be described below Complex

forma-tion of p22phoxwith Nox also contributes to the

stabil-ization of each protein [1–10] Formation of themutually stabilizing complex appears to require thecorrect folding of Nox, because heme incorporationinto gp91phox⁄ Nox2 is essential for heterodimer forma-tion [84]

It is known that human Duox2 associates with aspecific maturating protein named DuoxA2, whichcontains putative five transmembrane helices [67,85](Fig 6) The membrane protein DuoxA2 allows thetransition from the endoplasmic reticulum to the Golgiapparatus, maturation and translocation to the plasmamembrane of functional Duox2 [67,85] Interestingly,the DuoxA2 gene is arranged head-to-head and coex-pressed with the Duox2 gene; the gene for DuoxA1, aparalog of DuoxA2, is similarly linked to the Duox1gene [85] Biallelic inactivation of the DuoxA2 genehas recently been reported as a novel cause of congeni-tal hypothyroidism [86], confirming its crucial contri-bution to function of Duox2, which is directlyinvolved in thyroid hormone synthesis [60]

The Nox subfamilies in animals

The Nox enzymes in animals can be divided into threesubfamilies: one containing Nox1–Nox4 (the Nox1–4

Fig 5 Structure of the SH3 domain-containing enzyme NoxSH3 in

Na gruberi The two NoxSH3 enzymes in Na gruberi, tentatively named NoxSH3-1 and NoxSH3-2, contain 627 and 630 amino acids, respectively The amino acid sequences of NoxSH3-1 and NoxSH3-2 are shown: the heme-coordinated His residues in transmembrane segment 3 (TM3) and TM5 are shown in red; residues of FAD-bind- ing motifs are shown in green; residues of NADPH-binding motifs are shown in blue; and residues of the SH3 domain are shown in magenta A model for the structure of NoxSH3 is also shown The SH3 domain is inserted into the C-terminal NADPH-binding domain Cylinders represent six transmembrane a-helices.

Fig 6 Models for the structure of Duox1 ⁄ 2 complexed with A1 ⁄ 2 Cylinders represent six and five transmembrane a-helices of Duox1 ⁄ 2 and DuoxA1 ⁄ 2, respectively EF, Ca 2+ -binding EF-hand motif.

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Duox-subgroup), which form a heterodimer with p22phox[87–

93]; the Nox5 subfamily; and the Duox subfamily

(Fig 4) Although the Nox5 and Duox subfamilies are

not found in the sea anemone Ne vectensis of the

Cnidaria (the basal group of animals)

(http://geno-me.jgi/psf.org/euk_home.html) [94] (Fig 3), they were

probably present at the protostome–dueterostome

diver-gence This is because the Nox5 and Duox subfamilies

exist in both extant protostomes and deuterostomes,

with the exception that Nox5 has been lost in the lineage

of the phylum Nematoda and in that of the order

Rod-entia in mammals: Nox5 is absent in the nematode

Ca elegansand the rodents mouse and rat (Fig 3)

On the other hand, Nox2, a member of the Nox1–4

subgroup, was present before the divergence of the

Choanoflagellata and Metazoa (equivalent to animals):

Nox2 is found not only in the Cnidaria but also in the

choanoflagellate Mo brevicollis (http://genome.jgi/

psf.org/euk_home.html) [94] (Fig 3) During the

evolu-tion of protostomes, one of the two major groups of

animals, Nox2 has been lost in the lineage of the clade

Ecdysozoa, including the phyla Arthropoda and

Nem-atoda: Nox2 is absent in the fruitfly Drosophila and

the nematode Ca elegans On the other hand, Nox2 is

present in the Lophotrochozoa, another major

proto-stomian clade, including the phyla Mollusca and

Annelida: this oxidase exists in the limpet Lottia

gigan-tea (Mollusca) and the leech Capitella species

(Annel-ida) (Fig 3) Thus, it is likely that Nox2 is the closest

to the ancestral Nox in animals In contrast, Nox1,

Nox3 and Nox4 are not found in protostomes or the

Echinodermata, a phylum that belongs to the

deuter-ostomes (a sister group of protdeuter-ostomes) These three

Nox enzymes appear to have diverged from Nox2 at

distinct stages of evolution of the phylum Chordata in

deuterostomes

The Chordata is divided into three subphyla: the

Vertebrata, Urochordata (also known as the Tunicata),

and the Cephalochordata Although tunicates were

long considered to be the earliest offshoot of the

chor-date lineage, and cephalochorchor-dates (such as

amphi-oxus) as the closest group to vertebrates, recent

analyses have reversed their positions: amphioxus is

now viewed as the ‘basal chordate’ [95], and tunicates

as the sister group, or closest relatives, of the

verte-brates [96] (Fig 3) Thus, our understanding of the

evolution of a certain protein in the Chordata requires

information on the corresponding protein in the

sub-phylum Cephalochordata The present search for the

database of the amphioxus (lancelet) Branchiostroma

floridae (http://genome.jgi/psf.org/euk_home.html)

rev-ealed that, in addition to Nox2, Nox5, and Duox,

Nox4 exists in the Cephalochordata It is known that

Nox4 is present in Ciona intestinalis (the Urochordata)[97] but not in the sea urchin Strongylocentrotus purpu-ratus of the phylum Echinodermata, another majorgroup of the Chordata [90] Therefore, Nox4 appears

to have branched from a root close to Nox2 with theemergence of the Chordata Nox1 is found from fishes

to mammals, but not in the Urochordata or chordata, suggesting that this oxidase probably arosewith the emergence of the Vertebrata Nox3 hasemerged most recently, probably from a commonancestor of birds and mammals, because it is foundsolely in mammals and birds, but not in fishes oramphibians [98] (Fig 3)

Cephalo-The membrane protein p22phox has been strated to be complexed with mammalian Nox1–Nox4.Consistent with this, p22phox is absent in the Ecdyso-zoa, where the Nox1–4 subfamily is absent, but widelydistributed in species that have Nox2, including thechoanoflagellate Mo brevicollis and the cnidarian

demon-Ne vectensis The known exceptions are the leech itella species (the Annelida) and the sea urchin S pur-puratus (the Echinodermata) Nox2 of these species orgroups might be stable without p22phox, leading to loss

Cap-of the p22phox gene It may also be possible that thep22phox gene escaped cloning or correct sequencing forunknown reasons, which is known to often occur invarious genome projects

Regulation of the Nox1–4 subfamily

in animals

The phagocyte oxidase gp91phox⁄ Nox2 in mammals isdormant in resting cells, but becomes activated duringphagocytosis to produce superoxide, a precursor ofmicrobicidal ROS The oxidase activity is spatially andtemporally restricted to the phagosome, as inappropri-ate or excessive production of ROS results in damage

to surrounding cells and severe inflammation tion of gp91phox⁄ Nox2 requires stimulus-induced mem-brane translocation of p47phox, p67phox, p40phox, andRac, i.e formation of the active oxidase complex atthe membrane (Fig 7A) The essential role of theseregulatory proteins is evident from the following twolines of evidence First, the phagocyte NADPH oxi-dase activity can be reconstituted in a cell-free systemwith gp91phox, p22phox, p47phox, p67phox, and Rac, using

Activa-an Activa-anionic amphiphile, e.g arachidonic acid, as Activa-an

in vitro stimulant Second, defects in any of the fourgenes encoding gp91phox, p22phox, p47phox and p67phoxcause the primary immunodeficiency chronic granu-lomatous disease [11,12]

In the cytoplasm of resting cells, p47phox, p67phoxand p40phox form a ternary complex, whereas Rac is

Trang 10

complexed with Rho GDP dissociation inhibitor.

Upon cell stimulation, the three phox proteins are

en blocrecruited to the membrane; on the other hand,

Rac translocates independently but without Rho GDP

dissociation inhibitor, which remains in the cytoplasm

Although activation of gp91phox⁄ Nox2 complexed with

p22phoxin cells absolutely requires p47phox, p67phoxand

Rac as cytosolic regulators, p47phox is dispensable for

cell-free activation in the presence of excess amounts

of p67phox and Rac [99,100] It is thus considered that

p47phox functions as an organizer, whereas p67phox

serves as an activator that directly participates in

gp91phox⁄ Nox2 activation

Nox1 is abundantly expressed in colon epithelial

cells and also in vascular smooth muscle cells

[101,102], and seems to be involved in angiotensin

II-mediated hypertension [103–105] Nox1, as well as

Nox2, forms a complex with p22phox [88,106]

Although Nox1 is also inactive without an organizer

or an activator, it generates superoxide in the presence

of the p47phox paralog Noxo1 (Nox organizer 1) and

the p67phoxparalog Noxa1 (Nox activator 1) [106–109]

(Fig 7B) Rac is directly involved in Nox1 activation

as well [110–112]

In the inner ear of mice, Nox3 plays a crucial role in

formation of otoconia, tiny mineralized structures that

are required for perception of balance and gravity

[113] Although Nox3 also forms a functional

heterodi-mer with p22phox, this oxidase is capable of producing

superoxide in the absence of an organizer or an

activa-tor [88] The superoxide-producing activity can bestrongly enhanced by p47phox, Noxo1, and p67phox[89,110,114,115] In the presence of p67phoxor Noxa1,Nox3 activity is upregulated by Rac [110,116]

Although it is well known that Nox4 is highlyexpressed in epithelial cells of the adult and fetal kid-ney [117,118] and vascular endothelial cells [91,119], itsfunction remains to be elucidated Nox4 is complexedwith p22phox as well [80,82,84], and constitutively gen-erates superoxide in an NADPH-dependent manner[120] The mechanism of Nox4 regulation is largelyunknown at present: Nox4-mediated superoxide gener-ation appears to be independent of p47phox, Noxo1,p67phox, or Noxa1 [89,117,118], whereas the role ofRac remains controversial [79,121]

Nox2 activation

The oxidase organizer p47phoxis a 390 amino acid tein that contains, from the N-terminus, a phagocyteoxidase (PX) domain, tandem SH3 domains, and aPRR (Fig 7) The two SH3 domains cooperativelyinteract with the PRR in the C-terminal cytoplasmicregion of p22phox, an interaction that is essential forboth membrane translocation of p47phox and oxidaseactivation [122–124] The tandem SH3 domains sand-wich a short PRR of p22phox (amino acid resi-dues 151–160), containing a polyproline II (PPII) helix[125–127] (Fig 8) Pro152, Pro156 and Arg158 in thehuman p22phox PRR are indispensable for the inter-action with p47phox: Pro152 and Pro156 are recognized

pro-by the N-terminal SH3 domain, whereas Arg158directly contacts with the C-terminal one [127] (Fig 8)

On the other hand, Pro151, Pro155, Pro157 andPro160 are also involved in binding to p47phoxbut to alesser extent [127]

The gene encoding p22phoxexists in a wide variety ofanimals and also in the Choanoflagellata, a sistergroup of the Metazoa (Animalia) [128,129]; the p22phoxgene is absent in the Ecdysozoa, which is consistentwith the absence of the Nox1–4 subfamily in this clade(Fig 9) The p22phox region comprising the N-terminalcytoplasmic region and the two transmembrane seg-ments is functionally important [130] and well con-served in the Metazoa (animals) and Choanoflagellata,whereas the C-terminal cytoplasmic region is highlyvariable except for the PRR (Fig 8) The three resi-dues indispensable for binding to p47phox (Pro152,Pro156 and Arg158 in human p22phox) are invariant inall known animal p22phox proteins (Fig 8), althoughidentifiable p47phoxexists solely in the phylum Chorda-

ta, as described later (Fig 9)

Fig 7 Activation of gp91 phox ⁄ Nox2 and Nox1 (A) Interactions

required for activation of gp91 phox ⁄ Nox2 Interactions in a resting

state are indicated by blue arrows, stimulus-induced interactions by

arrows in magenta, and constitutive interactions by green arrows.

(B) Interactions required for activation of Nox1 Interactions in a

resting state are indicated by blue arrows; and stimulus-induced

interactions by arrows in magenta T1, T2, T3 and T4,

tetratricopep-tide repeats 1, 2, 3 and 4, respectively; AD, activation domain.

Trang 11

In the resting state, the two SH3 domains of p47phox

are inaccessible to the target protein, as they are masked

via an intramolecular interaction with the C-terminally

flanking region called the autoinhibitory region (AIR)

[125,131–133] (Fig 7) During phagocytosis of invading

microbes or with soluble stimuli such as N-formyl

che-motactic peptide and PMA, p47phox undergoes

phos-phorylation at multiple Ser residues, several of which

are present in the AIR [134,135] Simultaneous

phos-phorylation of Ser303, Ser304 and Ser328 in the AIR, in

cooperation with other agonists such as arachidonicacid, induces unmasking of the SH3 domains [136]; as aresult, the bis-SH3 domain interacts with the PRR ofp22phox [125–127] The SH3-mediated interaction withp22phoxalso participates in p47phox-dependent enhance-ment of Nox3 activation [88]

The domain architecture of p47phox (PX, bis-SH3,AIR, and a p67phox-binding PRR) is conserved fromfishes to mammals (Fig 10) In addition, the genome

of the amphioxus B floridae, which belongs to the phylum Cephalochordata, a basal group of the Chor-data [96], contains the gene for p47phox (http://genome.jgi/psf.org/euk_home.html), in which proteinthe whole domain structure is duplicated (Fig 10) Thepresence of the p47phox gene in the Cephalochordataindicates that it emerged early in chordate evolution

sub-On the other hand, a typical p47phox is absent in theascidian Ci intestinalis of the Urochordata, suggestingthat the p47phoxgene has been lost in the ascidian line-age This organism contains a typical p22phox carryingthe conserved PRR [97], which may imply the presence

of its interacting protein Although Ci intestinalis hasbeen reported to possess a protein harboring a PXdomain and three SH3 domains, but lacks an AIR and

a PRR [97] (Fig 10), there is no experimental evidenceshowing that this protein participates in oxidase activa-tion The residues in the AIR that strongly interactwith the SH3 domains are all conserved in chordatep47phox proteins (Fig 11): in human p47phox, the Pro–Pro–Arg sequence at the AIR N-terminus adopts aPPII helix conformation, which is lined in the grooveformed between the tandem SH3 domains Amongthese residues, Pro199 and Pro200 undergo hydro-phobic interactions as addition to forming hydrogenbonds via their backbone carbonyl groups; Arg201contacts Asp243 and Glu244 via electrostatic inter-actions In addition, Ser303 forms a hydrogen bondwith the side chain of Glu241 (Fig 11) The PPRRSregion, however, is not sufficient to make the SH3domains inaccessible to p22phox [131]; its C-terminalextension is required for efficient masking of the SH3domains [131] Besides Ser303, Ser310 and Ser328 formhydrogen bonds with the side chains of Glu211 andArg267, respectively (Fig 11) It is known that phos-phorylation of Ser303 and Ser328 plays a crucial role

in disruption of the intramolecular interaction to vate the bis-SH3 domain [131,136] In the p47phoxautoinhibited structure, furthermore, Arg318 under-goes an electrostatic interaction with Asp261 [132],whereas Ile305 is located in a hydrophobic pocket ofSH3(N), and Tyr324 probably points into a hydro-phobic pocket formed by the linker region and SH3(C)(Fig 11) Intriguingly, the amino acids of the AIR and

acti-Fig 8 (A) A model for the structure of p22 phox and alignment of

the PRR Large asterisks indicate residues crucial for interaction

with the p47 phox bis-SH3 domain, and small asterisks denote

resi-dues involved in the interaction Hs, H sapiens; Mm, Mus

muscu-lus; Tr, Ta rubripes; Dr, Da rerio; Ci, Ci intestinalis; Bf, B floridae;

Lg, Lot gigantea; Nv, Ne vectensis; Mb, Mo brevicollis (B) The

complex structure of the p47 phox bis-SH3 domain with the p22 phox

PRR Crucial residues in the p22 phox PRR (Pro152, Pro156, and

Pro158) are drawn as red sticks Secondary structures in the

p22 phox PRR complexed with the p47 phox bis-SH3 domain are

indi-cated below the sequence of human p22 phox The figure was

drawn using PYMOL software (http://www.pymol.org) and the

Protein Data Bank coordinates 1WLP.

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SH3 domains, which are involved in the intramolecular

interaction as described above, are invariant among

vertebrate and amphioxus p47phox: the exceptions are

that Ser328 is replaced by Thr in Branchiostoma and

that Glu241 is replaced by Gln in the puffer fish

Takifugu rubripes and by Ile in amphioxus Thus,

autoinhibition of the p47phox SH3 domains and

phos-phorylation-mediated regulation are probably

con-served in p47phoxof chordates

It was recently proposed that the p47phox paralog

Noxo1 in the medaka fish Oryzias latipes retains an

AIR [94] However, it seems unlikely that this region is

functional, as fewer than a half of the crucial residues

described above are conserved in this fish Noxo1 In

addition, an AIR is absent in Noxo1 of the zebrafish

Danio rerio, which belongs to a more basal group than

medaka in the teleost fish [137], suggesting that the

AIR was lost at an early stage after branching from

the p47phoxgene

The homology between the N-termini of p47phoxand

p40phox was recognized when the p40phox cDNA was

cloned [138] It was subsequently pointed out that

p47phox exhibits a similarity to a region of the yeast

polarity protein Bem1 [139] This module of about 120

amino acids was later found to exist in a variety of

pro-teins [140,141], and was named the PX domain [140]

The PX domain of p47phoxis capable of binding to phoinositides such as phosphatidylinositol 3,4-bisphos-phate [PtdIns(3,4)P2], albeit with a relatively low affinityand specificity [142,143] In neutrophils, PtdIns(3,4)P2ispredominantly formed from phosphatidylinositol3,4,5-trisphosphate, a product of type I phosphatidyl-inositol-3-kinase (PI3K), which is activated upon cellstimulation The binding requires Arg43 and Lys90 inhuman p47phox[144–146] (Fig 12) Intriguingly, in con-trast to the complete conservation of Lys90, Arg43 isreplaced by Lys in the mouse and by Thr in the pufferfish [147] In contrast, the neighboring residue Arg42 iswell conserved; this residue is required for stability ofp47phox [12] but is not directly involved in binding tophosphoinositides [145] Like the p22phox-interactingactivity of the SH3 domains, the lipid-binding activity ofthe PX domain is negatively regulated under restingconditions [144,145] The phosphorylation-induced con-formational change of p47phox also renders the PXdomain accessible to membrane phosphoinositides Thisinteraction, in cooperation with the binding to p22phox,allows p47phox to be targeted to flavocytochrome b558,which is crucial for phagocyte oxidase activation [144]

phos-In addition to the phosphoinositide-binding pocket, the

PX domain may have a binding site for acidic lipids such as phosphatidic acid and phosphatidylserine

phospho-Fig 10 Domain structures of p47 phox and its related proteins The total numbers of amino acid residues of each protein are indi- cated on the right: human, H sapiens; zebrafish, Da rerio; ascidian, Ci intestinalis; amphioxus, B floridae.

Fig 9 Distribution of Nox2, p22 phox , p47 phox , p67phoxand p40phoxin animals and choano- flagellates M b., Mo brevicollis; N v.,

Ne vectensis; L g., Lot gigantea; C sp I, Capitella sp I; C e., Ca elegans; D m.,

Dr melanogaster; S p., S purpuratus; B f.,

B floridae; C i., Ci intestinalis; D r.,

Da rerio; X t., X tropicalis; G g., Ga gallus;

H s., H sapiens Note that it remains unclear whether p22 phox , p47 phox , p67 phox and p40 phox are present or absent in the annelid Capitella sp., because sequencing of the whole gen- ome has not been completed Amino acid sequences of p22 phox , p47 phox , p67 phox and p40phoxin the Cephalochordata B floridae are shown in supplementary Fig S1.

Trang 13

(Fig 12), which facilitates membrane binding of the PX

domain [145,148] Another lipid-binding activity may

explain well why the p47phoxPX domain participates in

membrane translocation even in the absence of the

PI3K pathway products such as PtdIns(3,4)P2 [144]

The two residues Lys55 and Arg70 in the proposed

second binding site (Fig 12) are well conserved in

chordates, suggesting a role in oxidase activation

Noxo1, the organizer for Nox1

activation

Noxo1 plays an essential role in Nox1 activation This

organizer exhibits a domain architecture similar to that

of p47phox, except that it lacks an AIR (Fig 10).Noxo1 probably tethers the activator Noxa1 to Nox1:Noxo1 functions via its PRR by interactingwith Noxa1 and via its SH3 domains by binding to theNox1 partner p22phox [106,110,111,149] In cellsexpressing Noxo1 and Noxa1, Nox1 generates super-oxide without stimulants such as PMA, a potent

in vivoactivator of gp91phox⁄ Nox2, although the oxide production is further enhanced by PMA [106].The constitutive activity of Nox1 appears to be at leastpartially due to the absence of AIR in Noxo1; henceits SH3 domains are accessible to p22phox even in theresting state, in contrast to the p47phox SH3 domains[106,115] Regulation of the Noxo1 SH3 domains may

super-be more complicated than previously expected, as theyappear to interact intramolecularly with the N-terminalPRR, albeit with low affinity [149] It is likely that thebis-SH3 domain is partly accessible to the p22phoxPRR, and this intermolecular binding is facilitated bydisruption of the intramolecular interaction with thep47phoxPRR [149]

The PX domain of Noxo1 exhibits a tide-binding activity, which is also crucial for activa-tion of Nox1 [109,150,151] In addition to its essentialrole in Nox1 activation, Noxo1 is capable of enhanc-ing Nox3-catalyzed superoxide production[88,110,114,115,152]; the enhancement requires the PXdomain [150] and the SH3-mediated interaction withp22phox[88,157]

The oxidase activator p67phox of 526 amino acidstranslocates upon cell stimulation to the membrane in

Fig 11 Intramolecular interaction of the bis-SH3 domain with the

AIR in p47phox Residues crucial for the intramolecular interaction

with the bis-SH3 domain are highlighted (upper panel) The

sequence of the AIR in human p47 phox and the consensus AIR

sequence among p47phoxproteins derived from various species are

shown (middle panel) Large asterisks indicate residues crucial for

the intramolecular interaction with the bis-SH3 domain; small

aster-isks denote residues that play a role in the interaction Secondary

structure elements of the p67phox-binding region in p47phoxare

indi-cated below the sequence The three Ser residues Ser303, Ser310

and Ser328 directly interact with residues in the bis-SH3 domain

(Gle241, Glu211, and Arg267, respectively) (lower panel) The

figures were drawn using PYMOL software (http://www.pymol.org)

and the Protein Data Bank coordinates 1UEC.

Fig 12 Lipid-binding sites in the p47 phox PX domain Residues in the phosphoinositide-binding and second anion-binding pockets are shown in blue The sulfates bound in the two pockets (in a crystal

of the p47 phox PX domain [145]) are colored magenta The figure was drawn using PYMOL software (http://www.pymol.org) and the Protein Data Bank coordinates 1O7K.

Trang 14

a manner dependent on p47phox p67phox contains two

SH3 domains (Fig 7A), both of which play a role in

activation of the phagocyte NADPH oxidase [153]

Although the N-terminal (the first) SH3 domain is the

most conserved region in p67phox [154], it is unknown

how this module functions The C-terminal SH3

domain participates in membrane translocation of

p67phox by specifically binding to the C-terminal PRR

of p47phoxwith high affinity [155–157] The high

affin-ity and specificaffin-ity are achieved by the following

mecha-nism: in addition to the canonical PxxP binding site of

p67-SH3(C), which is occupied by the eight PRR

resi-dues of p47phox (Gln362–Pro369), which adopt a PPII

helix conformation (Fig 13), p67-SH3(C) makes direct

contacts with the remaining C-terminal segment of the

p47phox tail, which comprises two a-helices (Asp372–

Asn376 and Glu380–Ser386), linked by a turn of

Arg377–Ser379 [157] (Fig 13) Structural analysis and

comparison of p47phox proteins from various species

reveal the consensus sequence xPxøPxRP(S⁄

A)xxøIL-xRC(S⁄ T)xxT(K ⁄ R)(R ⁄ K)xØ, where x is any amino

acid and Ø is a hydrophobic residue (Fig 13) The

res-idue adjacent to the invariant Cys is a Ser or a Thr;

the corresponding residue in human p47phox(Ser379) isknown to undergo phosphorylation during cell stimu-lation [158] This phosphorylation attenuates the bind-ing to p67phox [158], and thus negatively regulatesoxidase activation [159]

The consensus sequence is also conserved in theC-terminal region of Noxo1, which is capable of inter-acting with p67phox as well as with Noxa1 [106] Theinteraction of the Noxa1 SH3 domain with the Noxo1PPR (Fig 7B) plays an important role in both mem-brane localization of Noxa1 and activation of Nox1[110,111]

Rac, a member of the Rho-family small GTPases,plays an essential role in gp91phox⁄ Nox2 activation[160–162] Among phagocytes, human neutrophils pre-dominantly express Rac2, whereas both Rac1 andRac2 are present in monocytes⁄ macrophages Apatient with abnormal neutrophil function was shown

to have an inhibitory (dominant-negative) mutation inRac2, resulting in decreased oxidase activity and otherneutrophil function defects [163,164] Upon cell stimu-lation, Rac is recruited to the membrane independently

of p47phox or p67phox The recruitment requires nylgeranylation of Cys189 at the C-terminus At themembrane, Rac is converted to the GTP-bound activeform via the function of guanine nucleotide-releasingfactors Rac in the GTP-bound form directly interactswith the p67phoxN-terminal region of about 200 aminoacids, which is crucial for activation of gp91phox[165,166] On the other hand, Cdc42 neither binds top67phoxnor activates gp91phox

gera-In the Rac-binding region, four tetratricopeptiderepeat (TPR) motifs are found (Fig 14): TPR motifsare degenerate 34 amino acid repeats that are present

in a variety of organisms, ranging from bacteria tohumans, and are involved in a variety of protein–pro-tein interactions [167] The TPR domain of p67phoxcontains an insertion of 19 amino acids between thea-helices of TPR3 and TPR4: the insertion containstwo short antiparallel b-strands and a 310helical turn[168,169], with the consensus sequence of LRGNxøID-YxxLGøx(Y⁄ F)KLx, where x is any amino acid and Ø

is a hydrophobic residue (Fig 14) The b-hairpin tion and the loops connecting TPR1 and TPR2, andTPR2 and TPR3, create the binding surface for Rac[168] (Fig 14) The invariant Arg in the b-hairpin(position 32 of TPR3; Arg102 in human p67phox) plays

inser-a key role in complex forminser-ation with Rinser-ac inser-and oxidinser-aseactivation, and the side chain of this residue undergoesdirect hydrogen bonding interactions with main and

Fig 13 Interaction of the p67phoxC-terminal SH3 domain with the

p47 phox C-terminus (A) Ribbon diagram of the structure of the

com-plex of the p67 phox C-terminal SH3 domain with the p47 phox

C-ter-minal region Residues involved in binding to the SH3 domains are

drawn as red sticks (residues in the PPII helix) or magenta sticks

(residues in the a-helices) The figure was drawn using PYMOL

software (http://www.pymol.org) and the Protein Data Bank

coordi-nates 1K4U (B) Secondary structure elements of the p67 phox

-bind-ing region in p47 phox are indicated below the sequence Asterisks

indicate residues crucial for interaction with p67 phox ; the dot

denotes Ser379, which becomes phosphorylated upon cell

stimu-lation.

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