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Hydrolysis of diadenosine polyphosphates by nucleotide pyrophosphatases/phosphodiesterases Petra Vollmayer 1 , Timothy Clair 2 , James W. Goding 3 , Kimihiko Sano 4 ,Jo¨ rg Servos 1 and Herbert Zimmermann 1 1 AK Neurochemie, Biozentrum der J. W. Goethe-Universitaet, Frankfurt am Main, Germany; 2 Laboratory of Pathology, NCI, National Institutes of Health, Bethesda, Maryland, USA; 3 Department of Pathology and Immunology, Monash University, Alfred Hospital, Prahran, Victoria, Australia; 4 Department of Pediatrics, Kobe University School of Medicine, Kobe, Japan Diadenosine polyphosphates (Ap n As) act as extracellular signaling molecules in a broad variety of tissues. They were shown to be hydrolyzed by surface-located enzymes in an asymmetric manner, generating AMP and Ap n-1 from Ap n A. The molecular identity of the enzymes responsible remains unclear. We analyzed the potential of NPP1, NPP2, and NPP3, the three members of the ecto-nucleotide pyro- phosphatase/phosphodiesterase family, to hydrolyze the diadenosine polyphosphates diadenosine 5¢,5¢¢¢-P 1 ,P 3 - triphosphate (Ap 3 A), diadenosine 5¢,5¢¢¢-P 1 ,P 4 -tetraphos- phate (Ap 4 A), and diadenosine 5¢,5¢¢ ¢-P 1 ,P 5 -pentaphosphate, (Ap 5 A), and the diguanosine polyphosphate, diguanosine 5¢,5¢¢¢-P 1 ,P 4 -tetraphosphate (Gp 4 G). Each of the three enzymes hydrolyzed Ap 3 A, Ap 4 A, and Ap 5 A at comparable rates. Gp 4 G was hydrolyzed by NPP1 and NPP2 at rates similar to Ap 4 A,butonlyathalfthisratebyNPP3. Hydrolysis was asymmetric, involving the a,b-pyrophos- phate bond. Ap n A hydrolysis had a very alkaline pH opti- mum and was inhibited by EDTA. Michaelis constant (K m ) values for Ap 3 Awere5.1l M ,8.0l M , and 49.5 l M for NPP1, NPP2, and NPP3, respectively. Our results suggest that NPP1, NPP2, and NPP3 are major enzyme candidates for the hydrolysis of extracellular diadenosine polyphos- phates in vertebrate tissues. Keywords: diadenosine polyphosphate; diguanosine poly- phosphate; ectonucleotidase; nucleotide pyrophosphatase; nucleotide phosphodiesterase. Diadenosine polyphosphates [adenosine-(5¢)-oligophospho- (5¢)-adenosines, Ap n As] comprise two adenosine residues linked together by a polyphosphate chain through phos- phoester bonds at their ribose 5¢ carbons. Ap n As are present intracellularly in prokaryotic and eukaryotic cells [1]. Recently, this group of nucleotides has attracted consider- able interest because its members act as extracellular signaling molecules in a broad variety of tissues [2,3]. They are involved, for example, in the modulation of synaptic transmission and sensory nerve function [2–4], inhibition of platelet aggregation [5], or in the control of vascular tone [6–9]. Vasoactive effects were also observed with adenosine polyphosphoguanosines (Ap n Gs) and diguanosine poly- phosphates (Gp n Gs) [10]. The diadenosine polyphosphates diadenosine 5¢,5¢¢¢-P 1 ,P 3 -triphosphate (Ap 3 A), diadenosine 5¢,5¢¢¢-P 1 ,P 4 - tetraphosphate (Ap 4 A), and diadenosine 5¢,5¢¢¢-P 1 ,P 5 -pen- taphosphate (Ap 5 A) are stored in chromaffin granules at millimolar concentrations together with noradrenaline and other nucleotides such as ATP and ADP [11,12]. In cholinergic synaptic vesicles, Ap 4 AandAp 5 A were found to be co-stored with acetylcholine [13]. They can be released from secretory cells in a stimulus-dependent manner [2]. Besides the adrenal medulla, platelets are thought to represent the main source of Ap n As in blood. Stimulated platelets release, from their storage granules, a mixture of Ap n As(uptoAp 7 A),aswellasAp n Gs and Gp n Gs, together with ATP, ADP and serotonin [14,15]. Ap n As exert their function via ionotropic (P2X) or metabotropic (P2Y) receptors for mononucleotides, or also via P1 adenosine receptors [3,16]. In addition, Ap n As may act on a separate group of receptors, termed dinucleotide receptors or P4 receptors [2,3,17]. In vertebrate tissues, extracellular Ap n As were shown to be metabolized and thus functionally inactivated by enzymes associated with the cell surface or present in body fluids [18]. Primary cleavage of Ap n As is asym- metric, generating AMP and Ap n-1 from Ap n A. Cellular systems analyzed include blood [19], the adrenal medulla Correspondence to H. Zimmermann, AK Neurochemie, Biozentrum der J.W. Goethe-Universitaet, Marie-Curie-Str. 9, D-60439 Frankfurt am Main, Germany. Fax: + 49 69 79829606, Tel.: + 49 69 79829602, E-mail: h.zimmermann@zoology.uni-frankfurt.de Abbreviations:Ap 4 , adenosine tetraphosphate; Ap 3 A, diadenosine 5¢,5¢¢¢-P 1 ,P 3 -triphosphate; Ap 4 A, diadenosine 5¢,5¢¢¢-P 1 ,P 4 -tetraphos- phate; Ap 5 A, diadenosine 5¢,5¢¢¢-P 1 ,P 5 -pentaphosphate; Ap n A, diadenosine polyphosphate (adenosine-(5¢)-oligophospho-(5¢)-adeno- sine); CHO, Chinese hamster ovary; E-NPP, ecto-nucleotide pyrophosphatase/phosphodiesterase; Gp 4 G, diguanosine 5¢,5¢¢¢-P 1 ,P 4 - tetraphosphate; pNP-TMP, p-nitrophenyl thymidine 5¢ monophos- phate; PC-1, plasma-cell differentiation antigen-1; PPADS, pyridoxal phosphate-6-azophenyl-2¢,4¢-disulfonic acid. Enzyme: nucleotide pyrophosphatase/phosphodiesterase (EC 3.1.4.1 or EC 3.6.1.9) (Received 20 March 2003, revised 29 April 2003, accepted 15 May 2003) Eur. J. Biochem. 270, 2971–2978 (2003) Ó FEBS 2003 doi:10.1046/j.1432-1033.2003.03674.x [20], vascular endothelial cells [21,22], synaptic membranes [23,24], airway epithelia [25], and Xenopus oocytes [26]. At present, little is known concerning the molecular identity of the enzymes involved. One group of enzymes with the potential to hydrolyze Ap n As are NPP1, NPP2, and NPP3, the three members of the ecto-nucleotide pyrophosphatase/phosphodiesterase (E-NPP) family (revised nomenclature) [27,28]. They reveal a surprisingly broad substrate specificity and are capable of hydrolyzing phosphodiester bonds of nucleotides and nucleic acids, and pyrophosphate bonds of nucleotides and nucleotide sugars, resulting in the release of nucleoside 5¢ monophosphates. Both purine and pyrimidine nucleotides are hydrolyzed. Substrates include ATP, NAD + ,andp-nitrophenyl thymi- dine 5¢ monophosphate (pNP-TMP) [29–31]. To date, three related mammalian NPPs have been cloned and function- ally characterized: NPP1 (plasma-cell differentiation anti- gen-1, PC-1) [32]; NPP2 (autotaxin) [33] and its splice variant, PD-Ia [34]; and NPP3 (gp130 RB13)6 , B10, PD-Ib) [35–37]. NPP1 and NPP3 share 50% amino acid identity and are more distantly related to NPP2 (39–41% identity). They have a broad and partially overlapping tissue distri- bution and may be co-localized within the same cell [37]. All can exist as integral glycoproteins (of  120 kDa) of the plasma membrane. They are disulfide-linked homodimers representing type II membrane proteins [18,29,30]. In addition, active soluble forms have been identified that presumably result from specific proteolytic cleavage near the transmembrane domain [38–40]. We analyzed the potential of heterologously expressed NPP1, NPP2, and NPP3 to hydrolyze the diadenosine polyphosphates Ap 3 A, Ap 4 AandAp 5 A, and the diguano- sine polyphosphate Gp 4 G.InthecaseofNPP1andNPP3, the membrane-bound form of the enzyme was analyzed, whereas, in the case of NPP2 (autotaxin), which was shown to promote cell motility in its soluble form [38], the soluble form was employed. Experimental procedures Materials Culture medium and genectin G-418 sulfate were obtained from Invitrogen (Karlsruhe, Germany). All nucleotides, penicillin, streptomycin, sodium butyrate, Cibacron Blue, suramin, heparin, heparan sulfate, benzamidine, and pyridoxal phosphate-6-azophenyl-2¢,4¢-disulphonic acid (PPADS) were obtained from Sigma-Aldrich (Deisenhofen, Germany). Leupeptin, pepstatin A, chymostatin, and anti- pain were from Calbiochem (Schwalbach, Germany), and aprotinin was from Roche (Mannheim, Germany). Cell culture and cell transfection Chinese hamster ovary (CHO) cells were cultured in HAM’s F-12 medium containing 10% fetal bovine serum, 100 UÆmL )1 penicillin and 100 lgÆmL )1 streptomycin. They were transfected by electroporation [41] with plasmid DNA containing human NPP1 (NPP1pSVT7) [42] or rat NPP3 (GenBank TM accession number D30649; NPP3pcDNA3). Transfection with the empty plasmid pSVT7 or pcDNA3 served as a control. Stable transfectants for NPP3 were selected for neomycin resistance using 800 lgÆmL )1 of genectin G-418 sulfate (Invitrogen) and subcloned by limiting dilution. Stably transfected cells were cultured in the presence of 750 lgofgenectinG-418sulfatepermLof culture medium. Sodium butyrate (6 m M )wasaddedtothe culture medium of stably transfected cells 16 h before preparation of membrane fractions or analysis of cell surface-located enzyme activity. Preparation of membrane fractions Transiently or stably transfected CHO cells were cultured in 150 · 25 mm culture dishes and membrane fractions were prepared 48 h after electroporation or 16 h after stimulation with sodium butyrate, respectively. After removal of culture medium, cells were washed twice with buffer A (140 m M NaCl, 5 m M KCl, 20 m M Hepes, pH 8.5), scraped off with 5 mL of ice-cold buffer A containing protease inhibitors (chymostatin, 2 lgÆmL )1 ;pepstatinA,1lgÆmL )1 ;benz- amidine, 1 m M ; antipain, 2 lgÆmL )1 ; aprotinin, 2 lgÆmL )1 ; leupeptin, 2 lgÆmL )1 ), and centrifuged (300 g for 5 min at 4 °C). Cells were homogenized in buffer A using a Potter– Elvehjem homogenizer and sonicated. The homogenate was then centrifuged (10 min at 825 g at 4 °C). The resulting supernatant fraction was centrifuged (100 000 g for 45 min at 4 °C) and the pellets were resuspended in protease inhibitor-containing buffer A prior to storage at )20 °C. Protein was determined according to the method of Peterson [43]. Measurement of nucleotide hydrolysis The hydrolysis of substrates Ap 3 A, Ap 4 A, Ap 5 Aand Gp 4 G was analyzed using membrane fractions containing heterologously expressed NPP1 and NPP3, or the soluble form of recombinant human NPP2. NPP2 was prepared and isolated from a vaccinia virus lysate of BS-C-1 cells, as described previously, through the concanavalin A–agarose step [44], and stored in a solution containing 50 m M Tris, pH 7.5, 100 m M NaCl, 10 m M CaCl 2 ,and 20% (v/v) ethylene glycol. Membrane fractions of mock- transfected cells (NPP1, NPP3) or storage solution (NPP2) served as controls. Hydrolysis was determined at 37 °C in buffer A (NPP1, NPP3) or buffer B (NPP2, 25 m M Tris/25 m M glycine, pH 9.0, 140 m M NaCl, 5 m M KCl, containing 500 lgÆmL )1 bovine serum albumin). Unless stated otherwise, CaCl 2 and MgCl 2 were added to the assay medium at a concentration of 1 m M .The reaction was started by addition of substrate and termin- ated by heat inactivation (95 °C for 4 min). Nucleotides were separated and quantified by HPLC. Samples were first centrifuged (20 min, 14 500 g,4°C) and then diluted with ultrapure water or buffer A. An aliquot was injected into a Sepsil C 18 reversed-phase column (Jasco, Grob- Umstadt, Germany) and eluted at 1.0 mLÆmin )1 with the mobile phase consisting of 50 m M potassium-phosphate buffer (pH 6.4), 5 m M tetrabutylammonium hydrogen sulfate and 10–18% methanol, depending on the nucleo- tide analyzed. The absorbance at 260 nm was continu- ously monitored and the nucleotide concentrations were determined from the area under the absorbance peaks. Hydrolysis rates represent initial rates. 2972 P. Vollmayer et al. (Eur. J. Biochem. 270) Ó FEBS 2003 pH dependence, ion dependence, and inhibitors Two different buffer systems were applied for analyzing pH dependence of Ap 3 A hydrolysis. For analysis from pH 6.0 to 7.5, a buffer solution containing 25 m M Hepes, 25 m M glycine, 140 m M NaCl, and 5 m M KClwasused.For analysis from pH 7.5–11.0, the buffer solution consisted of 25 m M Tris, 25 m M glycine, 140 m M NaCl, and 5 m M KCl. In these experiments the substrate concentration was 200 l M Ap 3 A for NPP1 and NPP3, and 2 m M for NPP2. The rate of the Ap 3 A hydrolysis in the presence of divalent metal cations was analyzed in buffer A (NPP1, NPP3) or buffer B (NPP2) containing 2 m M CaCl 2 ,2m M MgCl 2 , 2m M CaCl 2 and 2 m M MgCl 2 , or 500 l M EDTA. Because the storage solution of NPP2 contained CaCl 2 ,150l M EGTA was added to the solution containing 2 m M MgCl 2 . The substrate concentration was 200 l M Ap 3 AforNPP1, NPP2 and NPP3 1 . The inhibitory effect on Ap 4 Ahydrolysis of the following compounds was analyzed: PPADS; Ciba- cron Blue; suramin (all 100 l M ); NaF (500 l M ); heparin (0.1 mgÆmL )1 ), and heparan sulfate (0.1 mgÆmL )1 ). Enzymes were preincubated with the inhibitor for 10 min at 37 °C followed by addition of substrate at a final concentration of 200 l M . Analysis of cell surface-located catalytic activity For analysis of surface-located enzyme activity, CHO cells transiently transfected with NPP1 were seeded, 24 h after electroporation, in six-well plates (5 · 10 5 cells per well, 9.08 cm 2 ) and analyzed after an additional 24 h. Stably transfected CHO cells (NPP3) were seeded at a density of 2.5 · 10 5 cells per well and analyzed 2 days after seeding. Cells were washed twice with phosphate-free saline solution (140 m M NaCl, 5 m M KCl, 10 m M glucose, 20 m M Hepes, pH 7.4) and subsequently incubated for 60 min at 37 °Cin 1 mL of identical saline solution containing 200 l M of the substrate nucleotide, 1 m M MgCl 2 and 1 m M CaCl 2 .The physiological saline solution collected from the cultures was heat inactivated (95 °C for 4 min), followed by centrifuga- tion (14 500 g for 20 min). Aliquots of the supernatant were subjected to nucleotide analysis as described above. Results General biochemical properties of Ap n A hydrolysis by NPPs As members of the NPP family have been reported to share a strongly alkaline pH optimum [18,29], we first determined the pH dependence, using Ap 3 A as a substrate. Membrane fractions containing heterologously expressed NPP1 and NPP3 and soluble NPP2 revealed an alkaline pH optimum for the hydrolysis of Ap 3 A. The pH optimum was between 8.5 and 9.0 for NPP1 and NPP3 and pH 10 for NPP2 (n ¼ 2–3). At the physiological pH of 7.4, the hydrolysis rates for NPP1, NPP2, and NPP3 were approximately 10%, 15% and 30%, respectively, of maximal activity. In the following we analyzed the catalytic activity of NPP1 and NPP3 at pH 8.5 and that of NPP2 at pH 9. No diadenosine polyphosphate hydrolysis was detected in isolated membrane fractions or at the surface of mock-transfected CHO cells. Hydrolysis of Ap 3 A by NPP1- and NPP3-containing membrane fractions and by soluble NPP2 was determined in the presence of 2 m M CaCl 2 ,2m M MgCl 2 ,2m M CaCl 2 plus 2 m M MgCl 2 2 ,or500l M EDTA. As shown in 2 Fig. 1, the catalytic rates were similar in the presence of Ca 2+ or Mg 2+ . Activity was not further stimulated by the simultaneous addition of Ca 2+ and Mg 2+ , while EDTA greatly reduced the catalytic activity. In the following, catalytic activity was measured in the presence of 1 m M CaCl 2 and 1 m M MgCl 2 . Michaelis constant (K m )values were calculated from Lineweaver–Burk plots for Ap 3 Aas a substrate. Substrate concentrations tested ranged from 1 to 400 l M .TheK m and maximal rate (V max )values corresponded, respectively, to 5.1 ± 3.6 l M and 25.8 ± 11.3 nmolÆmin )1 Æmg protein )1 (n ¼ 3) for NPP1, 49.5 ± 17.7 l M and 153.7 ± 41.6 nmolÆmin )1 Æmg pro- tein )1 (n ¼ 4) for NPP3, and 8.0 ± 0.5 l M and 8.6 ± 0.8 nmolÆmin )1 ÆmL )1 (n ¼ 2) for NPP2. Substrate specificity and product pattern We subsequently analyzed the ability of NPP1 to NPP3 to hydrolyze various dinucleoside polyphosphates and determined the pattern of product formation. In order to avoid potential product inhibition, the enzyme concen- tration was adjusted to obtain low catalysis rates. Table 1 compares the hydrolysis rates of the three enzymes for the dinucleotides investigated. For each of the enzymes, catalyticrateswerenormalizedtothesubstrateAp 4 A. In the case of NPP1 and NPP3, substrates were added to the surface of transfected intact and viable cells, or to membrane fractions obtained from transfected cells. Ap 3 A, Ap 4 AandAp 5 A were hydrolyzed by each of the three enzymes at similar rates, and similar results were obtained with viable cells and membrane fractions. To investigate whether hydrolysis was restricted to diadenosine polyphosphates, we also analyzed the Fig. 1. Effect of divalent cations on the hydrolysis of diadenosine 5¢,5¢¢¢- P 1 ,P 3 -triphosphate (Ap 3 A) by NPP1, NPP2, and NPP3. Membrane fractions derived from CHO cells containing heterologously expressed NPP1 or NPP3, and soluble NPP2, were analyzed in the presence of 2m M CaCl 2 ,2m M MgCl 2 ,2m M CaCl 2 plus 2 m M MgCl 2 ,or500l M EDTA. In the case of NPP2, 150 l M EGTA was added to the 2 m M MgCl 2 -containing solution to chelate CaCl 2 contained in the storage solution. Substrate concentrations were 200 l M . The 100% values correspond to 9.3 ± 1.0 nmolÆmin )1 Æmg protein )1 (NPP1), 13.7 ± 0.2 nmolÆmin )1 ÆmL )1 (NPP2), and 26.6 ± 11.0 nmolÆmin )1 Æmg pro- tein )1 (NPP3). Values represent means ± SD of three experiments with duplicate determinations in each (NPP1, NPP3) or mean values ± range of two experiments (NPP2). Ó FEBS 2003 Hydrolysis of diadenosine polyphosphates (Eur. J. Biochem. 270) 2973 hydrolysis of diguanosine polyphosphates, choosing Gp 4 G as an example. Gp 4 G was hydrolyzed by NPP1 and NPP2 at rates similar to Ap 4 A, but only at half this rate by NPP3. Ap 3 A, Ap 4 AandAp 5 A were asymmetrically cleaved by all three members of the E-NPP family. Figure 2 shows representative HPLC profiles obtained with sol- uble NPP2, or with NPP1 or NPP3 following substrate application to the surface of transfected or mock- transfected cells. Mock-controls revealed no significant substrate hydrolysis. Ap 3 A was hydrolyzed to ADP and AMP, Ap 4 AtoATPandAMP,andAp 5 AtoAp 4 and AMP. Similarly, Gp 4 G was hydrolyzed to GTP and GMP (results not shown). Differential effect of inhibitors We further investigated the possibility that the enzymes differ regarding their sensitivity to potential inhibitors that have previously been reported to affect hydrolysis of diadenosine polyphosphates [18]. Ap 4 A(200l M )was chosen as the substrate (Fig. 3). Cibacron Blue (100 l M ) strongly inhibited the hydrolysis of Ap 4 Abyallthree enzymes. PPADS, at 100 l M , inhibited the hydrolysis of Table 1. Substrate preference of NPP1, NPP2 and NPP3. Activity was determined at the surface of viable and transfected CHO cells or using membrane fractions derived from transfected CHO cells (NPP1 and NPP3), or using soluble NPP2. Experiments were performed in the presence of 1m M CaCl 2 and 1 m M MgCl 2 . Substrate concentrations were 200 l M . Values are expressed relative to Ap 4 A hydrolysis. Absolute hydrolysis rates for Ap 4 A were 539 ± 278 pmolÆmin )1 Æ10 6 cells and 16.8 ± 12.1 nmolÆmin )1 Æmg protein )1 (NPP1, surface activity and activity of membrane fractions, respectively), 781.7 ± 193 pmolÆmin )1 Æ10 6 cells and 33.5 ± 10.6 nmolÆmin )1 Æmg protein )1 (NPP3, surface activity and activity of membrane fractions, respectively) and 15.6 ± 0.3 nmolÆmin )1 ÆmL )1 (NPP2). Values represent means ± SD of three experiments with duplicate determinations in each (NPP1, NPP3) or mean values ± range of two experiments (NPP2). ND, not determined. Substrate NPP1 (relative rate) NPP2 (relative rate) NPP3 (relative rate) Cell surface Membrane fraction Soluble Cell surface Membrane fraction Ap 4 A1 1 1 1 1 Ap 3 A 1.21 ± 0.03 1.06 ± 0.05 1.02 ± 0.02 1.19 ± 0.03 1.31 ± 0.08 Ap 5 A 0.98 ± 0.07 1.20 ± 0.13 1.07 ± 0.01 1.05 ± 0.05 1.54 ± 0.17 Gp 4 G ND 1.20 ± 0.20 1.14 ± 0.01 ND 0.45 ± 0.01 Fig. 2. Hydrolysis of diadenosine polyphosphates and product formation by heterologously expressed NPP1, NPP2 and NPP3. NPP1 and NPP3 were analyzed after expression in CHO cells. The substrates Ap 3 A, Ap 4 AandAp 5 A were applied for 60 min to the surface of either mock-transfected cells (control) or to the surface of transfected cells. In the case of NPP2, either storage buffer alone (control) or storage buffer containing the soluble enzyme were analyzed (120 min). Experiments were performed in the presence of substrate (200 l M ), 1 m M CaCl 2 and 1 m M MgCl 2 . Substrate hydrolysis and product formation were determined by HPLC. Absorbance was measured at 260 nm. AU, arbitrary units. 2974 P. Vollmayer et al. (Eur. J. Biochem. 270) Ó FEBS 2003 Ap 4 A by NPP1 and NPP3 by 82–88%, but was much less effective on NPP2 (42% inhibition). Whereas NPP1 and NPP2 were inhibited by suramin (100 l M ) by about 70% and 77%, respectively, NPP3 was not affected. Heparin and heparan sulfate inhibited NPP1 by 22%. No inhibition was obtained with NaF (500 l M ). Discussion A direct comparison of all three heterologously expressed members of the E-NPP family revealed that they are capable of hydrolyzing the diadenosine polyphosphates Ap 3 Ato Ap 5 A. This was true both for the membrane-bound enzymes NPP1 and NPP3 and for the soluble NPP2. In addition, all three enzymes hydrolyzed Gp 4 G. This suggests that they are generally capable of hydrolyzing physiologically released dinucleoside polyphosphates, including the vasoactive adenosine polyphosphoguanosines and diguanosine poly- phosphates [10]. Hydrolysis was asymmetric and involved the a,b-pyrophosphate bond, resulting in the production of AMP and Ap n-1 as the primary hydrolysis products. Hydrolysis of Ap n As had a very alkaline pH optimum, comparable to that of alkaline phosphatases [18]. Dinucleo- tide hydrolysis was inhibited by the divalent metal cation chelator, EDTA, as previously described for other substrates of the enzymes [29,30]. K m values for NPP1, NPP2 and NPP3 were in the low micromolar range for Ap 3 Aasa substrate. NPP2 (autotaxin) appears to be the most versatile member of the enzyme family. Two recent publications reported that it also exerts lysophospholipase D activity [45,46]. The K m value for lysophosphatidylcholine was found to be  250 l M . This is 30 times higher than that of NPP2 for Ap 3 A (present data). In contrast to NPP2, NPP1 and NPP3 do not display phospholipase D activity [47]. The general catalytic properties of the heterologously expressed E-NPPs compare well with previous data describing the hydrolysis of diadenosine polyphosphates in the blood or in association with the surface of cells [18], suggesting that members of the E-NPP family represent a major group of Ap n A-hydrolyzing enzymes in mammalian tissues. From the data available it is, however, difficult to conclude which of the isoenzymes has previously been characterized. The low K m value (8 l M ,Ap 4 A) dinucleoside tetraphosphatase isolated from rat liver [48] shares its general functional properties with members of the E-NPP family. As NPP1, NPP2, and NPP3 are all expressed in liver [49] it is difficult to assign the functional properties of the enzyme fraction identified to a specific member of the E-NPP family. Ap 3 AandAp 4 A are hydrolyzed asymmet- rically by human plasma, and an enzyme chromatographing at 230 kDa, with properties very similar to those of NPP1, has been purified from plasma [50]. In human serum, three isoenzymes splitting Ap 4 AandAp 3 A have been identified, with K m values for Ap 4 A in the range of 2–10 l M [51]. These isoenzymes may relate to the isoforms of the E-NPP family present in serum [18]. In contrast to ATP, Ap n As are not hydrolyzed by intact blood cells [19]. Cultured bovine chromaffin cells degrade members of the diadenosine polyphosphate family from Ap 3 AtoAp 6 A [2,20]. The pH optimum is in the alkaline range (8.5–9.0), and K m values are in the order of 2–4 l M . A partially purified enzyme isolated from bovine adrenal medullary plasma membranes co-chromatographed with a protein immunoreactive for an anti-NPP1 immunoglobulin [52], suggesting that NPP1 is mainly responsible for diadenosine polyphosphate hydrolysis in these cells. The K m value for Ap 4 A was determined as 2 l M and relates closely to the value obtained for Ap 3 A and recombinant NPP1 in this study. A partially purified alkaline phosphodiesterase from rat C6 glioma cells was found to hydrolyze Ap 4 A, Gp 4 G and NAD + , compatible with the catalytic properties of NPP1 [53]. Human airway epithelia contain mRNA enco- ding all three forms of NPPs [54]. Diadenosine polyphos- phates applied to the apical epithelial surface were hydrolyzed, as would be expected for NPPs, but catalytic activities cannot be assigned to an individual enzyme. Not all Ap n A-hydrolyzing enzymes described share the catalytic properties of NPPs. Whereas the diadenosine polyphosphate hydrolase activity in the blood [50], in synaptic membranes from the Torpedo electric organ, or on chromaffin cells are activated by Ca 2+ ions, the enzyme on cultured endothelial cells is inhibited by Ca 2+ [21,22]. The enzyme from adrenomedullary vascular endothelial cells also has a considerably lower K m for Ap n As (0.4 l M )than the NPPs and – in contrast to NPPs – is effectively inhibited by fluoride [22]. This implies the occurrence of Ap n A hydrolases unrelated to the presently identified members of the E-NPP family. Also unexplained is the release of Ap n A- hydrolyzing enzyme activity by phosphatidyl inositol-speci- fic phospholipase C, suggesting membrane anchorage via a glycosylphosphatidyl inositol-anchor [20,55–57]. Hydrolysis of Ap n As by the three expressed NPPs can be affected differentially by inhibitors. The non-specific P2 receptor inhibitor, Cibacron Blue, inhibits all enzymes to a similar extent. In contrast, PPADS, a frequently applied inhibitor of P2 receptors [16], has a considerably stronger inhibitory effect on NPP1 and NPP3 than on NPP2. Suramin inhibits only NPP1 and NPP2. This suggests that Fig. 3. Effect of inhibitors on hydrolysis of Ap 4 A by NPP1, NPP2, and NPP3. PPADS, Cibacron Blue, suramin (all 100 l M ), NaF (500 l M ), heparin, and heparan sulfate (both 0.1 mgÆmL )1 ) were applied at an Ap 4 A concentration of 200 l M . The 100% values correspond to 64.6 ± 16.1 nmolÆmin )1 Æmg protein )1 (NPP1), 12.3 ± 0.3 nmolÆ min )1 ÆmL )1 (NPP2), and 109.0 ± 24.4 nmolÆmin )1 Æmg protein )1 (NPP3). Values represent means ± SD of three experiments with triplicatedeterminationsineach(NPP1)ormeanvalues±rangeof two experiments with triplicate determinations in each (NPP2, NPP3). Ó FEBS 2003 Hydrolysis of diadenosine polyphosphates (Eur. J. Biochem. 270) 2975 differential inhibition by PPADS and suramin can be used to assign Ap n A hydrolysis in individual tissues to defined members of the E-NPP family. It should also be noted that application of these P2 receptor inhibitors will potentially obscure pharmacological experiments in which the effect of Ap n As on P2 receptors are investigated – because Ap n A hydrolysis and P2 receptors are simultaneously blocked. PPADS and, in particular, suramin, are effective inhibitors of ecto-Ap n AhydrolasefromTorpedo synaptic membranes [58], suggesting that this enzyme is related to NPP1. Submilligram quantities of heparin or heparan sulfate inhibit strongly the hydrolysis of pNP-TMP and, to a lesser extent, ATP hydrolysis by NPP1 endogenously expressed by Jurkat T cells [59]. We found only a small effect on Ap 4 A hydrolysis by heterologously expressed NPP1, suggesting that the hydrolysis of individual substrates may be differ- entially affected by the glycosaminoglycans. Taken together, all three functionally characterized members of the E-NPP family are capable of hydrolyzing dinucleoside polyphosphates. They comprise a versatile group of enzymes with a broad substrate specificity. In this sense they resemble intracellular dinucleoside polyphos- phate-hydrolyzing enzymes (Nudix hydrolases), unrelated to members of the E-NPP family, that reveal a comparably broad substrate specificity, including dinucleoside poly- phosphates, nucleoside triphosphates, nucleotide sugars, NADH and coenzyme A [60]. Our results suggest that NPP1, NPP2, and NPP3 are major enzyme candidates for the hydrolysis of extracellular dinucleoside polyphosphates released in vertebrate tissues. Acknowledgements This work was supported by grants from the Deutsche Forschungs- gemeinschaft (SFB 269, A4), from the Foerderfonds der Chemischen Industrie (to H. Zimmermann) and by the National Health and Medical Research Council of Australia (to J. W. Goding). References 1. McLennan, A.G. (1992) Ap 4 A and Other Dinucleoside Polyphos- phates. CRC Press, Boca Raton. 2. Miras-Portugal, M.T., Gualix, J., Mateo, J., Dı ´ az-Herna ´ ndez, M., Go ´ mez-Villafuertes, R., Castro, E. & Pintor, J. 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