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Abstract:

A new diMn III complex, Na[Mn 2(3-Me-5-SO 3-salpentO)(μ-MeO)(μ-AcO)(H 2O)]•4H 2O (1), where salpentOH = 1,5-bis(salicylidenamino) pentan-3-ol, was synthesized and structurally characterized. The complex possesses a bis(μ-alkoxo)(μ-acetato) triply bridged diMn III core, the structure of which is retained upon dissolution. Complex 1 is highly efficient to disproportionate H 2O 2 in an aqueous solution of pH ≥ 8.5 or in DMF, with only a slight decrease of activity. Electrospray ionization mass spectrometry, EPR, and UV-vis spectroscopy used to monitor the H 2O 2 disproportionation in buffered basic medium, suggest that the major active form of the catalyst during cycling occurs in the Mn III 2 oxidation state and that the starting complex retains the dinuclearity and composition during catalysis, with the acetate that moves from bridging to terminal ligand. UV-vis and Raman spectroscopy of H 2O 2 + 1 + Bu 4NOH mixtures in DMF suggest that the catalytic cycle involves Mn III 2/Mn IV 2 oxidation levels. At pH 10.6 in an Et 3N/Et 3NH + buffer, complex 1 catalyzes dismutation of H 2O 2 with saturation kinetics on the substrate, first order dependence on the catalyst, and k cat/K M = 16(1) ×10 2 s -1 M -1. During catalysis, the exogenous base contributes to retain the integrity of the bis(μ-alkoxo) doubly bridged diMn core and favors the formation of the catalyst-peroxide adduct (low value of K M), rendering 1 a highly efficient catalyst for H 2O 2 disproportionation. © 2011 American Chemical Society.

Registro:

Documento: Artículo
Título:Synthesis, characterization, and catalase activity of a water-soluble diMn III complex of a sulphonato-substituted schiff base ligand: An efficient catalyst for H 2O 2 disproportionation
Autor:Palopoli, C.; Bruzzo, N.; Hureau, C.; Ladeira, S.; Murgida, D.; Signorella, S.
Filiación:Departamento de Química Física/IQUIR-CONICET, Facultad de Ciencias Bioquímicas y Farmacéuticas, Universidad Nacional de Rosario, Suipacha 531, S2002LRK Rosario, Argentina
CNRS, LCC (Laboratoire de Chimie de Coordination), 205, route de Narbonne, F-31077 Toulouse, France
Institut de Chimie de Toulouse, FR2599, 118 route de Narbonne, F-31062 Toulouse, France
Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE-CONICET, Universidad de Buenos Aires, Pabellón 2, Buenos Aires C1428EHA, Argentina
Palabras clave:catalase; coordination compound; hydrogen peroxide; ligand; manganese; Schiff base; article; catalysis; chemical structure; chemistry; metabolism; spectroscopy; Catalase; Catalysis; Coordination Complexes; Hydrogen Peroxide; Ligands; Manganese; Models, Molecular; Schiff Bases; Spectrum Analysis
Año:2011
Volumen:50
Número:18
Página de inicio:8973
Página de fin:8983
DOI: http://dx.doi.org/10.1021/ic2011452
Título revista:Inorganic Chemistry
Título revista abreviado:Inorg. Chem.
ISSN:00201669
CODEN:INOCA
CAS:catalase, 9001-05-2; hydrogen peroxide, 7722-84-1; manganese, 16397-91-4, 7439-96-5; Catalase, 1.11.1.6; Coordination Complexes; Hydrogen Peroxide, 7722-84-1; Ligands; Manganese, 7439-96-5; Schiff Bases
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00201669_v50_n18_p8973_Palopoli

Referencias:

  • Bravo, J., Mate, M.J., Schneider, T., Switala, J., Wilson, K., Loewen, P.C., Fita, L., (1999) Proteins Struct., Funct., Bioinf., 34, pp. 155-166
  • Riggs-Gelasco, P.J., Mei, R., Penner-Hahn, J.E., (1995) Mechanistic Bioinorganic Chemistry, , Thorp, H. H. Pecoraro, V. L. American Chemical Society: Washington, DC, Ch 8
  • Sayre, L.M., Perry, G., Smith, M.A., (2008) Chem. Res. Toxicol., 21, pp. 172-188
  • Day, B.J., (2009) Biochem. Pharmacol., 77, pp. 285-296
  • Hanawa, T., Asayama, S., Watanabe, T., Owada, S., Kawakamai, H., (2009) J. Controlled Release, 135, pp. 60-64
  • Brazier, M.W., Doctrow, S.R., Masters, C.L., Collins, S.J., (2008) Free Radical Biol. Med., 45, pp. 184-192
  • Day, B.J., (2004) Drug Discovery Today, 9, pp. 557-566
  • McDonald, M.C., Di Villa Bianca, R.E., Wayman, N.S., Pinto, A., Sharpe, M.A., Cuzzocrea, S., Chatterjee, P.K., Thiemermann, C., (2003) Eur. J. Pharmacol., 466, pp. 181-189
  • Antonyuk, S.V., Melik-Adamyan, V.R., Popov, A.N., Lamzin, V.S., Hempstead, P.D., Harrison, P.M., Artymiuk, P.J., Barynin, V.V., (2000) Crystallogr. Rep., 45, pp. 105-116
  • Barynin, V.V., Whittaker, M.M., Antonyuk, S.V., Lamzin, V.S., Harrison, P.M., Artymiuk, P.J., Whittaker, J.W., (2001) Structure, 9, pp. 725-738
  • Wu, A.J., Penner-Hahn, J.E., Pecoraro, V.L., (2004) Chem. Rev., 104, pp. 903-938
  • Dubois, L., Xiang, D.F., Tan, X.S., Latour, J.M., (2005) Eur. J. Inorg. Chem., pp. 1565-1571
  • De Boer, J.W., Browne, W.R., Feringa, B.L., Hage, R., (2007) C. R. Chim., 10, pp. 341-354
  • Signorella, S., Tuchagues, J.P., Moreno, D., Palopoli, C., (2008) Inorganic Biochemistry Research Progress, pp. 243-279. , Hughes, J. G. Robinson, A. J. Nova Science Publishers Inc. New York
  • Berben, L.A., Peters, J.C., (2008) Inorg. Chem., 47, pp. 11669-11679
  • Kaizer, J., Csonka, R., Speier, G., (2008) React. Kinet. Catal. Lett., 94, pp. 157-163
  • Dubois, L., Pécaut, J., Charlot, M.F., Baffert, C., Collomb, M.N., Deronzier, A., Latour, J.M., (2008) Chem.-Eur. J., 14, pp. 3013-3025
  • Jiang, X., Liu, H., Zheng, B., Zhang, J., (2009) Dalton Trans., pp. 8714-8723
  • Berggren, G., Huang, P., Eriksson, L., Styring, S., Anderlund, M.F., Thapper, A., (2010) Dalton Trans., pp. 11035-11044
  • Shin, B.K., Kim, M., Han, J., (2010) Polyhedron, 29, pp. 2560-2568
  • Lessa, J.A., Horn Jr., A., Bull, E.S., Rocha, M.R., Benassi, M., Catharino, R.R., Eberlin, M.N., Fernandes, C., (2009) Inorg. Chem., 48, pp. 4569-4579
  • Doctrow, S.R., Huffman, K., Marcus, C.B., Tocco, G., Malfroy, E., Adinolfi, C.A., Kruk, H., Malfroy, B., (2002) J. Med. Chem., 45, pp. 4549-4558
  • Nishida, Y., Akamatsu, T., Tsuchiya, K., Sakamoto, M., (1994) Polyhedron, 13, pp. 2251-2254
  • Kani, I., Darak, C., Sahin, O., Büyükgüngör, O., (2008) Polyhedron, 27, pp. 1238-1247
  • Berry, K.J., Moya, F., Murray, K.S., Bergen A M B, V.D., West, B.O., (1982) J. Chem. Soc., Dalton Trans., pp. 109-116
  • Botsivali, M., Evans, D.F., Missen, P.H., Upton, M.W., (1985) J. Chem. Soc., Dalton Trans., pp. 1147-1149
  • Murase, I., Hatano, M., Tanaka, M., Ueno, S., Okawa, H., Kida, S., (1982) Bull. Chem. Soc. Jpn., 55, pp. 2404-2408
  • Palopoli, C., Chansou, B., Tuchagues, J.P., Signorella, S., (2000) Inorg. Chem., 39, pp. 1458-1462
  • (2010) CrysAlis Pro, , version 1.171.33.66; Oxford Diffraction Ltd. Oxford, U.K
  • Altomare, A., Cascarano, G., Giacovazzo, C., Guagliardi, A., (1993) J. Appl. Crystallogr., 26, pp. 343-350
  • Sheldrick, G.M., (1997) SHELXL-97, Program for Crystal Structure Refinement, , University of Göttingen: Göttingen, Germany
  • Walker, N., Stuart, D., (1983) Acta Crystallogr., Sect. A, 39, p. 158
  • Watkin, D.J., Prout, C.K., Pearce, L.J., (1996) CAMERON, , Chemical Crystallography Laboratory, Oxford, UK
  • Spek, A.L., (1990) Acta Crystallogr., Sect. A, 46, p. 34
  • Deacon, G.B., Phillips, R.J., (1980) Coord. Chem. Rev., 33, pp. 227-250
  • Nakamoto, K., (1997) Infrared and Raman Spectra of Inorganic and Coordination Compounds, p. 60. , 5 th ed. Wiley-Interscience: New York, Part B
  • Biava, H., Palopoli, C., Shova, S., De Gaudio, M., Daier, V., González- Sierra, M., Tuchagues, J.P., Signorella, S., (2006) J. Inorg. Biochem., 100, pp. 1660-1671
  • Moreno, D., Palopoli, C., Daier, V., Shova, S., Vendier, L., González Sierra, M., Tuchagues, J.P., Signorella, S., (2006) Dalton Trans., pp. 5156-5166
  • Daier, V., Biava, H., Palopoli, C., Shova, S., Tuchagues, J.P., Signorella, S., (2004) J. Inorg. Biochem., 98, pp. 1806-1817
  • Palopoli, C., González-Sierra, M., Robles, G., Dahan, F., Tuchagues, J.P., Signorella, S., (2002) J. Chem. Soc., Dalton Trans., pp. 3813-3819
  • Gelasco, A., Pecoraro, V.L., (1993) J. Am. Chem. Soc., 115, pp. 7928-7929
  • Gelasco, A., Kirk, M.L., Kampf, J.W., Pecoraro, V.L., (1997) Inorg. Chem., 36, pp. 1829-1837
  • Bertoncello, K., Fallon, G.D., Murray, K.S., Tiekink, E.R.T., (1991) Inorg. Chem., 30, pp. 3562-3568
  • Mikuriya, M., Yamato, Y., Tokii, T., (1992) Bull. Chem. Soc. Jpn., 65, pp. 1466-1468
  • Biava, H., Palopoli, C., Duhayon, C., Tuchagues, J.-P., Signorella, S., (2009) Inorg. Chem., 48, pp. 3205-3214
  • Zhang, Z., Brouca-Cabarrecq, C., Hemmert, C., Dahan, F., Tuchagues, J.-P., (1995) J. Chem. Soc., Dalton Trans., pp. 1453-1460
  • Zhang, J.J., Luo, Q.H., Duan, C.Y., Wang, Z.L., Mei, Y.H., (2001) J. Inorg. Biochem., 86, pp. 573-579
  • Miyasaka, H., Clérac, R., Wernsdorfer, W., Lecren, L., Bonhomme, C., Sugiura, K.I., Yamashita, M., (2004) Angew. Chem., Int. Ed., 43, pp. 2801-2805
  • Dubois, L., Xiang, D.F., Tan, X.S., Pécaut, J., Jones, P., Baudron, S., Le Pape, L., Deronzier, A., (2003) Inorg. Chem., 42, pp. 750-760
  • Karsten, P., Neves, A., Bortoluzzi, A.J., Strähle, J., Maichle-Mössmer, C., (2002) Inorg. Chem. Commun., 5, pp. 434-438
  • Sabater, L., Hureau, C., Blain, G., Guillot, R., Thuéry, P., Rivière, E., Aukauloo, A., (2006) Eur. J. Inorg. Chem., pp. 4324-4337
  • Hureau, C., Sabater, L., Gonnet, F., Blain, G., Sainton, J., Anxolabé hère-Mallart, E., (2006) Inorg. Chim. Acta, 359, pp. 339-345
  • Bonadies, J., Maroney, M.J., Pecoraro, V.L., (1989) Inorg. Chem., 28, pp. 2044-2051
  • Caudle, M.T., Riggs-Gelasco, P., Gelasco, A.K., Penner-Hahn, J.E., Pecoraro, V.L., (1996) Inorg. Chem., 35, pp. 3577-3584
  • Bermejo, M.R., González, A.M., Fondo, M., García-Deibe, A., Maneiro, M., Sanmartín, J., Hoyos, O.L., Watkinson, M., (2000) New J. Chem., 24, pp. 235-241
  • Bermejo, M.R., González-Noya, A.M., Abad, V., Fernández, M.I., Maneiro, M., Pedrido, R., Vásquez, M., (2004) Eur. J. Inorg. Chem., pp. 3696-3705
  • Boelrijk, A.E.M., Khangulov, S.V., Dismukes, G.C., (2000) Inorg. Chem., 39, pp. 3009-3019
  • Larson, E.J., Pecoraro, V.L., (1991) J. Am. Chem. Soc., 113, pp. 7809-7810
  • Bonadies, J.A., Kirk, M.L., Lah, M.S., Kessissoglou, D.P., Hatfield, W.E., Pecoraro, V.L., (1989) Inorg. Chem., 28, pp. 2037-2044
  • Larson, E.J., Pecoraro, V.L., (1991) J. Am. Chem. Soc., 113, pp. 3810-3818
  • Hureau, C., Sabater, L., Anxolabéhère-Mallart, E., Nierlich, M., Charlot, M.-F., Gonnet, F., Rivière, E., Blondin, G., (2004) Chem.-Eur. J., 10, pp. 1998-2010
  • Baldwin, M.J., Pecoraro, V.L., (1996) J. Am. Chem. Soc., 118, pp. 11325-11326
  • Schardt, B.C., Hollander, F.J., Hill, C.L., (1982) J. Am. Chem. Soc., 104, pp. 3964-3972
  • Czernuszewicz, R.S., Su, Y.O., Stern, M.K., MacOr, K.A., Kim, D., Groves, J.T., Spiro, T.G., (1988) J. Am. Chem. Soc., 110, pp. 4158-4165
  • Groves, J.T., Stern, M.K., (1988) J. Am. Chem. Soc., 110, pp. 8628-8638
  • Song, W.J., Seo, M.S., George, S.D., Ohta, T., Song, R., Kang, M.J., Tosha, T., Nam, W., (2007) J. Am. Chem. Soc., 129, pp. 1268-1277
  • Sakiyama, H., Tamaki, H., Kodera, M., Matsumoto, N., Okawa, H., (1993) J. Chem. Soc., Dalton Trans., pp. 591-595
  • Sakiyama, H., Okawa, H., Isobe, R., (1993) J. Chem. Soc., Chem. Commun., pp. 882-884
  • Higuchi, C., Sakiyama, H., Okawa, H., Fenton, D.E., (1995) J. Chem. Soc., Dalton Trans., pp. 4015-4020
  • Itoh, M., Motoda, K., Shindo, K., Kamiusuki, T., Sakiyama, H., Matsumoto, N., Okawa, H., (1995) J. Chem. Soc., Dalton Trans., pp. 3635-3641
  • Aono, T., Wada, H., Yonemura, M., Ohba, M., Okawa, H., Fenton, D.E., (1997) J. Chem. Soc., Dalton Trans., pp. 1527-1531
  • Gelasco, A., Bensiek, S., Pecoraro, V.L., (1998) Inorg. Chem., 37, pp. 3301-3309
  • Boelrijk, A.E.M., Dismukes, G.C., (2000) Inorg. Chem., 39, pp. 3020-3028
  • Triller, M.U., Hsieh, W.Y., Pecoraro, V.L., Rompel, A., Krebs, B., (2002) Inorg. Chem., 41, pp. 5544-5554
  • Signorella, S., Rompel, A., Buldt-Karentzopoulos, K., Krebs, B., Pecoraro, V.L., Tuchagues, J.-P., (2007) Inorg. Chem., 46, pp. 10864-10868
  • Godbole, M.D., Kloskowski, M., Hage, R., Rompel, A., Mills, A.M., Spek, A.L., Bouwman, E., (2005) Eur. J. Inorg. Chem., pp. 305-313
  • Shorter, J., (1983) Correlation Analysis of Organic Reactivity, pp. 146-153. , Research Studies Press: New York
  • Penner-Hahn, J.E., Pecoraro, V.L., (1992) Manganese Redox Enzymes, p. 29. , Pecoraro, V. L. VCH: New York
  • Shank, M., Barynin, V., Dismukes, G.C., (1994) Biochemistry, 33, pp. 15433-15436
  • Penner-Hahn, J.E., (1992) Manganese Redox Enzymes, pp. 29-45. , Pecoraro, V. L. VCH: New York
  • Whittaker, M.M., Barynin, V.V., Igarashi, T., Whittaker, J.W., (2003) Eur. J. Biochem., 270, pp. 1102-1116
  • Amo, T., Atomi, H., Imanaka, T., (2002) J. Bacteriol., 184, pp. 3305-3312
  • Allgood, G.S., Perry, J.J., (1986) J. Bacteriol., 168, pp. 563-567
  • Kagawa, M., Murakoshi, N., Nishikawa, Y., Matsumoto, G., Kurata, Y., Mizobata, T., Kawata, Y., Nagai, J., (1999) Arch. Biochem. Biophys., 362, pp. 346-355

Citas:

---------- APA ----------
Palopoli, C., Bruzzo, N., Hureau, C., Ladeira, S., Murgida, D. & Signorella, S. (2011) . Synthesis, characterization, and catalase activity of a water-soluble diMn III complex of a sulphonato-substituted schiff base ligand: An efficient catalyst for H 2O 2 disproportionation. Inorganic Chemistry, 50(18), 8973-8983.
http://dx.doi.org/10.1021/ic2011452
---------- CHICAGO ----------
Palopoli, C., Bruzzo, N., Hureau, C., Ladeira, S., Murgida, D., Signorella, S. "Synthesis, characterization, and catalase activity of a water-soluble diMn III complex of a sulphonato-substituted schiff base ligand: An efficient catalyst for H 2O 2 disproportionation" . Inorganic Chemistry 50, no. 18 (2011) : 8973-8983.
http://dx.doi.org/10.1021/ic2011452
---------- MLA ----------
Palopoli, C., Bruzzo, N., Hureau, C., Ladeira, S., Murgida, D., Signorella, S. "Synthesis, characterization, and catalase activity of a water-soluble diMn III complex of a sulphonato-substituted schiff base ligand: An efficient catalyst for H 2O 2 disproportionation" . Inorganic Chemistry, vol. 50, no. 18, 2011, pp. 8973-8983.
http://dx.doi.org/10.1021/ic2011452
---------- VANCOUVER ----------
Palopoli, C., Bruzzo, N., Hureau, C., Ladeira, S., Murgida, D., Signorella, S. Synthesis, characterization, and catalase activity of a water-soluble diMn III complex of a sulphonato-substituted schiff base ligand: An efficient catalyst for H 2O 2 disproportionation. Inorg. Chem. 2011;50(18):8973-8983.
http://dx.doi.org/10.1021/ic2011452