V2O5 Nanowires with an Intrinsic Peroxidase-Like Activity

被引:629
作者
Andre, Rute [1 ]
Natalio, Filipe [1 ]
Humanes, Madalena [2 ]
Leppin, Jana [1 ]
Heinze, Katja [1 ]
Wever, Ron [3 ]
Schroeder, H. -C. [4 ]
Mueller, Werner E. G. [4 ]
Tremel, Wolfgang [1 ]
机构
[1] Johannes Gutenberg Univ Mainz, Inst Inorgan Chem, D-55099 Mainz, Germany
[2] Univ Lisbon, Fac Sci, Dept Chem & Biochem, Ctr Chem & Biochem, P-1749016 Lisbon, Portugal
[3] Univ Amsterdam, Vant Hoff Inst Mol Sci, NL-1018 WS Amsterdam, Netherlands
[4] Johannes Gutenberg Univ Mainz, Inst Physiol Chem, Dept Appl Mol Genet, D-55099 Mainz, Germany
关键词
VANADIUM PENTOXIDE NANOBELTS; HYDROGEN-PEROXIDE; ELECTROCHEMICAL PROPERTIES; HORSERADISH-PEROXIDASE; OXIDATIVE BROMINATION; CATALYZED OXIDATION; OXIDE NANOTUBES; CHLOROPEROXIDASE; BROMOPEROXIDASE; INTERCALATION;
D O I
10.1002/adfm.201001302
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
V2O5 nanowires exhibit an intrinsic catalytic activity towards classical peroxidase substrates such as 2,2-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) and 3,3,5,5,-tetramethylbenzdine (TMB) in the presence of H2O2. These V2O5 nanowires show an optimum reactivity at a pH of 4.0 and the catalytic activity is dependent on the concentration. The Michaelis-Menten kinetics of the ABTS oxidation over these nanowires reveals a behavior similar to that of their natural vanadium-dependent haloperoxidase (V-HPO) counterparts. The V2O5 nanowires mediate the oxidation of ABTS in the presence of H2O2 with a turnover frequency (k(cat)) of 2.5 x 10(3) s(-1). The K-M values of the V2O5 nanowires for ABTS oxidation (0.4 mu M) and for H2O2 (2.9 mu M) at a pH of 4.0 are significantly smaller than those reported for horseradish peroxidases (HRP) and V-HPO indicating a higher affinity of the substrates for the V2O5 nanowire surface. Based on the kinetic parameters and similarity with vanadium-based complexes a mechanism is proposed where an intermediate metastable peroxo complex is formed as the first catalytic step. The nanostructured vanadium-based material can be re-used up to 10 times and retains its catalytic activity in a wide range of organic solvents (up to 90%) making it a promising mimic of peroxidase catalysts.
引用
收藏
页码:501 / 509
页数:9
相关论文
共 77 条
[1]   Vanadium haloperoxidases from brown algae of the Laminariaceae family [J].
Almeida, M ;
Filipe, S ;
Humanes, M ;
Maia, MF ;
Melo, R ;
Severino, N ;
da Silva, JAL ;
da Silva, JJRF ;
Wever, R .
PHYTOCHEMISTRY, 2001, 57 (05) :633-642
[2]   Selective photocatalytic oxidation of light alkanes over alkali-ion-modiried V2O5/SiO2;: Kinetic study and reaction mechanism [J].
Amano, F ;
Ito, T ;
Takenaka, S ;
Tanaka, T .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (21) :10973-10977
[3]   Steady-state photocatalytic epoxidation of propene by O2 over V2O5/Si2 photocatalysts [J].
Amano, F ;
Tanaka, T ;
Funabiki, T .
LANGMUIR, 2004, 20 (10) :4236-4240
[4]  
[Anonymous], 2010, Peroxidases and Catalases: Biochemistry, Biophysics, Biotechnology and Physiology
[5]  
[Anonymous], ANGEW CHEM
[6]  
Bernal H. G., 2005, INT J CHEM REACTOR E, V3, P1
[7]  
Bielanski A., 1991, OXYGEN CATALYSIS, DOI DOI 10.1201/9781482293289
[8]   Macroscopic fibers of oriented vanadium oxide ribbons and their application as highly sensitive alcohol microsensors [J].
Biette, L ;
Carn, F ;
Maugey, M ;
Achard, MF ;
Maquet, T ;
Steunou, N ;
Livage, T ;
Serier, H ;
Backov, R .
ADVANCED MATERIALS, 2005, 17 (24) :2970-+
[9]   Regioselective bromination of organic substrates by tetrabutylammonium bromide promoted by V2O5-H2O2:: An environmentally favorable synthetic protocol [J].
Bora, U ;
Bose, G ;
Chaudhuri, MK ;
Dhar, SS ;
Gopinath, R ;
Khan, AT ;
Patel, BK .
ORGANIC LETTERS, 2000, 2 (03) :247-249
[10]   Peroxometal-mediated environmentally favorable route to brominating agents and protocols for bromination of organics [J].
Bora, U ;
Chaudhuri, MK ;
Dey, D ;
Dhar, SS .
PURE AND APPLIED CHEMISTRY, 2001, 73 (01) :93-102