On the involvement of radical oxygen species O- in catalytic oxidation of benzene to phenol by nitrous oxide

被引:52
作者
Chernyavsky, Valery S.
Pirutko, Larisa V.
Uriarte, Anthony K.
Kharitonov, Alexander S.
Panov, Gennady I. [1 ]
机构
[1] Boreskov Inst Catalysis, Novosibirsk 630090, Russia
[2] Solutia Inc, Gonzalez, FL 32560 USA
基金
俄罗斯基础研究基金会;
关键词
selective oxidation; N2O; Fe-MFI; alpha-oxygen; oxygen radicals; benzene to phenol oxidation;
D O I
10.1016/j.jcat.2006.10.023
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Catalytic oxidation of benzene to phenol by nitrous oxide over Fe-MFI zeolites was studied in relation to the active oxygen species taking part in the oxidation. A linear dependence of the reaction rate on the concentration of independently identified active sites generating O- radicals (a sites) was obtained within a broad range of values. The dependence is interpreted as convincing evidence of the O- involvement in the catalytic (not only stoichiometric) oxidation of benzene to phenol. This conclusion is of particular importance in connection with a long discussion in the literature on a possible role of O- radicals in selective oxidation catalysis over V and Mo oxides. Reliable evidence of the catalytic role of O- obtained with zeolites may renew general interest in the once-suggested but not recognized role of radical oxygen in oxidation over widely used metal oxide catalysts. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:466 / 469
页数:4
相关论文
共 42 条
[1]  
Boreskov G.K., 2003, Heterogeneous Catalysis
[2]  
Centi G, 1999, CHEMTECH, V29, P48
[3]  
Centi G., 2001, Selective Oxidation by Heterogeneous Catalysis
[4]   CHARACTERIZATION AND REACTIVITY OF MONONUCLEAR OXYGEN SPECIES ON OXIDE SURFACES [J].
CHE, M ;
TENCH, AJ .
ADVANCES IN CATALYSIS, 1982, 31 :77-133
[5]   CHARACTERIZATION AND REACTIVITY OF MOLECULAR-OXYGEN SPECIES ON OXIDE SURFACES [J].
CHE, M ;
TENCH, AJ .
ADVANCES IN CATALYSIS, 1983, 32 :1-148
[6]   ACID CATALYSIS BY DEALUMINATED ZEOLITE-Y .1. METHANOL DEHYDRATION AND CUMENE DEALKYLATION [J].
DECANIO, SJ ;
SOHN, JR ;
FRITZ, PO ;
LUNSFORD, JH .
JOURNAL OF CATALYSIS, 1986, 101 (01) :132-141
[7]   Evolution of iron states and formation of α-sites upon activation of FeZSM-5 zeolites [J].
Dubkov, KA ;
Ovanesyan, NS ;
Shteinman, AA ;
Starokon, EV ;
Panov, GI .
JOURNAL OF CATALYSIS, 2002, 207 (02) :341-352
[8]   Kinetic isotope effects and mechanism of biomimetic oxidation of methane and benzene on FeZSM-5 zeolite [J].
Dubkov, KA ;
Sobolev, VI ;
Talsi, EP ;
Rodkin, MA ;
Watkins, NH ;
Shteinman, AA ;
Panov, GI .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1997, 123 (2-3) :155-161
[9]  
GOLODETS GI, 1983, STUD SURF SCI CATAL, V15
[10]   Surface species produced by the reaction between methane and oxygen radical anion O•- on MgO at 298 K [J].
Goto, A ;
Aika, K .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1998, 71 (01) :95-98