DECHEMA e. V. Subject Division Catalysis

4th World Congress on Oxidation Catalysis

Extended Abstracts of the 4th World Congress on Oxidation Catalysis September 16-21,2001 Berlin/Potsdam - Germany

Contents

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Topic 4 Stereoselective catalytic oxidation reactions A solid Os catalyst for cis-dihydroxylation of olefins A. Severeyns, D. E. De Vos, P. A. Jacobs*

3

Stereoselective oxidation of 2-thiomethyl-4,6-dimethyl-pyrimidine and 2-thiobenzyl-4,6-dimethyl-pyrimidine over titania-silica catalysts R. Mihaiu, D.C. Radu, V. Parvulescu, V.I. Parvulescu, V. Campeanu, E. Bartha, M.T. Caproiu, A. Jonas, P. Grange.V.I. Parvulescu

7

Chemo-, regio- and stereoselective epoxidation of allylic alcohols as a probe for the structure of Titania-Silica C. Beck, T. Mallat, A. Baiker

11

Hydroxy-directed diastereoselective epoxidation of terpenic unsaturated alcohols on mesoporous titanium silicates M. Guidotti, G. Moretti, R. Psaro, N. Ravasio

^

Tungstate-exchanged layered double hydroxides as catalysts for biomimetic bromination reactions B. F. Sels, D. E. De Vos, P. A. Jacobs

25

Stereoselective oxidation of menthols with H2O2 on lanthanium(III)-containing polyoxotungstates in an organic solvent free system: kinetic features and working states Y. Kera, N. Ishii, T. Tanaka, S. Tsujioka, H. Kominami

29

Heterogeneization of the Jacobsen catalyst over mesostructured materials for the enantioselective epoxidation of olefins J. Aguado, D.P. Serrano, M. Ramos, C. Vargas

33

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page Silica-supported titanium derivatives as catalysts for the epoxidation of alkenes with diluted aqueous hydrogen peroxide J. M. Fraile, J. I. Garcia, J. A. Mayoral, E. Vispe

Topic 5 Recent developments in oxidation catalysis

73

Partial oxidation of ethylene with water as oxidant over photocatalysts Y. Ichihashi, Y. Matsumura, M. Hatuta

41

New niobium-containing catalysts in the oxidation of large organic 79 molecules M. Ziolek, A. Lewandowska, B. Kilos, I. Nowak

Preparation and reactivity of surface modified ZrO2/SiO2 mixed oxides in the oxidation of olefins with hydrogen peroxide R. Gavagnin, G. Strukul

47

Pd-catalysed cyclohexane oxidation with tert-butyl hydroperoxide 87 U. Schuchardt, D. Mandelli, W. A. Carvalho

Noble metal supported on hydrophobic carbons for selective aerial oxidation of alcohols in supercritical carbon dioxide A. M. Steele, J. Zhu, S. C. Tsang

51

Supercritical CO2 as reaction medium for the partial oxidation of 57 propane B. Kerler, A. Martin, M. Baerns Control of oxidation catalysis by acoustic wave excitation: Activity 59 enhancement of Pd-catalyzed ethanol alcohol oxidation by thickness-extensional resonance oscillation H. Nishiyama, K. Izumi, N. Saito, Y. Inoue

Hydroperoxides: Interesting products from the oxidation of 91 cycloalkanes and alkylbenzenes by H2O2 catalysed by Keggin-type heteropolytungstates M. M. Q. Simoes, A. M. V. Cavaleiro, J. A. S. Cavaleiro, R. A. W. Johnstone Cyclopentene oxidation with H2O2 over B, Ga or Al modified titanium silicalites of MFI topology V. Hulea, E. Dumitriu, T. Hulea, C. Chelaru, S. Kaliaguine Detoxication of 1,1-dimethylhydrazine water containing by catalytic oxidation with dioxygen and hydrogen peroxide over Fehydroxides O. P. Pestunova, G. L. Elizarova,V. N. Parmon

Partial oxidation of alkenes by the activated oxygen from water on 61 Ir(acac)3/carbon-fiber anode I. Yamanaka, T. Furukawa, K. Otsuka Kinetic studies on the mechanism of gaseous hydrocarbons oxidation with hydrogen peroxide in presence of iron and copper hydroxides in aqueous solutions A.A. Lysova, A.O. Kuzmin, G.L. Elizarova, E.R. Savinova, V.N. Parmon

67

Natural phosphates as basic catalysts for the epoxidation of electron-deficient alkenes J. M. Fraile, J. I. Garcia, J. A. Mayoral, S. Sebti, R. Tahir

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Topic 6 Fundamentals and theory a) Structure-selectivity/activity relationships in oxidation catalysis Surface acidity-basicity of solid oxide catalysts

109

E. Bordes-Richard, B. Taouk, P. Courtine TAP reactor experiments over an unsupported polycrystalline Silver catalyst: the influence of different oxygen states on the reactivity in selective oxidation reactions A. C. van Veen, O. Hinrichsen, M. Muhler

147

Synergistic effect of Ga on Vanadium Phosphorus Oxides catalysts for n-Butane Oxidation to Maleic Anhydride L. Sartoni, R. Wells, A. Delimitis, A. Burrows, C. Kiely ,V. Martin, J.-M. Herrmann, H. Roussel, J.-C. Volta

149

Supported complex oxide monolayers as selective oxidation catalysts A.O. Taylor, A. Bhakoo, G. C. Bond, M.F. Portela, R. D. Rees, V. Rozanov, B. Sauerhammer, A.P.V. Soares, A. Subramaniam, I. York

155

Influence of the defect structure of perovskites on the catalytic oxidation of CH4 F. Froehlich, F. Seifert, W. Burckhardt

163

Structure-selectivity/activity relationships in metal/bromide homogeneous liquid phase oxygenations W. Partenheimer

167

113

A new role for Molybdenum in Vanadyl pyrophosphate catalysts for selective oxidation of Butane T. R. Felthouse, N. L. Brungard, W. Zou Properties of copper as catalyst in selective oxidation reactions H.-J. Wolk, G. Mestl

125

Design of mixed oxide catalysts for the oxidation of Methacrolein to Methacrylic acid J.C. Petzoldt, H. Bohnke, J.W. Gaube, H. Hibst

127

Alkene oxidation on metal oxide clusters: Model systems for active centers A. Fielicke, K. Rademann

133

Metal-support interactions in autothermal reforming catalysts based on transition metals on oxide ion conducting supports T. Krause, D. Carter, J.-M. Bae, S. Ahmed, M. Krumpelt

137

Characterization of Iron Centers in ex-Framework FeZSM-5 zeolite. An Active Catalyst in the Benzene to Phenol Oxidation with N2O. I.W.C.E. Arends, A. Ribera, R.A. Sheldon, S. de Vries, J. P6rez-Ramirez, G. Mul, A.R. Overweg, A.M. van der Kraan

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Mechanism of selective oxidation by ct-oxygen over FeZSM-5 zeolites G.I. Panov, K.A. Dubkov, E.V. Starokon, E.A. Paukshtis, A.M. Volodin

Supported silver and gold catalysts for the low temperature CO oxidation and the propene epoxidation " A. Wolf, A. Lange de Oliveira, F. Schuth

171

High temperature propane oxidation to CO and H2 on Ni catalysts. Effects of the nickel content and support on properties of catalysts N.N. Jovanovic, M.V. Stankovic, Z.D. Cupi6

177

Role of ionic states of metals in formation of catalyst active surface in alcohol oxidation processes A.N.Pestryakov, V.V. Lunin, N. Bogdanchikova

181

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Comparative studies in VOCs degradation over ZnO-TiO2 thin films: thermal and photocatalytic routes D. Dumitriu, A.R. Bally, N. Martin, R. Sanjines, P.E. Schmid, F. Levy, V.I. Parvulescu

187

Raman spectroscopic characterisation of the decomposition of heteropoly compounds of the Keggin-type M. Dieterle, J. Krohnert, F. Jentoft, R. Schlogl, G. Mestl, T. Ilkenhans, D. Spielbauer, H. Knozinger

217

Catalysts for the selective total oxidation of hydrocarbons: Comparison of binary and quaternary Fe- and Cu-oxides H.-J. Wolk, W. Gunther, G. Mestl, C. Elsasser, A. Rapp

191

TEM observation of Au/TiO2 propylene epoxidation catalysts T. Akita, K. Tanaka, S. Tsubota, M. Haruta

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193

Catalytic properties of novel nanostructured vanadia-based catalysts in the selective catalytic reduction of NO by NH3 G.A. Zenkovets, G.N: Kryukova, S.V. Tsybulya, V.N. Parmon, Z. Sobalik

225

A Comparison of the Factors Influencing Selectivity in Selective Oxidation and Epoxidation Reactions F. Cassidy, B. K. Hodnett Preparation and catalysis of isolated metal ions on silica for selective oxidation of lower alkanes Y. Yamada, A. Ueda, Z. Zhao, T. Kobayashi

199

VPO lattice oxygen mobility M. J. Lorences, G.S. Patience, F. V. Diez, J. Coca

227

Effect of acid sites on selective oxidation of n-Butane over (VO)2P2O7 as investigated by dimethylpyridine TemperatureProgrammed Desorption A. Satsuma, M. Yashiro, H. Nishiyama, Y. Kamiya, E. Nishikawa, T. Hatttori

231

A comparative study of photocatalytic oxidation of VOCs on sulfated TiO2 and Degussa P-25 L. Ding, D. S. Muggli

235

Sintering and wetting of silver on a-A!2O3 (1120) ethylene oxide model catalyst by heating alternately in ethylene and oxygen G.J. Feldmeyer, M. Kinne, RJ. Behm, K. Al-Shamery

207

Influence of the conditioning process on the formation of the active phase for total oxidation of ethylene on silica supported palladium catalysts S. Hackenberg, H. Hoffmann, RJ. Behm

209

Selective CO oxidation over Au/MyO, catalysts: Influence of composition and particle size of the metal oxide support Y.F. Han, M.J. Kahlich, M.M. Schubert, M. Kinne, RJ. Behm, V.Plzak

211

New applications of mesoporous Ti-containing silicate materials in 243 selective oxidation. Structure-selectivity/activity relationships N.N. Trukhan, V.N. Romannikov, O.A. Kholdeeva, J. Mrowiec-Bialon, A.B. Jarzebski

Nanostructured cobalt and nickel molybdate catalysts for oxidative dehydrogenation of propane R.X. Valenzuela, G. Bueno Sobrino, V. Cortes Corberan, D. Vie Giner, E. Martinez, F. Sapina

213

X-ray absorption studies on vanadium molybdenum oxides F. Haafl, T. Buhrmester, M. Martin

247

249

Investigation of the catalytic activity of a novel silver-copper-

215

Supramolecular metal complexes based on cyclodextrin and calixarenes in biphasic oxidations: relationship between the structure and the selectivity E. A.Karakhanov

oxide: Ag 2 Cu 2 O 3

H.-J. Wolk, U. Wild, G. Mestl, R. Schlogl, P. Gomez-Romero

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page Preparation, characterisation and reactivity of cobalt-based catalysts in the catalytic combustion of methane S.-F. Ji, T.-C. Xiao, H.-T. Wang, M.L.H. Green

Diffuse reflectance spectroscopy of Alumina supported Chromium 257 Oxides and catalytic measurements in Paraxylen partial oxidation S. Khaddar - Zine, A. Ghorbel, C. Naccache Enhancing the selectivity in the epoxidation of alkenes using TS-1 263 promoted catalyst M. C. Capel-Sanchez, J. M. Campos-Martin, J. L. G. Fierro Mechanistic study of allylic alcohols epoxidation over vanadiummontmorillonite as a heterogenous catalyst J. Khedher, A. Ghorbel

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269

Oxidation of methanol on silica supported alkali metal molybdates 273 A. Erdohelyi, A. Hancz, P. Tolmacsov, E. Novak Isothermal study of CO + O2 and NH3 + O2 reactions on Rh(l 11) using a molecular collimated beam doser V. Gorodetskii, S. Wehner, F. Zaera

277

Characterization and reactivity Vanadium Oxide catalysts supported on Zirconia K. V.R. Chary, G. Kishan, C. P. Kumar, K. Ramesh

279

Topic 6 Fundamentals and theory b) In-situ characterization of oxidation catalysts and reaction mechanisms Characterization of alumina supported Pd nanoparticles under reaction conditions by sum frequency generation spectroscopy G. Rupprechter, T. Dellwig, H. Unterhalt, L. Hu, H.-J. Freund

285

Supported catalysts based on Pd and P-Mo-V heteropolycomplexes for low-temperature CO oxidation: In situ IR study S. N. Pavlova, L. I. Kuznetsova, M. N. Bredikhin

287

The structure of active sites in metal vanadates and its influence on the catalytic performance in the oxidative dehydrogenation (ODH) of propane A. Bruckner, P. Rybarczyk, O. Buyevskaya, J. Radnik, H. Berndt, M. Baerns

291

Methane partial oxidation to syngas: I3C isotope-labelling study of 297 reaction pathways over Ni and Pt-containing catalysts Yu. P. Tulenin, V. V. Savkin, M. Yu. Sinev, V. N. Korchak, O. V. Krylov Bridging the "pressure gap": Investigation of the ammonia oxidation over copper with in situ NEXAFS in the soft X-ray range under mbar pressure conditions R.W. Mayer, M. Melzer, M. Havecker, D. Frickel, A. Knop-Gericke, R. Schlogl

303

Direct gas-phase epoxidation of propene - mechanistic studies A. Zwijnenburg, G. Mul, M. Makkee, J.A. Moulijn

307

Selectivity limiting factors in the partial oxidation of 309 methylaromatics on (VO)2P2O7 and modified V2O5 catalysts: New insight by using spectroscopic in situ methods U. Bentrup, A. Bruckner, A. Martin, B. Liicke

vni

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page In situ studies on the structure-activity relationships of ceriasupported oxide catalysts for ethane oxidative dehydrogenation M.A. Banares, M.V. Martinez-Huerta, J.L.G. Fierro, X. Gao, I.E. Wachs

315

Catalytic Olefin Epoxidation with Seven-coordinate Molybdenum 317 Oxobisperoxo Complexes: A Mechanistic Study W. R. Thiel Oxidation of ketones and a-ketols with dioxygen catalysed by copper complexes or Keggin-type heteropolymolybdates: from homogeneous systems to solid catalysts F. Launay, M. Vennat, L. El Aakel, A. Atlamsani, E. Duprey, J.-M. Bregeault

321

In situ examinations during the partial oxidation of ethylene and propylene on silver catalysts A. Drochner, M. Fehlings, J. Kunert, K. KrauB, H. Vogel

327

Transient response in methane combustion on perovskite - Study of O2 and CO2 adsorption/desorption elementary steps G. Vulpescu, F.C. Thyrion

329

The formation of carbon oxides in the ethylene oxidative chlorination process in the presence of copper chloride catalysts M.R. Flid, I.I. Kurlyandskaya, M.V. Babotina, Y.K. Dmitriev

337

The mechanism of oxidative carbonylation of the alkyne =C-H bond L.G. Bruk, I.V. Oshanina, V.R. Khabibulin, O.V. Kaljazina, O.N. Temkin, V.M. Nosova, Y.A. Ustynyuk

341

Theoretical aspects of the investigation of the number of steady states in catalytic oxidation reactions E.S. Patmar, N. Koltsov

343

On a resonance Raman effect of the molybdenum suboxide Mo4On M. Dieterle, G. Mestl

347

page Study of N2O adsorption and activation on zeolites by UV- and IR-spectroscopy and calorimetry A.L. Tarasov, L.M. Kustov, A.A. Tyrlov, A.M. Kulizade, V.L. Zholobenko

351

Interaction of nitrogen oxides with strong Lewis sites of HZSM-5 zeolite modified with zinc oxide: Relevance to selective oxidation of aromatic compounds and DENOX L.M. Kustov, A.L. Tarasov, A.M. Kulizade, A.A. Tyrlov, E.V. Smekalina

353

Insight in the thermal decomposition of ammonium heptamolybdate J. Wienold, R.E. Jentoft, O. Timpe, T. Ressler

355

In-situ studies on the structure and activity of copper oxide/zinc oxide catalyst in steam reforming of methanol using X-ray diffraction and absorption techniques M.M. Gunter, B. Bems, R. Schlogl, T. Ressler

357

In situ characterisation of iron phosphate and bismuth molybdate 359 catalysts prepared by hydrothermal methods A. M. Beale, G. Sankar A study of the nature of the oxidants in vanadyl pyrophosphate catalysts derived from a VOPO4-2H2O precursor Y.H. Taufiq-Yap, M.H. Looi, C.P. Ho, M.Z. Hussein, Z. Zainal, K.C. Waugh

365

Phosphine oxidation by Oxygen catalyzed by supported metal complex compounds of Copper(II) and Palladium(II) T. L. Rakitskaya, A.A. Ennan, V.Ya. Paina, A.S. Rakitskiy

369

Effect of a ligand nature on catalytic behavior of Silica-supported 375 Copper(II) in its reaction with Ozone T. L. Rakitskaya, A.S. Podmazko, A.Yu. Bandurko, L.A. Raskola, V.Ya. Paina

XI

Stater of atomic Oxygen in its complexes with transition meta1 utaiysts as studied by effective electron Hamiltonian approach

38 1

Topic 7 Catalytic reaction engineering

A.M.Tokmachev, A.L. Tchougreeff Catalytic Oxidations Under an NO Atmosphere U. Schuchardt, M.J. D. M. Jannini, M.C. Guerreiro

383

Perovskites of the composition RBa2Cu30,@=Y, Nd, Ho): Surface reduction and catalytic activity in CO oxidation Y.V. Guriev, A.V. Rogov, A. Galkin, V.V.Lunin

387

Physical adsorption and electron transfer on the surface of ionic crystals. Semiempirical quantum-chemical methods I.K. Vorontsova, I.A. Abronin, I.D. Mikheikin

39 1

Comparison between steady versus unsteady reactor operating modes for the selective oxidation of Isobutylene to Methacrolein J. F. Nicole, P. L. Mills

e

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E

'

399

Selective oxidation of H2S to elemental sulfur over SiC supported 407 iron-based catalyst N. Keller, C. Pham-Huu, M. J. Ledoux Determination of a high temporal resolution model for the selective oxidation of butane under unsteady-state conditions S. Weiss, S. Hess, M.A. Liauw, G. Emig

41 1

Tailormade high performance Phthalic Anhydride catalysts: An approach to optimize catalyst-reactor-interactions F. Rosowski, S. Storck, A. Tenten

415

Carbon monolithic catalysts in the selective oxidation of cyclohexanone E. Crezee, F. Kapteijn, J.A. Moulijn

417

Enhancement of selectivity of oxidative reactions in forced unsteady-state reactors A. A. Barresi, D. Fissore, M. Vanni, G. Baldi

419

Oxidative dehydrogenation of short chain alkanes in a two-zone fluidized bed reactor using VO,/A1203 as catalyst J.M. Lbpez Nieto, J. Soler, J. Herguido, B. Solsona, M. Menendez, J. Santamaria

427

~ a t a l y t i combustion c for process heat within fuel cell systems I. Hermann, A. Junge, D. Lemken

431

New catalysts for the oxidative steam reforming of methanol and ethanol to produce hydrogen for fuel cells S. Velu, S. Hashimoto, N. Satoh, K. Sumki, T. Mori

437

Reaction engineering investigations of the Hydroxylation of Benzene and Toluene with N20 on ZSM-5-zeolites A.. Reitzmann, B. Vogel, U. Hiemer, E. Klemm, G. Emig

Catalytic wet oxidation of reactive dye solutions at low pressure D.-K.Lee, D.-S. Kim, S. W. Kim

Complete catalytic oxidation of benzene T. Gürmen, E. Alpay, S. Atalay

Ti02photocatalytic oxidation of nitric oxide : Transient behavior and reaction kinetics S. Devahasdin, K. Li, D. H. Chen

Catalytic combustion of methane over Pd containing perovskites S. Petrovic, A. Terlecki-Baricevic, L. Karanovic, M. Zdujic '

Modeling of high pressure catalytic combustion in fuel rich regime F.W. Knebel, R. Reimert

Effect of sulphur compounds on the catalytic combustion of methane over precious meta1 catalysts P. Hurtado, S. Ordoiiez, H. Sastre, F.V. Diez Catalytic wet-air oxidation of industrial paper plant efiiuents in batch and trickle-bed reactors A. Pintar, M. Besson, P. Gallezot

Methane oxidative coupling in different operating modes N.I. Ilchenko, Yu.1. Pyatnitsky, L.N. Raevskaya, A.I. Bostan

493

497 Reduced NiMo04 as an efficient and durable oxidative dehydrogenation catalyst: periodic and continuous flow conditions R Del Rosso, A. Kaddouri, C. Mazzocchia, P. Gronchi, P. Centola

Deep oxidation of methane over iron 011) oxide catalysts J.R. Paredes, S. Ordofiez, F.V. Diez, H. Sastre

Kinetic study on cyclohexane oxidation over a NiOly-A1203-catalyst F. Patcas, F.C. Buciuman

Modified Wacker oxidation of long-chain terminal olefins J. Aguado, D. P. Serrano, R. Van Grieken, J.M. Escola, R. Garcia S. Carretero

i

Oxidative dehydrogenation of ethane and propane at short contact time B. Silberova, M. Fathi, A. Holmen

503

Study of Culy-A1203catalytic system for the combustion of Methane in fluidized bed reactor M. Iarnarino, R. Chirone, L. Lisi, R. Pirone, G. Russo, P. Salatino

507

Partial oxidation of ethane over s perovskite-based monolithic reactor F. Donsi, R. Pirone, G. Russo

51 1

Author index

Transient two-dimensional simulations of monoiithic catalysts using detailed models for heterogeneous and homogeneous reactions and transport phenomena for the catalytic partial oxidation of lower alkanes C. Correa, S. Tischer, R. Schwiedernoch, 0. Deutschmann Fuil Papers of the INVITED LECTURES wiii be pubiished in a special volume of "Topics in Catalysis", that is included in the Regular and Special tickets of the Congress