Flame Aerosol Synthesis of Vanadia–Titania Nanoparticles: Structural and Catalytic Properties in the Selective Catalytic Reduction of NO by NH3

Abstract Flame aerosol synthesis has been used to prepare vanadia–titania nanoparticles with high activity for the selective catalytic reduction of NO by NH 3 . The mixed oxides were prepared from vanadium and titanium alkoxides which were evaporated into an argon stream and burned in a methane oxygen diffusion flame. Silica-containing samples were produced in a similar way by mixing hexamethyldisiloxane vapor into the precursor stream. Different flame structures were investigated for the effect of temperature and residence time on particle morphology, vanadia surface species, and overall catalytic activity. By changing the oxygen flow rate into the flame, particles with specific surface areas between 23 and 120 m 2 /g could be produced. High-resolution transmission electron microscopy (HRTEM) revealed that nanoparticles were spherical with diameters of 10 to 50 nm. X-ray photoelectron spectroscopy analysis indicated that vanadia was dispersed on the surface of the titania spheres. No indication for the presence of crystalline V 2 O 5 could be found by X-ray diffraction or HRTEM. Catalysts with a vanadia surface loading of 10 μmol/m 2 showed high activity with less than 1% N 2 O formation up to 350°C. Catalytic activity strongly depended on the vanadia loading; an increase from 2.5 to 7 μmol/m 2 resulted in a 30 times higher activity per vanadium. Addition of silica lowered the overall activity but did not change the activation energy. Raman spectroscopy indicated the presence of vanadate clusters. Temperature-programmed reduction corroborated that no significant amount of vanadia entered the titania lattice to form an interstitial solution. The selective catalytic reduction activity of as-prepared vanadia–titania is comparable to the best catalysts obtained by wet chemical methods.

[1]  A. Baiker,et al.  Effect of grafting sequence on the behavior of titania-supported v V2O5-WO3 catalysts in the selective reduction of NO by NH3 , 2000 .

[2]  M. Reiche Vanadia grafted on TiO2–SiO2, TiO2 and SiO2 aerogels: Structural properties and catalytic behaviour in selective reduction of NO by NH3 , 1999 .

[3]  Alexis T. Bell,et al.  Structure and Catalytic Properties of Supported Vanadium Oxides: Support Effects on Oxidative Dehydrogenation Reactions , 1999 .

[4]  S. Pratsinis,et al.  The effect of precursor in flame synthesis of SiO2 , 1998 .

[5]  S. Pratsinis,et al.  PHOTOCATALYTIC DESTRUCTION OF PHENOL AND SALICYLIC ACID WITH AEROSOL-MADE AND COMMERCIAL TITANIA POWDERS , 1996 .

[6]  Bert M. Weckhuysen,et al.  Selective Catalytic Reduction of NO with NH 3over Supported Vanadia Catalysts , 1996 .

[7]  G. Deo,et al.  Reactivity of V2O5Catalysts for the Selective Catalytic Reduction of NO by NH3: Influence of Vanadia Loading, H2O, and SO2 , 1996 .

[8]  M. D. Amiridis,et al.  Selective Catalytic Reduction of Nitric Oxide by Ammonia over V2O5/TiO2, V2O5/TiO2/SiO2, and V2O5−WO3/TiO2 Catalysts: Effect of Vanadia Content on the Activation Energy , 1996 .

[9]  S. Pratsinis,et al.  Dopants in Flame Synthesis of Titania , 1995 .

[10]  E. Serwicka,et al.  Mechanism of surface spreading in vanadia-titania system , 1995 .

[11]  A. Baiker,et al.  Vanadia supported on titania aerogels morphological properties and catalytic behaviour in the selective reduction of nitric oxide by ammonia , 1994 .

[12]  Sotiris E. Pratsinis,et al.  Synthesis and evaluation of titania powders for photodestruction of phenol , 1994 .

[13]  W. R. Moser,et al.  Noble metal catalysts prepared by the high-temperature aerosol decomposition (HTAD) process , 1994 .

[14]  A. Baiker,et al.  Chapter 3.5 Characterization of V2O5/TiO2 Eurocat samples by temperature-programmed reduction , 1994 .

[15]  J. Katz,et al.  Formation and characterization of nanostructured V—P—O particles in flames: A new route for the formation of catalysts , 1994 .

[16]  J. Katz,et al.  Formation of V_2O_5-based mixed oxides in flames , 1993 .

[17]  J. Katz,et al.  Formation of mixed oxide powders in flames: Part I. TiO_2−SiO_2 , 1992 .

[18]  A. Bell,et al.  The effects of structure on the catalytic activity and selectivity of V2O5/TiO2 for the reduction of NO by NH3 , 1992 .

[19]  A. Wokaun,et al.  Selective catalytic reduction of nitric oxide over vanadia grafted on titania. Influence of vanadia loading on structural and catalytic properties of catalysts , 1992 .

[20]  M. Sanati,et al.  Vanadia Catalysts on Anatase, Rutile, and TiO2(B) for the Ammoxidation of Toluene: An ESR and High-Resolution Electron Microscopy Characterization , 1991 .

[21]  G. Bond,et al.  Vanadium oxide monolayer catalysts Preparation, characterization and catalytic activity , 1991 .

[22]  Alexis T. Bell,et al.  Laser raman spectroscopy of supported vanadium oxide catalysts , 1990 .

[23]  W. R. Moser,et al.  A NEW HIGH TEMPERATURE AEROSOL DECOMPOSITION PROCESS FOR THE SYNTHESIS OF MIXED METAL OXIDES FOR CERAMICS AND CATALYSTS AND THEIR CHARACTERIZATION , 1989 .

[24]  S. Ted Oyama,et al.  Oxygen chemisorption and laser Raman spectroscopy of unsupported and silica-supported vanadium oxide catalysts , 1989 .

[25]  G. Busca,et al.  Structure and surface area evolution of vanadia-on-titania powders upon heat treatment , 1989 .

[26]  P. Forzatti,et al.  On the surface structure of vanadia-titania catalysts: Combined laser-Raman and fourier transform-infrared investigation , 1989 .

[27]  H. Bosch,et al.  Structure and reactivity of titania-supported oxides. Part 1: vanadium oxide on titania in the sub- and super-monolayer regions , 1986 .

[28]  Patricia Layman,et al.  French Chemical Industry Completes Massive Restructuring: Regrouping of activities has greatly simplified industry's tangled structure; question remains if and when move will translate into higher profits , 1984 .

[29]  J. Livage,et al.  Infrared and Raman study of amorphous V2O5 , 1982 .

[30]  Margaret S. Wooldridge,et al.  Gas-phase combustion synthesis of particles , 1998 .

[31]  Sotiris E. Pratsinis,et al.  Flame aerosol synthesis of ceramic powders , 1998 .

[32]  R. Frischknecht,et al.  Capabilities of an Argon Fluoride 193 nm Excimer Laser for LaserAblation Inductively Coupled Plasma Mass Spectometry Microanalysis ofGeological Materials , 1997 .

[33]  Wenhua H. Zhu,et al.  The role of gas mixing in flame synthesis of titania powders , 1996 .

[34]  James A. Dumesic,et al.  Vanadia-Titania Catalysts for Selective Catalytic Reduction of Nitric-Oxide by Ammonia , 1995 .

[35]  J. Haber,et al.  Monolayer V2O5/TiO2 and MoO3/TiO2 catalysts prepared by different methods , 1991 .

[36]  A. Wokaun,et al.  Characterization of V2O5/SiO2- and TiO2/SiO2-mixed gel catalysts by Raman spectroscopy , 1991 .

[37]  A. Baiker,et al.  Selective catalytic reduction of nitric oxide with ammonia: I. Monolayer and Multilayers of Vanadia Supported on Titania , 1987 .

[38]  J. H. Scofield,et al.  Hartree-Slater subshell photoionization cross-sections at 1254 and 1487 eV , 1976 .