Dynamic X-ray diffraction computed tomography reveals real-time insight into catalyst active phase evolution.

Metals and metal oxides anchored to porous support materials are widely used as heterogeneous catalysts in a number of important industrial chemical processes. These catalysts owe their activity to the formation of unique metal/metal oxide support interactions, typically resulting in highly dispersed actives stabilized in a particular electronic or coordination state. They are employed in fixed-bed reactors as extruded or pelletized millimeter-sized “catalyst bodies” minimizing pressure drops along the length of the reactor. Since the efficiency of the whole catalytic system depends on the behavior and efficiency of the catalyst body per se, its design has very great importance. Crucial to this design is an understanding of the factors which influence the distribution and nature of the active phase during preparation. The type of desired distribution is very much dependant on catalytic process and required products; for example, an egg-shell distribution (as opposed to uniform, egg-white, or egg-yolk), where the active phase is located at the edges of the catalyst body, can be favored if the product forms readily.

[1]  U Neitzel,et al.  X-ray diffraction computed tomography. , 1987, Medical physics.

[2]  V. Rodríguez-González,et al.  Stabilization of hexagonal close-packed metallic nickel for alumina-supported systems prepared from Ni(II) glycinate , 2007 .

[3]  R J Cernik,et al.  X-ray colour imaging , 2007, Journal of The Royal Society Interface.

[4]  T. Schildhauer,et al.  Sulphur poisoning of Ni catalysts in the SNG production from biomass: A TPO/XPS/XAS study , 2009 .

[5]  B. Weckhuysen,et al.  Envisaging the physicochemical processes during the preparation of supported catalysts: Raman microscopy on the impregnation of Mo onto Al2O3 extrudates. , 2004, Journal of the American Chemical Society.

[6]  L. Gengembre,et al.  From Al2O3-supported Ni(II)-ethylenediamine Complexes to CO Hydrogenation Catalysts: Importance of the Hydrogen Post-treatment Evidenced by XPS , 2008 .

[7]  P. Bleuet,et al.  Probing the structure of heterogeneous diluted materials by diffraction tomography. , 2008, Nature materials.

[8]  W. Lee,et al.  Effect of Ni loading and calcination temperature on catalyst performance and catalyst deactivation of Ni/SiO2 in the hydrodechlorination of 1,2‐dichloropropane into propylene , 2000 .

[9]  B. Weckhuysen,et al.  Noninvasive in situ visualization of supported catalyst preparations using multinuclear magnetic resonance imaging. , 2005, Journal of the American Chemical Society.

[10]  J. Kosanetzky,et al.  Scattered X-ray beam nondestructive testing , 1989 .

[11]  G. Artioli,et al.  Towards three-dimensional quantitative reconstruction of cement microstructure by X-ray diffraction microtomography , 2011 .

[12]  M. Che,et al.  From Al2O3-supported Ni(II)–ethylenediamine complexes to CO hydrogenation catalysts: Characterization of the surface sites and catalytic properties , 2009 .

[13]  A. Beale,et al.  Chemical imaging of catalytic solids with synchrotron radiation. , 2010, Chemical Society reviews.

[14]  A. Beale,et al.  Tomographic energy dispersive diffraction imaging to study the genesis of Ni nanoparticles in 3D within gamma-Al2O3 catalyst bodies. , 2009, Journal of the American Chemical Society.

[15]  J. Grunwaldt,et al.  Catalysts at work: From integral to spatially resolved X-ray absorption spectroscopy , 2009 .

[16]  Andrew C. Jupe,et al.  Rapid whole-rock mineral analysis and composition mapping by synchrotron X-ray diffraction , 1996 .

[17]  A. Rack,et al.  X-ray diffraction microtomography (XRD-CT), a novel tool for non-invasive mapping of phase development in cement materials , 2010, Analytical and bioanalytical chemistry.

[18]  L. Gengembre,et al.  A systematic study of the interactions between chemical partners (metal, ligands, counterions, and support) involved in the design of Al2O3-supported nickel catalysts from diamine-Ni(II) chelates. , 2005, The journal of physical chemistry. B.

[19]  B. Weckhuysen,et al.  UV-Vis microspectroscopy: probing the initial stages of supported metal oxide catalyst preparation. , 2005, Journal of the American Chemical Society.

[20]  B. Weckhuysen,et al.  Effect of the Nickel Precursor on the Impregnation and Drying of γ-Al2O3 Catalyst Bodies: A UV−vis and IR Microspectroscopic Study , 2008 .

[21]  L. I. Kheifets,et al.  Theory of preparation of supported catalysts , 1981 .

[22]  Simon D M Jacques,et al.  Tomographic energy dispersive diffraction imaging as a tool to profile in three dimensions the distribution and composition of metal oxide species in catalyst bodies. , 2007, Angewandte Chemie.

[23]  A. Beale,et al.  Profiling physicochemical changes within catalyst bodies during preparation: new insights from invasive and noninvasive microspectroscopic studies. , 2010, Accounts of chemical research.

[24]  A. K. Tyagi,et al.  Temperature programmed decomposition of cobalt ethylene diamine complexes , 1999 .

[25]  A. Lycourghiotis,et al.  The Role of the Liquid‐Solid Interface in the Preparation of Supported Catalysts , 2006 .

[26]  P. Bleuet,et al.  Microstructural mapping of C60 phase transformation into disordered graphite at high pressure, using X‐ray diffraction microtomography , 2011 .

[27]  E. Scavetta,et al.  Combined Use of Synchrotron‐Radiation‐Based Imaging Techniques for the Characterization of Structured Catalysts , 2010 .