Combining synchrotron-based X-ray techniques with vibrational spectroscopies for the in situ study of heterogeneous catalysts: a view from a bridge.

The advantages, challenges, and future possibilities for combining synchrotron-based X-ray techniques with vibrational spectroscopies are considered in this critical review. Particular emphasis is given to (1) quantifying structure and structural change--on a wide range of length scales--in working heterogeneous catalytic systems; (2) relating that change to chemical speciation occurring at the surface of the catalyst; and (3) determining how such change relates to the overall function of the catalyst material. We will consider those resources that exist today and suggest some possible future directions yet to be ventured into or demonstrated. Lastly, we will consider how the catalysis community interacts with, and uses the resources offered by, modern synchrotron radiation facilities and whether this current relationship provides the best and most inclusive means for the exploitation of these resources in this field of research (83 references).

[1]  A. Dent,et al.  Particle size effects in Rh/Al2O3 catalysts as viewed from a structural, functional, and reactive perspective: the case of the reactive adsorption of NO , 2007 .

[2]  V. A. Solé,et al.  Ultrahigh vacuum/high-pressure flow reactor for surface x-ray diffraction and grazing incidence small angle x-ray scattering studies close to conditions for industrial catalysis. , 2010, The Review of scientific instruments.

[3]  P. Colarusso,et al.  Infrared Spectroscopic Imaging: From Planetary to Cellular Systems , 1998 .

[4]  S. Belin,et al.  New insights for materials science characterisation using different complementary techniques combined with x-ray absorption spectroscopy , 2005 .

[5]  P. L. Hansen,et al.  A combined QEXAFS/XRD method for on-line, in situ studies of catalysts: Examples of dynamic measurements of Cu-based methanol catalysts , 1993 .

[6]  D. W. Goodman,et al.  “Catalytically active Au on Titania:” yet another example of a strong metal support interaction (SMSI)? , 2005 .

[7]  J. Grunwaldt,et al.  Comparative in situ XAS investigations during aerobic oxidation of alcohols over ruthenium, platinum and palladium catalysts in supercritical CO2 , 2007 .

[8]  D. Rooney,et al.  A modified commercial DRIFTS cell for kinetically relevant operando studies of heterogeneous catalytic reactions , 2008 .

[9]  Jacques Jupille,et al.  Real-Time Monitoring of Growing Nanoparticles , 2003, Science.

[10]  Olivier Mathon,et al.  Invited article: the fast readout low noise camera as a versatile x-ray detector for time resolved dispersive extended x-ray absorption fine structure and diffraction studies of dynamic problems in materials science, chemistry, and catalysis. , 2007, The Review of scientific instruments.

[11]  M. Skoglundh,et al.  In Situ Spectroscopic Investigation of Low-Temperature Oxidation of Methane over Alumina-Supported Platinum during Periodic Operation† , 2011 .

[12]  J. Evans Brilliant opportunities across the spectrum. , 2006, Physical chemistry chemical physics : PCCP.

[13]  Michael J. Pellin,et al.  Reactivity of supported platinum nanoclusters studied by in situ GISAXS: clusters stability under hydrogen , 2006 .

[14]  J. Yarwood,et al.  A new radiation source for the infrared region , 1984, Nature.

[15]  W. Xu,et al.  Time Resolved IR and X-Ray Simultaneous Spectroscopy: New Opportunities for the Analysis of Fast Chemical-Physical Phenomena in Materials Science , 2009 .

[16]  A. Urakawa,et al.  On the local sensitivity of different IR techniques: Ba species relevant in NO(x) storage-reduction. , 2008, Physical chemistry chemical physics : PCCP.

[17]  P. Stair,et al.  Ultraviolet Raman spectroscopy characterization of coke formation in zeolites , 1997 .

[18]  A. Urakawa,et al.  Support Effects and Chemical Gradients along the Catalyst Bed in NOx Storage-Reduction Studied by Space- and Time-Resolved In Situ DRIFTS , 2009 .

[19]  John S. O. Evans,et al.  Parametric Rietveld refinement , 2007, Journal of applied crystallography.

[20]  S. Cuccaro,et al.  Erratum: 'New reactor dedicated to in operando studies of model catalysts by means of surface x-ray diffraction and grazing incidence small angle x-ray scattering' [Rev. Sci. Instrum. 78, 083902 (2007)] , 2007 .

[21]  M. Drakopoulos,et al.  High-energy X-ray diffraction using the Pixium 4700 flat-panel detector. , 2009, Journal of synchrotron radiation.

[22]  A. Dent,et al.  Combining diffuse reflectance infrared spectroscopy (DRIFTS), dispersive EXAFS, and mass spectrometry with high time resolution: Potential, limitations, and application to the study of NO interaction with supported Rh catalysts , 2007 .

[23]  C. Zhang,et al.  Influence of absorption on quantitative analysis in Raman spectroscopy , 2006 .

[24]  A. Dent,et al.  Tracing the conversion of aurichalcite to a copper catalyst by combined X-ray absorption and diffraction , 1991, Nature.

[25]  H. Topsøe,et al.  Developments in operando studies and in situ characterization of heterogeneous catalysts , 2003 .

[26]  A. Beale,et al.  Unraveling the crystallization mechanism of CoAPO-5 molecular sieves under hydrothermal conditions. , 2005, Journal of the American Chemical Society.

[27]  J. Grunwaldt,et al.  Axial variation of the oxidation state of Pt-Rh/Al2O3 during partial methane oxidation in a fixed-bed reactor: An in situ X-ray absorption spectroscopy study , 2005 .

[28]  Gwyn P. Williams The initial scientific program at the NSLS infrared beamline , 1990 .

[29]  Roberto Dinapoli,et al.  PILATUS: A single photon counting pixel detector for X-ray applications , 2009 .

[30]  B. Weckhuysen,et al.  Real time quantitative Raman spectroscopy of supported metal oxide catalysts without the need of an internal standard. , 2005, Physical chemistry chemical physics : PCCP.

[31]  M. Fernández-García,et al.  Multitechnique analysis of supported Pd particles upon dynamic, cycling CO/NO conditions: Size-dependence of the structure–activity relationship , 2010 .

[32]  B. Weckhuysen Chemical imaging of spatial heterogeneities in catalytic solids at different length and time scales. , 2009, Angewandte Chemie.

[33]  M. Newton Applying Dynamic and Synchronous DRIFTS/EXAFS to the Structural Reactive Behaviour of Dilute (≤1 wt%) Supported Rh/Al2O3 Catalysts using Quick and Energy Dispersive EXAFS , 2009 .

[34]  A. Marcelli,et al.  Infrared and X-ray simultaneous spectroscopy: a novel conceptual beamline design for time resolved experiments , 2010, Analytical and bioanalytical chemistry.

[35]  D. Ferri,et al.  First steps in combining modulation excitation spectroscopy with synchronous dispersive EXAFS/DRIFTS/mass spectrometry for in situ time resolved study of heterogeneous catalysts. , 2010, Physical chemistry chemical physics : PCCP.

[36]  U. Bentrup Combining in situ characterization methods in one set-up: looking with more eyes into the intricate chemistry of the synthesis and working of heterogeneous catalysts. , 2010, Chemical Society reviews.

[37]  D. E. Keller,et al.  Combining operando techniques in one spectroscopic-reaction cell: New opportunities for elucidating the active site and related reaction mechanism in catalysis , 2006 .

[38]  M. Janousch,et al.  In situ XAS and XRPD parametric rietveld refinement to understand dealumination of Y zeolite catalyst. , 2010, Journal of the American Chemical Society.

[39]  A. Urakawa,et al.  Space-Resolved Profiling Relevant in Heterogeneous Catalysis , 2009 .

[40]  D. Wermeille,et al.  The ID03 surface diffraction beamline for in-situ and real-time X-ray investigations of catalytic reactions at surfaces , 2009 .

[41]  B. Weckhuysen,et al.  Synchrotron radiation effects on catalytic systems as probed with a combined in-situ UV-vis/XAFS spectroscopic setup. , 2005, The journal of physical chemistry. B.

[42]  R. Bell,et al.  Tracking the formation of cobalt substituted ALPO-5 using simultaneous in situ X-ray diffraction and X-ray absorption spectroscopy techniques. , 2010, Physical chemistry chemical physics : PCCP.

[43]  Marco Milanesio,et al.  Studying modifications and reactions in materials by simultaneous Raman and X-ray powder diffraction at non-ambient conditions: methods and applications , 2009 .

[44]  B. Weckhuysen,et al.  Snapshots of a working catalyst: possibilities and limitations of in situ spectroscopy in the field of heterogeneous catalysis. , 2002, Chemical communications.

[45]  M. Fernández-García,et al.  "Oxidationless" promotion of rapid palladium redispersion by oxygen during redox CO/(NO+O2) cycling. , 2007, Angewandte Chemie.

[46]  Sergei G. Kazarian,et al.  Micro- and Macro-Attenuated Total Reflection Fourier Transform Infrared Spectroscopic Imaging , 2010 .

[47]  K. K. Hii,et al.  In situ investigation of the oxidative addition in homogeneous Pd catalysts by synchronised time resolved UV-Vis/EXAFS. , 2006, Chemical communications.

[48]  A. Dent,et al.  Rapid monitoring of the nature and interconversion of supported catalyst phases and of their influence upon performance: CO oxidation to CO2 by gamma-Al2O3 supported Rh catalysts. , 2006, Chemistry.

[49]  M. Fernández-García,et al.  Dynamic “operando” observation of 1 wt% Pd-based TWCs: Simultaneous XAS/DRIFTS/mass spectrometry analysis of the effects of Ce0.5Zr0.5O2 loading on structure, reactivity and performance , 2009 .

[50]  Marco Milanesio,et al.  Investigating Surface vs Bulk Kinetics in the Formation of a Molecular Complex via Solid-State Reaction by Simultaneous Raman/X-ray Powder Diffraction , 2009 .

[51]  N. A. Young,et al.  The first combined in situ FTIR and EXAFS study of a matrix isolated molecule , 1990 .

[52]  R. Prins,et al.  Application of synchrotron radiation to in situ characterization of catalysts , 1998 .

[53]  A. Marcelli,et al.  Time-resolved simultaneous detection of structural and chemical changes during self-assembly of mesostructured films , 2007 .

[54]  A. Dent,et al.  Identification of the surface species responsible for N2O formation from the chemisorption of NO on Rh/alumina. , 2007, Physical chemistry chemical physics : PCCP.

[55]  Marco Milanesio,et al.  In situ simultaneous Raman/high-resolution X-ray powder diffraction study of transformations occurring in materials at non-ambient conditions , 2007 .

[56]  Angelika Brückner,et al.  Looking on Heterogeneous Catalytic Systems from Different Perspectives: Multitechnique Approaches as a New Challenge for In Situ Studies , 2003 .

[57]  S. Belin,et al.  Time-resolved study of the oxidation of ethanol by cerium(IV) using combined quick-XANES, UV-vis, and Raman spectroscopies. , 2005, The journal of physical chemistry. A.

[58]  J R Helliwell,et al.  Synchrotron and neutron techniques in biological crystallography. , 2004, Chemical Society reviews.

[59]  A. Beale,et al.  Adding a third dimension to operando spectroscopy: a combined UV-Vis, Raman and XAFS setup to study heterogeneous catalysts under working conditions. , 2005, Chemical communications.

[60]  G. Somorjai,et al.  Molecular Studies of Catalytic Reactions on Crystal Surfaces at High Pressures and High Temperatures by Infrared−Visible Sum Frequency Generation (SFG) Surface Vibrational Spectroscopy , 1999 .

[61]  L. Rees,et al.  Spectroscopic Identification of the Active Site for CO Oxidation on Rh/Al2O3 by Concentration Modulation in situ DRIFTS , 1999 .

[62]  Stephen Naylor,et al.  Simultaneous Studies of Reaction Kinetics and Structure Development in Polymer Processing , 1995, Science.

[63]  W. Bras,et al.  Simultaneous monitoring of amorphous and crystalline phases in silicalite precursor gels. An in situ hydrothermal and time-resolved small- and wide-angle x-ray scattering study , 1994 .

[64]  U. Lienert,et al.  Synchrotron applications of an amorphous silicon flat-panel detector. , 2008, Journal of synchrotron radiation.

[65]  A. Beale,et al.  Spatiotemporal Multitechnique Imaging of a Catalytic Solid in Action: Phase Variation and Volatilization During Molybdenum Oxide Reduction , 2009 .

[66]  Cyril Petibois,et al.  A bright future for synchrotron imaging , 2009 .

[67]  Jork Leiterer,et al.  Linking Simultaneous In Situ WAXS/SAXS/Raman with Raman/ATR/UV–vis Spectroscopy: Comprehensive Insight into the Synthesis of Molybdate Catalyst Precursors , 2009 .

[68]  J. Grunwaldt,et al.  X-ray absorption spectroscopy under reaction conditions: suitability of different reaction cells for combined catalyst characterization and time-resolved studies , 2004 .

[69]  Williams,et al.  Synchrotron infrared spectroscopy at megabar pressures: Vibrational dynamics of hydrogen to 180 GPa. , 1992, Physical review letters.

[70]  A. Urakawa,et al.  Space- and time-resolved combined DRIFT and Raman spectroscopy: monitoring dynamic surface and bulk processes during NO(x) storage reduction. , 2008, Angewandte Chemie.

[71]  Duncan Akporiaye,et al.  SAPO-34 methanol-to-olefin catalysts under working conditions: A combined in situ powder X-ray diffraction, mass spectrometry and Raman study , 2009 .

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

[73]  M. Di Michiel,et al.  Combining time-resolved hard X-ray diffraction and diffuse reflectance infrared spectroscopy to illuminate CO dissociation and transient carbon storage by supported Pd nanoparticles during CO/NO cycling. , 2010, Journal of the American Chemical Society.

[74]  A. Beale,et al.  Probing the influence of X-rays on aqueous copper solutions using time-resolved in situ combined video/X-ray absorption near-edge/ultraviolet-visible spectroscopy. , 2006, The journal of physical chemistry. B.

[75]  A. Beale,et al.  Watching the crystallisation of complex oxides by in situ X-ray techniques , 2007 .

[76]  Rose-Noëlle Vannier,et al.  Elucidating the genesis of Bi2MoO6 catalyst by combination of synchrotron radiation experiments and Raman scattering. , 2009, Chemical communications.

[77]  B. Weckhuysen,et al.  Dealing with a local heating effect when measuring catalytic solids in a reactor with Raman spectroscopy. , 2006, Physical chemistry chemical physics : PCCP.

[78]  Annick Rubbens,et al.  Synthesis of γ-Bi2MoO6 catalyst studied by combined high-resolution powder diffraction, XANES and Raman spectroscopy , 2010 .

[79]  A. Dent,et al.  Synchronous, time resolved, diffuse reflectance FT-IR, energy dispersive EXAFS (EDE) and mass spectrometric investigation of the behaviour of Rh catalysts during NO reduction by CO. , 2004, Chemical Communications.

[80]  W. Duncan,et al.  Infrared synchrotron radiation from electron storage rings. , 1983, Applied optics.

[81]  A. Dent,et al.  Rhodium dispersion during NO/CO conversions. , 2007, Angewandte Chemie.

[82]  Arturo Martínez-Arias,et al.  Dynamic in situ observation of rapid size and shape change of supported Pd nanoparticles during CO/NO cycling. , 2007, Nature materials.