Towards the pressure and material gap in heterogeneous catalysis: hydrogenation of acrolein over silver catalysts
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1 Towards the pressure and material gap in heterogeneous catalysis: hydrogenation of acrolein over silver catalysts M. Bron 1, M. Bonifer 1, A. Knop-Gericke 2, D. Teschner 2, J. Kröhnert 2, F.C. Jentoft 2, R. Schlögl 2, P. Claus 1 1 Darmstadt University of Technology, Dep. Chemistry Chemical Technology II, Petersenstr. 20, Darmstadt, Germany 2 Department of Inorganic Chemistry, FHI Berlin, Faradayweg 4-6, Berlin, Germany
2 Hydrogenation of acrolein allyl alcohol (AyOH) acrolein = _ Ag S 1,2 = r 1 r 1 + r 2 = f (partial pressure, surface structure and composition) = _ propanal (PA) Control of intramolecular selectivity? Intrinsic selectivity to allyl alcohol when using Ag und Au catalysts [1, 2] [1] P. Claus, H. Hofmeister, J. Phys. Chem. B, 1999, 103, [2] P. Claus, A. Brückner, C. Mohr, H. Hofmeister, J. Am. Chem. Soc., 2000, 122, Poor selectivity to allyl alcohol when using Pt, Ru, Rh, Ni,... as hydrogenation catalysts
3 Pressure dependence of catalytic properties 9Ag/SiO 2 -IW M. Bron, E. Kondratenko, A. Trunschke, P. Claus, Z. Phys. Chem. 218 (2004) 405.
4 Acrolein hydrogenation: influence of preparation method (i.e., structural features of the silver catalyst) selectivity, conversion/% X AC S AyOH S PA S n-proh 0 10 bar 20 bar 0.2Ag/SiO 2 -S 10 bar 20 bar 10 bar 20 bar 9Ag/SiO 2 -P(NaOH) 9Ag/SiO 2 -IW
5 XPS/AES at Ag/SiO 2 catalysts Modified Augerparameter α α = E kin (Ag M 5 N 45 N 45 ) + E b (Ag 3d 5/2 ) independent of charging α = ev α = ev Ag α = ev α = ev Ag 2 O literature: E kin (Ag M 5 N 45 N 45 ) E b (Ag 3d 5/2 ) α Ag ev ev ev Ag 2 O ev ev ev L.H. Tjeng et al. PRB 41 (1990) A. Scheybal, A. Knop-Gericke, Electronic Structure, Dept. AC, Fritz-Haber-Institut (MPG), Berlin, Germany
6 TEM at Ag/SiO 2 catalysts 9Ag/SiO 2 -IW incipient wetness 9Ag/SiO 2 -P (NaOH) precipitation d Ag (9Ag/SiO 2 -IW) << d Ag (9Ag/SiO 2 -P(NaOH) Correlation particle size - product distribution/selectivity to allyl alcohol? M. Bron, E. Kondratenko, A. Trunschke, P. Claus, Z. Phys. Chem. 218 (2004) 405.
7 Structure sensitivity: particle size
8 Structure sensitivity: particle shape SC+ST MTP MTP Ag/SiO 2 SC: single crystalline, ST: single twinned, MTP: multiple twinned particles - Increasing defect number C. Mohr, H. Hofmeister, P. Claus, J. Catal. 213 (2003) 86.
9 In situ-xas under reaction conditions surface and gas phase related signal surface gas phase and gas related phase signal related signal Total Electron Yield [a.u.] C=C π * normal incidence grazing incidence C=O π * Ag(111) Photon Energy [ev] Total Total Electron Yield [a.u.] normal grazing incidence grazing incidence C=C C=C π * π * C=O π * normal incidence normal incidence grazing incidence C=O π * Ag(100) Photon Energie 288 [ev] Photon Energy [ev] Photon Energy [ev] Differences between Ag(100) und Ag(111) - Structure sensitivity of hydrogenation M. Bron, A. Knop-Gericke, D. Teschner, A. Scheybal, M. Hävecker, D. Wang, R. Födisch, D. Hönicke, R. Schlögl, P. Claus, submitted.
10 Orientation of reaction intermediates at the silver surface M. Bron, A. Knop-Gericke, D. Teschner, A. Scheybal, M. Hävecker, D. Wang, R. Födisch, D. Hönicke, R. Schlögl, P. Claus, submitted.
11 In situ-xas under reaction conditions M. Bron, A. Knop-Gericke, D. Teschner, A. Scheybal, M. Hävecker, D. Wang, R. Födisch, D. Hönicke, R. Schlögl, P. Claus, submitted.
12 Silver materials used within the GAP project Ag/SiO 2, Ag/ZnO Supported Ag with controlled particle size and shape Nanoscopic Ag (without support) Electrolyte silver Sputtered/electrochemically deposited Ag Ag foil Ag single crystals
13 Overview: Support free Silver materials used within the GAP project Silver Materials Catalysis Characterisation In situ experiments Single crystals No conversion at high pressures, beam-induced process in in situ- XAS-experiments (S AyOH low) In situ XAS: Orientation depends on crystal plane, C=O-accumulation at surface, In situ XPS Polycrystalline silver foil No conversion at high pressures, beam-induced process in in situ- XAS-experiments (S AyOH low) In situ XAS: C=O-accumulation at surface In situ XPS Electrolyte silver S AyOH 20 % (X = 2.5 % at 2 MPa) TAP: No interaction with hydrogen (as for pure SiO 2, but not Ag/SiO 2 ) Sputtered/electrochem S AyOH 23 % (X = 2.6 % at 2 MPa) XRD, XPS ically deposited silver nanoscopic silver: colloidal preparations precipitation S AyOH ca. 40 % (X = % at 2 MPa) TEM, XPS
14 Influence of ZnO-support on catalytic properties Conversion X, Selectivity S / % X Acrolein S Allyl alcohol S Propanal All catalysts: 5 % Ag Same preparation method (IW with AgNO 3 ) Reduction at 250 C Testing at 15 bar, 250 C 0 5Ag/ZnO "Merck" 5Ag/ZnO "EGA" 5Ag/ZnO "E" Different ZnO-support materials exhibit different selectivities with similar conversion
15 What influences selectivity? Hypothesis: selectivity depends on adsorption geometry. Adsorption geometry is is influenced by pressure (coverage) and structure of catalyst Pressure Increasing S AyOH with increasing partial pressure of acrolein at Ag/SiO 2 Why not with ZnO-supported catalyst?? Activation energy is not influenced by pressure - rate determing step Material Increasing S AyOH with smaller particles - larger number of kinks, edges, different exposed crystal planes, defects Support - can the support influence acrolein orientation?
16 Höhennormalisierte Intensität Hydrogen adsorption at silver: TAP-investigations H/D- Austausch an Ag/SiO 2 (iw) 1 (T=400 C) Zeit (s) H 2 HD D 2 HD-exchange occurs - dissociative adsorption of hydrogen at silver nanoparticles no hydrogen-activation when using electrolytic silver or pure SiO 2 -support M. Bron, E. Kondratenko, A. Trunschke, P. Claus, Z. Phys. Chem. 218 (2004) 405.
17 Flux (Moleküle / s) Hydrogen adsorption at silver: TAP-investigations H 2 - Pulse (Kat.: Ag/SiO 2 (NaOH), T=400 C) Experiment Simulation H 2 + ( ) <-> (H 2 ) (H 2 ) + ( ) <-> 2 (H) Zeit (s) k (400 C)/ s -1 E a / kj/mol 9Ag/SiO 2 -P k ads : (NaOH) k des : k dis : k ass : Ag/SiO 2 -IW k act : catalyst via precipitation (larger particles) H 2 + z z H H kads kdes k dis 2 + z k ass z H 2 2 z H catalyst via IW (smaller particles) k 2 z act z Different models have to be taken into account for the hydrogen adsorption at silver nanoparticles of different structure H
18 Flow adsorption calorimetry: hydrogen adsorption at silver catalysts Heat Flow/mW 0.28 cat.: 9Ag/SiO 2 -IW T Ads : 150 C pulse gas: 7% H 2 in Ar 0.26 Heat Flow/mW cat.: 9Ag/SiO 2 -F(NaOH) exothermic T Ads : 150 C pulse gas: H in Ar (increasing amount of pulsed gas) t/min t/min Different calorimetric responses - structure sensitivity of hydrogen adsorption at silver catalysts M. Bron, E. Kondratenko, A. Trunschke, P. Claus, Z. Phys. Chem. 218 (2004) 405.
19 Flow adsorption calorimetry: hydrogen adsorption at silver catalysts SiO 2 -supported catalysts: adsorption completely reversible 5Ag/ZnO Puls gas: 5 % H 2 in Ar Heat Flow / a.u. exothermic 150 C 250 C ZnO-supported catalysts: adsorption largely irreversible t / min
20 Infrared spectroscopy: H-D-exchange over Ag/SiO 2 catalysts A Ag/SiO 2 -P 523 K Reaktionsdauer min 1 min 2 min 3 min 4 min 5 min 10 min 20 min 30 min 40 min 60 min ~ u / cm -1 F. Jentoft et al., Poster Bunsentagung 2004
21 lnk Kinetics of isotope exchange from IR spectroscopy T / K D-H exchange (90 mbar) over Ag/SiO 2 -F) -4.5 E -5.0 A = 29.0 kj mol -1 R = T -1 / K -1 E A = 50.5 kj mol -1 R = Arrhenius plot of the isotopic exchange with H 2. Lower activation energy in presence of Ag.
22 Activation of hydrogen is structure sensitive weak (not dissoziative) adsorption of hydrogen at Ag(100) No measurable hydrogen activation using electrolytic silver Dissoziative adsorption of hydrogen at silver nanoparticles, mechanism depends on particle size/structure Different ratio edges/kinks to planes Different kind/number of defects Important role of support material Why is the selectivity to AyOH also influenced by partial pressure of hydrogen?
23 Schematic representation of the perimeter interface CH 3 CH 2 CHO "Perimeter- Interface" H 2 H* η 2 (C,O): π; di- σ "Macroligand" electronic effect η 2 (C,C): π; di- σ CHO O=C Ag, Au Oxidic support material + H* O η 4 (C,C,C,O) CH 2 =CH-CH 2 OH + H* OH co-ordination site for C=O (via MeOx?) steric effect
24 Thanks to GAP-project partners: Dr. R. Födisch, Prof. D. Hönicke (TU Chemnitz Further Cooperations: Dr. E. Kondratenko (ACA Berlin) TAP-measurements Dr. H. Hofmeister (MPI Halle) TEM-measurements AK Claus: Dipl.-Ing. M. Lucas N. Sargsyan J. Hohmeyer C. Breuer Dr. C. Mohr DFG for financial support within SP1091..and certainly you for your attention!
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