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" dd@   " @ `"  n?" dd@   @@``PR    @ ` ` p>> IA(     `8oQqaqa1 ?5 Q i1Cliquez pour modifier le style de titre du masque22  d  ZLrQqaqa1 ?: Q rCliquez pour modifier le style de texte du masque Second niveau Troisime niveau Quatrime niveau Cinquime niveau2s    TwQqaqa1?*` ~Preparation of catalysts - Exercises Dalian, March-April 2012 */xxCC>                              b  <V~v@޽h @ ?"` 'ka=^Z3ey___PPT10Y+D=' = @B +  bullec 0 0( \y0 d  Zl$ss1 ? K  rCliquez pour modifier le style de texte du masque Second niveau Troisime niveau Quatrime niveau Cinquime niveau2s  p  01 ?U     `|4ss1?B/  @Laboratoire de Catalyse en Chimie Organique, UMR 6503, Poitiers.AAp                    t::ttB  s *rllC ? a(80___PPT10.J~   0( >s0(4G>s0  B  s *rllC ? a(80___PPT10.  0  8(    ZLQqaqa̙1 ?Q` DICP Course - Dalian, 2012 Preparation of solid catalysts Exercises Supported by the Chinese Academy of Sciences Charles Kappenstein, Professor Emeritus, University of Poitiers, France JE$~-~G~ ~@    f     6    S VA Xenc11http://english.dicp.cas.cn/images/enc11.jpg"`2uP ^  6A1? QA  XA??Picture 4T    A&??.Logo Univ PoitiersImage 8Logo Univ Poitiers.jpga   |A9??Logo-SFAPicture 28Logo-SFA6 { '  A;??Logo+IC2MPImage 8Logo+IC2MP.jpgs `?b  <V~v@޽h @ ?"  'ka=^Z3ey___PPT10Y+D=' = @B +   0L0   0Tx (  T T N*Qqaqa1?i !k  Exercice 1 (2  &      hh88* T N_qaqa1?$  Ex.1. A transition alumina support has been prepared; the determination of the specific surface area (SBET) and the porous volume (Vp) gave the following results: SBET = 200 m2 g-1 Vp = 1 mL g-1 a) Calculate the size of the pores (hint: use the cylindrical pore model with constant diameter) b) Is this alumina microporous, mesoporous or macroporous? c) What is the accuracy of the experimental data? (hint: the accuracy can be expressed as estimated relative standard deviation)0xg           %                                                                                                                                                                                                      hx) < T c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +  0L0  4 (  4 4 N`qaqa1?i !k  Exercice 2 (2  &      hh88R  4 NPqaqa1?J &Ex.2. A transition alumina support display a specific surface area SBET = 180 m2 g-1. It is used for the preparation of platinum supported catalysts Pt/Al2O3. The maximum loading of H2PtCl6 precursor is: 1.6 mol m-2. The number of surface hydroxyl groups is 8 OH nm-2. a) Compare the number of surface OH groups able to adsorb the precursor to the total number of surface OH groups (assumption: the adsorption need one OH group per precursor molecule). b) Describe the different steps of the preparation procedure. c) Determine the maximum platinum loading (in term of mass percentage) that can be reach at the end of the catalyst preparation. d) What would you suggest for the surface loading for 10 g of support? Calculate the initial pH for different surface loadings. Conclusion.00xD   G    bj3bjb<                                                                                                                                                                                     hx) < 4 c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +   0L0   @<6 (  < < Nqaqa1?i !k  Exercice 3 (2  &      hh88 < N<qaqa1?  jEx.3. We have prepared a catalyst Ir/Al2O3 for the decomposition of hydrazine for space propulsion. The characteristics of the catalyst are: wt.-% Ir = 40 % Specific surface area of the support = 100 m2 g-1 Porous volume = 0.7 mL g-1 Ir crystallite size = 2 nm a) Estimate the pore diameter of the support b) Calcultate the distance x1 of Ir particles center to center on the surface c) Calculate the distance x2 of Ir particles center to center in the porous volume0x'     e L 6v                                                                                                                                                                                                hx) < < c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +   0L0 , $ `D(  D D Nxqaqa1?i !k  Exercice 4 (2      hh88 D NLqaqa1?`^  vEx.4. Preparation of a copper catalyst on silica (200 m2 g-1) We prepare a solution containing the complex tetraamminecopper(II) [Cu(NH3)4]2+ by adding commercial concentrated ammonia (28 wt.-%, density 0.898 kg L-1) to 50 mL of an aqueous solution containing copper nitrate 0.2 mol L-1; the final pH is 12. The pKa of the acid-base couple NH4+/NH3 is 9.25 at 25 C a) Concentration of the commercial ammonia solution? b) Concentration of ammonia in an aqueous solution of pH 12 at 25C? c) Volume of the commercial ammonia solution to be to be added to reach pH 12? d) Final volume, concentration of copper and pH? Conclusion$w0x8  I   H F     b,l    N     <                                                                                                            (                hx) < D c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +   0L0   X (  X6 X Nqaqa1?k &Exercice 4 (cont d)(2 2        hh88# X Npqaqa1?` Ex.4. Preparation of a copper catalyst on silica (200 m2 g-1) We dip 8.5 g of silica into the solution at room temperature and maintain agitation for 2 h. Then we remove the impregnated support by filtration, wash with water, dried, then calcined under air at 300 C. We observe that 57 % of initial copper remains on the support as CuO. e) How can we obtain experimentally this value? f) Describe the silica surface in ammonia solution? Compare with the aqueous solution. g) What happen in the presence of the copper complex; what is the best procedure to impregnate silica? What is the surface density of copper complex (in nm-2)? h) Determine the wt.-% of CuO and Cu in the sample. How can we obtain experimentally this value? A sample of 100 mg is followed by H2 TPR. At 300 C, the H2 consumption is 1.44 cm3 (20 C, 1 bar); at 500 C, the H2 consumption is 1.55 cm3 (20 C, 1 bar) i) Determine the reduction rate for copper at both temperatures. What is the final wt.-% of Cu in the sample?*0x8  8bjbjbjbj!bjbj~bRP                                                                                                   hx) < X c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +z  0L0 L%(  L L Nqaqa1?i !k  Exercice 5 (2      hh88 L Nqaqa1? eEx.5. Study of a silica-supported copper catalyst Cu/SiO2 Cu cubic cell, Bravais lattice F, a = 3.6147 Loading level xm = 1 wt.-% Cu Dispersion = 10 % a) Determine: (i) the diameter of a copper atom, (ii) the atom surface density for the three faces (100), (110) and (111), (iii) the mean density, and (iv) the average distance LCu between two Cu atoms. b) Determine: (i) the surface area of copper Am (m2 g-1), (ii) the size of the copper particles d (nm), (iii) the number of copper particles (g-1), the perimeter of the interface metal/support (hint: cubic particles with one face in contact with support, edge length d, surface density = mean density). c) Calculate: (i) the total number of copper atoms present in one particle; (ii) the number and percentage of Cu atoms on the free edges and corners; (iii) the number and percentage of Cu atoms on the free faces and (iv) the number and percentage of atoms in contact with the support.0x8 0bjbjEbjbjbjYbjbZJ    )        d  hx) < L c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +   0L0   `p (  ` ` NQqaqa1?i !k  Exercice 6 (2      hh88. ` NLQqaqa1? @Ex.6. Characterization of a silica-supported copper catalyst Cu/SiO2 hydrogen is adsorbed on copper at 25 C without dissociation; the adsorption enthalpy is close to -40 kJ mol-1. a) Can we use hydrogen to determine the number of surface Cu atoms? Nitrous oxide decomposes on copper between 25 and 80 C following the reaction: N2O(g) + 2 Cu(surface) Cu-O-Cu(surface) + N2(g) Using 150 mg of the catalyst, we obtain 0.43 cm3 N2 (STP). Take data from Ex. 4. b) Determine the dispersion of copper and the metallic surface area. c) Calculate the size of the copper particles. d) We use electron microscopy; how many copper particles can we expect to see on a picture 200 nm x 200 nm? The copper atoms in contact with the support are more difficult to reduce. e) How ca we explain the TPR results?!0xC l  3pbfT           J      `  hx) < ` c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +/  0L0 >6h(  h h N HT4&                                                                                                                                                                                                                                                                                                                                                                                                                                                hx) < h c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +  0L0 pP(  p1 p NIqaqa1?i dk Exercice 7 (cont'd)(2 @          hh88 p NKqaqa1? aEx.7. Preparation of a Rh/Al2O3 catalyst The rhodium surface contains two types of rhodium atoms; the chemisorption enthalpies for hydrogen are respectively -72 kJ mol-1 (sites 1) and 80 kJ mol-1 (sites 2). The entropy factor0x    ~                                                                     hx) < p c $@޽h ? 'ka=^Z3ey___PPT10Y+D=' = @B +`  0   X(  X X C x0?ss1 ? 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Preparation of a Rh/Al2O3 catalyst The rhodium precursor is "RhCl3xH2O" and contains 39.2 wt.-% Rh. 50.00 g alumina are dip in 100 cm3 of aqueous HCl 0.100 mol L-1. Then, 1.00 g of precursor RhCl3xH2O is added and the mixture is stirred for 1 h. After filtration, the impregnated alumina is dried at 120 C for 6 h. The sample contains 1.10 wt.-% Cl. A) Determine the value of x in the precursor formula. B) With the assumption that all the precursor has been adsorbed onto the alumina, calculate the wt.-% for Cl and Rh. Explain why the experimental value for Cl is different. Explain why this precursor is able to be adsorbed quantitatively in acidic conditions. The dried catalyst is reduced (1 vol.-% H2 in Ar, 300 C, 20 cm3 min-1, 1 h) and characterized by H-chemisorption at 20 C. The hydrogen uptake is 0.62 cm3 (STP) C) Determine the rhodium dispersion (hint: 1 surface Rh atom can adsorb 1 H atom) D) Calculate the metallic area (1 Rh atom, 7.9 2) and the average size of Rh particles (cubic model)0x     A HT4&                                                                                                                                                                                                                                                                                                                                                                                                                                                 hx) < h c $@޽h ? 'ka=^Z3ey___PPT10Y+D='  = @B +r< x ՜.+,0p    Format A4 (210x297mm)N   Times New Roman WingdingsSymbolbullecDiapositive 1Diapositive 2Diapositive 3Diapositive 4Diapositive 5Diapositive 6Diapositive 7Diapositiv