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by: Kobe Dare


Kobe Dare
GPA 3.6


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Class Notes
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This 25 page Class Notes was uploaded by Kobe Dare on Thursday October 22, 2015. The Class Notes belongs to THTR 2 at University of California Santa Barbara taught by Staff in Fall. Since its upload, it has received 29 views. For similar materials see /class/226857/thtr-2-university-of-california-santa-barbara in Theatre at University of California Santa Barbara.




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Date Created: 10/22/15
The Role of Au in Catalysis by PdAu Wayne Goodman Department of Chemistry Texas AampM University College Station TX USA The Role of Au in Catalysis by PdAu OUTLINE Introduction to issues and methodology Surface vs bulk composition IRAS amp TPD CO as a local probe of surface sites Isolated Pd as a reactive site AuPd Catalysis Vinyl Acetate VA Monomer PdA K 39139 CZH4 CH3COOH 12 02 3000 CH3COOCZH3 H20 510 atm gt100 2g 1 cm2 gagego 0093 0590 9000 Key Targets of Study 0 Mechanism of Au promotion 0 Active site description Vinyl Acetate VA Synthesis over Various Pd Catalysts 39lc2H439CH3co39oH 12 02 gt39 CH3050C2H3 Hzol 39 10392 Pd1quotoAu05 oSi02 VA Selectivity 96 Vw PC2H 75 kPa 10393 P02 10 kPa 90 VA reaction rate 1346011310 kpa Pd1 oSi02 molecules 39 25 nm 1 0 surface s1te lt 90 o Pd5Si02 38 nm Sec 1 104 lt20 Pd 100 a 10m 450 K 425 K 400 K 390 K 1 05 I I I I I I I I 39 220 225 230 235 240 245 250 255 1000TK391 YF Han D Kumar C Sivadinarayana and D W Goodman J CataL 224 60 2004 YF Han D Kumar C Sivadinarayana A Clearfield and D W Goodman CataL Lett 94 131 2004 YF Han D Kumar and D W Goodman J CataL 230 353 2004 YF Han JH Wang D Kumar Z You and D W Goodman LCataL 232 467 2005 Origin of Combustion Products C2H4 CH3COOH 12 02 gt CH3COOC2H3 H20 a Ethylene 02 gt C02 H20 3 AcOH20kPa 02 1 0 10OkPagt C02CO H20 r VA 02gtltgtC02 H20 No measurable rate of AcOH combustion at 413 K Only 50 increase in combustion rates upon addition of 35 kPa VA to mixture of CZH4 AcOH and 02 g Conclusion CO2 produced primarily from ethylene Y F Han D Kumar C Sivadinarayana and D W Goodman J Catal 224 60 2004 TPD Ethylene from Oxygencovered Pd100 VA RX HECQHMIWHEIM H2CCH2 3111 Zone Dun H2 1 g 439 7 V up I H chCads E E m in a I EU a H Hm 39 w 1 i I I I I 4 l I 1 EM 1m am 300 am 500 am 7m EDI WU 1cm IlII TEMPERATUREEK39J Figun L Tcmperaturbpmgrammad reacliun spectra uf ellhyiene admer on PM MUGFEE x IlaD at saturaticm ethyllena exposure The prnduct yields are listed in Table 2 ads Dlrod Mutation OHM r 2g commas Dom1466K Hpggmmn Inclinect Gombus nn t 7 Em 7 mumusual Wigwam wing2mm XC Guo and R J Madix J Am Chem Soc 1995117 5523 Key Issues Surface versus bulk composition Distribution of surface atoms I I l I 39I I I II P I 1 I 1 l l I 1 39 I 39 I 39 I 39 I 39 I 39 I 39 AuM0110 39 PdM01 0 1 monolayer 38 2 E ultil B 88 sec 39 39 m a er quot S E y 54133 multllayel g 39 5603 g was 739 E 003 E Baas 535MSZ JW 339 2415 39 15305 W Timil l lI all I 960 39103900 3911I00 3912I00 3913I00 3914I00 1500 b Temperature K Luo K eta J M01 Catalysis A Chemical 167 2001 191 AT CW Yi K Luo T Wei and D W Goodman J Phys Chem 109 18535 2005 PdAu Alloys Surface versus Bulk Composition Ion Scattering Spectroscopy USES Mo110 CW Yi K Luo T Wei and D W Goodman J Phys Chem 109 18535 2005 PdAu Alloys Surface versus Bulk Composition Pd Au Ion Scattering Spectroscopy USES ISS Intensity a u Mo110 03990 03995 13900 13905 13910 CW Yi K Luo T Wei andD W Goodman EEo J Phys Chem 109 18535 2005 ISS Intensity a u 090 Ion cattering pectrsc0py 095 5 ML Pds ML AuMo13910 Pd Au Ion Scattering Spectroscopy ISS Equilibrium surface achieved with 800 K anneal 13900 13905 13910 CW Yi K Luo T Wei andD W Goodman EEo J Phys Chem 109 18535 2005 ISS Intensity a u 090 Ion Scattering pectrscopy ISS 5 ML PdS ML AuMo1 10 095 Pd 100 EE Au 105 Surface Concentration of Pd Atomic 100 l 39 l 39 I 5ML Pd5ML AuMo110 5ML Au5ML PdMo110 200 39 l l I 39 400 600 800 Temperature K 100 Surface Concentration of Au Atomic oo 91 CW Yi K Luo T Wei and D W Goodman J Phys Chem 109 18535 2005 I 1 g 39 I I 39 39 2 39 39 39 g 80 s f I 39 ur ace s C D G Swartzfager 3 39 S B Ziemecki and E 60 l M Z Kelley JVST O o c Bulk 192 185 1982 9 0 395 i 2 40 o l I S o g 20 Annealed to 800 K o I m 0 O 20 4O 6O 80 100 Bulk Concentration of Au Atomic Surface Concentration of AuCu 0 20 40 60 80 Bulk Concentration of AuCu 100 Pd111 single crystal surface I mmquot raw 0quot 3 ABSORBANGE I 44 urpue ll 1151140 I I ma 1W 1W39 W MEHUHEERGMJJ Kuhn Szanyi and Goodman Surf Sci Lett 1992 274 L611 ABSOHBANGE 2200 a co Pd111 and Pd1 00 COde 1 2100 Frequency cm 2000 1mm 1 800 Szanyi Kuhn and Goodman J Vac Sci TechnolA 1993 11 1969 Absorbance IRAS COSML PdSML AuM0110 600 K anneal Pdrich surface Atop CO Bridging PdAu CO 1L l I l l l l 2200 2100 2000 1900 1800 1700 Wavenumber cm1 Absorbance 08 07 06 05 04 03 02 01 00 800 K anneal Aurich surface A 0 p Bridging CO P A C 0 d u 02L 01L K 005L H 002L l l I 2200 2100 2000 1900 1800 1700 Wavenumber cm1 quot 3 Pd monomers Pd dimers Aschoff et al Surf Sci 41 1998 L1051 O Pd multimers 10 Relative Amount 0 697 surface sites 86 Pd atoms Surface Pd coverage 12 f lNIo STM Pd in dark deposited onto Au111 Pd Atop siteUCO atop 2109 cm 1 2088 cm 1 2088 Absorbance Arbitrary Units oquot a m 2 m gt o u Pd7Au93 Pcl 5Aue5 2200 2100 2000 1900 Wavenumber cm391 F MarounF Ozanam 0 M Magnussen R J Behm Science 293 1811 2001 T PD COSML Pd 5 ML AuMo110 800 K Anneal CW Yi K Luo T Wei D W Goodman JPCB 2005 109 18535 28 QMS Intensity Arbitrary units mq 395ML39 Pdi5MI Au39IMo3911oj Anneal at 800 K for 20 min I 200 I I 300 400 Temperature K 4000 3000 m m o o 2000 1500 1000 QMS Intensity Arbitrary UnIts m o o 350010139 10 L39 COiQML39PdM39oa 10 bridge amp R threefold I 39 I 39 I 39 I 39 I 39 200 300 400 500 600 7 COPd111 Tods67K dr I2Ks 2 200 Temperature K 00 00100 TK X Guo and J T Yates JCP 9011 6761 1989 TPD CZH4 from Pd VS PdAu 0 10 ML Pd 2LC2D4TadS85K 50 ML Aul50 ML Pd 270 K 30au AMU 12039 16039 26039 22039 25039 32039 360 Temperature K Signi cant destabilization of ethylene on PdAu compared with pure Pd TPD Ethylene decomposition on Pd Au PdPdAulMo110 C2D4 ads ands E 100 Pd 3 39 Au 39 E lt 75Pd 50 Pd W 100 Au 200 300 400 500 600 Temperature K Hydrogen from adsorbed ethylene vs density of multiple Pd sites in PdAu Pd PdAulMo110 C2D4 ads ands 9997 05000 Production Yield a u 0 N As Pd multiple sites zero Ethylene dissociation zero 39 D2 00 02 04 06 08 139o Ethylene dissociation inhibited by formation of isolated Pd sites 3Fold HollowBridging Pd Site Density a u


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