A kinetic study of vinyl acetate synthesis over Pd-based catalysts: kinetics of vinyl acetate synthesis over Pd–Au/SiO and Pd/SiO catalysts

Han, Yi‐Fan; Wang, J.-H.; Kumar, Deepak; Yan, Zaoxue; Goodman, D. W.

doi:10.1016/j.jcat.2005.04.001

Cited by 126 publications

(76 citation statements)

References 35 publications

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“…The present results are discussed in the context of previous data reported from our laboratories for VA synthesis [12][13][14].…”

Section: Introductionsupporting

confidence: 76%

“…As evident in figure 3, changing p O 2 from 2.0 to 6.0 Torr while maintaining p C 2 H 4 and p AcOH constant at 9.0 and 4.0 Torr, respectively, the reaction rate increased from 4.5 Â 10 )5 to 7.5 Â 10 )5 s )1 at 423 K. Similarly, in changing p C 2 H 4 from 2.0 to 7.0 Torr (figure 4) while maintaining p O 2 and P AcOH constant at 8.5 and 3.2 Torr, respectively, the reaction rate decreased from 7.5Â10 )5 to 5.0Â10 )5 s )1 at 433 K. Varying p AcOH from 3.0 to 5.0 Torr (not shown) has little effect on the reaction rates for the Pd(100) catalyst [7,14], consistent with a similar behavior with respect to p AcOH reported earlier for Pd-5 and Pd-1 catalysts [12]. The reaction orders with respect to C 2 H 4 and O 2 , as summarized in table 1, were calculated by fitting the data to a power rate law:…”

Section: Kineticsmentioning

confidence: 95%

“…The reaction was carried out in a micro fixed-bed reactor connected to an online GC. The methodology for preparation of the supported catalyst and carrying out the reactivity measurements have been described in detail elsewhere [12,14]. The morphology, particle size, and chemical composition of the Pd catalysts, both fresh and used, were determined using transmission electron microscopy (TEM), X-ray diffraction (XRD) and XPS.…”

Section: Supported Catalystsmentioning

confidence: 99%

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Kinetic and Spectroscopic Studies of Vinyl Acetate Synthesis Over Pd(100)

et al. 2006

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A kinetic study of vinyl acetate (VA) synthesis over a Pd(100) catalyst is described, and the effect of particle-size on this reaction ascertained by comparing the single crystal data with data from supported Pd catalysts (5 wt% Pd/SiO 2 , d Pd =4.2 nm, and 1 wt% Pd/SiO 2 , d Pd =2.5 nm). A negative reaction order with respect to ethylene and a positive order with respect to oxygen were found for the model and supported catalytic systems, whereas the catalytic stability was strongly dependent on the particle size. The mechanism for VA synthesis is proposed to be identical on all catalysts studied based on the similarities of the kinetic parameters. Carbon-containing species on the poisoned Pd(100) catalyst were investigated by X-ray photoelectron spectroscopy (XPS), and the coverage was estimated to be approximately 1.5 ML after VA synthesis.KEY WORDS: kinetics of vinyl acehate synthesis; Pd(100) catalysts.

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“…The present results are discussed in the context of previous data reported from our laboratories for VA synthesis [12][13][14].…”

Section: Introductionsupporting

confidence: 76%

Section: Kineticsmentioning

confidence: 95%

Section: Supported Catalystsmentioning

confidence: 99%

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Kinetic and Spectroscopic Studies of Vinyl Acetate Synthesis Over Pd(100)

et al. 2006

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“…Bimetallic AuPd and AuPt catalysts have attracted much interest because of their enhanced performance compared to monometallic counterparts ( [19][20][21][22][23][24][25][26][27][28][29] and references therein), especially in hydrogenation [29], hydrodeoxygenation [20,26], hydrodesulfurisation [27,28], oxidation [21][22][23], and Catalysts 2017, 7, 233 6 of 10 other reactions (for review, see [19,24,25]). For example, the addition of gold to the bifunctional Pt/CsPW catalyst (CsPW = Cs 2.5 H 0.5 PW 12 O 40 ) for the hydrodeoxygenation of 3-pentanone has been found to increase catalyst activity and catalyst stability to deactivation, whereas the Au itself was inert in this reaction [26].…”

Section: Effect Of Gold Additivesmentioning

confidence: 99%

Selective Alkylation of Benzene by Propane over Bifunctional Pd-Acid Catalysts

et al. 2017

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Abstract:The alkylation of benzene by propane to yield isopropylbenzene (iPrPh) was studied using bifunctional Pd-acid catalysts, such as Pd-heteropoly acid and Pd-zeolite, in a fixed bed reactor at 300 • C and 1 bar pressure. Keggin-type tungstosilicic acid H 4 SiW 12 O 40 (HSiW) and zeolite HZSM-5 were used as the acid components in these catalysts. The reaction occurred most efficiently over 2%Pd/25%HSiW/SiO 2 , giving iPrPh with up to 88% selectivity. The Pd-HSiW catalyst was more selective than the Pd-HZSM-5; the latter gave only 11-18% iPrPh selectivity. The reaction proceeded via a bifunctional mechanism including the dehydrogenation of propane to form propene on Pd sites, followed by the alkylation of benzene with the propene on acid sites. The effect of Pd loading in Pd-HSiW and Pd-HZSM-5 catalysts indicated that the first step reached quasi-equilibrium at 1.5-2% Pd loading and the second step became rate limiting. The addition of gold to Pd-HSiW enhanced the activity of this catalyst, although the Au-HSiW without Pd was inert.

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“…In contrast, Pd-Au alloy catalysts have attracted much interest for their high stability under severe conditions. Pd-Au catalysts are frequently used as catalysts, for example, for CO and hydrocarbon oxidation, synthesis of vinyl acetate monomer, hydrocarbon hydrogenation, cyclotrimerization of acethylene, or CCl 2 F 2 (CFC-12) hydrodechlorination [4][5][6][7][8][9]. Pd and Au are completely miscible as a solid solution, and Pd is generally considered the catalytic center while the influence of Au is explained through either ''ensemble'' or ''ligand'' effects [10][11][12].…”

Section: Introductionmentioning

confidence: 99%

Experimental and Theoretical Study of CO Oxidation on PdAu Catalysts with NO Pulse Effects

Hao¹,

Shan²,

Hyun³

et al. 2009

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The effect of NO on CO oxidation was studied for Pt, Pd and PdAu catalysts. It was found that NO inhibits significantly the CO oxidation reactivity on both Pt and Pd catalysts. On PdAu catalyst, however, the presence of NO resulted in an enhancement of CO oxidation activity. In order to gain an atomistic understanding of this effect, densityfunction theory (DFT) calculations were performed on the adsorption and reaction properties of NO and CO on these metal surfaces. We have identified that the inhibition effects on Pt and Pd catalysts are due to stronger NO binding, and that the enhanced reactivity on PdAu is due to the reduced NO oxidation barrier on PdAu leading to NO 2 formation.

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A kinetic study of vinyl acetate synthesis over Pd-based catalysts: kinetics of vinyl acetate synthesis over Pd–Au/SiO and Pd/SiO catalysts

Cited by 126 publications

References 35 publications

Kinetic and Spectroscopic Studies of Vinyl Acetate Synthesis Over Pd(100)

Kinetic and Spectroscopic Studies of Vinyl Acetate Synthesis Over Pd(100)

Selective Alkylation of Benzene by Propane over Bifunctional Pd-Acid Catalysts

Experimental and Theoretical Study of CO Oxidation on PdAu Catalysts with NO Pulse Effects

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