Volcano-shape glycerol oxidation activity of palladium-decorated gold nanoparticles

Zhao, Zhifang; Arentz, J.; Pretzer, Lori A.; Limpornpipat, Pongsak; Clomburg, James M.; González, Ramón; Schweitzer, Neil M.; Wu, Tianpin; Miller, Jeffrey T.; Wong, Michael S.

doi:10.1039/c4sc01001a

Cited by 68 publications

(60 citation statements)

References 70 publications

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“…CO 2 might be the gaseous product formed (not identified in the present case) during the reaction according to the reports of Liu et al . and Zhao et al . The carbon balance noted in the present work is agreement with that observed for the oxidation of glycerol using gold catalyst…”

Section: Resultsmentioning

confidence: 99%

The Enhanced Catalytic Performance and Stability of Ordered Mesoporous Carbon Supported Nano‐Gold with High Structural Integrity for Glycerol Oxidation

Murthy

Selvam

2018

The Chemical Record

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Ordered mesoporous carbon (OMC) supported gold nanoparticles of size 3–4 nm having uniform dispersion were synthesized by sol‐immobilization method. OMCs such as CMK‐3 and NCCR‐56 with high surface area and uniform pore size were obtained, respectively, using ordered mesoporous silicas such as SBA‐15 and IITM‐56 as hard templates, respectively. The resulting OMC supported monodispersed nano‐gold, i. e., Au/CMK‐3 and Au/NCCR‐56, exhibited excellent performance as mild‐oxidizing catalysts for oxidation of glycerol with high hydrothermal stability. Further, unlike activated carbon supported nano‐gold catalysts (Au/AC), the OMC supported nano‐gold catalysts, i. e., Au/CMK‐3 and Au/NCCR‐56, show no aggregation of active species even after recycling. Thus, in the case of Au/CMK‐3 and Au/NCCR‐56, both the fresh and regenerated catalysts showed excellent performane for the chosen reaction owing to an enhanced textural integrity of the catalysts and that with remarkable selectivity towards glyceric acid. The significance of the OMC supports in maintaining the dispersion of gold nanoparticles is explicit from this study, and that the activity of Au/AC catalyst is considerably decreased (∼50 %) upon recycling as a result of agglomeration of the active gold nanoparticles over the disordered amorphous carbon matrix.

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Section: Resultsmentioning

confidence: 99%

The Enhanced Catalytic Performance and Stability of Ordered Mesoporous Carbon Supported Nano‐Gold with High Structural Integrity for Glycerol Oxidation

Murthy

Selvam

2018

The Chemical Record

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“…34,35 Using the catalyst with high activity, the effects of stirring speed, H 2 ow rate and catalyst particle size were studied. To eliminate the effect of external and internal diffusions so that the catalytic performance can be reliably compared, preliminary experiments were carried out to determine the reaction conditions.…”

Section: Catalytic Reactionmentioning

confidence: 99%

Catalytic hydrogenation of isophthalonitrile (IPN) over supported monometallic and bimetallic catalysts

Liu

Wang

2015

RSC Adv.

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The hydrogenation of Isophthalonitrile (IPN) to meta-xylylenediamine (m-XDA) is usually catalyzed by RANEY® or supported Ni based catalysts in the presence of a basic additive. The supported catalysts have better mechanical strength and are safer than RANEY® Ni catalysts. This work aimed to study the catalytic performance of g-Al 2 O 3 supported Ni and Ni-M (M ¼ Fe, Co, Cu) bimetallic catalysts in IPN hydrogenation. The H 2 -TPR results revealed that the introduction of a second metal enhanced the reducibility of Ni catalyst. The Ni-M bimetallic catalysts also had different metal dispersion, electronic properties and adsorption strength. Among Fe, Co and Cu, Fe showed the best promoting effect, which was attributed to the strong N-metal bonding and weak H-metal adsorption strength, which enhanced the catalytic activity and m-XDA selectivity. The catalytic performance also strongly depended on the Ni-Fe mass ratio. For the g-Al 2 O 3 supported Ni and Ni-M catalysts with a low Ni loading of 5 wt%, the rate constant k r increased from 0.024 mol 0.2 L À0.2 min À1 over 5Ni/Al 2 O 3 to 0.033 mol 0.2 L À0.2 min À1 over 5Ni-1.67Fe/Al 2 O 3 , meanwhile the m-XDA selectivity increased from 34.7% to 49.5%. Over the Ni-Fe bimetallic catalyst with high metal loading, 20Ni-5Fe/Al 2 O 3 , a very high m-XDA selectivity of 99.9% was obtained. Fig. 5 Effect of the Ni-Fe ratio on catalytic performance of Ni-Fe/ Al 2 O 3 catalysts (a) Ni + Fe ¼ 6.25 wt%, (b) Ni ¼ 5 wt%.This journal is

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“…74,75 However, since large amounts of glycolic acid are being formed within the first reaction hour, where the carbon mass balance is practically closed, glycolic acid is likely to be formed as a primary reaction product from glycerol via glyceraldehyde or dihydroxyacetone as intermediates, as it was also reported previously. 30,44,76,77 The direct generation of glycolic acid from glycerol as a primary reaction product is also supported by the formation of large quantities of formic acid in the beginning of the reaction, which is a side product of the reaction from glycerol to glycolic acid. After the first hour of the reaction, the selectivity towards glyceric and glycolic acid steadily decreases as a result of their further oxidation towards higher oxidation products (oxalic and formic acid).…”

Section: View Article Onlinementioning

confidence: 87%

Selective glycerol oxidation over ordered mesoporous copper aluminum oxide catalysts

Schünemann

Tüysüz

2017

Catal. Sci. Technol.

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Glycerol is a major by-product of the biodiesel production and is therefore produced in high quantities. While currently there are limited possible applications for this highly functionalized molecule, glycerol can be a cheap and abundant feedstock for value-added products that are accessible by selective oxidation.Usually, the selective oxidation of glycerol utilizes expensive noble metal catalysts, such as Au, Pt, and Pd. Here we report the selective oxidation of glycerol in basic media, using ordered mesoporous Cu-Al 2 O 3 catalysts with various Cu loadings prepared by a facile soft-templating method. The materials were characterized in detail by nitrogen physisorption, vis-NIR spectroscopy, EDX, low-and wide-angle XRD, XPS, and TEM. Subsequently the reaction conditions for glycerol oxidation were optimized. The catalytic oxidation of glycerol yields C 3 products, such as glyceric acid and tartronic acid, and also C 2 and C 1 products, such as glycolic acid, oxalic acid, and formic acid. Moreover, the role of the solvent on the catalytic reaction was investigated, and the addition of various co-solvents to the aqueous reaction mixture was found to increase the initial reaction rate up to a factor of three. The trends of the initial reaction rates correlate well with the polarity of the water/co-solvent mixtures. The prepared Cu-Al 2 O 3 catalysts are a more costefficient and environmentally viable alternative to the reported noble metal catalysts.

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Volcano-shape glycerol oxidation activity of palladium-decorated gold nanoparticles

Abstract: Activity and selectivity of glycerol oxidation were highly dependent upon Pd surface coverage of Pd-on-Au bimetallic catalysts.

Cited by 68 publications

References 70 publications

The Enhanced Catalytic Performance and Stability of Ordered Mesoporous Carbon Supported Nano‐Gold with High Structural Integrity for Glycerol Oxidation

The Enhanced Catalytic Performance and Stability of Ordered Mesoporous Carbon Supported Nano‐Gold with High Structural Integrity for Glycerol Oxidation

Catalytic hydrogenation of isophthalonitrile (IPN) over supported monometallic and bimetallic catalysts

Selective glycerol oxidation over ordered mesoporous copper aluminum oxide catalysts

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