Effects of Thiol Modifiers on the Kinetics of Furfural Hydrogenation over Pd Catalysts

Pang, Simon H.; Schoenbaum, Carolyn A.; Schwartz, Daniel K.; Medlin, J. Will

doi:10.1021/cs500598y

Cited by 114 publications

(138 citation statements)

References 33 publications

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“…The selective hydrogenation reaction of cinnamaldehyde has been demonstrated by modification of surface ligands on Pt nanocatalysts as shown in Figure 4a [37,[48][49][50]. By coating a variety of surface ligands on supported Pt nanocatalysts, the non-covalent interaction between cinnamaldehyde and surface ligands could be varied by simply tuning the chemical structures of ligands.…”

Section: Orientation Effect Of Surface Ligandsmentioning

confidence: 99%

Engineering Surface Ligands of Noble Metal Nanocatalysts in Tuning the Product Selectivity

Liu

Duay

et al. 2017

Catalysts

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Nanosized noble metal catalysts supported on high-surface-area support are of great importance for numerous industrial chemical processes to mediate reaction pathways in heterogeneous catalysis. Control of surface area and surface energy of nanocatalysts is a key to achieving high activity and selectivity for desired products. In the past decade, new synthetic methodologies for noble metal nanocatalysts with well-defined nanostructures have been developed. Wet-chemical preparation of noble metal nanocatalysts usually involves the utilization of specific surfactants that can bind the surface of nanocatalysts as ligands to control the nanostructures and prevent the coalescence of nanocatalysts. Surface ligands that form a densely packed self-assembled monolayer offer a facile solution to tune the surface energy of nanocatalysts, and, therefore, the selectivity of products. In this minireview, we highlight the recent advances in understanding the role of surface ligands in control over the product selectivity in a multi-product reaction using noble metal nanocatalysts. The review is outlined according to the three possible roles of surface ligands, including steric effect, orientation effect and surface charge state, in varying the adsorption/binding of reactants/transition states.

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Section: Orientation Effect Of Surface Ligandsmentioning

confidence: 99%

Engineering Surface Ligands of Noble Metal Nanocatalysts in Tuning the Product Selectivity

Liu

Duay

et al. 2017

Catalysts

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“…The initial hydrogenation step over noble metal catalysts is an aldehyde reduction followed by the reduction of the furan ring [22,24,25,56,57] as presented in Figure 1. Moreover, furfuryl alcohol can be hydrogenated into cyclopentanone almost quantitatively over Ru catalysts supported on acidic metal-organic frameworks [58].…”

Section: Hydrogenation Pathwaysmentioning

confidence: 99%

“…Nakagawa et al [22] demonstrated that introduction of Ir into Pd nanoparticles increases TOF due to increased adsorption of C=O bond. Pang et al [23,24] showed an increased aldehyde hydrogenation and hydrodeoxygenation selectivity with the introduction of thiols over Cu-based catalysts. O'Driscoll et al [25] demonstrated an excellent selectivity towards furfuryl alcohol over Pt-Sn catalysts in a range of solvents.…”

Section: Introductionmentioning

confidence: 99%

Hydrogenation of bio-oil into higher alcohols over Ru/Fe3O4-SiO2 catalysts

Cherkasov

Jadvani

Mann

et al. 2017

Fuel Processing Technology

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Permanent WRAP URL:http://wrap.warwick.ac.uk/91922 Copyright and reuse:The Warwick Research Archive Portal (WRAP) makes this work by researchers of the University of Warwick available open access under the following conditions. Copyright © and all moral rights to the version of the paper presented here belong to the individual author(s) and/or other copyright owners. To the extent reasonable and practicable the material made available in WRAP has been checked for eligibility before being made available.Copies of full items can be used for personal research or study, educational, or not-for-profit purposes without prior permission or charge. Provided that the authors, title and full bibliographic details are credited, a hyperlink and/or URL is given for the original metadata page and the content is not changed in any way. A note on versions:The version presented here may differ from the published version or, version of record, if you wish to cite this item you are advised to consult the publisher's version. Please see the 'permanent WRAP URL' above for details on accessing the published version and note that access may require a subscription. AbstractLiquid-phase hydrogenation of a solution of furfural, phenol and acetic acid has been studied in the 50-235 o C range over magnetic Ru/Fe3O4-SiO2 catalyst targeting the renewable production of second generation biofuels with minimum hydrogen consumption.Phenol was fully hydrogenated to cyclohexanol in the entire temperature range. Below 150 o C, furfural was mainly hydrogenated to tetrahydrofurfuryl alcohol while hydrogenolysis to cyclopentanol was the main reaction pathway above 200 o C. The hydrogenation rate was doubled in an acidic solution (pH=3) as compared to that at a pH 6. The spent catalyst was regenerated and reused in subsequent catalytic runs.

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“…Moreover, DFT calculations and UHV experiments have demonstrated that H 2 dissociative chemisorption on a pseudomorphic monolayer of Pd on Re(0 0 0 1) is unfavorable due to electronic perturbation (electron deficiency) of the Pd atoms [65][66][67][68]. Furfural decarbonylation requires contiguous Pd sites (e.g., on terraces), whereas hydrogenation can occur on edge or step sites [53,54,69]. Selectivity to the FAL increases with an increasing linear-to-bridging CO ratio in CO DRIFTS (indicating loss of threefold sites).…”

Section: Discussionmentioning

confidence: 99%

Catalysts for selective hydrogenation of furfural derived from the double complex salt [Pd(NH3)4](ReO4)2 on γ-Al2O3

Thompson

Lamb

2017

Journal of Catalysis

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a b s t r a c tThe double complex salt [Pd(NH 3 ) 4 ](ReO 4 ) 2 was employed as precursor of supported bimetallic catalysts for selective hydrogenation of furfural. Direct reduction of [Pd(NH 3 ) 4 ](ReO 4 ) 2 on c-Al 2 O 3 in flowing H 2 at 400°C yields bimetallic nanoparticles 1-2 nm in size that exhibit significant interaction between the metals, as evidenced by temperature-programmed hydride decomposition (complete suppression of b-PdH x formation), extended X-ray absorption fine structure spectroscopy at the Pd K and Re L III edges (PdARe distance = 2.72 Å), and scanning transmission electron microscopy with energy dispersive X-ray analysis. In contrast, calcination of [Pd(NH 3 ) 4 ](ReO 4 ) 2 on c-Al 2 O 3 at 350°C in air and subsequent reduction in H 2 at 400°C results in metal segregation and formation of large (>50 nm) supported Pd particles; Re species cover the Pd particles and c-Al 2 O 3 support. A PdRe 1:2 catalyst prepared by sequential impregnation and calcination using HReO 4 and [Pd(NH 3 ) 4 ](NO 3 ) 2 has a similar morphology.The catalyst derived by direct reduction of [Pd(NH 3 ) 4 ](ReO 4 ) 2 on c-Al 2 O 3 exhibits remarkably high activity for selective hydrogenation of furfural to furfuryl alcohol (FAL) at 150°C and 1 atm. Suppression of H 2 chemisorption via elimination of Pd threefold sites, as evidenced by CO diffuse-reflectance infrared Fourier transform spectroscopy, correlates with increased FAL selectivity.

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Effects of Thiol Modifiers on the Kinetics of Furfural Hydrogenation over Pd Catalysts

Cited by 114 publications

References 33 publications

Engineering Surface Ligands of Noble Metal Nanocatalysts in Tuning the Product Selectivity

Engineering Surface Ligands of Noble Metal Nanocatalysts in Tuning the Product Selectivity

Hydrogenation of bio-oil into higher alcohols over Ru/Fe3O4-SiO2 catalysts

Catalysts for selective hydrogenation of furfural derived from the double complex salt [Pd(NH3)4](ReO4)2 on γ-Al2O3

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