Gold catalysis at the gas–solid interface: role of the support in determining activity and selectivity in the hydrogenation of m-dinitrobenzene

Cárdenas‐Lizana, Fernando; Gómez‐Quero, Santiago; Perret, Noémie; Keane, Mark A.

doi:10.1039/c1cy00051a

Cited by 70 publications

(42 citation statements)

References 103 publications

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“…Over Pd/C and Pt/C catalysts, the reaction condition has significant effects on the product selectivity. Supported Au catalysts, such as Au/Al 2 O 3 , Au/Fe 2 O 3 and Au/TiO 2 , could deliver 100% selectivity to m-NAN at about a 10% conversion of m-DNB [7][8][9][10]; however, the highest selectivity to m-NAN could not achieve 90% after conversion reached above 70%, due to m-NAN being further hydrogenated to m-PDA [5,8,11]. Ru/C was found to be efficient in the selective partial hydrogenation of o-, m-and p-DNBs, and the selectivities to the corresponding NANs achieved over 95% [3].…”

Section: Introductionmentioning

confidence: 99%

Selective Hydrogenation of m-Dinitrobenzene to m-Nitroaniline over Ru-SnOx/Al2O3 Catalyst

Cheng

Lin

et al. 2014

Catalysts

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Series catalysts of Ru-SnO x /Al 2 O 3 with varying SnO x loading of 0-3 wt% were prepared, and their catalytic activity and selectivity have been discussed and compared for the selective hydrogenation of m-dinitrobenzene (m-DNB) to m-nitroaniline (m-NAN). The Ru-SnO x /Al 2 O 3 catalysts were characterized by X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and hydrogen temperature-programmed reduction (H 2 -TPR) and desorption (H 2 -TPD). Under the modification of SnO x , the reaction activity increased obviously, and the best selectivity to m-NAN reached above 97% at the complete conversion of m-DNB. With the increasing of the SnO x loading, the amount of active hydrogen adsorption on the surface of the catalyst increased according to the H 2 -TPD analysis, and the electron transferred from Ru to SnO x species, as determined by XPS, inducing an electron-deficient Ru, which is a benefit for the absorption of the nitro group. Therefore, the reaction rate and product selectivity were greatly enhanced. Moreover, the Ru-SnO x /Al 2 O 3 catalyst presented high stability: it could be recycled four times without any loss in activity and selectivity.

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Section: Introductionmentioning

confidence: 99%

Selective Hydrogenation of m-Dinitrobenzene to m-Nitroaniline over Ru-SnOx/Al2O3 Catalyst

Cheng

Lin

et al. 2014

Catalysts

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“…This spillover hydrogen contributes to hydrogenation activity [28]. Spillover has been reported for supported Au catalysts following hydrogen treatment at 423-673 K and can be quantified by TPD [29]. The TPD profile for Au/CeO 2 (Fig.…”

Section: Resultsmentioning

confidence: 99%

Overcoming the limitations of gold catalysts in hydrogenation: enhanced activity with full hydrogen utilization

Keane

Collado

et al. 2018

Reac Kinet Mech Cat

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Application of nano-scale supported Au in catalytic hydrogenation delivers high chemoselectivity but low activity using (pressurized) H 2 far in excess of stoichiometric requirements. We have tackled the issues of low reaction rate and inefficient hydrogen utilization through a series of approaches taking Au/CeO 2 (mean Au size = 2.8 nm) as a test catalyst. Increased spillover hydrogen (using physical mixtures of Au/CeO 2 with CeO 2 and SiO 2 ) and the promotional effect of water (via catalytic dissociation on surface oxygen vacancies) resulted in a fourfold increase in the selective rate of furfural hydrogenation to furfuryl alcohol. In contrast, Pd/CeO 2 and Ni/CeO 2 promoted decarbonylation (to furan), hydrogenolysis (to 2-methylfuran) and ring reduction (to tetrahydrofurfuryl alcohol). Coupling (2-butanol ? 2-butanone) dehydrogenation over Cu/SiO 2 (mean Cu size = 7.8 nm) with furfural hydrogenation over Au/CeO 2 further increased rate with full utilization of the hydrogen generated in dehydrogenation. The coupling strategy allows ''hydrogen free'' hydrogenation that circumvents the limitation of Au in standard catalytic hydrogenation. This can open new avenues to exploit the ultra-selectivity of Au for continuous production of high value commodity products.

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“…It has been shown that spillover hydrogen (i.e. H 2 dissociation at a metal site with migration to the support [80]) can contribute to nitroarene hydrogenation activity [8,20,81]. Experimental and theoretical work have established that surface oxygen groups on carbon substrates serve to accommodate spillover hydrogen [79].…”

Section: Catalyst Activitymentioning

confidence: 97%

“…Oxides have been the most widely used Au and Ag carriers where support surface chemistry (e.g. Lewis aciditybasicity) can impact on hydrogenation performance [8,9]. Carbon offers a number of advantages over oxide supports, notably cost effectiveness, stability in acid and base media and the possibility of adjusting porosity, specific surface area (SSA > 600 m 2 g −1 ) and surface chemistry for specific catalytic applications [10].…”

Section: Introductionmentioning

confidence: 99%

Carbon supported gold and silver: Application in the gas phase hydrogenation of m -dinitrobenzene

Cárdenas‐Lizana

Pedro

Gómez‐Quero

et al. 2015

Journal of Molecular Catalysis A: Chemical

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Gold catalysis at the gas–solid interface: role of the support in determining activity and selectivity in the hydrogenation of m-dinitrobenzene

Cited by 70 publications

References 103 publications

Selective Hydrogenation of m-Dinitrobenzene to m-Nitroaniline over Ru-SnOx/Al2O3 Catalyst

Selective Hydrogenation of m-Dinitrobenzene to m-Nitroaniline over Ru-SnOx/Al2O3 Catalyst

Overcoming the limitations of gold catalysts in hydrogenation: enhanced activity with full hydrogen utilization

Carbon supported gold and silver: Application in the gas phase hydrogenation of m -dinitrobenzene

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