Liquid phase oxidation of cyclohexane using bimetallic Au–Pd/MgO catalysts

Liu, Xi; Conte, Marco; Sankar, Meenakshisundaram; He, Qian; Murphy, D. M.; Morgan, David; Jenkins, Robert L.; Knight, David W.; Whiston, Keith; Kiely, Christopher J.; Hutchings, Graham J.

doi:10.1016/j.apcata.2015.02.034

Cited by 50 publications

(38 citation statements)

References 53 publications

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“…Nanometallic catalysts, in particular, often show superior performance compared to their bulk counterparts [1,2]. These catalysts, which are widely used in the chemical industry, have motivated experiments on new materials on the nanoscale with high catalytic activity and/or selectivity [3][4][5] and have inspired the development of computational methods for predicting new catalyst candidates and optimizing their efficiency [6,7].…”

Section: Introductionmentioning

confidence: 99%

Application of a parallel genetic algorithm to the global optimization of medium-sized Au–Pd sub-nanometre clusters

2018

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Abstract. To contribute to the discussion of the high activity and reactivity of Au-Pd system, we have adopted the BPGA-DFT approach to study the structural and energetic properties of medium-sized AuPd sub-nanometre clusters with 11-18 atoms. We have examined the structural behaviour and stability as a function of cluster size and composition. The study suggests 2D-3D crossover points for pure Au clusters at 14 and 16 atoms, whereas pure Pd clusters are all found to be 3D. For Au-Pd nanoalloys, the role of cluster size and the influence of doping were found to be extensive and non-monotonic in altering cluster structures. Various stability criteria (e.g. binding energies, second differences in energy, and mixing energies) are used to evaluate the energetics, structures, and tendency of segregation in sub-nanometre Au-Pd clusters. HOMO-LUMO gaps were calculated to give additional information on cluster stability and a systematic homotop search was used to evaluate the energies of the generated global minima of monosubstituted clusters and the preferred doping sites, as well as confirming the validity of the BPGA-DFT approach.

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Section: Introductionmentioning

confidence: 99%

Application of a parallel genetic algorithm to the global optimization of medium-sized Au–Pd sub-nanometre clusters

2018

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“…These data prompted us to consider the use of supported Ag–Pd nanoalloys prepared by using a sol‐immobilisation protocol to explore the possibility of synergistic effects between Ag and Pd, analogous to that observed for Au–Pd nanoalloys supported over MgO . A sample with a molar ratio of 1:1 between these two metals was initially prepared and tested (Table ).…”

Section: Resultsmentioning

confidence: 99%

“…Low cyclohexane conversion is therefore required to control the process at acceptable selectivities >80 % towards the two major commercial products cyclohexanol and cyclohexanone. In a previous study, by using Au–Pd nanoalloys supported on MgO, we found that these catalysts were capable of an enhanced conversion for cyclohexane oxidation of >10 % in the absence of organic initiators, while still preserving a high selectivity to cyclohexanol, as shown by Au/MgO catalysts . It was noted however that monometallic Au nanoparticles supported on MgO required the presence of a radical initiator such as azobisisobutyronitrile (AIBN) or tert ‐butyl hydroperoxide (TBHP) to show an appreciable catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

Catalytic Partial Oxidation of Cyclohexane by Bimetallic Ag/Pd Nanoparticles on Magnesium Oxide

Liu

Conte

et al. 2017

Chemistry A European J

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Abstract:The liquid phase oxidation of cyclohexane to cyclohexanol and cyclohexanone was investigated by synthesizing and testing an array of heterogeneous catalysts comprising: monometallic Ag/MgO, monometallic Pd/MgO and a set of bimetallic AgPd/MgO catalysts. Interestingly, Ag/MgO was capable of a conversion comparable to current industrial routes of ca. 5%, and with a high selectivity (up to 60%) to cyclohexanol, thus making Ag/MgO an attractive system for the synthesis of intermediates for the manufacture of nylon fibres. Furthermore, following the doping of Ag nanoparticles with Pd, the conversion increased up to 10% whilst simultaneously preserving a high selectivity to the alcohol. Scanning transmission electron microscopy and energy dispersive spectroscopy of the catalysts showed a systematic particle size composition variation with the smaller Ag-Pd nanoparticles being statistically richer in Pd. Analysis of the reaction mixture by Electron Paramagnetic Resonance (EPR) spectroscopy coupled with the spin trapping technique showed the presence of large amounts of alkoxy radicals, thus providing insights for a possible reaction mechanism.

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“…Furthermore, the catalytic performance of Cr 2 O 3 / MgO may further improve via treatment with a few portions of other transition metal oxides. For instance, the surface structure of Cr 2 O 3 /MgO has an impact on doping with small quantities of Co or manganese oxide, and an effort is made to associate the oxide-oxide or oxide-support interaction with catalytic activity (Liu et al 2015). This system is recorded to be promising for the catalytic conversion of isopropanol at 200°C-400°C using the flow system and catalytic decomposition of hydrogen peroxide at 20°C-40°C.…”

Section: Cr 2 O 3 /Mgo Heterogeneous Catalystmentioning

confidence: 97%

Magnesium oxide as a heterogeneous catalyst support

Julkapli

Bagheri

2016

Reviews in Inorganic Chemistry

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AbstractResearchers normally consider MgO as a promising high-surface-area heterogeneous catalyst support, additive, and promoter for many kinds of chemical reactions due to its certain properties, including stoichiometry and composition, cation valence, redox properties, acid-base character, and crystal and electronic structure. The presence of MgO as a support catalyst also modifies the electronic state of the overall catalytic performance by electron transfer between the native catalyst and MgO as support. The influence is clarified by alteration of acid-base properties of the catalyst-supported MgO. Meanwhile, the method, chemical composition, and condition in the preparation of MgO are the important factors affecting its surface and catalytic properties. Therefore, MgO with a high surface area and nanocrystalline structure has encouraging applications for some reactions, including as dry reforming, dehydrohalogenation, oxidative dehydrogenation of butane, nonoxidative dehydrogenation of ethylbenzene, decomposition of CCl

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Liquid phase oxidation of cyclohexane using bimetallic Au–Pd/MgO catalysts

Cited by 50 publications

References 53 publications

Application of a parallel genetic algorithm to the global optimization of medium-sized Au–Pd sub-nanometre clusters

Application of a parallel genetic algorithm to the global optimization of medium-sized Au–Pd sub-nanometre clusters

Catalytic Partial Oxidation of Cyclohexane by Bimetallic Ag/Pd Nanoparticles on Magnesium Oxide

Magnesium oxide as a heterogeneous catalyst support

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