Applying Topological and Economical Principles in Catalyst Design: New Alumina–Cobalt Core–Shell Catalysts

Calderone, V. Roberto; Shiju, N. Raveendran; Ferré, Daniel Curulla; Rose, Amadeus; Thiessen, Johannes; Jess, Andreas; Roest, Els van der; Wiewel, Barbara V.; Rothenberg, Gadi

doi:10.1007/s11244-014-0313-5

Cited by 4 publications

(4 citation statements)

References 22 publications

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“…[26] Here, one might expect am uch better activity as the fit between the oxide support and the metal oxide crystals would enable the formation of smaller (and thus more active) particles. [26][27][28][29] The fact that this materialg ave < 5% conversion supports our hypothesis that the nitrogen-doped carbon is responsible for oxygen activation. We also studied the effect of metal-oxide loading on the catalytic activity.A ll metal oxides were prepared at two different loadings, 0.43 mmol g À1 and 1.3 mmol g À1 .T he higher loadings (shown in Ta ble 1) gave consistently highery ields by 20-30 %.…”

supporting

confidence: 65%

“…To rule out the possibility that carbon is simply not the ideal support for cobalt oxide, we synthesized an equivalent catalyst on γ‐Al 2 O 3 . Here, one might expect a much better activity as the fit between the oxide support and the metal oxide crystals would enable the formation of smaller (and thus more active) particles . The fact that this material gave <5 % conversion supports our hypothesis that the nitrogen‐doped carbon is responsible for oxygen activation.…”

Section: Catalytic Oxidation Of Cinnamyl Alcohol With Molecular Oxygementioning

confidence: 69%

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Cooperative Catalysis for Selective Alcohol Oxidation with Molecular Oxygen

Slot

Eisenberg

Noordenne

et al. 2016

Chemistry A European J

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The activation of dioxygen for selective oxidation of organic molecules is a major catalytic challenge. Inspired by the activity of nitrogen-doped carbons in electrocatalytic oxygen reduction, we combined such a carbon with metal-oxide catalysts to yield cooperative catalysts. These simple materials boost the catalytic oxidation of several alcohols, using molecular oxygen at atmospheric pressure and low temperature (80 °C). Cobalt and copper oxide demonstrate the highest activities. The high activity and selectivity of these catalysts arises from the cooperative action of their components, as proven by various control experiments and spectroscopic techniques. We propose that the reaction should not be viewed as occurring at an 'active site', but rather at an 'active doughnut'-the volume surrounding the base of a carbon-supported metal-oxide particle.

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confidence: 65%

Section: Catalytic Oxidation Of Cinnamyl Alcohol With Molecular Oxygementioning

confidence: 69%

Cooperative Catalysis for Selective Alcohol Oxidation with Molecular Oxygen

Slot

Eisenberg

Noordenne

et al. 2016

Chemistry A European J

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“…However, the carbon in question must also be made cheaply and simply in ton quantities 6. 22, 23 It is this combination of economic and scientific constraints that makes the search for platinum alternatives such an exciting challenge.…”

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confidence: 99%

A Simple Synthesis of an N‐Doped Carbon ORR Catalyst: Hierarchical Micro/Meso/Macro Porosity and Graphitic Shells

Eisenberg

Stroek

Geels

et al. 2015

Chemistry A European J

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Replacing platinum as an oxygen reduction catalyst is an important scientific and technological challenge. Herein we report a simple synthesis of a complex carbon with very good oxygen reduction reaction (ORR) activity at pH 13. Pyrolysis of magnesium nitrilotriacetate yields a carbon with hierarchical micro/meso/macro porosity, resulting from in situ templating by spontaneously forming MgO nanoparticles and from etching by pyrolysis gases. The mesopores are lined with highly graphitic shells. The high ORR activity is attributed to a good balance between high specific surface area and mass transport through the hierarchical porosity, and to improved electronic conductivity through the graphitic shells. This novel carbon has a high surface area (1320 m(2) g(-1) ), and high nitrogen content for a single precursor synthesis (∼6 %). Importantly, its synthesis is both cheap and easily scalable.

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“… − Hence, for selective hydrogenolysis of HMF to DMF, the challenge is how to keep the furan ring intact during the efficient hydrogenolysis of formyl and hydroxyl groups. Currently, to address the challenge, many heterogeneous catalysts, including Cu-, Ni-, Co-, Ru-, Pd-, and Pt-based monometallic catalysts, and their bimetallic catalysts, have been explored. ,− …”

Section: Introductionmentioning

confidence: 99%

Facile Synthesis of Kilogram-Scale Co-Alloyed Pt Single-Atom Catalysts via Ball Milling for Hydrodeoxygenation of 5-Hydroxymethylfurfural

Gan

Liu

et al. 2020

ACS Sustainable Chem. Eng.

113

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Catalytic conversion of biomass-derived 5-hydroxymethylfurfural (HMF) into high-quality biofuel 2,5-dimethylfuran (DMF) is significant for the utilization of biomass but remains a substantial challenge. Herein, we report a straightforward, eco-friendly, and scalable ball milling method for the synthesis of Co-alloyed Pt (Pt1/Co) single-atom alloy (SAA) catalysts at kilogram levels. The catalysts exhibit superior catalytic performance for the hydrodeoxygenation of HMF to DMF, obtaining 100% HMF conversion and 92.9% selectivity to DMF under 1.0 MPa H2 at 180 °C for 2 h. The reaction pathway is also investigated, which shows that the hydrogenolysis of the CO bond in HMF to form 2,5-dihydroxymethylfuran is the main route during the hydrodeoxygenation and promoted by the synergistic effect of Pt and Co. Pt1/Co SAA catalysts display excellent stability without aggregation after five successive runs. More inspiringly, our method achieves the mass production of Pt1/Co at the kilogram scale, rendering its potential for practical applications. Moreover, by varying acetylacetonate precursors, we show the general synthesis of different Co-supported noble metal SAA catalysts (M1/Co, M = Pd, Ru, Ir, and Rh). Our findings not only offer a facile and readily scalable synthetic approach of SAA catalysts but also open new avenue to the exploitation of biomass.

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Applying Topological and Economical Principles in Catalyst Design: New Alumina–Cobalt Core–Shell Catalysts

Cited by 4 publications

References 22 publications

Cooperative Catalysis for Selective Alcohol Oxidation with Molecular Oxygen

Cooperative Catalysis for Selective Alcohol Oxidation with Molecular Oxygen

A Simple Synthesis of an N‐Doped Carbon ORR Catalyst: Hierarchical Micro/Meso/Macro Porosity and Graphitic Shells

Facile Synthesis of Kilogram-Scale Co-Alloyed Pt Single-Atom Catalysts via Ball Milling for Hydrodeoxygenation of 5-Hydroxymethylfurfural

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