Synthesis of methanol using copper–f block element bimetallic oxides as catalysts and greenhouse gases (CO2, CH4) as feedstock

Branco, Joaquim B.; Ferreira, Ana C.; Gonçalves, A.P.; Soares, C. O.; Gasche, T. Almeida

doi:10.1016/j.jcat.2016.06.007

Cited by 24 publications

(10 citation statements)

References 61 publications

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“…Noble metal-based compounds have been demonstrated to be very active for the catalytic syngas formation from methane. − However, aiming for less-expensive catalysts with comparable performances, bimetallic cobalt-actinide, copper-actinide, and nickel-actinide oxides were prepared and tested for partial oxidation of methane. , The first generation of catalysts was synthesized by Choudhary et al. via mixing of nickel or cobalt nitrate with uranyl nitrate and subsequent decomposition in air at higher temperatures .…”

Section: Heterogeneous Catalysis: Small-molecule Activation Using Ura...mentioning

confidence: 99%

“…In particular, the copper–cerium oxide catalyst derived from the intermetallic compound exhibited the highest intrinsic activity of ∼900 mL MeOH /m 2 Cu ·h. The high performance was ascribed to the synergetic interaction of copper oxide with the lanthanide oxide phase resulting in an electronic enrichment of the copper …”

Section: Heterogeneous Catalysis: Small-molecule Activation Using Ura...mentioning

confidence: 99%

“…180−183 However, aiming for less-expensive catalysts with comparable performances, bimetallic cobalt-actinide, copperactinide, and nickel-actinide oxides were prepared and tested for partial oxidation of methane. 133,184 The first generation of catalysts was synthesized by Choudhary et al via mixing of nickel or cobalt nitrate with uranyl nitrate and subsequent decomposition in air at higher temperatures. 185 Thereby, the order of performance was the following: NiO-ThO 2 > NiO-UO 2 > NiO-ZrO 2 with NiO-ThO 2 showing the highest conversion of methane (∼95%) with a CO and H 2 selectivity of >96% at 800 °C.…”

Section: Solar Thermal and Electrocatalyticmentioning

confidence: 99%

“…Both bimetallic copper-lanthanide/copper-actinide oxides derived from the oxidation of intermetallic compounds and the corresponding bimetallic oxides supported on alumina were tested as catalysts for the formation of methanol from carbon dioxide and hydrogen in the presence of methane according to reaction (Scheme 7). 184 However, Branco et al have shown that the addition of methane is detrimental for the formation of methanol, especially in the case of alumina supported catalysts, and consequently, the reaction was performed solely in the presence of carbon dioxide and molecular hydrogen (Scheme 8). 184 In the absence of methane, all copper f-block element oxide catalysts showed a higher activity than the commercial copper catalyst.…”

Section: Solar Thermal and Electrocatalyticmentioning

confidence: 99%

“…184 However, Branco et al have shown that the addition of methane is detrimental for the formation of methanol, especially in the case of alumina supported catalysts, and consequently, the reaction was performed solely in the presence of carbon dioxide and molecular hydrogen (Scheme 8). 184 In the absence of methane, all copper f-block element oxide catalysts showed a higher activity than the commercial copper catalyst. In particular, the copper−cerium oxide catalyst derived from the intermetallic compound exhibited the highest intrinsic activity of ∼900 mL MeOH /m 2 Cu •h.…”

Section: Solar Thermal and Electrocatalyticmentioning

confidence: 99%

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Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

et al. 2019

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The chemistry of actinide molecules and materials has shown remarkable conceptual advancements in the past decade illustrating their unique reactivity profiles, when compared with lanthanides and transition elements, but there are still some challenging questions on the intriguing stability of low valent states and the significant role of 5f orbitals in bonding and reactivity of actinides. The distinctive electronic flexibility of actinide centers makes them potential catalysts for heterogeneous molecular transformations because of the kinetic lability of their coordination states and facile switching among oxidaton states. Actinide-enabled chemical transformations such as the six-electron reduction of dinitrogen into two reactive ammonia molecules or four-electron oxidation of water into oxygen under mild conditions are promising pathways in the quest of high-efficiency heterogeneous catalysts. This Review provides a comprehensive account on actinide-mediated catalytic transformation of small molecules such as CO, CO2, N2, O2, H2O, CH4, HCl, and NH3. The emphasis is placed on the emerging phenomena in actinide-based solid catalysts and controlled synthesis of nanostructured actinide materials as pristine and substrate-grown phases. The mechanistic investigations highlight the influence of the 5f electrons in multielectron transfer reactions and the propensity of actinide centers to achieve higher oxidation states that defines the surface termination in actinide oxides. Finally, the status and perspectives of actinide-containing materials beyond the nuclear fuel applications is discussed, underlining their exciting chemistry and unexplored potential toward alternative catalytic energy production processes.

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Section: Heterogeneous Catalysis: Small-molecule Activation Using Ura...mentioning

confidence: 99%

Section: Heterogeneous Catalysis: Small-molecule Activation Using Ura...mentioning

confidence: 99%

Section: Solar Thermal and Electrocatalyticmentioning

confidence: 99%

Section: Solar Thermal and Electrocatalyticmentioning

confidence: 99%

Section: Solar Thermal and Electrocatalyticmentioning

confidence: 99%

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Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

et al. 2019

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Promotierungseffekte in der Methanolsynthese: Verständnis eines industriellen Katalysators für die Umsetzung von CO₂

Behrens

2016

Angewandte Chemie

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CO 2 -Umsetzung ·Heterogene Katalyse ·Katalysatorpromotierung ·Kupfer ·M ethanolsynthese Methanol ist eine wichtige Grundchemikalie,die im industriellen Maßstab über einem kupferbasierten Katalysator hergestellt wird. Die Kupfernanopartikel sind auf Zinkoxid fixiert und gleichzeitig mit einer Zinkspezies promotiert. Das eingespeiste Gas ist eine Mischung aus CO 2 ,C Ou nd H 2 (Synthesegas), und der Prozess wird industriell seit den 1960er Jahren bis auf kleinere Modifikationen und inkrementelle Optimierungen nahezu unverändert durchgeführt. Der Cu/ZnO-Katalysator,d er üblicherweise in der Industrie noch durch weitere Additive verbessert wird, wurde über Jahrzehnte im Hinblick auf die industrielle Methanolproduktion intensiv untersucht. Das Synthesegas wird dabei üblicherweise durch die Dampfreformierung von Erdgas oder die Kohlevergasung erhalten. Vora llem im späten 20. Jahrhundert wurden viele bahnbrechende Ergebnisse erarbeitet, wie die Struktursensitivitätd er Methanolsynthese oder die Identifizierung von CO 2 als direkte Kohlenstoffquelle für Methanol (und nicht CO) gemäßder Reaktion CO 2 + 3H 2 ! CH 3 OH + H 2 O. [1] Allerdings hat es hat den Anschein, dass die internationale Katalyseforschung diesen etablierten Katalysator danach etwas aus den Augen verloren hat. Einige wichtige Aspekte im Zusammenhang mit der Funktion von ZnO,d as von manchen als inerter Tr äger,v on anderen zusätzlich als "elektronischer Promoter" betrachtet wurde,oder die strukturelle Dynamik von Cu und Zn sowie der exakte Reaktionsmechanismus blieben zumindest teilweise noch kontrovers. Die Methanolsynthese über Cu/ZnO ist nun wieder in den Fokus vieler Forschungsgruppen gerückt, was mit einer stark wachsenden Anzahl an Publikationen einhergeht. Dieses wiedererwachte Interesse konnte z. B. auf dem kürzlich abgehaltenen internationalen Katalysekongress (ICC 2016) in Peking beobachtet werden, wo eine hochinteressante Sitzung diesem Thema gewidmet war. Die in jüngster Zeit erzielten und z. T. dort vorgestellten Fortschritte sind eindrucksvoll und basieren auf einer sehr breiten experimentellen und theoretischen Basis,d ie neue Synthesemethoden, [2] neue Einblicke aus der Quantenchemie, [3] der Modellkatalyse, [4] kinetische Experimente [5] und ausgeklügelte Katalysatorcharakterisierung [6] beinhaltet. Kürzlich haben außerdem Kuld et al. [7] eine exzellente Studie publiziert, die viele dieser Aspekte in einer einzigen Verçffentlichung kombiniert, um so die Rolle des Zn-Promoters umfassend zu dechiffrieren. Hohen Anteil an der Motivation fürdieses neue Interesse an Cu/ZnO hat das Faktum, dass dieses Material über seine Rolle in der konventionellen Synthesegaschemie hinaus eines der seltenen Beispiele füre inen Katalysator ist, der die Umsetzung von CO 2 in eine hçherwertige Chemikalie in einem industriellen Prozess katalysiert. Methanol kann als Tr eibstoff fürV erbrennungsmotoren oder Brennstoffzellen genutzt werden, und somit wäre ein Übergang vom fossilstämmigen Synthesegas hin zu einer Einspeisung von anthropogenem CO 2 (z. B. aus Punkt...

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Promoting the Synthesis of Methanol: Understanding the Requirements for an Industrial Catalyst for the Conversion of CO₂

Behrens

2016

Angew Chem Int Ed

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Synthesis of methanol using copper–f block element bimetallic oxides as catalysts and greenhouse gases (CO2, CH4) as feedstock

Cited by 24 publications

References 61 publications

Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

Promotierungseffekte in der Methanolsynthese: Verständnis eines industriellen Katalysators für die Umsetzung von CO₂

Promoting the Synthesis of Methanol: Understanding the Requirements for an Industrial Catalyst for the Conversion of CO₂

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Synthesis of methanol using copper–f block element bimetallic oxides as catalysts and greenhouse gases (CO2, CH4) as feedstock

Cited by 24 publications

References 61 publications

Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

Promotierungseffekte in der Methanolsynthese: Verständnis eines industriellen Katalysators für die Umsetzung von CO2

Promoting the Synthesis of Methanol: Understanding the Requirements for an Industrial Catalyst for the Conversion of CO2

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Product

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Promotierungseffekte in der Methanolsynthese: Verständnis eines industriellen Katalysators für die Umsetzung von CO₂

Promoting the Synthesis of Methanol: Understanding the Requirements for an Industrial Catalyst for the Conversion of CO₂