Transformation of Methane to Propylene: A Two‐Step Reaction Route Catalyzed by Modified CeO<sub>2</sub> Nanocrystals and Zeolites

He, Jieli; Xu, Ting; Wang, Zhihui; Zhang, Qinghong; Deng, Weiping; Wang, Ye

doi:10.1002/ange.201104071

Cited by 99 publications

(6 citation statements)

References 48 publications

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“…Ceria can uptake and release oxygen via the transformation between Ce 3+ and Ce 4+ , thus it can be widely used as active component or support in many catalytic reactions. [262][263][264][265][266][267][268] In recent years, CeO 2 nanomaterials with different morphologies have been extensively used in catalytic reactions and display excellent catalytic activity.…”

Section: Catalytic Applicationsmentioning

confidence: 99%

Shape-controlled synthesis and catalytic application of ceria nanomaterials

et al. 2012

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Because of their excellent properties and extensive applications, ceria nanomaterials have attracted much attention in recent years. This perspective provides a comprehensive review of current research activities that focus on the shape-controlled synthesis methods of ceria nanostructures. We elaborate on the synthesis strategies in the following four sections: (i) oriented growth directed by the crystallographic structure of cerium-based materials; (ii) oriented growth directed by the use of an appropriate capping reagent; (iii) growth confined or dictated by various templates; (iv) other potential methods for generating CeO(2) nanomaterials. In this perspective, we also discuss the catalytic applications of ceria nanostructures. They are often used as active components or supports in many catalytic reactions and their catalytic activities show morphology dependence. We review the morphology dependence of their catalytic performances in carbon monoxide oxidation, water-gas shift, nitric oxide reduction, and reforming reactions. At the end of this review, we give a personal perspective on the probable challenges and developments of the controllable synthesis of CeO(2) nanomaterials and their catalytic applications.

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Section: Catalytic Applicationsmentioning

confidence: 99%

Shape-controlled synthesis and catalytic application of ceria nanomaterials

et al. 2012

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“…In regard to nitrile synthesis from hydrocarbon feedstocks, the challenge of potentially practical and sustainable routes rely on activating C-H bonds at mild temperatures, as well as hindering the side reactions to selectively form nitriles. Today in the chemical industry, metal catalysts dominate the technology for producing chemicals25262728293031, and significant advances in green synthesis processes are mostly combined by the development of new catalysts. The metal catalysts for efficiently oxidative cyanation of C-H bonds are in great demand but extremely difficult to achieve.…”

mentioning

confidence: 99%

Controllable cyanation of carbon-hydrogen bonds by zeolite crystals over manganese oxide catalyst

Wang

Zhang

et al. 2017

Nat Commun

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The synthesis of organic nitriles without using toxic cyanides is in great demand but challenging to make. Here we report an environmentally benign and cost-efficient synthesis of nitriles from the direct oxidative cyanation of primary carbon-hydrogen bonds with easily available molecular oxygen and urea. The key to this success is to design and synthesize manganese oxide catalysts fixed inside zeolite crystals, forming a manganese oxide catalyst with zeolite sheath (MnOx@S-1), which exhibits high selectivity for producing nitriles by efficiently facilitating the oxidative cyanation reaction and hindering the side hydration reaction. The work delineates a sustainable strategy for synthesizing nitriles while avoiding conventional toxic cyanide, which might open a new avenue for selective transformation of carbon-hydrogen bonds.

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“…This performance does not meet the standard that is reported in the literature where S CHd 3 Cl > 70% at X CHd 4 > 10% is typically achieved. 11,13,23,46 A large part of the methane is converted to CO, which was the dominant product at temperatures above 490 °C.…”

Section: Methane Oxychlorination Over Mgmentioning

confidence: 99%

“…To put this conversion rate into a broader context, EuMg 3 Al MMO is one of the most active catalysts •h −1 under similar conditions. 13 The functionalization of the Mg x Al MMO was further evidenced by the preservation of the activity under 80% HCl, conditions under which the Mg x Al MMO did not perform well. The addition of Eu 3+ enhanced the methane conversion rate from 1.17 mmol•g cat…”

Section: Methane Oxychlorination Over Eu 3+mentioning

confidence: 99%

“…9−17 Several reported catalyst materials showed promising catalytic behavior in the MOC reaction. 9,11,13,18 High conversion levels of methane and good selectivity to the desired CH 3 Cl reaction product are achieved at a relatively mild temperature and pressure for benchmark catalysts. Even though the development of MOC catalysts is still in an early phase, a redox-active center apparently seems essential for enhanced catalytic performance in MOC chemistry.…”

Section: Introductionmentioning

confidence: 99%

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Europium–Magnesium–Aluminum-Based Mixed-Metal Oxides as Highly Active Methane Oxychlorination Catalysts

Terlingen

Bos

Ahr³

et al. 2023

ACS Catal.

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Methane oxychlorination (MOC) is a promising reaction for the production of liquefied methane derivatives. Even though catalyst design is still in its early stages, the general trend is that benchmark catalyst materials have a redox-active site, with, e.g., Cu2+, Ce4+, and Pd2+ as prominent showcase examples. However, with the identification of nonreducible LaOCl moiety as an active center for MOC, it was demonstrated that a redox-active couple is not a requirement to establish a high activity. In this work, we show that Mg2+–Al3+-based mixed-metal oxide (MMO) materials are highly active and stable MOC catalysts. The synergistic interaction between Mg2+ and Al3+ could be exploited due to the fact that a homogeneous distribution of the chemical elements was achieved. This interaction was found to be crucial for the unexpectedly high MOC activity, as reference MgO and γ-Al2O3 materials did not show any significant activity. Operando Raman spectroscopy revealed that Mg2+ acted as a chlorine buffer and subsequently as a chlorinating agent for Al3+, which was the active metal center in the methane activation step. The addition of the redox-active Eu3+ to the nonreducible Mg2+–Al3+ MMO catalyst enabled further tuning of the catalytic performance and made the EuMg3Al MMO catalyst one of the most active MOC catalyst materials reported so far. Combined operando Raman/luminescence spectroscopy revealed that the chlorination behavior of Mg2+ and Eu3+ was correlated, suggesting that Mg2+ also acted as a chlorinating agent for Eu3+. These results indicate that both redox activity and synergistic effects between Eu, Mg, and Al are required to obtain high catalytic performance. The importance of elemental synergy and redox properties is expected to be translatable to the oxychlorination of other hydrocarbons, such as light alkanes, due to large similarities in catalytic chemistry.

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Transformation of Methane to Propylene: A Two‐Step Reaction Route Catalyzed by Modified CeO₂ Nanocrystals and Zeolites

Cited by 99 publications

References 48 publications

Shape-controlled synthesis and catalytic application of ceria nanomaterials

Shape-controlled synthesis and catalytic application of ceria nanomaterials

Controllable cyanation of carbon-hydrogen bonds by zeolite crystals over manganese oxide catalyst

Europium–Magnesium–Aluminum-Based Mixed-Metal Oxides as Highly Active Methane Oxychlorination Catalysts

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Transformation of Methane to Propylene: A Two‐Step Reaction Route Catalyzed by Modified CeO2 Nanocrystals and Zeolites

Cited by 99 publications

References 48 publications

Shape-controlled synthesis and catalytic application of ceria nanomaterials

Shape-controlled synthesis and catalytic application of ceria nanomaterials

Controllable cyanation of carbon-hydrogen bonds by zeolite crystals over manganese oxide catalyst

Europium–Magnesium–Aluminum-Based Mixed-Metal Oxides as Highly Active Methane Oxychlorination Catalysts

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Transformation of Methane to Propylene: A Two‐Step Reaction Route Catalyzed by Modified CeO₂ Nanocrystals and Zeolites