Solid Catalysts for the Selective Low‐Temperature Oxidation of Methane to Methanol

Palkovits, Regina; Antonietti, Markus; Kuhn, Pierre; Thomas, Arne; Schüth, Ferdi

doi:10.1002/anie.200902009

Cited by 545 publications

(412 citation statements)

References 27 publications

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“…Remarkably, a small amount of Pt 0 and Pd 0 nanoparticles are also visible in the TEM (Fig. 9c), which is in agreement with the findings of Palkovits et al 18 Note that the total amount of Pd 0 found in the samples is significantly higher than that of Pt 0 . In both cases, however, the amount of metal formed is too small to be seen by XRD.…”

Section: Metal Dopingsupporting

confidence: 91%

A functional triazine framework based on N-heterocyclic building blocks

et al. 2012

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Covalent organic frameworks constitute a subclass of polymeric materials offering enhanced porosity, functionality and stability. In this work a covalent triazine framework based on bipyridine building blocks is presented, along with a comprehensive elucidation of its local structure, porosity, and capacity for metal uptake. A typical synthesis was carried out under ionothermal conditions at 400 700 C using ZnCl 2 as a Lewis acidic trimerization catalyst. A high degree of local order and the presence of triazine and bipyridine moieties are ascertained at a synthesis temperature of 400 C, along with micropores and specific surface areas of up to 1100 m 2 g 1 . Mesopores are increasingly formed at synthesis temperatures above 450 C, yielding highly porous frameworks with hierarchical porosity and exceptionally large surface areas in excess of 3200 m 2 g 1 at 700 C. We demonstrate the capability of the bipyridine unit to provide specific and strong binding sites for a large variety of transition metal ions, including Co, Ni, Pt and Pd. The degree of metal loading (up to 38 wt%) can be tuned by the metal concentration in solution and is dependent on both the type of metal as well as the temperature at which the CTF was synthesized. Evidence for site specific metal coordination bodes well for the use of metal loaded CTFs as heterogeneous catalysts carrying homogeneous type active sites.

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Section: Metal Dopingsupporting

confidence: 91%

A functional triazine framework based on N-heterocyclic building blocks

et al. 2012

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“…Palkovits et al [91] used Periana's molecular template and developed a covalent triazine-based framework (CTF) by trimerization of 2,6-dicyanopyridine in molten ZnCl 2 . This solid ligand coordinates PtCl 2 forming a solid analog to Periana's ðbpymÞPtCl 2 system (Fig.…”

Section: Methane Oxidation To Methanolmentioning

confidence: 99%

“…The catalyst undergoes an activation period but eventually reaches TONs above 250. The work of Palkovits et al [91] is an example of a low temperature heterogeneously catalyzed methane oxidation pathway. It illustrates nicely how heterogeneous catalysis can benefit from concepts of homogeneous catalysis.…”

Section: Methane Oxidation To Methanolmentioning

confidence: 99%

Methane Activation by Heterogeneous Catalysis

2014

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Methane activation by heterogeneous catalysis will play a key role to secure the supply of energy, chemicals and fuels in the future. Methane is the main constituent of natural gas and biogas and it is also found in crystalline hydrates at the continental slopes of many oceans and in permafrost areas. In view of this vast reserves and resources, the use of methane as chemical feedstock has to be intensified. The present review presents recent results and developments in heterogeneous catalytic methane conversion to synthesis gas, hydrogen cyanide, ethylene, methanol, formaldehyde, methyl chloride, methyl bromide and aromatics. After presenting recent estimates of methane reserves and resources the physico-chemical challenges of methane activation are discussed. Subsequent to this recent results in methane conversion to synthesis gas by steam reforming, dry reforming, autothermal reforming and catalytic partial oxidation are presented. The high temperature methane conversion to hydrogen cyanide via the BMA-process and the Andrussow-process is considered as well. The second part of this review focuses on one-step conversion of methane into chemicals. This includes the oxidative coupling of methane to ethylene mediated by oxygen and sulfur, the direct oxidation of methane to formaldehyde and methanol, the halogenation and oxyhalogenation of methane to methyl chloride and methyl bromide and finally the non-oxidative methane aromatization to benzene and related aromates. Opportunities and limits of the various activation strategies are discussed.

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“…56,57 For example, platinum coordinated at CTF (Pt-CTF) shows a promising performance as a solid catalyst for direct low-temperature oxidation of methane to methanol with high selectivity, activity, and stability. This catalyst shows a turnover frequency of ca.…”

Section: Synthesis and Applications Of Ctfsmentioning

confidence: 99%

Carbon- and Nitrogen-Based Porous Solids: A Recently Emerging Class of Materials

Sakaushi

Antonietti

2014

Bulletin of the Chemical Society of Japan

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118

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In this account, the emergence of a new family of porous solid-state materials based on carbon and nitrogen is discussed. This started with the observation that carbon nitride, a polymeric material with a composition close to C 3 N 4 , is not only unexpectedly thermally and chemically stable, but a semiconductor at the same time and able to catalyze a variety of chemical reactions, such as DielsAlder cyclizations, oxidations, and photochemical water splitting. Carbon nitride is however already sufficiently reviewed but related materials with similar potential have essentially been not sufficiently covered. The remaining structures are manifold and cover the range from on the one hand covalent triazine frameworks (CTFs) as new semiconducting porous solid-state materials to the other porous nitrogen-doped carbons (NdCs) as catalysts which are known to be applicable in a variety of electrocatalytic reactions. CTFs are porous polymeric frameworks constituted of triazine rings and other aromatic rings. Chemical binding motifs and crystal structures can be used to control the band structure of such an (organic) solid-state material. Porous NdCs are usually made by adding nitrogen sources to classical carbonization recipes, and they are attracting a lot of interest because of their catalytic activity for electrochemical processes, such as oxygen reduction reaction (ORR). This account will summarize state-ofthe-art work on those systems being next-generation catalysts for different kinds of reactions, which are affordable and high-performance catalysts with unique principle for emergence of catalytic activities, combining theoretical and experimental studies together with basic and applied science in a range of scientific fields from chemistry to physics. Indeed, the first exploration of the above materials as candidates for components of fuel cells and rechargeable metalair batteries are discussed.

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Solid Catalysts for the Selective Low‐Temperature Oxidation of Methane to Methanol

Cited by 545 publications

References 27 publications

A functional triazine framework based on N-heterocyclic building blocks

A functional triazine framework based on N-heterocyclic building blocks

Methane Activation by Heterogeneous Catalysis

Carbon- and Nitrogen-Based Porous Solids: A Recently Emerging Class of Materials

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