New catalytic materials for the high-temperature synthesis of hydrocyanic acid from methane and ammonia by high-throughput approach

Moehmel, S.; Steinfeldt, Norbert; Engelschalt, S.; Holeňa, Martin; Kolf, S.; Baerns, M.; Dingerdissen, Uwe; Wolf, Dorit; Weber, Robert S.; Bewersdorf, Martin

doi:10.1016/j.apcata.2007.09.035

Cited by 36 publications

(30 citation statements)

References 21 publications

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“…However, high throughput experimentation combined with genetic algorithm, analysis of variance and regression trees revealed that additives such as Ir, Au, Ni and Re and also alternative supports such as Si 3 N 4 or SiC have a positive effect on the HCN yield [52]. Addition of oxygen to a CH 4 =NH 3 feed enhances HCN formation rate by several orders of magnitude.…”

Section: Methane To Hydrogen Cyanidementioning

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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Section: Methane To Hydrogen Cyanidementioning

confidence: 99%

Methane Activation by Heterogeneous Catalysis

2014

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“…During the last decade, high-throughput (HT) methods have become an established tool for the evaluation of heterogeneous catalysts for different chemical processes [3][4][5][6][7][8][9][10][11][12][13][14][15][16]. hte's approach to HT testing is based on a patent filed on 3 March 1998, which relates to parallel reactor systems for testing the activity of solid catalysts simultaneously exposed to gaseous feed streams [17].…”

Section: Introductionmentioning

confidence: 99%

High-Throughput Screening as a Supplemental Tool for the Development of Advanced Emission Control Catalysts: Methodological Approaches and Data Processing

Sundermann¹,

Gerlach²

2016

Catalysts

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Abstract:A high-throughput (HT) screening platform developed at hte with the application focus on automotive catalysis is described. hte HT units are configured for performing steady-state testing, as well as dynamic tests with fast feed switches, such as lean/rich excursions for the evaluation of NO x storage capacity and efficiency of lean NO x traps (LNT), ammonia storage capacity for selective catalytic reduction (SCR), evaluation of oxygen storage capacity (OSC), as well as lambda sweep tests for screening of three-way catalysts (TWC). Even though catalysts are screened on a rather small scale (~100 mg powder), experience showed that dosing rather complex gas mixtures in concentrations close to that found in real exhaust for the given application is mandatory to generate relevant data. The objective of this work is to give additional insight into HT technology. In the industrial research laboratory, HT screening has matured to become a reliable approach for rapid screening of both reaction parameter spaces, as well as material properties relevant for exhaust gas catalyst development. Due to the speed of optimized screening involving 48 parallel reactors, automated handling of primary data is an imported requirement. Software for data reduction, like estimation of light-off temperature, needs to be robust and handle results for diverse sample libraries in an unattended fashion. In combination with the statistical design of experiment and multivariate data analysis, HT testing has become a valuable enhancement to automotive catalyst development.

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“…Baerns et al have studied the oxidative dehydrogenation of propane, using gaseous oxygen, [22][23][24] total propane oxidation, [25] and the production of hydrocyanic acid. [26] Yamada et al have investigated methanol synthesis, [27][28][29] and others have performed studies on (selective) oxidation, [30][31][32][33] reduction, [34] methane reforming, [35] and isomerisation. [36] Most of the catalysts used in these studies are mixed oxides containing four to five different metals.…”

Section: Qcementioning

confidence: 99%

Selective Hydrogen Oxidation Catalysts via Genetic Algorithms

et al. 2008

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Solid "oxygen reservoirs," such as doped ceria, can be successfully applied in a novel process for the oxidative dehydrogenation of propane. The ceria lattice oxygen selectively burns hydrogen from the dehydrogenation mixture at 550 8C. This gives three key advantages: it shifts the dehydrogenation equilibrium to the desired product side, generates heat in situ, which aids the endothermic dehydrogenation, and simplifies product separation. We have applied a genetic algorithm to screen doped cerias for their performance in the selective hydrogen oxidation. Three generations of doped ceria catalysts (61 catalysts in total), were synthesised. Dopants were chosen from a set of 26 elements, and with a maximum of two dopants per catalyst, at five different concentrations. The catalyst performance (activity and selectivity), is expressed by a fitness value. Each generation shows a higher average fitness value. The dopant type has a large effect on the catalyst fitness. We identified six dopant atoms which lead to selective hydrogen combustion catalysts, namely bismuth (Bi), chromium (Cr), copper (Cu), potassium (K), manganese (Mn), lead (Pb) and tin (Sn) ("good" dopants). Analysis of the effect of electronegativity, ionic radius and dopant concentration shows that most elements yielding a high fitness have electronegativities ranging from 1.5-1.9. Generally, the properties of catalysts containing two dopants can be predicted from the behaviour of singly doped ones. Synergy does occur for certain copper-, iron-and platinum-containing catalysts. The addition of calcium (Ca) or magnesium (Mg) to copper-doped catalysts doubles the activity, and the selectivity of iron doped catalysts can be improved by adding chromium (Cr), manganese (Mn) or zirconium (Zr). Importantly, the doped cerias show a high stability in the redox cycling, much higher than that of supported oxides. A Cr-and Zr-doped catalyst (Ce 0.90 Cr 0.05 Zr 0.05 O 2 ) was highly selective and active over 250 redox cycles (a total of 148 h on stream), with no phase segregation or change in particle size.

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New catalytic materials for the high-temperature synthesis of hydrocyanic acid from methane and ammonia by high-throughput approach

Cited by 36 publications

References 21 publications

Methane Activation by Heterogeneous Catalysis

Methane Activation by Heterogeneous Catalysis

High-Throughput Screening as a Supplemental Tool for the Development of Advanced Emission Control Catalysts: Methodological Approaches and Data Processing

Selective Hydrogen Oxidation Catalysts via Genetic Algorithms

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