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Increasing the efficiency of optimized v-sba-15 catalysts in the selective oxidation of methane to formaldehyde by artificial neural network modelling

2020, Kunkel, Benny, Kabelitz, Anke, Buzanich, Ana Guilherme, Wohlrab, Sebastian

The present study investigates the possibility of improving the selective oxidation of methane to formaldehyde over V-SBA-15 catalysts in two different ways. In a classical approach of catalyst optimization, the in situ synthesis of V-SBA-15 catalysts was optimized with regard to the applied pH value. Among the set of catalysts synthesized, a higher amount of incorporated vanadium, a higher content of polymeric VOx species as well as a less ordered structure of the support material were observed by increasing the pH values from 2.0 to 3.0. An optimum in performance during the selective oxidation of methane to formaldehyde with respect to activity and selectivity was found over V-SBA-15 prepared at a pH value of 2.5. With this knowledge, we have now evaluated the possibilities of reaction control using this catalyst. Specifically, artificial neural network modelling was applied after the collection of 232 training samples for obtaining insight into the influence of different reaction parameters (temperature; gas hourly space velocity (GHSV); and concentration of O2, N2 and H2O) onto methane conversion and selectivity towards formaldehyde. This optimization of reaction conditions resulted in an outstanding high space-time yield of 13.6 kgCH2O·kgcat·h−1. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.

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Rice husk derived porous silica as support for pd and CeO2 for low temperature catalytic methane combustion

2019, Liu, Dongjing, Seeburg, Dominik, Kreft, Stefanie, Bindig, René, Hartmann, Ingo, Schneider, Denise, Enke, Dirk, Wohlrab, Sebastian

The separation of Pd and CeO2 on the inner surface of controlled porous glass (CPG, obtained from phase-separated borosilicate glass after extraction) yields long-term stable and highly active methane combustion catalysts. However, the limited availability of the CPG makes such catalysts highly expensive and limits their applicability. In this work, porous silica obtained from acid leached rice husks after calcination (RHS) was used as a sustainable, cheap and broadly available substitute for the above mentioned CPG. RHS-supported Pd-CeO2 with separated CeO2 clusters and Pd nanoparticles was fabricated via subsequent impregnation/calcination of molten cerium nitrate and different amounts of palladium nitrate solution. The Pd/CeO2/RHS catalysts were employed for the catalytic methane combustion in the temperature range of 150–500◦C under methane lean conditions (1000 ppm) in a simulated off-gas consisting of 9.0 vol% O2, and 5.5 vol% CO2 balanced with N2. Additionally, tests with 10.5 vol% H2O as co-feed were carried out. The results revealed that the RHS-supported catalysts reached the performance of the cost intensive benchmark catalyst based on CPG. The incorporation of Pd-CeO2 into RHS additionally improved water-resistance compared to solely Pd/CeO2 lowering the required temperature for methane combustion in presence of 10.5 vol% H2O to values significantly below 500◦C (T90 = 425◦C). © 2019 by the authors. Licensee MDPI, Basel, Switzerland.

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Synthesis and molecular structures of the lowest melting odd- and even-numbered a,b-unsaturated carboxylic acids—(E)-hept-2-enoic acid and (E)-oct-2-enoic acid

2016, Sonneck, Marcel, Spannenberg, Anke, Wohlrab, Sebastian, Peppel, Tim

The molecular structures of the two lowest melting odd- and even-numbered α,β-unsaturated carboxylic acids—(E)-hept-2-enoic acid (C7) and (E)-oct-2-enoic acid (C8)—are herein reported. The title compounds were crystallized by slow evaporation of ethanolic solutions at −30 °C. C7 crystallizes in the triclinic space group P1¯ with two molecules in the unit cell and C8 in the monoclinic space group C2/c with eight molecules in the unit cell. The unit cell parameters for C7 are: a = 5.3049(2) Ă…, b = 6.6322(3) Ă…, c = 11.1428(5) Ă…, α = 103.972(3)°, β = 97.542(3)°, γ = 90.104(3)°, and V = 376.92(3) Ă…3 (T = 150(2) K). The unit cell parameters for C8 are: a = 19.032(10) Ă…, b = 9.368(5) Ă…, c = 11.520(6) Ă…, β = 123.033(11)°, and V = 1721.80(16) Ă…3 (T = 200(2) K).