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The synthesis and characterization of sol-gel-derived cornhusk support for low-temperature catalytic methane combustion (LTCMC) were investigated in this study. The prepared cornhusk support was impregnated with palladium and cerium oxide (Pd/CeO2) via the classical incipient wetness method. The resulting catalyst was characterized using various techniques, including X-ray diffraction (XRD), N2 physisorption (BET), transmission electron microscopy (TEM), and hydrogen temperature-programmed reduction (H2-TPR). The catalytic performance of the Pd/CeO2/CHSiO2 catalyst was evaluated for methane combustion in the temperature range of 150–600 °C using a temperature-controlled catalytic flow reactor, and its performance was compared with a commercial catalyst. The results showed that the Pd/CeO2 dispersed on SiO2 from the cornhusk ash support (Pd/CeO2/CHSiO2) catalyst exhibited excellent catalytic activity for methane combustion, with a conversion of 50% at 394 °C compared with 593 °C for the commercial silica catalyst (Pd/CeO2/commercial). Moreover, the Pd/CeO2/CHSiO2 catalyst displayed better catalytic stability after 10 h on stream, with a 7% marginal loss in catalytic activity compared with 11% recorded for the Pd/CeO2/commercial catalyst. The N2 physisorption and H2-TPR results indicated that the cornhusk SiO2 support possessed a higher surface area and strong reducibility than the synthesized commercial catalyst, contributing to the enhanced catalytic activity of the Pd/CeO2/SiO2 catalyst. Overall, the SiO2 generated from cornhusk ash exhibited promising potential as a low-cost and environmentally friendly support for LTCMC catalysts. [ABSTRACT FROM AUTHOR]

In the present day, methanol is mainly produced from methane via reforming processes, but research focuses on alternative production routes. Herein, we present a chemo-/biocatalytic oxidation cascade as a novel process to currently available methods. Starting from synthetic biogas, in the first step methane was oxidized to formaldehyde over a mesoporous VOx/SBA-15 catalyst. In the second step, the produced formaldehyde was disproportionated enzymatically towards methanol and formic acid in equimolar ratio by formaldehyde dismutase (FDM) obtained from Pseudomonas putida. Two processing routes were demonstrated: (a) batch wise operation using free formaldehyde dismutase after accumulating formaldehyde from the first step and (b) continuous operation with immobilized enzymes. Remarkably, the chemo-/biocatalytic oxidation cascades generate methanol in much higher productivity compared to methane monooxygenase (MMO) which, however, directly converts methane. Moreover, production steps for the generation of formic acid were reduced from four to two stages. [ABSTRACT FROM AUTHOR]

Fe2O3, CoO4 and NiO nanoparticles were prepared via a citrate method and further functionalized with Pd by impregnation. The pure oxides as well as Pd/Fe2O3, Pd/CoO4, and Pd/NiO (1, 5 and 10 wt % Pd) were employed for catalytic methane combustion under methane lean (1 vol %)/oxygen rich (18 vol %, balanced with nitrogen) conditions. Already, the pure metal oxides showed a high catalytic activity leading to complete conversion temperature of T100 ≤ 500 ?°C. H2-TPR (Temperature-programmed reduction) experiments revealed that Pd-functionalized metal oxides exhibited enhanced redox activity compared to the pure oxides leading to improved catalytic combustion activity at lower temperatures. At a loading of 1 wt % Pd, 1Pd/CoO4 (T100 = 360 ?°C) outperforms 1Pd/Fe2O3 (T100 = 410 ?°C) as well as 1Pd/NiO (T100 = 380 ?°C). At a loading of 10 wt % Pd, T100 could only be slightly reduced in all cases. 1Pd/CoO4 and 1Pd/NiO show reasonable stability over 70 h on stream at T100. XPS (X-ray photoelectron spectroscopy) and STEM (Scanning transmission electron microscopy) investigations revealed strong interactions between Pd and NiO as well as CoO4, respectively, leading to dynamic transformations and reoxidation of Pd due to solid state reactions, which leads to the high long-term stability. [ABSTRACT FROM AUTHOR]

The molecular structures of the two lowest melting odd- and even-numbered a,b-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) Å, b = 6.6322(3) Å, c = 11.1428(5) Å, α = 103.972(3)°, β = 97.542(3)°, γ = 90.104(3)°, and V = 376.92(3) ų (T = 150(2) K). The unit cell parameters for C8 are: a = 19.032(10) Å, b = 9.368(5) Å, c = 11.520(6) Å, β = 123.033(11)°, and V = 1721.80(16) ų (T = 200(2) K). [ABSTRACT FROM AUTHOR]

Literature on zeolite membranes in catalytic reactions is reviewed and categorized according to membrane location. From this perspective, the classification is as follows: (i) membranes spatially decoupled from the reaction zone; (ii) packed bed membrane reactors; (iii) catalytic membrane reactors and (iv) zeolite capsuled catalyst particles. Each of the resulting four chapters is subdivided by the kind of reactions performed. Over the whole sum of references, the advantage of zeolite membranes in catalytic reactions in terms of conversion, selectivity or yield is evident. Furthermore, zeolite membrane preparation, separation principles as well as basic considerations on membrane reactors are discussed. [ABSTRACT FROM AUTHOR]

The molecular structures of (E)-non-2-enoic acid (C9) and (E)-dec-2-enoic acid (C10) are reported. The title compounds were crystallized by slow evaporation of ethanolic solutions at -30 °C. C9 crystallizes in the monoclinic space group P21/c and C10 in the tri clinic space group P-1, each with 4 molecules in the unit cell. The unit cell parameters for C9 are: a = 10.6473(4) Å, b = 5.2855(2) Å, c = 17.0313(7) Å; β = 106.0985(10)° and V= 920.87(6) ų. The unit cell parameters for C10 are: α = 4.1405(2) Å, b = 15.2839(6) Å, c = 17.7089(7) Å; α = 68.3291(11)°, β = 83.3850(13)°, γ = 85.0779(12)° and V= 1033.39(8) ų. [ABSTRACT FROM AUTHOR]

The valorization of carbon dioxide by diverting it into useful chemicals through reduction has recently attracted much interest due to the pertinent need to curb increasing global warming, which is mainly due to the huge increase of CO2 emissions from domestic and industrial activities. This approach would have a double benefit when using the green hydrogen generated from the electrolysis of water with renewable electricity (solar and wind energy). Strategies for the chemical storage of green hydrogen involve the reduction of carbon dioxide to value-added products such as methane, syngas, methanol, and their derivatives. The reduction of CO2 at ambient pressure to methane or carbon monoxide are rather facile processes that can be easily used to store renewable energy or generate an important starting material for chemical industry. While the methanation pathway can benefit from existing infrastructure of natural gas grids, the production of syngas could be also very essential to produce liquid fuels and olefins, which will also be in great demand in the future. In this review, we focus on the recent advances in the thermocatalytic reduction of CO2 at ambient pressure to basically methane and syngas on the surface of supported metal nanoparticles, single-atom catalyst (SACs), and supported bimetallic alloys. Basically, we will concentrate on activity, selectivity, stability during reaction, support effects, metal-support interactions (MSIs), and on some recent approaches to control and switch the CO2 reduction selectivity between methane and syngas. Finally, we will discuss challenges and requirements for the successful introduction of these processes in the cycle of renewable energies. All these aspects are discussed in the frame of sustainable use of renewable energies. [ABSTRACT FROM AUTHOR]

The separation of CO2 from gas streams is a central process to close the carbon cycle. Established amine scrubbing methods often require hot water vapour to desorb the previously stored CO2. In this work, the applicability of MFI membranes for H2O/CO2 separation is principally demonstrated by means of realistic adsorption isotherms computed by configurational-biased Monte Carlo (CBMC) simulations, then parameters such as temperatures, pressures and compositions were identified at which inorganic membranes with high selectivity can separate hot water vapour and thus make it available for recycling. Capillary condensation/adsorption by water in the microporous membranes used drastically reduces the transport and thus the CO2 permeance. Thus, separation factors of αH2O/CO2 = 6970 could be achieved at 70 °C and 1.8 bar feed pressure. Furthermore, the membranes were tested for stability against typical amines used in gas scrubbing processes. The preferred MFI membrane showed particularly high stability under application conditions. [ABSTRACT FROM AUTHOR]

For the determination of suitable catalysts, a high-throughput approach was chosen by Lenk et al. [[5]] to evaluate catalyst activity and to investigate interactions with pollutant gases or aging effects based on them. Choya et al. [[1]] investigated the influence of undesirable impurities, specifically alkali metals and in this case Na SP + sp , which may remain in the catalyst after the synthesis of Co SB 3 sb O SB 4 sb bulk catalysts. Liu and co-workers [[2]] used a metal foam monolithic catalyst Pd/Al SB 2 sb O SB 3 sb /Fe-Ni, which was placed in a quartz tube burner. [Extracted from the article]

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. [ABSTRACT FROM AUTHOR]

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). [ABSTRACT FROM AUTHOR]

Low-temperature hydrogen production from natural gas via steam reforming requires novel processing concepts as well as stable catalysts. A process using zeolite membranes of the type MFI (Mobile FIve) was used to enrich natural gas with liquefied petroleum gas (LPG) alkanes (in particular, propane and n-butane), in order to improve the hydrogen production from this mixture at a reduced temperature. For this purpose, a catalyst precursor based on Rh single-sites (1 mol% Rh) on alumina was transformed in situ to a Rh1/Al2O3 catalyst possessing better performance capabilities compared with commercial catalysts. A wet raw natural gas (57.6 vol% CH4) was fully reformed at 650 °C, with 1 bar absolute pressure over the Rh1/Al2O3 at a steam to carbon ratio S/C = 4, yielding 74.7% H2. However, at 350 °C only 21 vol% H2 was obtained under these conditions. The second mixture, enriched with LPG, was obtained from the raw gas after the membrane process and contained only 25.2 vol% CH4. From this second mixture, 47 vol% H2 was generated at 350 °C after steam reforming over the Rh1/Al2O3 catalyst at S/C = 4. At S/C = 1 conversion was suppressed for both gas mixtures. Single alkane reforming of C2–C4 showed different sensitivity for side reactions, e.g., methanation between 350 and 650 °C. These results contribute to ongoing research in the field of low-temperature hydrogen release from natural gas alkanes for fuel cell applications as well as for pre-reforming processes. [ABSTRACT FROM AUTHOR]