Simulation of methane partial oxidation over silica‐supported MoO3 and V2O5

Amiridis, Michael D.; Rekoske, James E.; Dumesic, James A.; Rudd, Dale F.; Spencer, Nicholas D.; Pereira, Candido

doi:10.1002/aic.690370108

Cited by 53 publications

(49 citation statements)

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“…In contrast, formaldehyde is the primary product over V O /SiO catalyst. A microkinetic approach, using a single set of physically realistic input assumptions, has identi"ed the elementary steps needed to "t the data for both of these catalysts (Amiridis et al, 1991). Reaction pathways for each catalyst are shown in Fig.…”

Section: Researchmentioning

confidence: 99%

Environmentally friendly processes

Pereira

1999

Chemical Engineering Science

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Environmental concerns have raised public awareness of environmental issues and are driving forces for regulation. The impact of regulation on the cost of production is expected to become important in determining the international competitiveness of the US chemical industry. In response to cost pressures, industry has launched a number of initiatives aimed at improving e$ciency and reducing environmental impact. Some of these environmental success stories are receiving increased national attention due to programs such as the Presidential Green Chemistry Challenge Awards Program. In addition to traditional metrics for evaluating process performance, such as productivity, environmental considerations increasingly are important in process development. Chemical processes evolve through life cycle phases, beginning with research, and then moving to process engineering, plant operation, and eventually, decommissioning. The number of technology options available for reducing environmental impact are highest early on in the life cycle and then decrease drastically. In contrast, costs associated with resolving an environmental problem typically increase exponentially as the process matures and the scale of equipment gets larger. There is, therefore, a considerable incentive to address and resolve environmental issues early in the life cycle. Chemical reactions responsible for producing high value-added products are, in most cases, also responsible for generating by-products and pollutants. New chemical and biochemical approaches are providing new reaction concepts. As in the development of traditional chemical and petrochemical processes, reaction engineering, broadly de"ned as the "eld that quanti"es the engineering aspects of chemically reactive systems, is providing enabling tools that accelerate the development of environmentally friendly processes. Core reaction engineering methods are being utilized for kinetic modeling, reactor selection, scale-up, and design. Meanwhile, the research frontiers are providing new reaction engineering tools, from computational chemistry to probe the nature of catalytic active sites to computational #uid dynamics modeling for designing the internals of reaction-separation systems. The long-term goal is to develop processes having 100% raw materials utilization, or zero waste. The near-term strategy for controlling emissions is to institute pollution prevention programs and install cost-e!ective end-of-pipe technologies. These technologies typically control generic classes of air pollutant emissions such as carbon monoxide, volatile organic compounds (VOCs), nitrogen oxides (NO V) and sulfur oxides (SO V). Technologies for treating wastewater are also available. Over time, a shift in focus is expected, from mere compliance to a point where environmentalism, like safety, is fully integrated into the corporate culture. The present paper discusses the role of reaction engineering in the development of environmentally-friendly processes. Select examples of processes, from the author's exper...

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Section: Researchmentioning

confidence: 99%

Environmentally friendly processes

Pereira

1999

Chemical Engineering Science

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“…The ion-radical mechanism has been reported for catalysts based on metal oxides containing ambivalent metals that are able to easily change their oxidation states, such as MoO 3 or V 2 O 5 . As a matter of fact, these two oxides supported on SiO 2 are the catalytic systems grabbing a majority of studies concerning the oxidation of methane into formaldehyde [4][5][6][7]. Similarly, the cited ambivalence is also present in the mixed iron oxide from magnetite, the major component in our catalytic system.…”

Section: Discussionmentioning

confidence: 89%

“…In any case, the direct oxidation of methane into methanol, formaldehyde, and other oxygenated products is still very far from being competitive for commercial implementation [2,3]. Among the catalysts employed for direct oxidation of methane to formaldehyde using molecular oxygen, those based on vanadium, molybdenum [4][5][6][7], and especially iron [3,[8][9][10][11][12][13][14][15][16][17] have shown the most promising performance. Nevertheless, the yield of formaldehyde reported with these catalysts does not exceed 5% [2,4,8,[18][19][20], although higher yields can be found in the literature for other catalysts.…”

Section: Introductionmentioning

confidence: 99%

(Ag)Pd-Fe3O4 Nanocomposites as Novel Catalysts for Methane Partial Oxidation at Low Temperature

et al. 2020

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Nanostructured composite materials based on noble mono-(Pd) or bi-metallic (Ag/Pd) particles supported on mixed iron oxides (II/III) with bulk magnetite structure (Fe3O4) have been developed in order to assess their potential for heterogeneous catalysis applications in methane partial oxidation. Advancing the direct transformation of methane into value-added chemicals is consensually accepted as the key to ensuring sustainable development in the forthcoming future. On the one hand, nanosized Fe3O4 particles with spherical morphology were synthesized by an aqueous-based reflux method employing different Fe (II)/Fe (III) molar ratios (2 or 4) and reflux temperatures (80, 95 or 110 °C). The solids obtained from a Fe (II)/Fe (III) nominal molar ratio of 4 showed higher specific surface areas which were also found to increase on lowering the reflux temperature. The starting 80 m2 g−1 was enhanced up to 140 m2 g−1 for the resulting optimized Fe3O4-based solid consisting of nanoparticles with a 15 nm average diameter. On the other hand, Pd or Pd-Ag were incorporated post-synthesis, by impregnation on the highest surface Fe3O4 nanostructured substrate, using 1–3 wt.% metal load range and maintaining a constant Pd:Ag ratio of 8:2 in the bimetallic sample. The prepared nanocomposite materials were investigated by different physicochemical techniques, such as X-ray diffraction, thermogravimetry (TG) in air or H2, as well as several compositions and structural aspects using field emission scanning and scanning transmission electron microscopy techniques coupled to energy-dispersive X-ray spectroscopy (EDS). Finally, the catalytic results from a preliminary reactivity study confirmed the potential of magnetite-supported (Ag)Pd catalysts for CH4 partial oxidation into formaldehyde, with low reaction rates, methane conversion starting at 200 °C, far below temperatures reported in the literature up to now; and very high selectivity to formaldehyde, above 95%, for Fe3O4 samples with 3 wt.% metal, either Pd or Pd-Ag.

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“…As described above, a number of studies have concerned the selective oxidation of methane by oxygen over the MoO x /SiO 2 catalysts [39,41,44,48,[49][50][51][52][53]. However, it remains questionable whether or not the supported MoO x catalysts are effective for the selective oxidation of ethane by oxygen to such oxygenates as CH 3 CHO.…”

Section: Selective Oxidation Of Ethane To Acetaldehyde and Formaldehymentioning

confidence: 96%

“…As far as the reaction mechanism is concerned, many early studies considered that the lattice oxygen species, particularly the terminal oxygen species (i.e. Mo=O and V=O), were responsible for the activation and oxidation of methane to HCHO [39][40][41][42][43][44] . Such a mechanism may be represented by the following reactions:…”

Section: Selective Oxidation Of Methane To Formaldehyde Over Heterogementioning

confidence: 99%

Catalytic selective oxidation or oxidative functionalization of methane and ethane to organic oxygenates

Wang

Zhang

2010

Sci. China Chem.

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Selective oxidation or oxidative functionalization of methane and ethane by both homogeneous and heterogeneous catalysis is presented concerning: (1) selective oxidation of methane and ethane to organic oxygenates by hydrogen peroxide in a water medium in the presence of homogeneous osmium catalysts, (2) selective oxidation of methane to formaldehyde over highly dispersed iron and copper heterogeneous catalysts, (3) selective oxidation of ethane to acetaldehyde and formaldehyde over supported molybdenum catalysts, and (4) oxidative carbonylation of methane to methyl acetate over heterogeneous catalysts containing dual sites of rhodium and iron.National Natural Science Foundation of China [20433030, 20625310, 20773099, 20873110]; National Basic Program of China [2005CB221408, 2010CB732303]; Key Scientific Project of Fujian [2009HZ0002-1]; Program for New Century Excellent Talents in Fujia

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Simulation of methane partial oxidation over silica‐supported MoO₃ and V₂O₅

Abstract: Microkinetic simulations have been carried out to describe the partial oxidation

Cited by 53 publications

References 24 publications

Environmentally friendly processes

Environmentally friendly processes

(Ag)Pd-Fe3O4 Nanocomposites as Novel Catalysts for Methane Partial Oxidation at Low Temperature

Catalytic selective oxidation or oxidative functionalization of methane and ethane to organic oxygenates

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