Formaldehyde Synthesis Via the Partial Oxidation of Methane Over Supported Metal Oxide Catalysts PDF Download

Author: Aidan William Sexton
Publisher:
ISBN:
Category :
Languages : en
Pages : 294

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Author: Maria-Guadalupe Cardenas-Galindo
Publisher:
ISBN:
Category :
Languages : en
Pages : 440

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Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 135

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Catalytic oxidation of methane to partial oxidation products, primarily formaldehyde and C[sub 2] hydrocarbons, was found to be directed by the catalyst used. In this project, it was discovered that a moderate oxidative coupling catalyst for C[sub 2] hydrocarbons, zinc oxide, is modified by addition of small amounts of Cu and Fe dopants to yield fair yields of formaldehyde. A similar effect was observed with Cu/Sn/ZnO catalysts, and the presence of a redox Lewis acid, Fe[sup III] or Sn[sup IV], was found to be essential for the selectivity switch from C[sub 2] coupling products to formaldehyde. The principle of double doping with an oxygen activator (Cu) and the redox Lewis acid (Fe, Sn) was pursued further by synthesizing and testing the CuFe-ZSM-5 zeolite catalyst. The Cu[sup II](ion exchanged) Fe[sup III](framework)-ZSM-5 also displayed activity for formaldehyde synthesis, with space time yields exceeding 100 g/h-kg catalyst. However, the selectivity was low and earlier claims in the literature of selective oxidation of methane to methanol over CuFe-ZSM-5 were not reproduced. A new active and selective catalytic system (M=Sb, Bi, Sn)/SrO/La[sub 2]O[sub 3] has been discovered for potentially commercially attractive process for the conversion of methane to C[sub 2] hydrocarbons, (ii) a new principle has been demonstrated for selectivity switching from C[sub 2] hydrocarbon products to formaldehyde in methane oxidations over Cu, Fe-doped zinc oxide and ZSM-5, and (iii) a new approach has been initiated for using ultrafine metal dispersions for low temperature activation of methane for selective conversions. Item (iii) continues being supported by AMOCO while further developments related to items (i) and (ii) are the objective of our continued effort under the METC-AMOCO proposed joint program.

Author: Benoit J. Kartheuser
Publisher:
ISBN:
Category :
Languages : en
Pages : 410

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Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 135

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Book Description
Catalytic oxidation of methane to partial oxidation products, primarily formaldehyde and C2 hydrocarbons, was found to be directed by the catalyst used. In this project, it was discovered that a moderate oxidative coupling catalyst for C2 hydrocarbons, zinc oxide, is modified by addition of small amounts of Cu and Fe dopants to yield fair yields of formaldehyde. A similar effect was observed with Cu/Sn/ZnO catalysts, and the presence of a redox Lewis acid, Fe{sup III} or Sn{sup IV}, was found to be essential for the selectivity switch from C2 coupling products to formaldehyde. The principle of double doping with an oxygen activator (Cu) and the redox Lewis acid (Fe, Sn) was pursued further by synthesizing and testing the CuFe-ZSM-5 zeolite catalyst. The Cu{sup II}(ion exchanged) Fe{sup III}(framework)-ZSM-5 also displayed activity for formaldehyde synthesis, with space time yields exceeding 100 g/h-kg catalyst. However, the selectivity was low and earlier claims in the literature of selective oxidation of methane to methanol over CuFe-ZSM-5 were not reproduced. A new active and selective catalytic system (M=Sb, Bi, Sn)/SrO/La2O3 has been discovered for potentially commercially attractive process for the conversion of methane to C2 hydrocarbons, (ii) a new principle has been demonstrated for selectivity switching from C2 hydrocarbon products to formaldehyde in methane oxidations over Cu, Fe-doped zinc oxide and ZSM-5, and (iii) a new approach has been initiated for using ultrafine metal dispersions for low temperature activation of methane for selective conversions. Item (iii) continues being supported by AMOCO while further developments related to items (i) and (ii) are the objective of our continued effort under the METC-AMOCO proposed joint program.

Author: T.H. Fleisch
Publisher: Elsevier
ISBN: 0080537316
Category : Technology & Engineering
Languages : en
Pages : 577

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This volume contains peer-reviewed manuscripts describing the scientific and technological advances presented at the 6th Natural Gas Conversion Sumposium held in Alaska in June 2001. This symposium continues the tradition of excellence and the status as the premier technical meeting in this area established by previous meetings. The 6th Natural Gas Conversion Symposium is conducted under the overall direction of the Organizing Committee. The Program Committee was responsible for the review, selection, editing of most of the manuscripts included in this volum. A standing International Advisory Board has ensured the effective long-term planning and the continuity and technical excellence of these meetings.

Author: Marianne Rose Smith
Publisher:
ISBN:
Category :
Languages : en
Pages : 462

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Author: Adam Bielanski
Publisher: CRC Press
ISBN: 1482293285
Category : Science
Languages : en
Pages : 489

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A description of catalytic systems commonly used as model systems in the laboratory and as industrial catalysts in large-scale operations, and a discussion of the mechanisms operating in these reactions. Attempts to describe the elementary steps by quantum chemical methods are also shown, as are rec

Author: Remegia Mmalewane Modibedi
Publisher:
ISBN:
Category : Catalysis
Languages : en
Pages : 210

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In this study a catalyst that works at low temperature and atmospheric pressure for the oxidation of methane to methanol and formaldehyde was developed. Catalyst preparation was based on the fact that the higher activity and selectivity to the desired products obtained over supported catalysts, compared to bulk oxides, can be attributed to the formation of easily reducible supported metal oxide phases.

Author: Rafael Alfredo Díaz Real
Publisher:
ISBN:
Category :
Languages : en
Pages : 0

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The kinetics of the vapor phase air oxidation of methanol to formaldehyde over molybdenum oxide catalysts, antimony oxide catalyst, and their mixtures (both supported and unsupported), at atmospheric pressure and different operating conditions, have been studied in a fixed-bed integral reactor heated by a fluidized sand bath. The effect of various process variables, namely the process temperature (T), the ratio of catalysts to feed flow rate or space time (W/F), and the ratio of methanol fed to air (R), on conversion and yield have been determined. A screening study at varying operating conditions was performed to determine the optimum composition of a Sb$\sb2\rm O\sb4$-MoO$\sb3$ mixture. On the basis of this study a catalyst containing 67% $\rm Sb\sb2O\sb4$-33% MoO$\sb3$ was selected for the detailed kinetic study of oxidation of methanol to formaldehyde. The operating conditions studied were as follows: temperature in the range 623 to 698 K, space times from 5 to 50 $\rm g\sb{cat}/mol\sb{CH\sb3OH}h\sp{-1},$ and methanol to air ratios in the range 0.04 to 0.10 mol$\rm\sb{CH\sb3OH}h\sp{-1}/mol\sb{air}h\sp{-1}.$ This catalyst proved to be highly active and selective to formaldehyde formation. Yields up to $\sim$100% were obtained. Best operating conditions found were obtained at a space time of 27.5 for a methanol/air ratio of 0.06 and a temperature of 698 K. The rate equation for the oxidation of methanol to formaldehyde was derived on the basis of a two-stage redox mechanism$$\eqalign{\rm CH\sb3OH\sb{(g)} + S\sb{ox}\ {\buildrel{k\sb1}\over{\to}}\ &\rm HCHO\sb{(g)} + H\sb2O\sb{(g)} + S\sb{red}\cr\rm O\sb{2\sb{(g)}} + &\rm S\sb{red}\ {\buildrel{k\sb2}\over{\to}}\ S\sb{ox}\cr}$$where S$\rm\sb{ox}$ represents an active site of lattice oxygen and S$\rm\sb{red}$ represents a reduced site of lattice oxygen. The rate equation for the temperature of 648 to 698 K which correlated the data was$$\rm r = {k\sb1P\sb{M}\over 1+{k\sb1P\sb{M}\over 2k\sb2P\sb{O\sb2}}}$$where k$\sb1$ and k$\sb2$ are the temperature dependent rate constants of steps one and two. The equations relating k$\sb1$ and k$\sb2$ with temperature were$$\eqalign{&\rm ln\ k\sb1 = -6.4039-{6.9153\times10\sp3\over T}\cr&\rm ln\ k\sb2 = -3.0154 + {1.8809\times10\sp3\over T}\cr}$$ Several spectroscopic and analytical techniques, viz, electron spin resonance (ESR), x-ray diffraction spectroscopy (XRD), scanning electron microscopy (SEM), and adsorption studies were used to characterize the catalysts. The surface are of the catalyst used in the kinetic study was 6.1 m$\sp2$/g as determined by the BET method. A preliminary study of the Sb-Mo oxide mixture (load of $\sim$5 wt%) supported on Y zeolite was also carried out. Maximum yield obtained was comparable to that obtained with pure MoO$\sb3.$ A new catalyst has been developed that gave nearly 100% conversion and 100% yield. The industrial potential of this catalyst is very promising.