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1999 Progress Report: Investigation of the Partial Oxidation of Methane to Methanol in a Simulated Countercurrent Moving Bed Reactor

EPA Grant Number: R825370C048
Subproject: this is subproject number 048 , established and managed by the Center Director under grant R825370
(EPA does not fund or establish subprojects; EPA awards and manages the overall grant for this center).

Center: EERC - National Center for Clean Industrial and Treatment Technologies (CenCITT)
Center Director: Crittenden, John C.
Title: Investigation of the Partial Oxidation of Methane to Methanol in a Simulated Countercurrent Moving Bed Reactor
Investigators: Carr, R.W.
Institution: University of Minnesota
EPA Project Officer: Karn, Barbara
Project Period:    
Project Period Covered by this Report: January 1, 1998 through January 1, 1999
RFA: Exploratory Environmental Research Centers (1992)
Research Category: Center for Clean Industrial and Treatment Technologies (CenCITT) , Targeted Research

Description:

Objective:

The goal of this project is to develop a simulated countercurrent moving bed chromatographic reactor (SCMCR) for the production of methanol from methane (natural gas).

Progress Summary:

The partial oxidation of methane to methanol is a process that utilizes a clean source material in an energy efficient manner to produce a substance that is both a clean fuel and a useful chemical feedstock. Simulated countercurrent moving bed chromatographic reactors are chemical reactors in which reaction and separation occur simultaneously in integrated reactor/adsorbers.

The adsorptive separation has very low energy requirements, so the SCMCR is environmentally benign from the standpoint of CO2 emissions. The separation of product(s) from reactant(s) enables equilibrium limited reactions to be carried to higher conversions than would be possible in conventional non-separative reactors. The SCMCR is also capable of improving yields of other intrinsically low conversion processes.

The partial oxidation of methane to methanol is a low conversion process if it is carried out at conditions where deep oxidation to CO2 and H2O is minimized. The consequent low yields of methanol have made commercialization unattractive. The present investigation seeks to determine to what extent the SCMCR can improve methanol yields, and whether a commercially feasible process might result.

The homogeneous gas phase partial oxidation of methane was carried out at total pressures from 60 to 100 atm in a multiple column configuration SCMCR. The reactor design and operating conditions were optimized for methanol production on the basis of a program of experimentation. A mathematical model has been developed as a basis for refinement of the design and for potential scale-up.

The SCMCR system has been designed, built, and operated. A suitable adsorbent that separates methane from methanol and does not significantly spread the methane block wave, (10% Carbowax on 80/100 Supelcoport) was selected and used in the adsorber columns. Parts of the system have been redesigned and replaced in order to reduce methane spreading due to dispersion. It was found that using nitrogen instead of helium as a carrier gas has a favorable effect on the viscosity and the flow characteristics of the mixture at high pressures.

The effect of temperature, total pressure, and methane to oxygen ratio in the make-up feed, on methane conversion, methanol selectivity, and methanol yield, have been determined. The optimum SCMCR performance was obtained at 477°C, 100 atm, and CH4/O2 = 2. For these conditions methane conversion is 50%, methanol selectivity is 50%, and the methanol yield is 25%. The per-pass methanol yield in the tubular reactor alone at these operating conditions is 3%. Thus, the SCMCR improves the methanol productivity by a factor of 8. Furthermore, the best methanol yields, from conventional tubular reactors, that have been reported in the literature are 6-8%. The SCMCR betters these reactors by a factor of 3 to 4.

Journal Articles:

No journal articles submitted with this report: View all 4 publications for this subproject

Supplemental Keywords:

Sustainable Industry/Business, Scientific Discipline, RFA, Technology for Sustainable Environment, Sustainable Environment, Chemical Engineering, Chemistry, cleaner production/pollution prevention, New/Innovative technologies, Engineering, clean technology, clean technologies, catalysts, partial oxidation, oxidation, oxidation reactions, waste streams, mathematical models, reactors, energy efficiency, methanol, reaction engineering, feedstocks, feedstock, environmentally benign reactor, simulated countercurrent moving bed chromatographic reactor (SCMCR)

Progress and Final Reports:
Original Abstract


Main Center Abstract and Reports:
R825370    EERC - National Center for Clean Industrial and Treatment Technologies (CenCITT)

Subprojects under this Center: (EPA does not fund or establish subprojects; EPA awards and manages the overall grant for this center).
R825370C032 Means for Producing an Entirely New Generation of Lignin-Based Plastics
R825370C042 Environmentally Conscious Design for Construction
R825370C046 Clean Process Advisory System (CPAS) Core Activities
R825370C048 Investigation of the Partial Oxidation of Methane to Methanol in a Simulated Countercurrent Moving Bed Reactor
R825370C054 Predictive Tool for Ultrafiltration Performance
R825370C055 Heuristic Reactor Design for Clean Synthesis and Processing - Separative Reactors
R825370C056 Characterization of Selective Solid Acid Catalysts Towards the Rational Design of Catalytic Reactions
R825370C057 Environmentally Conscious Manufacturing: Prediction of Processing Waste Streams for Discrete Products
R825370C064 The Physical Properties Management System (PPMS™): A P2 Engineering Aid to Support Process Design and Analysis
R825370C065 Development and Testing of Pollution Prevention Design Aids for Process Analysis and Decision Making
R825370C066 Design Tools for Chemical Process Safety: Accident Probability
R825370C067 Environmentally Conscious Manufacturing: Design for Disassembly (DFD) in De-Manufacturing of Products
R825370C068 An Economic Comparison of Wet and Dry Machining
R825370C069 In-Line Copper Recovery Technology
R825370C070 Selective Catalytic Hydrogenation of Lactic Acid
R825370C071 Biosynthesis of Polyhydroxyalkanoate Polymers from Industrial Wastewater
R825370C072 Tin Zeolites for Partial Oxidation Catalysis
R825370C073 Development of a High Performance Photocatalytic Reactor System for the Production of Methanol from Methane in the Gas Phase
R825370C074 Recovery of Waste Polymer Generated by Lost Foam Technology in the Metal Casting Industry
R825370C075 Industrial Implementation of the P2 Framework
R825370C076 Establishing Automated Linkages Between Existing P2-Related Software Design Tools
R825370C077 Integrated Applications of the Clean Process Advisory System to P2-Conscious Process Analysis and Improvement
R825370C078 Development of Environmental Indices for Green Chemical Production and Use

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The perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Conclusions drawn by the principal investigators have not been reviewed by the Agency.


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