Processes employing multiple successive chemical reaction process steps and apparatus therefore

• US 20040013587A1
• Filed: 07/16/2002
• Published: 01/22/2004
• Est. Priority Date: 07/16/2002
• Status: Active Grant

• Current Assignee: The 323 Trust
• Original Assignee: Kreido Laboratories (Namliong SkyCosmos, Inc.)
• Inventors: Gulliver, Eric A., Doss, James E., Holl, Richard A.
• Granted Patent: US 7,098,360 B2
• Time in Patent Office: Days
• US Class Current: 422/224
• CPC Class Codes: B01F 27/272 with means for moving the materials to be mixed axially between the surfaces of the rotor and the stator, e.g. the stator rotor system formed by conical or cylindrical surfaces
• CPC Class Codes: B01F 35/92 for heating the outside of the receptacle, e.g. heated jackets or burners
• CPC Class Codes: B01J 19/0093 Microreactors, e.g. miniaturised or microfabricated reactors laboratory containers with capillary fluid transport in microfabricated channels or chambers B01L3/5027
• CPC Class Codes: B01J 19/1887 forming a thin film
• CPC Class Codes: B01J 2219/00096 Plates
• CPC Class Codes: B01J 2219/00788 Three-dimensional assemblies, i.e. the reactor comprising a form other than a stack of plates
• CPC Class Codes: B01J 2219/00835 Comprising catalytically active material
• CPC Class Codes: B01J 2219/00867 Microreactors placed in series, on the same or on different supports
• CPC Class Codes: B01J 2219/00869 Microreactors placed in parallel, on the same or on different supports
• CPC Class Codes: B01J 2219/00873 Heat exchange
• CPC Class Codes: B01J 2219/00889 Mixing micromixers B01F33/30
• CPC Class Codes: C07C 51/09 from carboxylic acid esters or lactones
• CPC Class Codes: C07C 51/265 having alkyl side chains which are oxidised to carboxyl groups
• CPC Class Codes: C07C 63/04 Monocyclic monocarboxylic acids
• CPC Class Codes: C07C 63/26 1,4 - Benzenedicarboxylic acid

Abstract

The invention provides processes and apparatus for the production of materials requiring a plurality of chemical reaction steps. In the prior art the number of reaction vessels is minimized by performing two or more reactions together in the same vessel. Instead each process is separated into separate successive steps, in each of which at least two principal components are reacted together, with or without at least one catalyst. In each step the components are reacted under optimum conditions for that reaction, using motion-augmented, sub-Kolmogoroff, micro-agitation provided by a separate discrete motor-operated, micro-agitation means. Such means are much smaller in size, but are extremely flexible as to the flow rate and reaction conditions, so that they can be adjusted to suit the reaction, without compromises dictated by attempting to perform other reactions in the same vessel. Multiple micro-agitation means in parallel and/or in series can be used in each step to increase capacity without scale-up problems, and units can be serviced or capacity reduced without the need to close down the process. Motor-operated micro-agitation means performing a non-chemical action can be provided at any stage of the process. Between each two steps the resultant mixture is separated to give a principal component used in the subsequent step, while at least one new principal component is added in the next step. Micro-agitation processes and the micro-agitation means therefore is described and claimed in prior U.S. Pat. Nos. 5,279,463 and 5,438,191 and application Ser. No. 09/802,037 entitled Method and Apparatus for Materials Processing. The materials to be produced preferably comprise organic di-carboxylic acids, and more preferably dimethyl terephthalate and terephthalic acid.

Claims

1. Processes for the production of materials requiring a plurality of chemical reaction steps, the processes being characterized by:

separation of the process into a plurality of separate successive process steps, each process step involving the reaction together of at least two principal step reaction components, with or without at least one catalyst component;

in each process step the principal step reaction components are reacted together with the employment of motion augmented sub-Kolmogoroff micro-agitation provided by motor-operated, micro-agitation means to facilitate the reaction, thereby producing a mixture of process step output materials;

between each two successive process steps a principal step reaction component for the subsequent process step is separated from the mixture of process step output materials from the prior process step and is supplied to the subsequent process step; and

at least one new principal step reaction component is supplied to the subsequent process step for reaction with the thus separated principal step reaction component from the prior process step.

2. Processes as claimed in claim 1, and including at least one non-reaction process step employing motion-augmented, sub-Kolmogoroff micro-agitation provided by motor-operated, micro-agitation means, the said step being disposed in the process sequence at a location selected from the group comprising prior to all of the process steps, prior to any of the process steps involving a reaction, subsequent to any of the process steps involving a reaction, subsequent to all of the process steps, and interposed between any two successive process steps involving a reaction.

3. Processes as claimed in claim 1, wherein such motor-operated, micro-agitation means comprise:

a cylindrical stator tube having at least a part along its length of uniform internal diameter about a longitudinal axis to provide a corresponding inner cylindrical surface;

a rotor mounted for rotation within the tube with its longitudinal axis parallel with the tube axis and providing an outer cylindrical surface parallel to the inner tube surface to provide an annular passage between them; and

means for rotating the rotor about its longitudinal axis;

wherein the radial dimension of the passage is at most about equal to the combined thicknesses of two boundary layers back-to-back formed on the surfaces with no room between them for an intervening bulk layer such that would permit Taylor vortices to be formed.

4. Processes as claimed in claim 1, wherein the materials to be produced are organic di-carboxylic acids.

5. Processes as claimed in claim 1, wherein the material to be produced is dimethyl terephthalate, the processes including the steps of:

oxidation in a first step of one methyl group of p-xylene to a carboxylic acid group;

esterification in a second step of the carboxylic acid group;

oxidation in a third step of the second methyl group of the p-xylene to the corresponding second carboxylic acid group; and

esterification in a fourth step of the second carboxylic acid group to give the dimethyl terephthalate.

6. Processes as claimed in claim 1, wherein the material to be produced is terephthalic acid, the processes including the steps of.

oxidation in a first step of one methyl group of p-xylene to a carboxylic acid group;

esterification in a second step of the carboxylic acid group;

oxidation in a third step of the second methyl group of the p-xylene to the corresponding second carboxylic acid group;

esterification in a fourth step of the second carboxylic acid group; and

hydrolysis in a fifth step of the resulting di-ester to terephthalic acid.

7. Processes as claimed in claim 1, wherein the material to be produced is terephthalic acid, the processes including the steps of.

oxidation in a first step of one methyl group of p-xylene to a carboxylic acid group;

esterification in a second step of the carboxylic acid group;

oxidation in a third step of the second methyl group of the p-xylene to the corresponding second carboxylic acid group; and

hydrolysis in a fourth step of the second carboxylic acid group to result terephthalic acid.

8. Processes for the production of organic carboxylic acids including at least two carboxylic acid groups, the processes being characterized by separate successive process steps, namely:

in a first process step reacting together at least two principal first step reaction components, with the employment of motion augmented, sub-Kolmogoroff, micro-agitation to facilitate the reaction, the first of which components has methyl groups which are to be converted to carboxylic acid groups, and the second of which will oxidize a methyl group of the first component to the corresponding carboxylic acid, and separating out the converted product from the first step;

in a second process step reacting together, with the employment of motion augmented, sub-Kolmogoroff, micro-agitation to facilitate the reaction, the converted product from the first step as a principal second step first reaction component and a second step second reaction component which will esterify the carboxylic acid group, and separating out the converted product from the second step;

in a third process step reacting together, with the employment of motion augmented sub-Kolmogoroff micro-agitation to facilitate the reaction, the converted product from the second step as a principal third step first reaction component and a third step second reaction component which will oxidize another methyl group of the converted product from the second step to a second carboxylic acid group, and separating out the converted product from the third step;

in a fourth process step reacting together, with the employment of motion augmented sub-Kolmogoroff micro-agitation to facilitate the reaction, the converted product from the third step as a principal fourth step first reaction component and a fourth step second reaction component which will esterify the second carboxylic acid group, and separating out the converted product from the fourth step; and

in a fifth process step reacting together, with the employment of motion augmented sub-Kolmogoroff micro-agitation to facilitate the reaction, the converted product from the fourth step as a principal fifth step first reaction component and a fifth step second reaction component which will hydrolyse the esterified carboxylic acid groups, and separating out the converted product from the fifth step.

9. Processes as claimed in claim 8, wherein the materials to be produced are organic di-carboxylic acids.

10. Processes as claimed in claim 8, wherein the material to be produced is dimethyl terephthalate and the first principal first step reaction component is p-xylene.

11. Processes as claimed in claim 8, wherein the material to be produced is terephthalic acid and the principal first step reaction component is p-xylene.

12. Processes as claimed in claim 8, wherein the material to be produced is terephthalic acid, the principal first step reaction component is p-xylene, and the process is terminated at the fourth step in which the principal fourth step first reaction component is hydrolysed by a fourth step second reaction component to result in the terephthalic acid.

13. Apparatus for the production of materials requiring a plurality of chemical reaction steps:

wherein the process for which the process apparatus is employed has been separated into a plurality of separate successive process steps, each process step involving the reaction together of at least two principal step reaction components, with or without at least one catalyst component;

wherein each process step is carried out in a separate, respective process step apparatus comprising;

motor-operated, micro-agitation means;

means for feeding the respective principal step reaction components to the motor-operated micro-agitation means wherein they are reacted together while subjected to motion-augmented, sub-Kolmogoroff, micro-agitation to facilitate the reaction between them, the operation of the motor-operated micro-agitation means resulting in a mixture of process step output materials; and

means for discharging such a mixture therefrom;

and wherein each process step apparatus also comprises;

process step separator means for separating from the mixture of process step output materials received from the micro-agitation means a principal step reaction component for supply to a subsequent process step apparatus;

means for feeding a mixture discharged from the micro-agitation means to the process step separator means; and

means for discharging at least the separated principal step reaction component from the process step separator means for supply to the subsequent process step apparatus.

14. Apparatus as claimed in claim 13, wherein the process includes at least one non-reaction process step employing motion-augmented, sub-Kolmogoroff micro-agitation provided by motor-operated, micro-agitation means, the apparatus including at least one such motor-operated, micro-agitation means disposed in the process sequence at a location selected from the group comprising prior to all of the process steps, prior to any of the process steps involving a reaction, subsequent to any of the process steps involving a reaction, subsequent to all of the process steps, and interposed between any two successive process steps involving a reaction.

15. Apparatus as claimed in claim 14, wherein such motor-operated, micro-agitation means comprise:

a cylindrical stator tube having at least a part along its length of uniform internal diameter about a longitudinal axis to provide a corresponding inner cylindrical surface;

a rotor mounted for rotation within the tube with its longitudinal axis parallel with the tube axis and providing an outer cylindrical surface parallel to the inner tube surface to provide an annular passage between them; and

means for rotating the rotor about its longitudinal axis;

wherein the radial dimension of the passage at most about equal to the combined thicknesses of two boundary layers back-to-back formed on the surfaces with no room between them for an intervening bulk layer such that would permit Taylor vortices to be formed.