Methanol synthesis reactor

The modular reactor design addresses the challenges of scaling, access, and process control in methanol synthesis reactors by featuring a scalable tube bundle, improved access, and enhanced catalyst and temperature management, resulting in increased efficiency and safety.

JP7695726B2Active Publication Date: 2025-06-19CRI HF
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Patent Information

Application Number
JP2023543122
Authority / Receiving Office
JP · JP
Patent Type
Patents
Current Assignee / Owner
Priority Date
2021-01-15
Filing Date
2022-01-13
Publication Date
2025-06-19
Estimated Expiration
2042-01-13

AI Technical Summary

Technical Problem

Existing reactor designs for methanol synthesis are difficult to scale up or down, lack efficient access and maintainability, and struggle with proper catalyst management and temperature measurement, leading to inefficiencies and safety concerns.

Method used

A modularly configured reactor with a scalable tube bundle arrangement, improved access mechanisms, and enhanced catalyst management and temperature measurement systems, allowing for efficient scaling, maintenance, and process control.

Benefits of technology

The reactor design enables flexible scaling to meet changing facility needs, improves catalyst distribution and heat management, and enhances process control and safety by providing accurate temperature measurements.

✦ Generated by Eureka AI based on patent content.

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Patent Text Reader

Abstract

The improved reactor comprises a shell and at least one reactor internal including a tube bundle comprising a plurality of tubes mounted by at least one tube support plate comprising at least one radial strut and at least one bracket configured to secure to at least one tube of the tube bundle, the plurality of tubes being arranged in concentric bands about a longitudinal axis of the reactor, the reactor comprising a gas introduction plate, a catalyst support plate, and a top plate.
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Description

Technical Field

[0001] The present disclosure relates to a reactor, particularly a reactor for methanol synthesis.

Background Art

[0002] Global climate change is considered to be "the most pressing environmental problem of the modern era." The National Aeronautics and Space Administration (NASA) states that "the scientific basis for the warming of the climate system is clear." Climate change is caused by the warming effects of greenhouse gases such as water vapor, nitrous oxide, methane, and carbon dioxide. Among these, carbon dioxide emissions are the main cause. This is because the global atmospheric CO2 concentration has increased by one-third since the start of the Industrial Revolution. CO2 emissions are mainly due to human activities such as the consumption of fossil fuels, and their by-products are emitted into the atmosphere.

[0003] As a solution to the problem that renewable energy sources such as wind power and solar power generation are inherently intermittent and unpredictable, chemical energy storage has been explored. Due to the intermittency of wind power and solar power generation, power grids and power companies must rely on fossil fuel-based energy sources to meet baseline electricity demand, but incorporating suddenly available wind power and solar power generation into the grid is difficult because it is difficult to quickly reduce and expand such fossil fuel-based energy sources as coal-fired power plants. Since many renewable energy sources are difficult to expand as alternatives to conventional fossil fuel-based power sources, high-density energy storage of renewable energy, in which the renewable energy can be stored and used when the grid can handle the energy, is important for addressing climate change.

[0004] Existing energy storage modalities, including thermal energy storage, compressed air energy storage, hydrogen storage, pumped hydroelectric storage, and large batteries, have so far proven to be prohibitively expensive and / or difficult to scale up. For example, chemical storage of renewable energy in the form of electrolyzing water to produce hydrogen for combustion, fuel cell consumption, or chemical synthesis such as methanol synthesis is a promising approach as it provides a sufficiently high density of renewable energy that can be used when needed, and stable storage, enabling renewable energy to supply energy demand constantly without change rather than intermittently.

[0005] The reactors used in methanol synthesis from syngas are typically limited to boiling water reactors (BWRs) due to the high heat profile of a typical reaction suite containing a significant amount of CO. BWRs are complex and expensive devices but are usually necessary to mitigate the heat generated from the exothermic production of methanol from syngas in order to protect the reaction products, reactors, and catalysts.

[0006] Shell and tube reactors for the synthesis of methanol from CO2 and H2 using a catalyst and / or an exothermic reaction, such as a suitable catalyst like a copper and zinc oxide (Cu / ZnO)-based catalyst or other suitable catalysts, have to undergo regular maintenance, such as catalyst loading, and / or removal and refilling, removal of fouling of the reactor shell, implementation of repairs of various components, or otherwise. The ability to access the interior of the reactor for catalyst loading, maintenance implementation, and other purposes has to be balanced with the need to maintain the tubes within the bundle.

[0007] The design of existing shell and tube reactors is difficult to scale up or down based on the needs of a particular facility, such as the desired throughput. The throughput of the facility may change over time due to bottleneck elimination efforts, which can increase the reactor throughput requirements. Scaling up the reactor to eliminate a facility bottleneck can be a difficult, expensive, and time-consuming endeavor, where the entire reactor, including the interior, often needs to be improved or redesigned.

[0008] This can require a significant amount of design and engineering effort. As an engineer, when scaling up the design, essentially a "from-scratch" redo is required, especially considering tube placement and cross-sectional area, shell size and configuration, and the volume and cross-sectional surface area of the catalyst bed. Existing shell and tube reactor designs and providers are not well-suited to adapting the reactor design in an efficient manner to changing requirements. If the reactor is not properly designed, non-uniform distribution of the catalyst, reactants, and heat can occur, which can damage the catalyst and / or reactor components and reduce the efficiency of the reaction. In many cases, a runaway exothermic reaction can result in catastrophic failure of the reactor.

[0009] Furthermore, it is difficult to scale up / down and properly fabricate the feed tubes within and / or for the reactor. Improperly designed, placed, and / or fabricated feed tubes often lead to blockages, eddies, and non-uniform regions of reactants within the reactor, which can, detrimentally, reduce the reactor efficiency and throughput, as well as result in hot spots. Hot spots in exothermic reactions are particularly dangerous and can damage the reactor and catalyst.

[0010] Another problem in reactor design is the difficulty of measuring the temperature inside the reactor at one or more desired locations. In particular, it is difficult to properly control a process involving a reactor, especially in high-risk applications such as exothermic reactions, without understanding the temperature profile inside the reactor at different locations along the reactor body corresponding to different stages of the reaction and / or different reactor states.

[0011] However, thermocouple junctions including gasket seats can be damaged over time, leading to leakage of the thermocouple junction. Such leaks can be repaired, but to do so requires deactivating the catalyst and replacing the gasket seat. This is costly, potentially dangerous, and involves time-consuming shutdowns, catalyst deactivation, and startups, each of which incurs high costs including significant opportunity costs. Considering that the expected lifespan of the catalyst is 3 to 5 years, such repairs result in very costly interruptions to the operation of the facility. Furthermore, in high-pressure and / or temperature reactions involving hydrogen, the risk of leakage from the flange joint to the outside of hydrogen or other reactants / products and to the inside of oxygen, a catalyst poison, is particularly high.

[0012] Therefore, the design of existing reactors incorporating multiple thermowells for providing thermocouples at different height positions along the reactor body is vulnerable to significant operation interruptions due to leakage of the thermocouple junction, and the reactor design that omits such thermowells to avoid interruptions lacks the reactor state data necessary to properly control the reaction. Furthermore, the existing thermowell configuration inside the reactor inserts the thermocouple laterally with respect to the flow direction, for example, radially into the reactor body. This disadvantageously results in temperature measurements being closer to the outer shell in the case of larger reactors, which further complicates the scaling up / down of the reactor design. The reactor design is also unsuitable for enabling the thermocouple to be inserted into the reactor body without damaging the thermocouple when a catalyst is present.

[0013] Existing reactor designs may include one or more nozzles for removing spent catalyst, for example, from the bottom of the reactor body. The configuration of the catalyst removal nozzles of existing reactors is not well-suited to effectively and quickly remove the catalyst such that the operator does not have to scrape the catalyst out of the reactor body.

[0014] Certain shell and tube reactors and other types of reactors may include an inlet nozzle through which reactant gas is fed from a pipe extending through the center of the reactor body. The pipe may be perforated to fit one or more supply tubes, each of which may be connected to the pipe and then bent upward to supply reactants through the reactor body. The configuration of such reactors is not well-suited to accommodate the precise and tube-specific adjustments that must be made to connect the pipe to each of the multiple supply tubes, for example, when scaling up to hundreds of tubes.

[0015] The inlet pipe in a particular reactor configuration is further utilized to support supply tubes at different heights within the reactor body, and one or more flat bars are welded and extending between the inlet pipe and the one or more supply tubes. This configuration is particularly time-consuming for the manufacture, assembly, and maintenance of large reactors, which complicates the task of scaling the reactor design up or down according to the requirements of the facility. Further, disadvantageously, the inlet pipe occupies a significant cross-sectional area that could otherwise be occupied by catalyst. Tie rods have been considered for supporting supply tubes within shell and tube reactors, but such supports occupy catalyst space and pose an obstacle during catalyst loading and removal. SUMMARY OF THE INVENTION PROBLEMS TO BE SOLVED BY THE INVENTION

[0016] Based on the above, there is a need for an improved reactor configured to maintain the interior of the reactor, manage the catalyst, expand or contract based on the need for the processing capacity of the facility, improve the measurement of the reactor state without compromising the integrity and maintainability of the reactor, effectively remove spent catalyst, improve production, and solve the problems of constructing a shell and tube reactor.

Means for Solving the Problems

[0017] Embodiments of the reactor according to the present disclosure advantageously provide a reactor that is scalable and / or configured for improved access and maintainability of the reactor, particularly the interior of the reactor, to address the drawbacks of existing reactor designs. The embodiments of the reactor described above can be configured to facilitate access to the interior of the reactor without sacrificing the strength and robustness inside the reactor, such as a reactor tube bundle comprising one or more tubes and one or more support structures, while keeping the tube bundle intact and undamaged.

[0018] The reactor embodiments described above further comprise a tube arrangement configured to be easily expanded or reduced based on the needs of a particular facility. In existing reactor designs, tubes cannot be easily added to or removed from a tube bundle according to the reactor shell shape when constructing a reactor without significant redesign work, whereas embodiments of the present disclosure advantageously enable an annular band of tubes or other arrangements to be modularly arranged based on the required processing capacity of the reactor and associated facilities. In the above embodiments, the tube arrangement may define a regular and / or repeating pattern that can be simply added to the design of an existing tube bundle and / or removed from the design of the existing tube bundle when designing a reactor. This has the advantage of making bottleneck elimination work or other design work much easier and less costly from a manufacturing perspective.

[0019] The arrangement of the tube bundle further facilitates the distribution of heat and reactants throughout the interior of the reactor, particularly through the catalyst bed, without interrupting the catalyst loading that occurs as the operator typically loads or discards catalyst particles between the open upper end of the reactor and the interior of the reactor. The reactor and tube bundle arrangements of the embodiments advantageously result in both modularity of design for improved constructability and maintenance of desired characteristics regarding heat and reactant distribution while ensuring that the catalyst particles are evenly distributed within the reactor.

[0020] The tube bundle of the reactor embodiments according to the present disclosure is further configured to provide improved structural support for one or more tubes for increased robustness of the reactor during construction, transportation, and installation, as well as during operation. In embodiments, one or more structural supports and / or one or more of the plurality of tubes are given an increased thickness to ensure structural support at desired locations of the tube bundle.

[0021] In an embodiment, the reactor and its components are configured to facilitate easy access for maintenance of critical parts. One or more plates configured to support the tube bundle are modular such that an operator can easily load, remove, or access the catalyst between the inside of the reactor and the components inside the reactor as compared to existing reactors, and components such as support plates are welded to the inner surface of the reactor shell and can prohibit access to the components inside the reactor.

[0022] An embodiment of the reactor addresses the problem that existing reactor designs are inadequate to provide proper flow and reactant distribution, and thus heat distribution, within the reactor and the catalyst bed, by providing an improved inlet nozzle and distribution mechanism configured to direct reactants into a tube bundle disposed within the interior of the reactor. In an embodiment, the inlet nozzle is provided near a gas introduction plate and is arranged in a flow direction that is transverse to the flow direction of the plurality of tubes of the tube bundle. A second inlet nozzle may be provided at the bottom of the reactor and may be configured with a structure for evenly distributing the flow into the plurality of tubes of the tube bundle. In an embodiment, one or more catalyst removal nozzles are provided with an improved configuration for removing the catalyst, and the removal nozzles are configured with a downward angle.

[0023] The tube bundle and the plurality of tubes can be arranged such that the cross-sectional area of the plurality of tubes relative to the cross-sectional area of the catalyst is improved for even heat and flow distribution without hindering the structural and modular characteristics of the tube bundle.

[0024] An embodiment of the reactor is further configured to reduce the occurrence of blockages, eddies, and / or non-uniform regions of reactants within the reactor body and the associated hot spots by providing for improved distribution of the catalyst, the interior of the reactor, and the reactants during the course of the reaction.

[0025] Embodiments of the reactor of the present disclosure further address the drawbacks of existing reactor designs with respect to process control and temperature measurement. In an embodiment, the reactor is configured to provide one or more thermowells configured to receive one or more respective thermocouples. The thermocouples may be configured to measure the temperature inside the reactor at a plurality of positions each using a single thermowell arranged axially or longitudinally with respect to the reactor body.

[0026] Example embodiments according to the present disclosure may relate to a reactor comprising a shell defining an internal space, at least one inlet nozzle, and a tube bundle comprising one or more tubes.

[0027] Embodiments may further comprise a catalyst support plate.

[0028] Embodiments may further comprise at least one tube support plate.

[0029] Embodiments may further comprise a gas introduction plate.

[0030] Embodiments may further comprise an upper plate.

[0031] Embodiments may further comprise an upper plate and a tube support plate.

[0032] Embodiments may be further configured where the shell is configured to receive at least one catalyst.

[0033] In an embodiment, at least one catalyst is a solid catalyst. Such a solid catalyst may comprise balls of a first diameter.

[0034] In an embodiment, the solid catalyst comprises balls of a second diameter.

[0035] In an embodiment, the shell is configured to receive at least one solid catalyst. Such a solid catalyst may have a shape defining at least one of pellets, rings, tablets, and spheres.

[0036] In an embodiment, the catalyst support plate is configured to support the solid catalyst at a predetermined height.

[0037] In an embodiment, the catalyst support plate defines one or more openings.

[0038] In an embodiment, the one or more openings include a plurality of openings of a first size and a plurality of openings of a second size, and the plurality of openings extend through at least a portion of the thickness of the catalyst support plate.

[0039] In an embodiment, the first size corresponds to the circumference of at least one tube of the tube bundle.

[0040] In an embodiment, the second size is smaller than the first size.

[0041] In an embodiment, the second size is a function of the thickness of the catalyst support plate.

[0042] In an embodiment, the plurality of openings of the first size are defined through the catalyst support plate according to the arrangement of the plurality of tubes.

[0043] In an embodiment, the gas introduction plate includes a plurality of openings defined through the thickness of the gas introduction plate.

[0044] In an embodiment, the plurality of openings are a plurality of circular openings defined through the gas introduction plate according to the arrangement of the plurality of tubes.

[0045] In an embodiment, the gas introduction plate includes a second plurality of openings defined through the thickness of the gas introduction plate, and the second plurality of openings have a size and / or shape different from those of the plurality of circular openings.

[0046] In an embodiment, the shell defines an outlet nozzle.

[0047] In an embodiment, the outlet nozzle is located on a side portion of the shell.

[0048] In an embodiment, the inlet nozzle is located near the bottom of the shell.

[0049] In an embodiment, the inlet nozzle is arranged laterally with respect to the direction of the flow through the shell.

[0050] In an embodiment, the inlet nozzle is arranged substantially parallel to the direction of the flow through the shell.

[0051] In an embodiment, the gas introduction plate is arranged near the inlet nozzle.

[0052] In an embodiment, the at least one tube support plate includes at least one annular band.

[0053] In an embodiment, the at least one annular band includes at least one bracket configured to extend around a portion of the tubes of the tube bundle.

[0054] In an embodiment, the at least one bracket extends around the entire tube.

[0055] In an embodiment, the shell defines a startup nozzle configured for the supply of a heating fluid.

[0056] In an embodiment, the reactor further includes at least one catalyst removal nozzle.

[0057] In an embodiment, the reactor further comprises a handhole.

[0058] In an embodiment, the at least one tube support plate defines a plurality of concentric annular bands.

[0059] In an embodiment, the tube bundle comprises at least one tube of a first size and at least one tube of a second size.

[0060] In an embodiment, the inlet nozzle is disposed below the gas introduction plate.

[0061] In an embodiment, the shell defines an outlet nozzle, and the outlet nozzle is disposed below the catalyst support plate.

[0062] In an embodiment, catalysts (e.g., balls) of a first size (e.g., diameter) and catalysts (e.g., balls) of a second size (e.g., diameter) are disposed in respective individual layers near the catalyst support plate.

[0063] In an embodiment, the shell is at least one solid catalyst, and the catalyst is configured to receive at least one solid catalyst that defines a first height within the shell in an unreduced state and a second height within the shell in a reduced state (e.g., due to settling that may occur during operation).

[0064] In an embodiment, the second height is lower than the first height.

[0065] In an embodiment, the at least one tube support plate defines at least one radial support member connected to at least one of the plurality of annular bands.

[0066] In an embodiment, the at least one radial support member is connected to at least one of the plurality of annular bands and to the outer support band.

[0067] In an embodiment, the innermost annular band of the at least one tube support plate comprises any number (e.g., six) of brackets, each configured to correspond to the same number of innermost rings of tubes of a first size.

[0068] In an embodiment, the second annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to the preceding band (e.g., 10), and the brackets of the second annular band are each configured to correspond to the same number of concentric bands (e.g., rings) of tubes within a second concentric band or ring of the plurality of tubes of the tube bundle. Such plurality of tubes may be of a first size.

[0069] In an embodiment, the third annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to the preceding band (e.g., 14), and the brackets of the third annular band are each configured to correspond to the same number of concentric bands (e.g., rings) of tubes within a third concentric band or ring of the plurality of tubes of the tube bundle. Such plurality of tubes may be of a second size.

[0070] In an embodiment, the fourth annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to the preceding band (e.g., 18), and the brackets of the fourth annular band are each configured to correspond to the same number of concentric bands (e.g., rings) of tubes within a fourth concentric band or ring of the plurality of tubes of the tube bundle. Such plurality of tubes may be of a first size.

[0071] In an embodiment, the fifth annular band of the at least one tube support plate has an equal or greater number of brackets compared to a preceding band (e.g., 22), and the brackets of the fifth annular band are each configured to correspond to a concentric band (e.g., a ring) of the same number of tubes of the tube bundle, located within a fifth concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a first size.

[0072] In an embodiment, the sixth annular band of the at least one tube support plate has an equal or greater number of brackets compared to a preceding band (e.g., 26), and the brackets of the sixth annular band are each configured to correspond to a concentric band (e.g., a ring) of the same number of tubes of the tube bundle, located within a sixth concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a first size.

[0073] In an embodiment, the seventh annular band of the at least one tube support plate has an equal or greater number of brackets compared to the plurality of brackets of a preceding band (e.g., 30), and the brackets of the seventh annular band are each configured to correspond to a concentric band (e.g., a ring) of the same number of tubes of the tube bundle, located within a seventh concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a second size.

[0074] In an embodiment, the eighth annular band of the at least one tube support plate has an equal or greater number of brackets compared to a preceding band (e.g., 34), and the brackets of the eighth annular band are each configured to correspond to a concentric band (e.g., a ring) of the same number of tubes of the tube bundle, located within an eighth concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a first size.

[0075] In an embodiment, the ninth annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to a preceding band (e.g., 36), and the brackets of the ninth annular band are each configured to correspond to a concentric band (e.g., ring) of the same number of tubes of the tube bundle located within a ninth concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a first size.

[0076] In an embodiment, the tenth annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to a preceding band (e.g., 42), and the brackets of the tenth annular band are each configured to correspond to a concentric band (e.g., ring) of the same number of tubes of the tube bundle located within a tenth concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a first size.

[0077] In an embodiment, the eleventh annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to a preceding band (e.g., 46), and the brackets of the eleventh annular band are each configured to correspond to a concentric band (e.g., ring) of the same number of tubes of the tube bundle located within an eleventh concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a second size.

[0078] In an embodiment, the twelfth annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to a preceding band (e.g., 50), and the brackets of the twelfth annular band are each configured to correspond to a concentric band (e.g., ring) of the same number of tubes of the tube bundle located within a twelfth concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a first size.

[0079] In an embodiment, the 13th annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to a preceding band (e.g., 54), and the brackets of the 13th annular band are each configured to correspond to a concentric band (e.g., a ring) of the same number of tubes of the tube bundle located within the 13th concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a first size.

[0080] In an embodiment, the 14th annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to a preceding band, and the brackets of the 13th annular band are each configured to correspond to a concentric band (e.g., a ring) of the same number of tubes of the tube bundle located within the 14th concentric band or ring of the plurality of tubes. Such a plurality of tubes can be of a second size.

[0081] It will be apparent that any number of annular bands can be provided.

[0082] In an embodiment, any one of the plurality of annular bands of the at least one tube support plate further comprises brackets corresponding to at least one thermocouple insertion tube. Such thermocouple insertion tubes can be of a similar size (e.g., of a first or second size) to the plurality of tubes of the tube bundle.

[0083] In an embodiment, at least four tube support plates are arranged longitudinally along the tube bundle.

[0084] In an embodiment, at least one tube support plate is arranged longitudinally along the tube bundle, and an annular band of the at least one tube support plate further includes a bracket corresponding to at least one thermocouple insertion tube, and the at least one thermocouple insertion tube is configured to receive a temperature measuring device.

[0085] In an embodiment, the temperature measuring device is configured to obtain temperatures at a plurality of longitudinal positions within the reactor.

[0086] In an embodiment, the temperature measuring device is configured to obtain temperatures longitudinally, for example, at a plurality of positions (e.g., at least eight different positions), along the reactor.

[0087] In an embodiment, the shell defines at least one flange at the upper part of the shell to facilitate attachment and detachment between the main body of the shell.

[0088] In an embodiment, the shell is configured to be attached to a skirt at the bottom of the shell.

[0089] In an embodiment, the skirt defines an opening configured to receive an introduction spool.

[0090] In an embodiment, the at least one tube support plate defines at least one radial member connected to at least one of a plurality of annular bands of the tube support plate, and the at least one radial member of the at least one tube support plate is axially aligned with at least one radial member of another tube support plate.

[0091] In an embodiment, the at least one radial member of the at least one tube support plate is axially offset with respect to at least one radial member of an adjacent tube support plate.

[0092] In an embodiment, the at least one tube support plate defines a plurality of radial members arranged symmetrically about the longitudinal axis of the reactor. Yes.

[0093] In an embodiment, the at least one tube support plate defines at least one radial member connected to at least one of a plurality of annular bands of the tube support plate, and the at least one annular band of the at least one tube support plate is removably fixed to the at least one radial member.

[0094] In an embodiment, at least one tube of the tube bundle defines a uniform thickness longitudinally within the reactor.

[0095] In an embodiment, at least one tube of the tube bundle defines a tapered thickness longitudinally within the reactor.

[0096] In an embodiment, at least one tube of the tube bundle is configured to facilitate a greater degree of heat transfer near the bottom of the reactor relative to the top of the reactor.

[0097] Any of the plurality of features described above, or any of the other plurality of features described herein, may be combined with each other and used alone or in combination with other features.

[0098] Other methods, embodiments, and variations of the system will be described in more detail in the following description.

[0099] These and other features, aspects, and advantages of the present invention will become readily apparent and better understood in view of the following specification, appended claims, and accompanying drawings.

Brief Description of the Drawings

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Best Mode for Carrying Out the Invention

[0101] A better understanding of the different embodiments of the present invention can be obtained from the following description read in conjunction with the accompanying drawings in which like reference numerals represent like components.

[0102] This disclosure is susceptible to various modifications and alternative configurations, but specific illustrative embodiments are shown in the drawings and described below. However, it is not intended to limit the present disclosure to the disclosed embodiments, but rather, it is intended to cover all modifications, alternative configurations, combinations, and equivalents that fall within the spirit and scope of the present disclosure and are defined by the appended claims.

[0103] It will be understood that unless a term is defined in this patent as having a stated meaning, there is no intention to explicitly or implicitly limit the meaning of such term beyond its plain or ordinary meaning.

[0104] Referring to FIG. 1A, a reactor 100 according to an embodiment of the present disclosure is shown. The reactor 100 includes a shell 102 that defines an internal space 103 (FIG. 4) and includes at least one inlet nozzle 120. The reactor 100 receives at least one reactor internal component, such as a tube bundle 130 (FIG. 3) including one or more tubes 131, and is configured to cooperate with the at least one reactor internal component. The reactor 100 extends longitudinally about axis 1A-1A from an upper end 105 to a bottom end 107 and may define a generally cylindrical shape.

[0105] The inlet nozzle 120 is disposed near the bottom end 107, and one or more reactants enter through the inlet nozzle 120 and move upward in the direction F1 (FIG. 4) through the one or more tubes 131 and through the internal space 103 of the reactor 100, and then exit the tube 131 near the upper end 105 and change direction downward in the direction F2 toward an outlet nozzle 124 that defines a corresponding flange 125. As the reactants travel upward through the one or more tubes 131, the reactants exchange heat with the catalyst and exchange heat with the reactants and products traveling downward in the direction F2 (FIG. 4).

[0106] In an exothermic reaction such as methanol synthesis, the reactants advantageously absorb the heat generated by the reaction in the tubes 131 to preheat the reactants before supplying them to the catalyst bed 140. This is further advantageous in reducing the formation of catalyst hot spots and associated catalyst sintering and product degradation. This further reduces the likelihood of a runaway reaction, as the reactants define a heat exchange medium for removing heat from the catalyst bed. Due to the distribution of the tubes 131, the reactants form a heat exchange modality that is much more effective than, for example, a cooling water sleeve surrounding the reactor 100.

[0107] In addition to the inlet nozzle 120 and the outlet nozzle 124, the reactor 100 may define one or more catalyst removal nozzles 116 and / or one or more handholes 118 that provide access to the internal space 103 through the one or more catalyst removal nozzles 116 and / or the one or more handholes 118. The one or more catalyst removal nozzles 116 may be angled downward to facilitate gravity-based removal of catalyst from the catalyst bed 140, for example, when removing and refilling spent catalyst. The one or more handholes 118 may facilitate maintenance by allowing a technician to insert a hand, tool, or instrument into the internal space 103 near the catalyst support plate 154, the catalyst bed 140, or any other suitable location.

[0108] As seen in FIGS. 1A and 1B, the reactor 100 defines a startup nozzle 110 configured for the supply of a heating fluid. During startup operation, if the reaction has not yet reached steady-state operation, the reactants may not receive the necessary amount of preheating as they travel through the tube bundle 130 in the direction F1. The startup nozzle 110 may receive a heating fluid, such as an inert gas like heated nitrogen gas, that may pass through the internal space 103 and supply sufficient enthalpy to achieve steady-state operation without adversely affecting the yield of the reaction.

[0109] The shell 102 may further define at least one thermocouple port 106. Each thermocouple port 106 may facilitate the insertion of a temperature measuring device axially or longitudinally into the reactor 100, in an embodiment, into the tube bundle 130. By disposing the thermocouple port 106 at the upper portion 105 of the reactor 100, a single temperature measuring device, such as a thermocouple, through which temperature can be measured at multiple positions, can be inserted therethrough. In an embodiment, the temperature measuring device is elongate and may be provided with a plurality of measuring devices, such as a plurality of thermocouples, thereon at a plurality of predetermined distances so that the reactor conditions at each of the plurality of predetermined distances can be measured for improved control of the reaction.

[0110] Two thermocouple ports 106 are shown in FIGS. 1A and 1B on both sides of the startup nozzle 110, but it will be understood that more or fewer thermocouple ports 106 can be provided at any suitable location. By providing a temperature measuring device through the thermocouple port 106, the reactor 100 advantageously enables the measurement of reactor conditions at different height positions within the reactor while minimizing the number of thermocouple junctions, thereby facilitating improved process control and throughput while minimizing the risk of leakage into or out of the shell 102. The location of the thermocouple port 106, regardless of the size of the reactor 100, is in contrast to existing reactor designs where the thermocouple is inserted radially near the shell unevenly such that a larger reactor is sampled, and further enables sampling of the reactor conditions at a desired radial position of the reactor 100.

[0111] Moving on to FIG. 4, the shell 102 defines an inlet nozzle 120, with a corresponding flange 121 disposed at an arbitrary distance below the gas introduction plate 156, and both can be disposed near the bottom end 107 of the reactor 100. The inlet nozzle 120 can be disposed transversely to the longitudinal extent of the reactor 100 such that as reactants flow through the inlet nozzle 120 in the flow direction F4, the reactants change direction and flow into one or more of the tubes 131 of the tube bundle 130 in the direction F1 through the gas introduction plate 156.

[0112] The inlet nozzle 120 can be arranged as shown so as to optimize the distance between the inlet nozzle 120 and the bottom of the tube bundle 130 and to evenly distribute the reactants to the tubes 131 such that eddies that cause blockage, hot spots, and non-uniform flow are avoided. The flange 121 can be configured to facilitate attachment of the reactant supply line to the nozzle 120. Although the inlet nozzle 120 is illustrated and described, it will be understood that the distance between the inlet nozzle 120 and the bottom of the tube bundle 130 may be appropriately larger or smaller.

[0113] Furthermore, or alternatively, the shell 102 further defines a second inlet nozzle 132 with a corresponding flange 133, as shown in FIG. 5A. The flange 133 can be configured to facilitate attachment of the reactant supply line to the nozzle 132. The second inlet nozzle 132 is arranged to direct the reactants vertically in a direction F3 corresponding to or parallel to the upward flow direction F1 through the tubes 131. The reactor shell 102 can be secured by a skirt 108 that defines an opening 122 through its thickness and configured to receive an inlet spool 135 connected to the second inlet nozzle 132.

[0114] The skirt 108 may be cylindrical in shape and extend downward from the bottom end 107 with a substantially the same spread as the reactor shell 102. The skirt 108 may define the reactor 100 and the ring 109 that fixes the skirt 108 in a predetermined position on the same plane. The inlet spool 135 may be curved so that the reactants are supplied in a flow direction generally transverse to the flow direction F3, for example, in a direction substantially parallel to the direction F4 of the inlet nozzle 120, toward the reactor 100. The inlet nozzle 120 and the second inlet nozzle 132 may be configured to act simultaneously or independently of each other. Although the skirt is illustrated and described, any suitable support may be used, and the present disclosure is not limited to the use of the skirt.

[0115] In an embodiment, the diverter 137 may be removably disposed within the second inlet nozzle 132 or the shell 102 to direct the flow direction of the reactants when the second inlet nozzle 132 is in use. The diverter 137 may define a shape that distributes a portion of the flow of reactants from the second inlet nozzle 132 radially outward such that the flow is evenly distributed among a plurality of central tubes that are generally aligned with the second inlet nozzle 132 and the plurality of outer tubes. Although the diverter 137 is illustrated and described, it will be understood that any suitable structure, configuration, or arrangement may be utilized. In an embodiment, the diverter 137 defines a plurality of openings and / or protrusions configured to distribute the flow of reactants flowing in through the nozzle 132.

[0116] Moving on to FIG. 5B, the reactor 100 can be removable from the shell 102 and can further include a domed head portion 104 that is releasably attached thereto at flanges 112, 114 that can include any suitable means for attaching the domed head portion 104 and the shell 102, such as openings and corresponding fasteners. The domed head portion 104 can define a space 113 above the upper extent of the tube bundle 130. The space 113 provides a space for the preheated reactants to mix and return downward through the catalyst bed 140. The nozzle 110 can be defined through the thickness of the domed head portion 104 to allow for the addition of a heating medium during startup operation, as described above.

[0117] Although a domed head portion that can be releasably fixed to the shell is illustrated and described, the present disclosure is not limited thereto, and it will be understood that for any size of reactor, a fixed head with a flanged manhole, for example, can be used instead.

[0118] The thermocouple ports 106 can be aligned with respective thermocouple insertion tubes 126 that can extend any distance above the upper extent of the tube bundle 130. The thermocouple ports 106 can extend through a part or all of the thickness of the domed head portion 104 to allow access to the interior 103 of the reactor. The thermocouple ports 106 can cooperate with a gasket seal, their combination, or any other suitable means, such as by defining an opening sized to be flush with the surface of the temperature measuring device so that pressure can be maintained within the interior 103 of the reactor, to facilitate access to the interior 103 of the reactor. Any suitable means can be used. By extending any distance above the upper extent of the tube bundle 130, the thermocouple insertion tubes 126 are configured to be more readily identifiable during installation of the thermocouples, especially when the domed head 104 is in a given position, as access is limited. The thermocouple insertion tubes 126 can extend along the length of the reactor 100 substantially parallel to or aligned with the supply tube 131.

[0119] Reactor 100 includes one or more catalyst support plates 154, at least one tube support plate 162, 163, 164, 165, a gas introduction plate 156, an upper feed tube support plate 150, and / or an upper plate 190. Providing these can advantageously facilitate fixing the tube bundle 130 within the shell 102 while allowing access to the interior 103 of the reactor as needed for maintenance or other purposes. The gas introduction plate 156 and the catalyst support plate 154 can advantageously be welded to the inner surface of the shell 102 to fix the tube bundle 130 therein.

[0120] The tubes 131 of the tube bundle 130 can be welded to the gas introduction plate 156, the upper feed tube support plate 150, and / or at least one tube support plate 162, 163, 164, 165. In an embodiment, only the gas introduction plate 156 is welded or otherwise fixed to the inner surface of the reactor shell 102, and the upper feed tube support plate 150 and at least one tube support plate 162, 163, 164, 165 are not fixed so as to accommodate thermal expansion of the tubes 131.

[0121] Turning to FIG. 4, the catalyst bed 140 can include one or more sections of catalyst such as a solid catalyst. The catalyst bed 140 can additionally or alternatively include one or more inert sections 142, 144 that include support ceramic balls of a first diameter, such as 1 - 30 mm, more specifically 5 - 20 mm, or in an embodiment 9 mm. The catalyst bed 140 can further include support ceramic balls of a second diameter, such as 1 - 30 mm, more specifically 10 - 25 mm, or in an embodiment 19 mm. The catalyst bed 140 can define separate sections 142, 144 corresponding to ceramic balls that substantially include only balls of a single size.

[0122] For example, in the illustrated embodiment, section 142 substantially comprises only balls having a diameter of 9 mm, while section 144 comprises only balls having a diameter of 19 mm. Sections 142, 144 may have any suitable height within the reactor 100, for example 5 - 500 mm, more specifically 100 - 300 mm, or in the embodiment 200 mm for each of sections 142, 144. The heights of sections 142, 144 may be the same or different from each other. The catalyst bed 140 may further or alternatively comprise a solid catalyst having a shape defining at least one of pellets, rings, tablets, and spheres. Sections 142, 144 may be disposed near (e.g., above or directly above) the catalyst support plate 154 and substantially under section 141 which comprises only solid catalysts of different shapes and / or sizes with respect to the support ceramic balls of sections 142, 144.

[0123] The support ceramic ball sections 142, 144 advantageously support the weight of the catalyst within the catalyst bed while promoting an effective and even distribution of the flow. By providing separate first and second sections 142, 144, the flow of reactants, products, and by-products through the interior 103 of the reactor towards the outlet nozzle 124 allows for the gas flow between the catalyst particles within the catalyst bed 140, between the smaller first diameter support ceramic balls within the first section 142, and finally between the larger second diameter support ceramic balls within the second section 144, improving the gas flow before passing through the catalyst support plate 154. The support ceramic balls may advantageously be inert and configured to withstand thermal shock and corrosion from various reactants, products, and / or by-products. Although support ceramic balls are described, it will be understood that sections 142, 144 may have more or fewer sections and may comprise support structures of different shapes or sizes such as rings, cylinders, polygons, or others.

[0124] In an embodiment, section 141 of catalyst bed 140 has, or may define, a first height 148 corresponding to the height of the non-reduced catalyst and a second height 146 corresponding to the height of the reduced catalyst.

[0125] Section 141 of catalyst bed 140 may comprise catalyst particles of a single size and / or shape, although it will be understood that separate sections within catalyst bed 140 of catalyst particles of different sizes and / or shapes are contemplated within the scope of the present disclosure. The catalyst particles may have any suitable shape or configuration, such as spheres, pellets, cylinders, trilobes, quadrilobes, pyramids, cones, stars, or otherwise, and may have any suitable number and size of apertures defined therethrough, and / or a plurality of notches or grooves defined on a portion of their surface. Separate sections corresponding to a single, different type of catalyst size and / or shape may be provided within catalyst bed 140, for example, as axial or radial layers or pockets. In an embodiment, catalyst particles of different sizes and shapes may be provided and mixed together within the catalyst body in any suitable configuration.

[0126] The catalyst particles within catalyst bed 140 may function as the support ceramic balls within sections 142, 144, and may cooperate with the support ceramic balls, and vice versa. In an embodiment, the catalyst particles are selected independently of the support ceramic balls.

[0127] The tube bundle 130 according to the embodiment is shown in FIGS. 6 and 7. The tube bundle 130 is configured to extend substantially longitudinally about the axis 1A-1A within the shell 102, and is maintained by, in order from the top to the bottom, an upper plate and a tube support plate 150, a plurality of tube support plates 162, 163, 164, 165, a catalyst support plate 154, and a gas introduction plate 156. The distance 161 between the upper plate and the tube support plate 150 and the tube support plate 162, as well as between the tube support plates 162, 163, 164, and 165, may be uniform along the length of the tube bundle 130. In an embodiment, the distance 161 may vary. The distance 167 between the tube support plate 165 and the catalyst support plate 154 may be greater than the distance 161. The distance 169 between the catalyst support plate 154 and the gas introduction plate 156 may be smaller than the distance 167. It will be understood that the depicted embodiments are merely exemplary and that any arrangement of the tube bundle 130 may be used.

[0128] The plurality of tubes 131 may define a uniform thickness and diameter along the longitudinal length of the tube bundle 130. In an embodiment, the plurality of tubes 131 have a tapered thickness along the length of the tube bundle, with the thickness and / or diameter increased in the vicinity of one or more plates 150, 162, 163, 164, 165, 154, 156 to support the plurality of plates. In an embodiment, one or more of the tubes 131 of the tube bundle 130 may have an increased thickness relative to the other plurality of tubes 131 to increase structural support. For example, the plurality of tubes 131 extending closer to the center or outer edge of the tube bundle 130 may have an increased thickness relative to the other plurality of tubes of, for example, 10%, 20%, 25%, 33%, 50% or any other suitable thickness. That is, the plurality of walls of such plurality of tubes 131 may have an increased thickness while maintaining the same inner diameter in an embodiment. This advantageously allows the plurality of tubes 131 having an increased thickness to carry reactants while supporting the tube bundle 130, thereby freeing up cross-sectional area for increased catalyst loading and more evenly distributed catalyst relative to other structural arrangements.

[0129] In an embodiment, the plurality of tubes 131 have a reduced thickness and / or an increased diameter near the bottom of the reactor 100 to facilitate more efficient heat transfer near the bottom of the reactor 100, for example, compared to the top of the reactor 100. Alternatively, one or more of the plurality of tubes 131 of the tube bundle 130 may comprise an internal tube rod configured to increase the velocity of the reactants preheated therein. The internal tube rod may extend a portion or all of the distance from the bottom of the plurality of tubes 131 to the top of the plurality of tubes 131.

[0130] Generally, the tube bundle 130 and the reactor 100 are advantageously configured modularly in design and implementation. Existing shell-and-tube reactors are not easily scalable due to the significant rework that must be done to properly balance the tube length and diameter, catalyst bed, shell, and other components, but the design of the reactor 100 advantageously allows for expansion or contraction based on a plurality of concentric banded arrangements of the plurality of tubes 131 on the tube bundle 130. The tube bundle 130 can be such that other geometric features of the reactor can remain unchanged even when multiple annular bands of the plurality of tubes 131 are added (to increase the capacity of the reactor design for higher throughput or during bottleneck resolution efforts) or removed (to decrease the capacity of the reactor design). As a result, large-scale redesign work can be avoided.

[0131] The tube bundle 130 can be configured such that one or more geometric constraints or ratios are maintained in any design, whether the reactor and tube bundle are configured for reduced throughput or increased throughput in various designs. To ensure that the tube density is improved, the average tube pitch of the tube bundle (i.e., the center-to-center distance between the plurality of tubes) is substantially constant across the tube bundle, and the plurality of annular bands and tubes that define it are spaced to maintain a constant tube pitch.

[0132] As another example, the tube bundle 130 advantageously achieves a desired ratio of the cumulative cross-sectional area of the catalyst bed in a plan view of the reactor to the cumulative cross-sectional area of the plurality of tubes 131 (i.e., the combined total radial surface area of the plurality of tubes) in the same plan view. In embodiments, the ratio of the cumulative cross-sectional area of the catalyst to the cumulative cross-sectional area of the plurality of tubes is in the range of 2 to 20, more specifically 5 to 12.

[0133] Even if an annular band of a plurality of tubes 131 is added to or removed from the design of the tube bundle 130, the cross-sectional area of the plurality of tubes 131 with respect to the catalyst bed can be simply and easily adjusted so as to remain within a suitable range such that the performance of the reactor, and in particular its safety profile, is suitable. In embodiments, the addition or removal of one or more annular bands of the plurality of tubes may not substantially change the cumulative cross-sectional area of the catalyst with respect to the cumulative cross-sectional area of the plurality of tubes. In other embodiments, the tube bundle 130 is designed such that the removal or addition of a plurality of annular bands of the plurality of tubes does not require a major redesign, but rather allows an engineer to simply and easily adjust the reactor to new required capacities or other requirements, such that any other geometric or process-related parameters are targeted. By providing the tube bundle 130 with a specified relationship between the cross-sectional areas of the plurality of tubes and the catalyst bed, heat distribution is improved, which reduces the hot spot and reduces the likelihood of a runaway reaction by improving the overall throughput through the reactor 100.

[0134] The reactor 100 can be controlled and maintained during operation so as to control one or more characteristics of the catalyst bed 140 and / or the tube bundle 130. In some embodiments, the reactor 100 is configured to utilize a temperature measuring device to evaluate the distribution of heat across the cross-sectional area of the catalyst bed. In particular, the reactor 100 can be controlled by evaluating the radial temperature gradient within the reactor as a function of depth (from the upper end 105 to the lower end 107) within the reactor 100, and / or evaluating the growth of said gradient as a function of depth.

[0135] Moving to FIGS. 12 and 13, the catalyst support plate 154 is configured to support the total height of the solid catalyst, such as the heights of sections 142 and 144, in combination with the height of section 141. The catalyst support plate 154 is further configured to advantageously support the forces resulting from the differential pressure on the catalyst bed 140. The catalyst support plate 154 can be disposed within the shell 102 in the vicinity of the catalyst removal nozzle 116 and / or the handhole 118. The catalyst support plate 154 may define one or more openings 180, 181. The openings 180, 181 comprise or may define a plurality of openings including a plurality of openings of a first size corresponding to the opening 180 and a plurality of openings of a second size corresponding to the opening 181, and the plurality of openings extend through at least a portion of the thickness of the catalyst support plate 154.

[0136] The first size of the opening 180 may correspond to the circumference of at least one tube 131 of the tube bundle 130. In an embodiment, the first size of the opening 180 is larger than the circumference of the plurality of tubes 131 to allow for any degree of movement and / or thermal expansion of the plurality of tubes within the opening 180. The opening 180 may be defined through the catalyst support plate 154 depending on the arrangement of the plurality of tubes 131 within the tube bundle 130. The second size of the opening 181 is smaller than the first size of the opening 180, and the second size of the opening 181 may serve to allow the flow of reactants, reaction products, and reaction by-products therethrough in the path to the outlet nozzle 124.

[0137] In an embodiment, one or more of the openings 180 may define the termination of a temperature measuring device. The opening 182 may be sized and configured to receive the thermocouple insertion tube 126 and terminate an extension of the thermocouple insertion tube 126 (FIG. 7). The opening 182 may, in an embodiment, extend only through a portion of the thickness of the catalyst support plate 154. In an embodiment, the thermocouple insertion tube 126 may be welded to and sealed at the catalyst support plate 154. The plurality of tubes 131 may not be welded to the catalyst support plate 154 to account for the effects of thermal expansion.

[0138] The size of the plurality of openings 181 and / or the average distance between the plurality of openings 181 can be a function of the thickness of the catalyst support plate 154 such that the size of the plurality of openings 181 is proportional to the thickness of the catalyst support plate 154 and / or the distance between the plurality of openings 181 is inversely proportional to the thickness of the catalyst support plate 154. That is, the greater the thickness of the catalyst support plate 154, the larger the diameter of the plurality of openings 181 and / or the smaller the distance between the plurality of openings 181. In an embodiment, the catalyst support plate 154 can have a thickness of 20 to 500 mm, more specifically 50 to 300 mm, and in an embodiment 110 mm, while the plurality of openings 181 can have a diameter of 1 to 50 mm, more specifically 5 to 25 mm, and in an embodiment 10 mm.

[0139] As can be seen in the enlarged view of FIG. 13, the plurality of openings 180 can extend in a pattern or arrangement corresponding to the arrangement of the plurality of tubes 131 within the tube bundle 130, as described in more detail herein. The plurality of openings 181 can extend between each of the plurality of openings 180. The plurality of openings 181 can define any suitable pattern or arrangement, such as an extending direction 183A defining a straight line and / or a transverse extending direction 183B. Other patterns or arrangements of the plurality of openings 181 are envisioned within the scope of the present disclosure. The plurality of openings 181 can be spaced apart from each other by any distance, for example, in an embodiment, 1 to 30 mm, more specifically 5 to 20 mm, and in an embodiment 15 mm, between the centers of adjacent ones of the plurality of openings 181, along one or both of the directions 183A, 183B. The distance between the centers of adjacent ones of the plurality of openings 181 need not be uniform across the entire surface of the catalyst support plate 154, but rather can vary as appropriate.

[0140] The catalyst support plate 154 may define a band 184 of the material forming the catalyst support plate 154 that does not define either of the openings 180, 181 at the outer periphery. The band 184 extends partially or entirely around the outer periphery of the catalyst support plate 154 and advantageously facilitates welding or other suitable attachment of the catalyst support plate 154 to the inner surface of the shell 102. In an embodiment, the band 184 extends into a recess defined by the inner surface of the shell 102 and may then be welded to the recess. The band 184 may extend radially a distance of any suitable distance, such as 5 mm.

[0141] Referring to FIG. 11, the gas introduction plate 156 may be disposed under the catalyst support plate 154 and may comprise a plurality of openings 155 defined through at least a portion of the thickness of the gas introduction plate 156. The plurality of openings 155 may be defined through the gas introduction plate 156 according to the arrangement of the plurality of tubes 131 of the tube bundle 130 and may be circular openings that are aligned with the arrangement of the plurality of openings 180 of the catalyst support plate 154. In an embodiment, the gas introduction plate 156 is substantially solid with no openings other than the plurality of openings 155 and pushes the incoming reactants into the plurality of tubes 131. The plurality of tubes 131 may be seal welded and / or strength welded to the gas introduction plate 156. It will be understood that when one component is described herein as being welded to another component, seal welding, strength welding, combinations thereof, or any other type of attachment may be contemplated.

[0142] Referring to FIGS. 8 - 9, the reactor 100 may further include at least one tube support plate 150, 162, 163, 164, 165 that may be longitudinally spaced along the axial or longitudinal length of the tube bundle 130. Although tube support plates 150, 162, 163, 164, 165 are shown and represented, it will be understood that more or fewer support plates may be provided. The upper supply tube support plate 150 is substantially the same as tube support plates 162, 163, 164, 165 and may include or omit one or more features. For example, the upper supply tube support plate 150 may have the same features as tube support plates 162, 163, 164, 165 and may further include one or more spacers configured to cooperate with the upper plate, as will be described in more detail below.

[0143] The tube support plates 150, 162, 163, 164, 165 may include at least one annular band 168 configured to maintain the position of at least one tube 131. The at least one annular band 168 includes at least one bracket 172 configured to extend around a portion of the tubes 131 of the tube bundle 130. In an embodiment, the at least one bracket 172 extends around the entire tube 131. The bracket 172 may be configured to be removably attached to the tube 131.

[0144] In an embodiment, the bracket 172 may extend around only a portion rather than the entire tube. The bracket 172 may advantageously cooperate with a beam portion 173 that extends between the bracket 172 and an adjacent bracket 172 attached to an adjacent tube 131. The bracket 172 may be connected to the beam portion 173 removably or non - removably and may define, for example, a fillet connection. The annular band 168 may be defined by a series of connected brackets 172 and beam portions 173 that define a generally annular arrangement with the corresponding tube 131.

[0145] The annular band 168 is arranged concentrically with the adjacent annular bands 168 of the tube support plates 150, 162, 163, 164, 165, and the annular band 168 may optionally be arranged about the longitudinal axis 1A-1A of the reactor. The tube support plates are defined by the cooperation of the brackets 172, the beam portion 173, the radial members 166, and the annular band 168. Although the annular band 168 is shown and represented, it will be understood that any suitable configuration including an asymmetric arrangement, an offset arrangement, or a non-annular arrangement may be used. Although the cooperation of various components has been described as defining the tube support plates, it will be understood that the tube support plates may take any suitable configuration and are thus not limited thereby.

[0146] At least one of the tube support plates 150, 162, 163, 164, 165 defines at least one radial member 166 connected to at least one annular band 168 at attachment point 169 and / or to the outer support band 170 at attachment point 171. The tube support plates may define a plurality of radially symmetrically arranged radial members 166, for example, at 22.5° increments, at 30° increments, at 45° increments, at 90° increments, at 120° increments, at 180° increments, at another increment evenly divisible by 360°, or in other ways. In other embodiments, the plurality of radial members 166 are arranged asymmetrically in any suitable manner.

[0147] The outer support band 170 may define a substantially continuous band of a support material such as stainless steel that provides sufficient rigidity, strength, and / or support to the tube support plate and / or facilitates attachment of the outer support band 170 to the inner surface of the reactor shell 102. Eight radial supports 166 are illustrated and represented with respect to the embodiments of FIGS. 9 and 10, although more or fewer radial supports 166 may be provided, and it will be understood that all of the tube support plates 150, 162, 163, 164, 165 need not have the same number or arrangement of radial supports or other components.

[0148] The plurality of radial supports 166 may extend straight outwardly from the center of the tube support plate to the outer support band 170 or may define a curved, bent, serpentine, or other configuration. The plurality of radial supports 166 may be formed of any suitable material such as stainless steel and may define heat resistant properties to maintain the desired rigidity and strength in the reactor condition. The plurality of radial supports 166 advantageously define attachment points 169 between the annular band 168 and the plurality of radial supports 166. The attachment points 169 may be removable or non-removable and may define any suitable connection such as being welded together or attached by suitable fasteners. The tube support plate may be configured to move with the plurality of tubes 131 due to thermal expansion and contraction and may be formed of a high temperature resistant material such as steel (e.g., stainless steel), ceramic, polymeric material, composite material, or otherwise.

[0149] In embodiments, the tube support plates 150, 162, 163, 164, 165 may be manufactured using any suitable means. In embodiments, the tube support plates 150, 162, 163, 164, 165 are formed from a single solid plate from which material is removed, for example by water jet cutting. In other embodiments, the radial supports and the annular band are manufactured separately and assembled to form the tube support plate.

[0150] The upper supply tube support plate 150 may further define one or more spacers 174 on its upper surface. The spacer 174 can be attached to one or more structures of the upper supply tube support plate 150 in any suitable manner, such as by welding. The spacer 174 may extend a predetermined height and may define an opening within its central portion. The opening may comprise one or more threads configured to mate with one or more threads of a fastener, as described in further detail below with respect to the upper plate 190. The spacer 174 can extend around the upper supply tube support plate 150 in any suitable arrangement and in any suitable number.

[0151] For example, when the spacer 174 is attached to a plurality of radial supports 166, the spacer 174 can define three concentric ring patterns 175 (FIG. 9) around the upper supply tube support plate 150. In an embodiment, the spacer 174 extends along four radial supports 166 between the first and second annular bands, between the seventh and eighth annular bands, and between the thirteenth and fourteenth annular bands. A total of four spacers 174 can be arranged on each concentric ring pattern 175 such that the corner portions of each segment of the upper plate 190 are fixed thereto, as described below.

[0152] The arrangement of the plurality of radial supports 166 advantageously provides for secure attachment of the plurality of tubes 131 of the tube bundle 130 while minimizing interference with the distribution of the catalyst as the catalyst is loaded from the upper portion 105 of the reactor 100. For example, as catalyst particles are poured into the shell 102, the plurality of radial supports 166 are configured to minimize non-uniform distribution of the catalyst. In an embodiment, the plurality of radial supports 166 of adjacent tube support plates 162, 163, 164, 165 can be axially aligned along the longitudinal extent of the reactor 100.

[0153] In other embodiments, as seen in FIG. 10B, the plurality of radial supports 167 of adjacent tube support plates may be offset from the plurality of radial supports 166 to facilitate an even distribution of the catalyst being loaded. The degree of offset can be any suitable degree. In an embodiment, the plurality of radial supports 167 are offset by a distance corresponding to half of the angular distance between the plurality of radial supports 166. In the embodiment of FIG. 10B, the radial supports 166 are offset from each other by 45°, and the offset of the plurality of radial supports 167 is 22.5°. Subsequent tube support plates may be arranged alternately. The plurality of radial supports 166 of adjacent tube support plates may be offset downward in the longitudinal length of the reactor to define a spiral or helical pattern. The illustrated embodiments are exemplary, and any other arrangement may be used as appropriate.

[0154] The tube bundle 130 may be arranged such that the innermost annular band 168A of at least one tube support plate comprises six brackets each configured to correspond to a ring of the six innermost tubes of the first size. The first size can be, for example, a diameter of 0.5 to 3 mm, more specifically a diameter of 1 to 2 mm, and in an embodiment 1.5 mm. The second annular band 168B of at least one tube support plate comprises ten brackets each configured to correspond to a ring of ten tubes of the tube bundle of the first size. The third annular band 168C of at least one tube support plate comprises fourteen brackets each configured to correspond to a ring of fourteen tubes of the tube bundle of the second size. The second size can be, for example, a diameter of 0.5 to 5 mm, more specifically 1 to 4 mm, and in an embodiment 2.5 mm.

[0155] The fourth annular band 168D of at least one tube support plate comprises 18 brackets each configured to correspond to a ring of 18 tubes of a tube bundle of a first size. The fifth annular band 168E of at least one tube support plate comprises 22 brackets each configured to correspond to a ring of 22 tubes of a tube bundle of a first size. The sixth annular band 168F of at least one tube support plate comprises 26 brackets each configured to correspond to a ring of 26 tubes of a tube bundle of a first size.

[0156] The seventh annular band 168G of at least one tube support plate comprises 30 brackets each configured to correspond to a ring of 30 tubes of a tube bundle of a second size. The eighth annular band 168H of at least one tube support plate comprises 34 brackets each configured to correspond to a ring of 34 tubes of a tube bundle of a first size. The ninth annular band 168I of at least one tube support plate comprises 36 brackets each configured to correspond to a ring of 36 tubes of a tube bundle of a first size. The tenth annular band 168J of at least one tube support plate comprises 42 brackets each configured to correspond to a ring of 42 tubes of a tube bundle of a first size.

[0157] The 11th annular band 168K of at least one tube support plate comprises 46 brackets each configured to correspond to a ring of 46 tubes of a tube bundle of a second size. The 12th annular band 168L of at least one tube support plate comprises 50 brackets each configured to correspond to a ring of 50 tubes of a tube bundle of a first size. The 13th annular band 168M of at least one tube support plate comprises 54 brackets each configured to correspond to a ring of 54 tubes of a tube bundle of a first size. The 14th annular band 168N of at least one tube support plate comprises 58 brackets each configured to correspond to a ring of 58 tubes of a tube bundle of a second size.

[0158] Although the 1st to 14th annular bands are illustrated and represented, it will be understood that embodiments of the reactor of the present disclosure facilitate a modular reactor configuration that better accommodates different processing capacity requirements of different facilities than existing reactor designs. If desired, for example, an engineer may modify the depicted tube bundle 130 to have more, fewer, and / or different annular bands. Additional annular bands may be added to increase the number of tubes in a simple retrofit and to expand the tube bundle outwardly in order to expand the tube bundle 130 and reactor 100 as a whole to accommodate a higher annual production capacity of the plant, such as during efforts to eliminate bottlenecks. For example, the attachment 171 between the radial support 166 and the outer band 170 may be removed so that additional annular bands can be added to the tube support plate, and the outer band 170 around the new annular band may be replaced. For this purpose, the outer band 170 may be configured to have an expandable circumference.

[0159] Conversely, to reduce the reactor 100, the annular zones, such as the outermost annular zone, can be removed to fit a smaller reactor shell and / or to reduce the size of the tube bundle to provide a corresponding lower annual plant production capacity. This can be done, for example, by removing the attachment 169 between the annular zone and the radial support.

[0160] Furthermore, the arrangement of the annular zones as shown allows for the addition or removal of annular zones, as well as the accompanying plurality of brackets and plurality of tubes, while corresponding to the structure of the radial supports. As can be seen, the annular zones are arranged in the space between the plurality of tubes such that the plurality of tubes are in a substantially even distribution and the catalyst and reactants can pass between them, and such that the addition or removal of the annular zones is possible without substantially compromising the design of the radial supports and tube supports, as the number of brackets and tubes increases.

[0161] In an embodiment, the ninth annular zone 168I (or any other) of at least one tube support plate further comprises a bracket 172 corresponding to at least one thermocouple insertion tube 126, where the at least one thermocouple insertion tube 126 is of a first tube size. By providing the bracket 172 on the thermocouple insertion tube 126, it becomes possible to insert a temperature measuring device into the tube bundle, preferably into any region of the tube bundle surrounded by the catalyst and the plurality of tubes, in order to obtain an accurate temperature measurement value along the longitudinal length of the reactor.

[0162] The upper and supply tube support plates may include, similar to tube support plates 162, 163, 164, 165, one or more radial supports 166, an outer band 170, and one or more brackets 172 configured to engage and / or surround tube 131 of tube bundle 130. The radial supports 166 of the upper supply tube support plate 150 may be arranged similar to or corresponding to the supports 166 of the supply tube support plates 162, 163, 164, 165 and may be axially split at a suitable angle 176 (FIG. 9), for example 45°. It will be understood that other angles or arrangements are contemplated by the present disclosure.

[0163] The bracket 172 of the upper supply tube support plate 150 forms or extends near the end of the tube 131 where preheated reactants exit the tube 131 and then flow downward in a second direction F2. The thermocouple insertion tube 126 extends at any distance above the uppermost distance or extent of the tube 131, which may facilitate easier insertion of a temperature measuring device from the thermocouple port 106 into the thermocouple insertion tube 126. Similar to the tube support plates 162, 163, 164, 165, the upper supply tube support plate 150 may be configured to be sized up or down to suit the desired capacity of the reactor 100.

[0164] The arrangement of the tube bundle 130 and the tube support plates 150, 162, 163, 164, 165 may advantageously indicate the cause of reactor heat transfer and reactor kinetics.

[0165] Moving on to FIGS. 14 - 16, the upper plate 190 is shown. The upper plate 190 can be installed on or above the upper supply tube support plate 150. The upper plate 190 has a modular configuration and can define four separate segments 192 surrounded by a flange 191. The upper plate 190 can define a plate edge 194, one or more tube holes 202 defined through at least a portion of the thickness of the plate 190, and one or more gas openings 204 defined through at least a portion of the thickness of the plate 190. The tube holes 202 can be generally aligned with the arrangement of the tubes 131 of the tube bundle 130 and can be configured to facilitate the passage of preheated reactants from the tubes 131 into the space 113 (FIG. 5B) of the reactor 100.

[0166] The gas openings 204 facilitate the passage of preheated reactants into the catalyst bed 140 and ensure proper flow distribution. The upper plate 190 can be configured to create a small pressure drop to make the flow entering the catalyst bed as uniform as possible. The upper plate 190 is advantageously illustrated and configured to use a simplified design as shown and represented, as opposed to existing techniques that may utilize heavy, and / or costly designs that are difficult to manufacture and / or operate for maintenance purposes and / or complex designs, to achieve improved uniformity of flow distribution.

[0167] Since the upper plate 190 can extend outwardly to the flange 191, the gas openings 204 can extend substantially to the edge 194 without leaving a gap such as within the catalyst support plate 154. The upper plate 190 can have a reduced thickness compared to the catalyst support plate 154. In embodiments, the upper plate 190 has a thickness of 1 - 25 mm, more specifically 5 - 15 mm, and in an embodiment 8 mm.

[0168] The upper plate 190 is configured to be removably attached to the shell 102 and / or to the upper plate and the tube support plate 150 by any suitable mechanism, for example, by use of fastening members 196 that cooperate with corresponding openings 193 (FIG. 15) at the edges of each section of the plate 190. The fastening members 196 of the upper plate 190 extend between the upper plate 190 and the upper supply tube support plate 150 and can cooperate with one or more spacers 174 that are welded, for example tack welded, to the upper supply tube support plate 150.

[0169] In an embodiment, the spacer 174 has a height and / or perimeter sufficient to receive the mating end of the fastening member 196 within a track or recess defined through a portion of the thickness of the spacer 174, which can enable a secure attachment of the upper plate 190 to the upper supply tube support plate 150. The height of the spacer 174 can be from 1 to 30 mm, more specifically 5 to 20 mm, and in an embodiment 15 mm. The spacer 174 can be welded to the radial support 166, the annular band 168, the bracket 172, or others. As can be seen, the fastening member 196, and the corresponding spacer 174, may be positioned such that the fastening member, and the spacers 196, 174 are provided at each corner and along the inner edges of the section 194 of the upper plate 190.

[0170] The upper plate 190 further comprises, or may cooperate with, one or more load rings 195. The load rings 195 can be any suitable component configured to facilitate positioning and / or removal of the section 194 of the upper plate 190. The load rings 195 can be attached through one or more gas openings 204 or at any other suitable location, and removably fixed to the upper plate 190 and can define components for manipulating the upper plate 190. In an embodiment, the load rings 195 are configured to enable an operator to grip the upper plate 190 by means of a tool for lifting the upper plate 190 in a direction away from the reactor shell 102.

[0171] By modularly providing a plurality of separate sections 194 on the upper plate 190, the upper plate 190 can be more easily removable and replaceable during maintenance operations without sacrificing the upper plate 190's ability to distribute reactants and fix the catalyst bed 140. The modular configuration of the upper plate 190 allows for the production of a plurality of identical sections 192 instead of a monolithic plate 190, making the manufacturing process less costly and less complex. One advantage of the arrangement of the upper plate 190 is that a factory worker can stand on one of the plurality of sections 194 of the upper plate 190 while loading catalyst through the provided openings by the removed section 194.

[0172] Referring to FIGS. 17 - 19, a retaining plate 210 for use with one or more nozzles of the reactor 100 is illustrated and represented. The retaining plate 210 can secure the catalyst removal nozzle 116 and / or the handhole 118. The retaining plate 210 may comprise a handle 212 and is configured to cooperate with a defined lip 214 by the nozzle 116. In an embodiment, the nozzle 116 defines a plurality of lips 214 circumferentially disposed around the opening of the nozzle in any suitable pattern, and the retaining plate 210 is configured to abut the inner surface of the lip 214 as seen in FIG. 17. In an embodiment, the plurality of lips 214 are spaced apart at any angle, such as 15°, 20°, 30°, 45°, 60°, 90°, or others. The arrangement of the plurality of lips 214 can be symmetric or asymmetric. The flange 117 of the nozzle 116 can define one or more openings 211 through which a suitable fastener can be received to connect the nozzle 116 to a suitable spool.

[0173] In certain embodiments, the plurality of lips 214 do not extend around the bottom - most section B of the circumferential opening defined by the catalyst removal nozzle 116 or the handhole 118. Rather, as seen in FIG. 19, the bottom - most section B is unobstructed so that catalyst particles can freely flow under the influence of gravity during catalyst removal. The arrangement of the retaining plate 210 prevents the catalyst from flowing too fast during catalyst removal.

[0174] Turning to FIG. 20, a reactor 300 according to an embodiment is illustrated and represented. Reference numerals in the "300" series may include features similar to or identical to those already represented by reference numerals in the "100" series. The reactor 300 may receive and secure a tube bundle having an upper plate 350 as described above, and includes a shell 302 that defines an inlet nozzle 320 and an outlet nozzle 324. The shell 302 further includes a dome-shaped upper portion 304 that defines and / or supports a thermocouple insertion nozzle 306, or may cooperate with the dome-shaped upper portion 304. The dome-shaped upper portion 304 may be fixed to the shell 302 by a flange 312. The reactor 300 extends longitudinally about the axis 20A-20A. The catalyst bed 340 may extend to a suitable height within the internal space defined by the reactor shell 302.

[0175] The reactor 300 further defines a thermocouple insertion tube 326 that extends about the longitudinal axis 20A-20A, or substantially parallel to or aligned with the longitudinal axis 20A-20A and through the catalyst bed 340. The thermocouple insertion tube 326 may be integrated with or independent of the tube bundle as described above. The thermocouple insertion tube 326 is configured to receive a temperature measuring device 310 that also extends about the longitudinal axis 20A-20A. The temperature measuring device 310 may be a multi-element thermocouple. The multi-element thermocouple is configured to obtain temperature measurements at a plurality of locations along the reactor 300.

[0176] As shown in FIG. 20, the temperature measurement device 310 may include eight measurement positions 382A, 382B, 382C, 382D, 382E, 382F, 382G, 382H along the length of the reactor 300 and extend to the end 327. The temperature measurement device 310 may have an overall length 330I. The positions 382A, 382B, 382C, 382D, 382E, 382F, 382G, 382H may be spaced apart by distances 330A, 330B, 330C, 330D, 330E, 330F, 330G, respectively. The distances 330A, 330B, 330C, 330D, 330E, 330F, 330G may be the same distance such that the measurement positions are equally spaced along the reactor 300, or may be different distances depending on the requirements of a particular process.

[0177] The thermocouple insertion tube 326 may be configured to preferably define an opening within the thermocouple insertion tube 326 at or near the positions 382A, 382B, 382C, 382D, 382E, 382F, 382G, 382H, for example, to enable the temperature measurement device 310 to measure the temperature inside the reactor, so that the temperature measurement device 310 can obtain measurement values at the positions 382A, 382B, 382C, 382D, 382E, 382F, 382G, 382H. Although a temperature measurement device is shown, it will be understood that the present disclosure is not limited to other types of sensors and, in particular, to multi-element thermocouples. In embodiments, different sensors may be arranged at different positions as required.

[0178] The temperature measurement device 310, the reactor 300, and the thermocouple insertion tube 326 advantageously reduce the number of thermocouple junctions, thereby providing highly resolved reactor state data at multiple positions within the reactor, particularly in the case of high pressure and / or high temperature service, and / or in the case of reactions involving catalysts sensitive to hydrogen or oxygen, while simultaneously minimizing the risk of leakage, facilitating improved process control. The configuration of the temperature measurement device 310, the reactor 300, and the thermocouple insertion tube 326 further improves the scalability of the reactor design as the arrangement of the thermocouple insertion tube 326 and the temperature measurement device 310 enables accurate measurement of the internal reactor state regardless of the reactor size, monitors a reactor with thermowells arranged radially from the side wall surface of the reactor, and reduces the difficulty of disproportionally measuring the conditions near the shell rather than near the center of the reactor in the case of a larger reactor.

[0179] Furthermore, as can be seen at least in FIGS. 2 and 7, the reactor may comprise a plurality of temperature measurement devices. The temperature measurement devices may be arranged in any suitable configuration relative to the reactor shell and relative to each other. In the embodiments of FIGS. 2 and 7, for example, the temperature measurement devices may be offset from the central longitudinal axis of the reactor by the same distance and arranged on opposite sides of each other. The distance between the plurality of temperature measurement devices may be configured to minimize interference with or disturbance of the heat distribution within the reactor, particularly within the catalyst bed. The distance may be selected to be above a minimum threshold at which hot spots occur between or in the vicinity of the plurality of temperature measurement devices due to the resulting interruption to the flow of reactants and products and thus to the heat distribution. Arranging the plurality of temperature measurement devices above the minimum threshold thereby avoids disruption of the reactor performance and improves the accuracy of the measured values.

[0180] Multiple temperature measuring devices may serve different purposes and / or may be complementary to each other. In the embodiments of FIGS. 2 and 7, the temperature measuring device is a plurality of multi-element thermocouples as represented with respect to FIG. 20. One of the plurality of multi-element thermocouples may be connected to a process control system, while a second one of the plurality of multi-element thermocouples may be connected to a safety instrumentation system.

[0181] By providing a plurality of multi-element thermocouples, advantageously, the measurement of the temperature at a specific location, i.e., height, within the reactor is confirmed. If there is a difference between the plurality of signals obtained from the plurality of multi-element thermocouples, it can be used, for example, to determine the occurrence of a hot spot at a specific height and enable an operator to make adjustments as needed. It will be appreciated that any suitable number of thermocouples in any suitable configuration may be used.

[0182] Embodiments of the reactor comprise a plurality of supply tubes extending longitudinally through the reactor and the catalyst bed. The tube bundle may define a plurality of thermocouple insertion tubes that extend parallel to the plurality of supply tubes and are configured to receive temperature measuring devices, such as multi-element thermocouples, therethrough. The plurality of thermocouple insertion tubes may be configured to extend at different distances from the center of the reactor.

[0183] The plurality of distances may be configured to enable the measurement of the temperature distribution at a plurality of different distances from the center. In particular, this may help verify the design of the reactor at a particular scale and further enhance the scalability of the reactor of the embodiments of the present disclosure. This improves the subdivision of the temperature measurement and enables the associated response to be adjusted using a process control system, further strengthening the process control of the reactor. In an embodiment, the radial configuration of the plurality of thermocouple insertion tubes may be determined to coincide with a predicted hot spot.

[0184] This enables the operator to quickly and accurately determine when a hot spot is formed and respond accordingly, thereby preventing a runaway reaction. The configuration of the plurality of thermocouple insertion tubes can further be determined for the tube bundle to correspond to the size of the reactor shell. In a smaller reactor, for example, fewer thermocouple insertion tubes may be utilized, but the number of thermocouple insertion tubes and the complexity of their configuration can increase in a larger reactor.

[0185] By providing a reactor according to the disclosed embodiments, the problems that existing reactors are difficult to access when maintenance is required and difficult to expand / contract based on the need for facility throughput are addressed. Embodiments of the reactors of the present disclosure are advantageously modularly arranged based on the need for facility design throughput, are easily accessible for maintenance and catalyst loading, facilitate improved even distribution of catalyst, reactants, and heat, and / or provide a robust but flexible reactor interior configured to provide robust structural support during construction, transportation, installation, and operation.

[0186] In the drawings and the foregoing description, reactors have been illustrated and described, but they are to be regarded as illustrative and not restrictive, and only the preferred embodiments have been illustrated and described, and it is understood that all changes, equivalents, and modifications falling within the scope of the spirit of the embodiments defined by the following claims are to be protected.

[0187] Thus, the plurality of features of the disclosed embodiments can be combined or arranged by those skilled in the art to achieve specific advantages as would be understood from the present disclosure. Similarly, the plurality of features of the disclosed embodiments can provide independent benefits applicable to other embodiments not detailed herein. In particular, any feature from one disclosed embodiment can be employed in another disclosed embodiment.

[0188] It is to be understood that not necessarily all objectives or advantages may be achieved under any embodiment of the present disclosure. One skilled in the art will recognize that the reactor may be implemented or performed in a manner that realizes or optimizes one advantage or group of advantages as taught, without realizing other objectives or advantages as taught or suggested.

[0189] One skilled in the art will recognize the interchangeability of the various features disclosed. Other known equivalents for each feature, in addition to the variations described, may be mixed and matched by one skilled in the art to manufacture or use a reactor under the principles of the present disclosure. One skilled in the art will understand that the features described may be adapted to other types of reactors, reaction suites, chemical species, and processes. Thus, the present disclosure, as well as its embodiments and variations, is not limited to the methanol synthesis process or to shell and tube reactors, but may be utilized in any chemical process.

[0190] While the present disclosure describes specific exemplary embodiments and examples of reactors, it will thus be understood by one skilled in the art that the present disclosure extends beyond the specifically disclosed embodiments to other alternative embodiments and / or uses of the present disclosure, as well as obvious modifications and equivalents thereof. It is intended that the present disclosure not be limited by the above specifically disclosed embodiments.

[0191] Furthermore, unless otherwise indicated, any numerical values used in the specification and claims to represent quantities, components, distances, or other measurements should be understood to be optionally modified by the term "about" or its synonyms. When terms such as "about", "approximately", "substantially", etc. are used with a stated amount, value, or condition, it can be understood to mean an amount, value, or condition that deviates by less than 20%, less than 10%, less than 5%, less than 1%, less than 0.1%, or less than 0.01% from the stated amount, value, or condition. As used herein, the term "between" includes any of the referenced endpoints. For example, "between 2 and 10" includes both 2 and 10.

Claims

1. A reactor, comprising a shell defining an internal space configured to receive a catalyst, at least one inlet nozzle, and a tube bundle comprising a plurality of tubes arranged in a concentric band shape centered on the longitudinal axis of the reactor and comprising: The reactor further comprises at least one tube support plate, the at least one tube support plate comprises at least one annular band, and the at least one annular band comprises at least one bracket configured to extend around a portion of the tubes of the tube bundle. A reactor.

2. at least one catalyst support plate, at least one tube support plate, a gas introduction plate, an upper plate, or an upper plate and a tube support plate The reactor according to claim 1, further comprising.

3. The catalyst is a solid catalyst, and the solid catalyst comprises catalyst balls of a first diameter. The reactor according to claim 1.

4. The solid catalyst further comprises catalyst balls of a second diameter. The reactor according to claim 3.

5. The reactor further comprises a catalyst support plate, and the catalyst balls of the first diameter and the catalyst balls of the second diameter are arranged in respective individual layers near the catalyst support plate. The reactor according to claim 4.

6. The shell is configured to receive at least one solid catalyst, and the solid catalyst has a shape defining at least one of pellets, rings, tablets, and spheres. The reactor according to claim 1.

7. The reactor further comprises a catalyst support plate, and the catalyst support plate is configured to support a solid catalyst having a predetermined height, the reactor according to claim 1.

8. The reactor further comprises a catalyst support plate, and the catalyst support plate defines one or more openings, the reactor according to claim 1.

9. The one or more openings include a plurality of openings of a first size and a plurality of openings of a second size, and the plurality of openings extend through at least a part of the thickness of the catalyst support plate, the reactor according to claim 8.

10. The first size corresponds to the circumference of at least one tube of the tube bundle, and the second size is smaller than the first size, the reactor according to claim 9.

11. The plurality of openings of the first size are defined through the catalyst support plate according to the arrangement of the plurality of tubes of the tube bundle, the reactor according to claim 10.

12. The reactor further comprises a gas introduction plate, and the gas introduction plate includes a plurality of openings defined through the thickness of the gas introduction plate, and the plurality of openings are a plurality of circular openings defined through the gas introduction plate according to the arrangement of the plurality of tubes of the tube bundle, the reactor according to claim 1.

13. The gas introduction plate includes a second plurality of openings defined through the thickness of the gas introduction plate, and the second plurality of openings have a size and / or shape different from that of the plurality of circular openings, the reactor according to claim 12.

14. The at least one tube support plate defines a plurality of concentric annular bands, the reactor according to claim 1.

15. The reactor according to claim 14, wherein the at least one tube support plate defines at least one radial support member connected to at least one of the plurality of annular bands. **Claim 16** The innermost annular band of the at least one tube support plate comprises a predetermined number of brackets each configured to correspond to a concentric circumferential ring of the same predetermined number of the innermost tubes of the tube bundle, and the second annular band of the at least one tube support plate comprises an equal or greater number of brackets compared to the innermost annular band, and the brackets of the second annular band are each configured to correspond to a corresponding number of tubes within a second concentric circumferential ring of the tube bundle. The reactor according to claim 14. **Claim 17** The reactor according to claim 16, wherein one of the plurality of annular bands of the at least one tube support plate comprises brackets corresponding to at least one thermocouple insertion tube, the at least one thermocouple insertion tube being configured to receive a temperature measuring device, and the temperature measuring device being configured to obtain temperatures at a plurality of longitudinal positions within the reactor. **Claim 18** A methanol synthesis reactor, a shell defining an internal space configured to receive a solid catalyst; a tube bundle comprising a plurality of tubes, the plurality of tubes being arranged in concentric circumferential bands about the longitudinal axis of the reactor; at least one inlet nozzle; an outlet nozzle located near the bottom of the shell; a catalyst support plate with the outlet nozzle disposed below the catalyst support plate; A plurality of tube support plates, each of the plurality of tube support plates comprising a plurality of annular bands, each of the plurality of annular bands comprising at least one bracket configured to extend around a tube of the tube bundle, a tube support plate; A gas introduction plate; comprising; Each of the plurality of tube support plates defines a plurality of radial supports, each of the plurality of radial supports being connected between the plurality of annular bands of the tube support plate; Each of the plurality of radial supports is removably fixed to at least one of the plurality of annular bands of each of the plurality of tube support plates; The gas introduction plate is disposed near the inlet nozzle, and the inlet nozzle is disposed below the gas introduction plate, a methanol synthesis reactor.

19. The tube bundle has a reduced thickness and / or an increased diameter near the bottom of the reactor so as to facilitate a greater degree of heat transfer near the bottom of the reactor relative to the upper part of the reactor, the reactor according to claim 18.

20. A reactor, A shell defining an internal space configured to receive a catalyst; At least one inlet nozzle located near the bottom of the shell; A tube bundle comprising a plurality of tubes arranged in concentric bands centered on the longitudinal axis of the reactor; comprising; The plurality of tubes of the tube bundle receive reactants from at least one of the inlet nozzles, the reactants exiting the plurality of tubes at the open upper ends of the plurality of tubes near the upper end of the reactor, the reactants flowing downward through the reactor for reaction; The reactor further comprises a gas introduction plate; The gas introduction plate includes a plurality of openings defined through the thickness of the gas introduction plate, and the plurality of openings are a plurality of circular openings defined through the gas introduction plate according to the arrangement of the plurality of tubes of the tube bundle. The gas introduction plate includes a plurality of second openings defined through the thickness of the gas introduction plate, and the plurality of second openings have sizes and / or shapes different from those of the plurality of circular openings. The plurality of second openings are within the internal space defined by the shell, and the plurality of second openings function to allow the flow of reactants, reaction products, and reaction by-products.

21. The reactor according to claim 20, further comprising at least one tube support plate above the gas introduction plate.

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