Multi-stage reactor system and method for conversion of oxygenates

Abstract

An exemplary process for converting one or more oxygenates to one or more olefins is disclosed. In one exemplary aspect, the method may include introducing a first input feed into an adiabatic multi-stage reactor having a first reactor bed and a second reactor bed. The method may further include contacting the first input feed with a first reactor bed to maintain a first temperature of the first reactor bed within a first temperature range and produce a first reaction mixture, and introducing a second input feed into a multi-stage reactor, the first reaction mixture is mixed with the second input feed to produce a first effluent. The method may also include contacting the first effluent with a second reactor bed, thereby maintaining a second temperature of the second reactor bed within a second temperature range and producing a second reaction mixture. The invention also discloses an exemplary system.

Description

Cross-references to related applications

[0001] This application claims priority to U.S. Provisional Application No. 63 / 488,867, filed March 7, 2023, the entire contents of which are expressly incorporated herein by reference. Technical Field

[0002] The present invention provides a multi-stage reactor system and method for the conversion of oxygenates (e.g., alcohols or ethers), and more specifically, an adiabatic method for converting oxygenates into olefins. Background Technology

[0003] The present invention provides a multi-stage reactor system and method for the conversion of oxygen-containing compounds (e.g., alcohols or ethers), and more specifically, an adiabatic method for converting oxygen-containing compounds into olefins.

[0004] Fixed-bed adiabatic reactors are among the cheapest reactors available, but they present a challenge for processes that release or absorb large amounts of heat. Endothermic reactions can lower process temperatures depending on the extent of the reaction and may quench the process without adding heat. Exothermic reactions can raise process temperatures depending on the extent of the reaction and may cause the reaction to lose selectivity or proceed uncontrollably without removing heat. In such processes, adding or removing heat requires expensive heat exchange equipment, ultimately increasing net heat demand, increasing system pressure drop, and increasing the difficulty of controlling the process. In processes with high heat exchange requirements, the fixed bed is often segmented and heated or cooled, or a more expensive multi-tube fixed-bed reactor is used, where the reactor itself acts as a heat exchanger. However, such systems can be inefficient, and their applicability can be severely limited (e.g., steam methane reforming or partial oxidation of propylene to acrylic acid) and they are generally not suitable for systems with a combination of exothermic and endothermic steps.

[0005] Therefore, there is still a need for improved, efficient, cost-effective, and more versatile systems and methods that can combine endothermic and exothermic reactions. Attached Figure Description

[0006] The accompanying drawings, which are incorporated in and form part of this application, illustrate certain aspects of the subject matter disclosed herein. These drawings, together with the description, help to explain some principles related to the disclosed embodiments. In the drawings: Figure 1 This is a schematic diagram of an exemplary system for the conversion of oxygen-containing compounds, wherein the first input feed contains at least ethanol; and Figure 2 This is a schematic diagram of another exemplary system for the conversion of oxygen-containing compounds, wherein the first input feed contains at least methanol and ethanol.

[0007] In practical applications, similar reference numerals indicate similar structures, features, or elements. Summary of the Invention

[0008] In certain aspects of the subject matter of this invention, challenges associated with the conversion of oxygen-containing compounds can be addressed by employing one or more of the features described herein or equivalent methods that can be understood by those skilled in the art. Various aspects of the subject matter of this invention relate to methods and systems for converting one or more oxygen-containing compounds into one or more olefins.

[0009] In some respects, one or more of the following features may be optionally included in any feasible combination.

[0010] This invention discloses an exemplary method for converting one or more oxygen-containing compounds into one or more olefins. In one exemplary aspect, the method includes introducing a first input feed into a first end of an adiabatic multistage reactor, the first input feed comprising one or more first oxygen-containing compounds and one or more first olefins, the multistage reactor having at least a first reaction stage and a second reaction stage. The first reaction stage is upstream of the second reaction stage and has a first reactor bed, and the second reaction stage has a second reactor bed. The method further includes contacting the first input feed with the first reactor bed to maintain a first temperature of the first reactor bed within a first temperature range of about 300°C to 550°C and produce a first reaction mixture; introducing a second input feed downstream of the first reaction stage of the multistage reactor such that, upon exiting the first reaction stage, the first reaction mixture mixes with the second input feed to produce a first effluent with a different composition relative to the first reaction mixture, the second input feed comprising one or more second oxygen-containing compounds. The method further includes contacting the first effluent with the second reactor bed to maintain a second temperature of the second reactor bed within a second temperature range of about 300°C to 550°C and produce a second reaction mixture.

[0011] In some aspects, the multistage reactor may have a third reaction stage with a third reactor bed. In this case, the method may further include introducing a third input feed downstream of the second reaction stage of the multistage reactor, such that upon exiting the second reaction stage, the second reaction mixture can be mixed with the third input feed to produce a second effluent with a different composition relative to the second reaction mixture, the third input feed comprising one or more third oxygen-containing compounds. The method further includes contacting the second effluent with the third reactor bed to maintain a third temperature of the third reactor bed within a third temperature range of about 300°C to 550°C and to produce the third reaction mixture.

[0012] In some aspects, no external heat is added to the multistage reactor during or between each reaction stage. In some aspects, no heat is removed from the multistage reactor during or between each reaction stage. In some aspects, the first effluent is not removed from the multistage reactor. In some aspects, the second effluent is not removed from the multistage reactor. In some aspects, heat is not removed from the first reaction mixture before mixing with the second input feed. In some aspects, heat is not removed from the second reaction mixture before being removed from the multistage reactor or subsequently mixed with the third input feed. In some aspects, heat is not removed from the third reaction mixture before being removed from the multistage reactor or subsequently mixed with the fourth input feed.

[0013] In some aspects, the one or more first oxygen-containing compounds include a predominant first oxygen-containing compound, and the one or more first olefins include a predominant first olefin, wherein the predominant first oxygen-containing compound may be ethanol and the predominant first olefin may be ethylene. In some aspects, the molar ratio of ethylene to ethanol in the first feed may be from about 0.25 to 10. In some aspects, the molar ratio of ethylene to ethanol in the first feed may be from about 0.25 to 5. In some aspects, the first temperature range may be from about 350°C to 500°C. In some aspects, the second temperature range may be from about 350°C to 500°C. In some aspects, the third temperature range may be from about 350°C to 500°C.

[0014] In some aspects, at least one of the first or second reactor beds may be a fixed bed. In some aspects, the third reactor bed may be a fixed bed. In some aspects, at least one of the first or second reactor beds may be a fluidized bed. In some aspects, the third reactor bed may be a fluidized bed. In some aspects, at least one of the first or second reactor beds may be a moving bed. In some aspects, the third reactor bed may be a moving bed.

[0015] In some aspects, the one or more first oxygen-containing compounds and the one or more second oxygen-containing compounds may be the same. In some aspects, the one or more first oxygen-containing compounds, the one or more second oxygen-containing compounds, and the one or more third oxygen-containing compounds may be the same. In some aspects, the one or more first oxygen-containing compounds comprise one or more C2+ alcohols. In some aspects, the one or more second oxygen-containing compounds comprise one or more C2+ alcohols. In some aspects, the one or more third oxygen-containing compounds comprise one or more C2+ alcohols.

[0016] In some aspects, the one or more first oxygen-containing compounds include a predominant first oxygen-containing compound, wherein the predominant oxygen-containing compound may be ethanol. In some aspects, the one or more second oxygen-containing compounds include a second predominant oxygen-containing compound, wherein the predominant oxygen-containing compound may be ethanol. In some aspects, the one or more third oxygen-containing compounds include a predominant third oxygen-containing compound, wherein the predominant oxygen-containing compound may be ethanol.

[0017] In some aspects, the method may further include introducing a second reaction mixture into a single-stage reactor containing one or more catalysts, and contacting the second reaction mixture with the one or more catalysts to produce an output stream containing one or more product olefins. Prior to introducing the second reaction mixture into the single-stage reactor, the method may further include lowering the temperature of the second reaction mixture.

[0018] In some aspects, the method may also include introducing the output stream into the separation subsystem to generate a first stream and a second stream.

[0019] In some aspects, the second stream may contain at least one C3+ olefin. In some aspects, the method may further include combining the first stream with one or more first oxygen-containing compounds to produce a first input feed. In some aspects, the first stream may contain a primary olefin, wherein the primary olefin may be ethylene.

[0020] In some aspects, the method may further include condensing the output stream into a condensed output stream and introducing the condensed output stream into a separation subsystem to produce a first stream and a second stream. In some aspects, the method may further include combining the first stream with one or more first oxygen-containing compounds to produce a first input feed. In some aspects, the first stream may contain a primary olefin, wherein the primary olefin may be ethylene. In some aspects, the second stream may contain at least one C3+ olefin.

[0021] In some aspects, the method may further include introducing a third reaction mixture into a single-stage reactor containing one or more catalysts, and contacting the third reaction mixture with the one or more catalysts to produce an output stream containing one or more product olefins.

[0022] In some aspects, the method may further include lowering the temperature of the third reaction mixture before introducing it into the single-stage reactor. In some aspects, the method may further include introducing an output stream into a separation system to produce a first stream and a second stream. In some aspects, the method may further include combining the first stream with one or more first oxygen-containing compounds to produce a first input feed. In some aspects, the first stream may contain a major olefin, wherein the major olefin may be ethylene. In some aspects, the second stream may contain at least one C3+ olefin.

[0023] In some aspects, the method may further include condensing the output stream into a condensate output stream and introducing the condensate reaction mixture into a separation subsystem to produce a first stream and a second stream. In some aspects, the method may further include combining the first stream with one or more first oxygen-containing compounds to produce a first input feed. In some aspects, the first stream may contain a primary olefin, wherein the primary olefin may be ethylene. In some aspects, the second stream may contain at least one C3+ olefin.

[0024] In some aspects, the method may further include superheating the one or more first oxygen-containing compounds before introducing the first input stream into the adiabatic multistage reactor. In some aspects, the method may further include superheating the one or more second oxygen-containing compounds before introducing the second input stream into the adiabatic multistage reactor. In some aspects, the method may further include superheating the one or more third oxygen-containing compounds before introducing the third input stream into the adiabatic multistage reactor.

[0025] In some aspects, the gauge pressure of the multistage reactor can be from 0 to about 30 bar. In some aspects, the weight hourly space velocity (WHSV) of the multistage reactor can be from about 0.25 to 15.

[0026] In some aspects, at least one of the first or second reactor beds may contain a catalyst mixture. In some aspects, the catalyst mixture may contain zeolite and an alcohol dehydration catalyst. In some aspects, a third reactor bed may contain a catalyst mixture. In some aspects, the catalyst mixture of the third reactor bed may contain zeolite and an alcohol dehydration catalyst.

[0027] In some aspects, the second input feed can be introduced into the adiabatic multistage reactor at a temperature higher than the temperature of the first reaction mixture. In some aspects, the third input feed can be introduced into the adiabatic multistage reactor at a temperature higher than the temperature of the second reaction mixture.

[0028] In some aspects, a multistage reactor may include one or more additional reaction stages downstream of a third reaction stage, each of which has a corresponding reactor bed. In this case, the method may further include introducing a subsequent feed downstream of a previous reaction stage of the multistage reactor, such that upon exiting the previous reaction stage, the previous reaction mixture can be mixed with the subsequent feed to produce an additional effluent having a composition different from the previous reaction mixture, the subsequent feed containing one or more additional oxygen-containing compounds. The method may further include contacting the previous effluent with a corresponding reactor bed of one of the one or more additional reaction stages, thereby maintaining the temperature of the corresponding reactor bed in a temperature range of about 300°C to 550°C and producing an additional reaction mixture downstream of the previous reaction stage.

[0029] In some aspects, the one or more first oxygen-containing compounds may include ethanol and methanol. In some aspects, the one or more first olefins may include ethylene, propylene, butene, or any combination thereof.

[0030] In some aspects, the one or more first oxygen-containing compounds are methanol-free. In some aspects, the one or more second oxygen-containing compounds are methanol-free. In some aspects, the one or more third oxygen-containing compounds are methanol-free.

[0031] In another aspect, the present invention provides another method for converting one or more oxygen-containing compounds into one or more olefins. In some aspects, the method includes introducing a first input feed into a first end of an adiabatic multistage reactor, the first input feed comprising one or more first oxygen-containing compounds, said one or more first oxygen-containing compounds including ethanol and at least one of methanol or dimethyl ether, said multistage reactor having at least a first reaction stage and a second reaction stage, wherein the first reaction stage is upstream of the second reaction stage and the first reaction stage has a first reactor bed and the second reaction stage has a second reactor bed. The method further includes contacting the first input feed with the first reactor bed to maintain a first temperature of the first reactor bed within a first temperature range of about 300°C to 550°C and produce a first reaction mixture, and introducing a second input feed downstream of the first reaction stage of the multistage reactor such that, upon exiting the first reaction stage, the first reaction mixture mixes with the second input feed to produce a first effluent with a different composition relative to the first reaction mixture, the second input feed comprising one or more second oxygen-containing compounds. The method further includes contacting the first effluent with the second reactor bed to maintain a second temperature of the second reactor bed within a second temperature range of about 300°C to 550°C and produce a second reaction mixture.

[0032] In some aspects, the multistage reactor may have a third reaction stage having a third reactor bed, and the method may further include: introducing a third input feed downstream of the second reaction stage of the multistage reactor such that, upon exiting the second reaction stage, the second reaction mixture can be mixed with the third input feed to produce a second effluent with a different composition relative to the second reaction mixture, the third input feed comprising one or more third oxygen-containing compounds. The method may further include: contacting the second effluent with the third reactor bed to maintain a third temperature of the third reactor bed within a third temperature range of about 300°C to 550°C and to produce a third reaction mixture. In some aspects, the one or more first oxygen-containing compounds may include ethanol and methanol. In some aspects, the one or more first oxygen-containing compounds may include ethanol or dimethyl ether. In these aspects, the one or more first oxygen-containing compounds may also include methanol.

[0033] In some aspects, the one or more second oxygen-containing compounds may include ethanol, methanol, or a combination thereof. In some aspects, the one or more second oxygen-containing compounds do not contain methanol.

[0034] In some aspects, the one or more third oxygen-containing compounds may include ethanol, methanol, or a combination thereof. In some aspects, the one or more third oxygen-containing compounds do not contain methanol.

[0035] On the other hand, the present invention provides a system that uses the above-described method to convert one or more oxygen-containing compounds into one or more olefins. In some aspects, the system may include the above-described adiabatic multistage reactor.

[0036] In another aspect, a method for converting one or more oxygen-containing compounds into one or more compounds may include: introducing a first input feed into a first end of an adiabatic multistage reactor assembly, the first input feed comprising one or more first oxygen-containing compounds and at least one or more first olefins and methanol, wherein the multistage reactor assembly has at least a first reaction stage and a second reaction stage, and the first reaction stage is upstream of the second reaction stage. The first reaction stage has a first reactor bed, and the second reaction stage has a second reactor bed. The method further includes: contacting the first input feed with the first reactor bed to maintain a first temperature of the first reactor bed within a first temperature range of about 300°C to 550°C and produce a first reaction mixture; and introducing a second input feed downstream of the first reaction stage of the multistage reactor assembly such that, upon exiting the first reaction stage, the first reaction mixture mixes with the second input feed to produce a first effluent with a different composition relative to the first reaction mixture. The second input feed comprises one or more second oxygen-containing compounds. The method further includes contacting the first effluent with the second reactor bed to maintain a second temperature of the second reactor bed within a second temperature range of about 300°C to 550°C and produce a second reaction mixture.

[0037] In some aspects, the multistage reactor assembly may have a third reaction stage, wherein the third reaction stage has a third reactor bed. In these aspects, the method may include introducing a third input feed downstream of the second reaction stage of the multistage reactor assembly, such that the reaction mixture exiting the second reaction stage can be mixed with the third input feed to produce a second effluent that may have a different composition relative to the second reaction mixture. The third input feed may contain one or more third oxygen-containing compounds. The method may further include contacting the second effluent with the third reactor bed to maintain a third temperature of the third reactor bed within a third temperature range of about 300°C to 550°C and to produce a third reaction mixture.

[0038] In some respects, a multistage reactor assembly may include two or more reactors, wherein the first and second stages may be carried out in the first reactor and the third stage may be carried out in the second reactor.

[0039] In some aspects, a multistage reactor assembly may include two or more reactors, wherein a first reactor bed may be located in a first reactor, a second reactor bed may be located in a second reactor, and in other aspects, a third reactor bed may be located in a third reactor.

[0040] In some respects, the first input feed may include one or more first oxygen-containing compounds, one or more first olefins, and methanol.

[0041] In some respects, the first input feed may include one or more first oxygen-containing compounds as well as methanol.

[0042] In some respects, the first input feed may include one or more first oxygen-containing compounds and one or more first olefins.

[0043] In some respects, the one or more second oxygen-containing compounds do not contain methanol.

[0044] In some respects, the one or more third oxygen-containing compounds do not contain methanol.

[0045] In some aspects, the one or more first olefins may include one or more recycled olefins, wherein the one or more recycled olefins may include ethylene, propylene, butene, pentene, or any combination thereof. Detailed Implementation

[0046] Certain exemplary aspects will now be described to provide a comprehensive understanding of the principles governing the structure, function, manufacture, and use of the systems and methods disclosed herein. One or more examples of these aspects are illustrated in the accompanying drawings. It will be understood by those skilled in the art that the systems and methods specifically described herein and illustrated in the accompanying drawings are non-limiting exemplary embodiments and that the scope of the invention is not limited solely by the claims. Features shown or described in conjunction with one exemplary aspect may be combined with features of other aspects. Such modifications and variations are intended to be covered within the scope of the invention.

[0047] Dehydrating alcohols to olefins (e.g., ethanol to ethylene) is particularly difficult to achieve in a cost-effective manner. This is a significant problem, for example, because producing ethylene from ethanol is the first step in the production of most bulk renewable chemicals (such as bio-based polyethylene or bio-based ethylene glycol) and the first step in many industrial methods for producing renewable hydrocarbon fuels (especially sustainable aviation fuel (SAF)) from ethanol. Because the dehydration reaction is highly endothermic, multiple reaction stages, very high recycling levels, or low feed concentrations are typically required to achieve high conversion rates. All conventional methods result in both very high equipment costs and energy consumption.

[0048] In the systems and methods of the present invention described herein, one or more oxygen-containing compounds (e.g., C1+ alcohols, dimethyl ethers, or mixtures thereof) and optionally present olefin co-feeds are converted into an olefin mixture. The conversion method involves a combination of two processes: endothermic dehydration of the alcohol or ether to olefins, followed by net exothermic oligomerization and cracking of the resulting low-carbon-number olefins to high-carbon-number olefins. To maximize the thermal integration potential between these reactions and minimize equipment costs and overall process heat requirements, the systems and methods are designed to balance the heat released or absorbed throughout the process by controlling the relative rates of the two reactions through the phased addition of the one or more oxygen-containing compounds during the entire process.

[0049] In this disclosure, an adiabatic multistage reactor is designed to balance the endothermic dehydration of oxygenated compounds and the exothermic oligomerization of olefins. This is achieved by diverting the oxygenated compound feed to multiple stages of the adiabatic reactor in such a manner that the endothermic dehydration reaction of the oxygenated compound offsets the heat generated by the exothermic oligomerization process, maintaining the internal reactor temperature within the limits required for the reactor bed. Therefore, compared to conventional conversion methods involving only a single-agent oxygenated compound feed, the conversion process in this adiabatic multistage reactor proceeds under a more uniform temperature distribution. Furthermore, this heat offsetting avoids the need for material removal between reactor stages during operation, the large-scale recycling of unconverted or partially converted oxygenated compounds, or the over-diluting of the oxygenated compound feed, which would be necessary if the oxygenated compound feed were provided as a single agent. It should be noted that the reactor contents can be cooled or heated by supplying a second feed at a temperature lower or higher than the reactor contents at that stage, without removing or adding heat.

[0050] Generally, the systems disclosed herein for converting one or more oxygen-containing compounds into one or more olefins include an adiabatic multistage reactor having multiple inputs (e.g., at least first and second input feeds), at least a first reaction stage and a second reaction stage, wherein the first reaction stage is upstream of the second reaction stage. The first reaction stage includes a first reactor bed, and the second reaction stage includes a second reactor bed. In use, the first input feed can be fed into a first end (e.g., an inlet) of the adiabatic multistage reactor and then contacted with the first reactor bed to produce a first reaction mixture. A second input feed can be introduced into the adiabatic multistage reactor downstream of the first reaction stage and then mixed with the first reaction mixture to produce a first effluent with a different composition relative to the first reaction mixture. The first effluent can then be contacted with the second reactor bed to produce a second reaction mixture. This second reaction mixture can then be fed into a subsequent reaction stage of the reactor (e.g., a third reaction stage) through the reactor output, or in other cases.

[0051] In some respects, no external heat is added to the adiabatic multistage reactor during or between each reaction stage. The phrase "external heat" refers to heat supplied to the adiabatic multistage reactor that is not generated by the chemical reactions within the reactor or by any input feed (e.g., the first, second, or third input feed). Alternatively or additionally, no heat is removed from the adiabatic multistage reactor during or between each reaction stage.

[0052] In some aspects, the first effluent is not removed from the adiabatic multistage reactor. The components of the first effluent may include water, oxygenated compounds, and co-products. Alternatively or additionally, in some aspects, the second effluent is not removed from the adiabatic multistage reactor. The components of the second effluent may include water, oxygenated compounds, olefins, and co-products (e.g., alkanes and aromatic compounds).

[0053] In some respects, heat is not removed from the first reaction mixture before mixing with the second input feed. Alternatively or additionally, in some respects, heat is not removed from the second reaction mixture before being removed from the multistage reactor or then mixed with the third input feed.

[0054] The first input feed comprises one or more first oxygen-containing compounds. For the purposes of this disclosure, "oxygen-containing compound" is a hydrocarbon containing oxygen as part of its chemical structure. Non-limiting examples of first oxygen-containing compounds include methanol, ethanol, butanol, pentanol, one or more esters, and / or one or more ethers. In some aspects, the one or more first oxygen-containing compounds do not contain methanol. In some aspects, the one or more first oxygen-containing compounds may comprise the same oxygen-containing compound; in other aspects, the one or more first oxygen-containing compounds may comprise a mixture of different oxygen-containing compounds. For example, in some aspects, the one or more first oxygen-containing compounds may comprise a dominant first oxygen-containing compound, such as ethanol. In these aspects, the one or more first oxygen-containing compounds may also comprise one or more other oxygen-containing compounds, such as methanol, propanol, one or more esters, and / or one or more ethers. The weight percentage of the "dominant first oxygen-containing compound" as used herein may be higher than the weight percentage of any other single oxygen-containing compound in the one or more first oxygen-containing compounds, for example, it may be present in an amount of at least 25% by weight, at least 50% by weight, or at least 75% by weight of the one or more first oxygen-containing compounds. In some aspects, the dominant first oxygen-containing compound may be present in amounts of 25% to 99% by weight, 25% to 90% by weight, 50% to 99% by weight, or 75% to 99% by weight of the one or more first oxygen-containing compounds. Further consideration is that the amount of the dominant first oxygen-containing compound may be between any of these stated ranges.

[0055] In some aspects, the one or more first oxygen-containing compounds may include ethanol and methanol. Alternatively or additionally, the one or more first oxygen-containing compounds may include dimethyl ether. Furthermore, the molar ratio of methanol to ethanol in the first input feed may be about 0.5 to 6, or the molar ratio may be about 1 to 5, or the molar ratio may be about 2 to 5, or the molar ratio may be about 3 to 6, or the molar ratio may be about 3 to 5.

[0056] The one or more first oxygen-containing compounds can be introduced into an adiabatic multistage reactor at various temperatures. For example, in some aspects, the temperature of the one or more first oxygen-containing compounds can be about 300°C to 550°C or about 400°C to 500°C. In one aspect, the temperature of the one or more first oxygen-containing compounds can be about 300°C to 480°C. In another aspect, the temperature of the one or more first oxygen-containing compounds can be about 480°C to 550°C or about 450°C to 500°C. It is also considered that the temperature of the one or more first oxygen-containing compounds does not exceed any of these stated ranges. Further consideration is that the temperature of the one or more first oxygen-containing compounds can be between any of these stated ranges.

[0057] The first input feed may also contain other materials, such as one or more first olefins. Non-limiting examples of first olefins include ethylene, propylene, butene, etc. In some aspects, the one or more first olefins may comprise the same olefin; in other aspects, the one or more first olefins may comprise a mixture of different olefins. For example, in some aspects, the one or more first olefins may comprise a predominant first olefin, such as ethylene. The weight percentage of "predominant first olefin" as used herein may be higher than the weight percentage of any other single olefin in the one or more first olefins, for example, it may be present in an amount of at least 25 wt%, at least 50 wt%, or at least 75 wt% of the one or more first olefins. In some aspects, the content of the predominant first olefin may be present in an amount of 25 wt% to 99 wt%, 25 wt% to 90 wt%, 50 wt% to 99 wt%, or 75 wt% to 99 wt% of the one or more first olefins. Further consideration is that the content of the predominant first olefin may be between any of these stated ranges. In some aspects, the first input feed may contain ethanol and ethylene. For example, the molar ratio of ethylene to ethanol in the first input feed can be from about 0.25 to 10, or the molar ratio of ethylene to ethanol in the first input feed can be from about 0.25 to 5.

[0058] In some aspects, at least one of the one or more first olefins is provided via olefin recycling within an adiabatic multistage system. Such olefins are referred to herein as "recycled olefins". Non-limiting examples of suitable recycled olefins include ethylene, propylene, butene, pentene, or any combination thereof. For example, in some aspects, at least one of the one or more first olefins may comprise ethylene alone or in combination with other olefins (e.g., one or more C3+ olefins) by recycling ethylene produced within an adiabatic multistage reactor and combining it with the one or more first oxygen-containing compounds (e.g., ethanol) to form a first input feed. In some aspects, at least one of the one or more first olefins may comprise a recycled C2-C4 olefin mixture, while in other aspects, at least one of the one or more first olefins may comprise C2-C5 olefins.

[0059] The first input feed can be introduced into the adiabatic multistage reactor at a variety of temperatures. For example, in some aspects, the temperature of the first input feed can be about 300°C to 550°C, or about 400°C to 500°C. It is also considered that the temperature of the first input feed does not exceed any of these stated ranges. Further consideration is that the temperature of the first input feed can be between any of these stated ranges.

[0060] In use, the components of the first input feed are designed to maintain a first temperature in the first reactor bed within a first temperature range. In some aspects, the first temperature range can be about 300°C to 550°C. In some aspects, the first temperature range can be about 300°C to 500°C, about 350°C to 500°C, about 300°C to 400°C, about 350°C to 450°C, about 400°C to 460°C, about 400°C to 480°C, or about 370°C to 480°C. It is also considered that the first temperature does not exceed any of these stated ranges. Further consideration is that the first temperature can be between any of these stated ranges.

[0061] In addition to the composition of the first input feed, the temperature of the first reactor bed can also depend at least on the composition of the first reactor bed. The first reactor bed may contain one or more first catalysts. Therefore, in some aspects, the first reactor bed may contain a single catalyst, while in others, it may contain a mixture of two or more catalysts. It should be noted that the design of the first reactor bed should avoid over-conversion of the one or more first oxygen-containing compounds and the one or more olefins (e.g., low-carbon olefins) present in the first input feed, which could lead to either undercooling or overheating of the first reaction stage, respectively. Therefore, the composition of the first reactor bed can be designed based on the desired rate and composition of the one or more first olefins relative to the total flow rate of the one or more first oxygen-containing compounds.

[0062] In some aspects, the one or more first catalysts comprise doped or undoped zeolite catalysts. Non-limiting examples of suitable zeolite catalysts include pentasilicone ring types, such as ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or dealuminated crystalline silicates of the group ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or phosphorus and / or boron modified crystalline silicates of the group ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or molecular sieves of the AEL group of silica-aluminophosphate types. Non-limiting examples of suitable dopants for zeolite catalysts include phosphorus and / or boron. In some aspects, the zeolite catalyst can be boron- and phosphorus-doped zeolite. Additional additives for mixing with the doped zeolite include a SiO2 support doped with a metal dopant, which may include sodium (Na), potassium (K), lithium (Li), beryllium (Be), magnesium (Mg), calcium (Ca), strontium (Sr), barium, radium, iron (Fe), cobalt (Co), nickel (Ni), lanthanum (La), chromium (Cr), zirconium (Zr), ruthenium (Ru), molybdenum (Mo), iridium (Ir), tungsten (W), copper (Cu), manganese (Mn), vanadium (V), zinc (Zn), titanium (Ti), rhodium (Rh), rhenium (Re), gallium (Ga), palladium (Pd), silver (Ag), indium (In), or any combination thereof.

[0063] In other respects, the one or more first catalysts may also include catalysts specifically for alcohol or ether dehydration, such as solid acids, doped or undoped alumina, such as zirconated alumina, γ-alumina, high-purity γ-alumina or doped γ-alumina, or doped or undoped zeolites with limited olefin oligomerization activity (e.g., such zeolites, under application conditions, would dehydrate alcohols to their corresponding olefins with a selectivity of at least 80 mol%), such as H-MFI type zeolites with a high Si / Al2 ratio (e.g. >190) or dealuminated, and under certain conditions (Si / Al2 ratio), H-FER, H-BEA or HY type zeolites may also be considered monofunctional dehydration catalysts.

[0064] An exemplary catalyst combination physically mixed within a first reactor bed may include a portion (e.g., the first catalyst in one or more first catalysts) of doped zeolite, such as crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or dealuminated crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or phosphorus and / or boron modified crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or molecular sieves of the aluminosilicate type of AEL group. The additional additives used for mixing with the doped zeolite consist of a SiO2 support doped with a metal dopant, including iron (Fe), strontium (Sr), cobalt (Co), nickel (Ni), lanthanum (La), chromium (Cr), zirconium (Zr), ruthenium (Ru), molybdenum (Mo), iridium (Ir), magnesium (Mg), tungsten (W), copper (Cu), manganese (Mn), vanadium (V), zinc (Zn), titanium (Ti), rhodium (Rh), rhenium (Re), gallium (Ga), palladium (Pd), silver (Ag), indium (In), or any combination thereof. A second portion of the catalyst mixture (e.g., a second catalyst in one or more of the first catalysts) may comprise a catalyst specifically for the dehydration of alcohols or ethers as described above.

[0065] The first reactor bed can have various structural configurations. For example, in some aspects, the first reactor bed is a fixed reactor bed. In some aspects, the fixed bed reactor is an axial flow fixed bed reactor. In some aspects, the fixed bed reactor is a radial flow fixed bed reactor. In other aspects, the first reactor bed is a fluidized bed. In other aspects, the first reactor bed is a moving bed.

[0066] The second input feed comprises one or more second oxygen-containing compounds, so named because they are second oxygen-containing compounds introduced into the reactor at the second stage or reactor bed. Non-limiting examples of second oxygen-containing compounds include methanol, ethanol, butanol, pentanol, one or more esters, and / or one or more ethers. In some aspects, the one or more second oxygen-containing compounds do not contain methanol. In some aspects, the one or more second oxygen-containing compounds may comprise the same oxygen-containing compound, while in other aspects, the one or more second oxygen-containing compounds may comprise a mixture of different oxygen-containing compounds. For example, in some aspects, the one or more second oxygen-containing compounds may comprise a dominant second oxygen-containing compound, such as ethanol. The weight percentage of the “dominant second oxygen-containing compound” as used herein may be higher than any other single oxygen-containing compound among the one or more second oxygen-containing compounds, for example, it may be present in an amount of at least 25% by weight, at least 50% by weight, or at least 75% by weight of the one or more second oxygen-containing compounds. In some aspects, the dominant second oxygen-containing compound may be present in amounts of 25% to 99% by weight, 25% to 90% by weight, 50% to 99% by weight, or 75% to 99% by weight of the one or more second oxygen-containing compounds. Further consideration is that the amount of the dominant second oxygen-containing compound may be between any of these stated ranges.

[0067] Typically, the one or more second oxygen-containing compounds are identical to the one or more first oxygen-containing compounds, such that the overall conversion process within the adiabatic multistage reactor involves two or more injections of oxygen-containing compounds, more specifically, separate injections of oxygen-containing compounds at different reaction stages. This allows the system to control the temperature of the reactor bed, thereby maximizing the thermal integration of the adiabatic multistage reactor. In some aspects, the primary second oxygen-containing compound of the one or more second oxygen-containing compounds may include ethanol. In these aspects, the one or more second oxygen-containing compounds may also include one or more other oxygen-containing compounds, such as methanol, propanol, butanol, pentanol, one or more esters and / or one or more ethers.

[0068] The one or more second oxygen-containing compounds can be introduced into an adiabatic multistage reactor at various temperatures. For example, in some aspects, the temperature of the one or more second oxygen-containing compounds can be about 300°C to 550°C or about 400°C to 500°C. In one aspect, the temperature of the one or more second oxygen-containing compounds can be about 300°C to 480°C. In another aspect, the temperature of the one or more second oxygen-containing compounds can be about 480°C to 550°C or about 450°C to 500°C. It is also considered that the temperature of the one or more second oxygen-containing compounds does not exceed any of these stated ranges. Further consideration is that the temperature of the one or more second oxygen-containing compounds can be between any of these stated ranges.

[0069] The second input feed can be introduced into the adiabatic multistage reactor at a variety of temperatures. For example, in some aspects, the temperature of the second input feed can be about 200°C to 550°C, about 200°C to 500°C, about 300°C to 500°C, about 360°C to 400°C, about 400°C to 500°C, or about 450°C to 550°C. It is also considered that the temperature of the one or more second input feeds does not exceed any of these stated ranges. Further consideration is that the temperature of the second input feed can be between any of these stated ranges. In some aspects, the second input feed can be introduced into the adiabatic multistage reactor at a temperature higher than the temperature of the first reaction mixture.

[0070] In use, the components of the second input feed are designed to maintain the second temperature of the second reactor bed within a second temperature range. In some aspects, the second temperature range can be about 300°C to 550°C. In other aspects, the second temperature range can be about 300°C to 500°C, about 350°C to 500°C, about 300°C to 400°C, about 350°C to 450°C, about 400°C to 480°C, or about 380°C to 450°C. It is also considered that the second temperature does not exceed any of these stated ranges. Further consideration is that the second temperature can be between any of these stated ranges.

[0071] In addition to the composition of the second input feed, the temperature of the second reactor bed can also depend at least on the composition of the bifunctional catalyst or a specific catalyst mixture in the second reactor bed. The second reactor bed may contain one or more second catalysts. Therefore, in some aspects, the second reactor bed may contain a single catalyst, while in others, it may contain a mixture of two or more monofunctional or bifunctional catalysts. It should be noted that the design of the second reactor bed should avoid over-conversion of the one or more second oxygen-containing compounds and the one or more second olefins (e.g., low-carbon olefins) present in the first reaction mixture, which could lead to either undercooling or overheating of the second reaction stage, respectively. Therefore, the composition of the second reactor bed can be designed based on the desired rate and composition of the one or more second olefins relative to the total flow rate of the one or more second oxygen-containing compounds.

[0072] In some aspects, the one or more second catalysts comprise doped or undoped zeolite catalysts. Non-limiting examples of suitable zeolite catalysts include pentasilicone ring types, such as ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or dealuminated crystalline silicates of the group ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or phosphorus and / or boron modified crystalline silicates of the group ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or molecular sieves of the AEL group of silica-aluminophosphate types. Non-limiting examples of suitable dopants for zeolite catalysts include phosphorus and / or boron. Additional additives for mixing with doped zeolites include a SiO2 support doped with metal dopants, which may include sodium (Na), potassium (K), lithium (Li), beryllium (Be), magnesium (Mg), calcium (Ca), strontium (Sr), barium, radium, iron (Fe), cobalt (Co), nickel (Ni), lanthanum (La), chromium (Cr), zirconium (Zr), ruthenium (Ru), molybdenum (Mo), iridium (Ir), tungsten (W), copper (Cu), manganese (Mn), vanadium (V), zinc (Zn), titanium (Ti), rhodium (Rh), rhenium (Re), gallium (Ga), palladium (Pd), silver (Ag), and / or indium (In).

[0073] In other respects, the one or more second catalysts may also include catalysts specifically for alcohol or ether dehydration, such as solid acids, doped or undoped alumina, such as zirconated alumina, γ-alumina, high-purity γ-alumina or doped γ-alumina, or doped or undoped zeolites with limited olefin oligomerization activity (e.g., such zeolites, under application conditions, would dehydrate alcohols to their corresponding olefins with a selectivity of at least 80 mol%), such as H-MFI type zeolites with a high Si / Al2 ratio (e.g. >190) or dealuminated, and under certain conditions (Si / Al2 ratio), H-FER, H-BEA or HY type zeolites may also be considered monofunctional dehydration catalysts.

[0074] An exemplary catalyst combination physically mixed within the second reactor bed may include a portion (e.g., the first catalyst of the one or more second catalysts) of doped zeolite, such as crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or dealuminated crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or phosphorus and / or boron modified crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or molecular sieves of the aluminosilicate type of AEL group. Additional additives for mixing with the doped zeolite consist of a SiO2 support doped with metal dopants, including iron (Fe), strontium (Sr), cobalt (Co), nickel (Ni), lanthanum (La), chromium (Cr), zirconium (Zr), ruthenium (Ru), molybdenum (Mo), iridium (Ir), magnesium (Mg), tungsten (W), copper (Cu), manganese (Mn), vanadium (V), zinc (Zn), titanium (Ti), rhodium (Rh), rhenium (Re), gallium (Ga), palladium (Pd), silver (Ag), and / or indium (In). A second portion of the catalyst mixture (e.g., a second catalyst of the one or more first catalysts) may comprise a catalyst specifically for the dehydration of alcohols or ethers as described above.

[0075] The second reactor bed can have various structural configurations. For example, in some aspects, the second reactor bed is a fixed reactor bed. In some aspects, the fixed bed reactor is an axial flow fixed bed reactor. In some aspects, the fixed bed reactor is a radial flow fixed bed reactor. In other aspects, the second reactor bed is a fluidized bed. In other aspects, the second reactor bed is a moving bed.

[0076] In some aspects, an adiabatic multistage reactor may include one or more additional reaction stages, each with a corresponding reactor bed. For example, an adiabatic multistage reactor may include a third reaction stage with a third reactor bed. The third reactor bed may have various configurations. For example, in some aspects, the third reactor bed is a fixed reactor bed. In some aspects, the fixed bed reactor is an axial flow fixed bed reactor. In some aspects, the fixed bed reactor is a radial flow fixed bed reactor. In other aspects, the third reactor bed is a fluidized bed. In other aspects, the third reactor bed is a moving bed.

[0077] In operation, a third input feed is introduced downstream of the second reaction stage of the adiabatic multistage reactor, such that upon exiting the second reaction stage, the second reaction mixture can be mixed with the third input feed to produce a second effluent with a different composition relative to the second reaction mixture. The second effluent is then contacted with the third reactor bed, thereby maintaining the third temperature of the third reactor bed within a third temperature range of approximately 300°C to 550°C and producing the third reaction mixture. In some aspects, heat is not removed from the third reaction mixture before removal from the adiabatic multistage reactor or subsequent mixing with the fourth input feed.

[0078] The third input feed comprises one or more third oxygen-containing compounds, so named because they are third oxygen-containing compounds introduced into the reactor at the third stage or reactor bed. Non-limiting examples of third oxygen-containing compounds include methanol, ethanol, propanol, butanol, pentanol, one or more esters, and / or one or more ethers. In some aspects, the one or more third oxygen-containing compounds do not contain methanol. In some aspects, the one or more third oxygen-containing compounds may contain the same oxygen-containing compound, while in other aspects, the one or more third oxygen-containing compounds may contain a mixture of different oxygen-containing compounds. For example, in some aspects, the one or more third oxygen-containing compounds may contain a dominant third oxygen-containing compound, such as ethanol. The weight percentage of the “dominant third oxygen-containing compound” as used herein may be higher than any other single oxygen-containing compound among the one or more third oxygen-containing compounds, for example, it may be present in an amount of at least 25% by weight, at least 50% by weight, or at least 75% by weight of the one or more third oxygen-containing compounds. In some aspects, the dominant third oxygen-containing compound may be present in amounts of 25% to 99% by weight, 25% to 90% by weight, 50% to 99% by weight, or 75% to 99% by weight of the one or more third oxygen-containing compounds. Further consideration is that the content of the dominant third oxygen-containing compound may be within any of these stated ranges.

[0079] Typically, the one or more third oxygen-containing compounds are identical to the one or more first oxygen-containing compounds and the one or more second oxygen-containing compounds, such that the overall conversion process within the adiabatic multistage reactor includes two or more injections of oxygen-containing compounds, more specifically, injections of oxygen-containing compounds at different reaction stages. This further enables the system to control the temperature of the reactor bed, thereby maximizing the thermal integration of the entire adiabatic multistage reactor. In some aspects, the primary third oxygen-containing compound of the one or more third oxygen-containing compounds may include ethanol. In these aspects, the one or more third oxygen-containing compounds may also include one or more other oxygen-containing compounds, such as methanol, propanol, one or more esters and / or one or more ethers.

[0080] The one or more third oxygen-containing compounds can be introduced into an adiabatic multistage reactor at various temperatures. For example, in some aspects, the temperature of the one or more third oxygen-containing compounds can be about 300°C to 550°C or about 400°C to 500°C. In one aspect, the temperature of the one or more third oxygen-containing compounds can be about 300°C to 480°C. In another aspect, the temperature of the one or more third oxygen-containing compounds can be about 480°C to 550°C or about 450°C to 500°C. It is also considered that the temperature of the one or more third oxygen-containing compounds does not exceed any of these stated ranges. Further consideration is that the temperature of the one or more third oxygen-containing compounds can be between any of these stated ranges.

[0081] A third input feed can be introduced into the adiabatic multistage reactor at various temperatures. For example, in some aspects, the temperature of the third input feed can be about 200°C to 550°C, about 200°C to 500°C, or about 300°C to 500°C. In some aspects, the third input feed can be introduced into the adiabatic multistage reactor at a temperature higher than that of the second reaction mixture.

[0082] In use, the components of the third input feed are designed to maintain the third temperature of the third reactor bed within a third temperature range. In some aspects, the third temperature range can be about 300°C to 550°C. In other aspects, the third temperature range can be about 300°C to 500°C, about 350°C to 500°C, about 300°C to 400°C, about 350°C to 450°C, about 400°C to 460°C, about 400°C to 480°C, or about 370°C to 480°C. It is also considered that the third temperature does not exceed any of these stated ranges. Further consideration is that the second temperature can be between any of these stated ranges.

[0083] In addition to the composition of the third input feed, the temperature of the third reactor bed can also depend at least on the composition of the third reactor bed. The third reactor bed may contain one or more third catalysts (e.g., bifunctional catalysts). Therefore, in some respects, the third reactor bed may contain a single catalyst, while in others, it may contain a mixture of two or more catalysts. It should be noted that the design of the third reactor bed should avoid over-conversion of the one or more third oxygen-containing compounds and the one or more third olefins (e.g., low-carbon olefins) present in the second reaction mixture, which could lead to either undercooling or overheating of the third reaction stage, respectively. Therefore, the composition of the third reactor bed can be designed based on the desired rate and composition of the one or more third olefins relative to the total flow rate of the one or more third oxygen-containing compounds.

[0084] In some aspects, the one or more third catalysts comprise doped or undoped zeolite catalysts. Non-limiting examples of suitable zeolite catalysts include pentasilicone ring types, such as ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or dealuminated crystalline silicates of the group ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or phosphorus and / or boron modified crystalline silicates of the group ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON with a Si / Al ratio greater than 10; or molecular sieves of the AEL group of silica-aluminophosphate types. Non-limiting examples of suitable dopants for zeolite catalysts include phosphorus and / or boron. In some aspects, the zeolite catalyst can be boron- and phosphorus-doped zeolite. Additional additives used for mixing with the doped zeolite include a SiO2 support doped with a metal dopant, which may include sodium (Na), potassium (K), lithium (Li), beryllium (Be), magnesium (Mg), calcium (Ca), strontium (Sr), barium, radium, iron (Fe), cobalt (Co), nickel (Ni), lanthanum (La), chromium (Cr), zirconium (Zr), ruthenium (Ru), molybdenum (Mo), iridium (Ir), tungsten (W), copper (Cu), manganese (Mn), vanadium (V), zinc (Zn), titanium (Ti), rhodium (Rh), rhenium (Re), gallium (Ga), palladium (Pd), silver (Ag), and / or indium (In).

[0085] In other respects, the one or more third catalysts may also include catalysts specifically for alcohol or ether dehydration, such as solid acids, doped or undoped alumina, such as zirconated alumina, γ-alumina, high-purity γ-alumina or doped γ-alumina, or doped or undoped zeolites with limited olefin oligomerization activity (e.g., such zeolites, under application conditions, would dehydrate alcohols to their corresponding olefins with a selectivity of at least 80 mol%), such as H-MFI type zeolites with a high Si / Al2 ratio (e.g. >190) or dealuminated, and under certain conditions (Si / Al2 ratio), H-FER, H-BEA or HY type zeolites may also be considered monofunctional dehydration catalysts.

[0086] An exemplary catalyst combination physically mixed within a third reactor bed may include a portion (e.g., the first catalyst of the one or more third catalysts) of doped zeolites, such as crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or dealuminated crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or phosphorus and / or boron modified crystalline silicates of the ZSM-5 (MFI or BEA framework), CHA, FER, FAU, MWW, MOR, EUO, MFS, ZSM-48, MTT, or TON group with Si / Al greater than 10, or molecular sieves of the aluminosilicate type of AEL group. Additional additives for mixing with the doped zeolite consist of a SiO2 support doped with metal dopants, including iron (Fe), strontium (Sr), cobalt (Co), nickel (Ni), lanthanum (La), chromium (Cr), zirconium (Zr), ruthenium (Ru), molybdenum (Mo), iridium (Ir), magnesium (Mg), tungsten (W), copper (Cu), manganese (Mn), vanadium (V), zinc (Zn), titanium (Ti), rhodium (Rh), rhenium (Re), gallium (Ga), palladium (Pd), silver (Ag), and / or indium (In). A second portion of the catalyst mixture (e.g., a second catalyst of the one or more first catalysts) may comprise a catalyst specifically for the dehydration of alcohols or ethers as described above.

[0087] As described above, an adiabatic multistage reactor can contain any number of reaction stages, equal to or greater than two, to achieve the desired output composition. Therefore, in a further aspect, the multistage reactor includes one or more additional reaction stages downstream of a third reaction stage. Each of the one or more additional reaction stages has a corresponding reactor bed. In use, a subsequent input feed is introduced into the multistage reactor downstream of previous reaction stages (e.g., the first, second, and third reaction stages), such that upon exiting the previous reaction stage (e.g., the third reaction stage), the previous reaction mixture (e.g., the third reaction mixture) mixes with the subsequent input feed to produce an additional effluent with a composition different from the previous reaction mixture. The subsequent input feed may contain one or more additional oxygen-containing compounds. The previous effluent can then be contacted with the corresponding reactor bed of the one or more additional reaction stages, thereby maintaining the temperature of the corresponding reactor bed within a certain temperature range (e.g., about 300°C to 550°C) and producing an additional reaction mixture downstream of the previous reaction stage.

[0088] While the foregoing discussion of adiabatic multistage reactors includes all beds within a single adiabatic multistage reactor, this document also considers the possibility that each reactor bed may reside in a separate adiabatic reactor. For example, in some aspects, the aforementioned first, second, and third reactor beds are each located in their respective adiabatic reactors. This approach allows for the use of mobile beds and enables individual access to and maintenance or replacement of each bed. This document also considers the implementation of two or more adiabatic reactors, where at least one of these reactors comprises two or more catalyst beds. For example, in some aspects, the first adiabatic reactor comprises a first reactor bed and a second reactor bed, while the second adiabatic reactor comprises a third reactor bed and, optionally, a fourth reactor bed.

[0089] In the presence of two or more adiabatic reactors, these reactors may be collectively referred to herein as a reactor assembly (e.g., two or more adiabatic multistage reactors may be collectively referred to herein as an adiabatic multistage reactor assembly). In some aspects, a method for converting one or more oxygen-containing compounds into one or more olefins may include introducing a first input feed into a first end of an adiabatic multistage reactor assembly having at least a first reaction stage and a second reaction stage, wherein the first reaction stage is upstream of the second reaction stage and has a first reactor bed, and the second reaction stage has a second reactor bed. The first input feed may include one or more first oxygen-containing compounds and at least one of one or more first olefins or methanol. The method may further include: contacting the first input feed with the first reactor bed to maintain a first temperature of the first reactor bed within a first temperature range of about 300°C to 550°C and produce a first reaction mixture; and introducing a second input feed downstream of the first reaction stage of the multistage reactor assembly such that, upon exiting the first reaction stage, the first reaction mixture mixes with the second input feed to produce a first effluent with a different composition relative to the first reaction mixture. The second input feed may contain one or more second oxygen-containing compounds. The method may further include: contacting the first effluent with the second reactor bed to maintain the second temperature of the second reactor bed within a second temperature range of about 300°C to 550°C and to produce a second reaction mixture.

[0090] In some aspects, the multistage reactor assembly may include a third reaction stage, wherein the third reaction stage has a third reactor bed. In these aspects, the method may further include introducing a third input feed into a downstream system of the second reaction stage of the multistage reactor, such that, upon exiting the second reaction stage, the second reaction mixture is mixed with the third input feed to produce a second effluent with a different composition relative to the second reaction mixture. The third input feed may contain one or more third oxygen-containing compounds. The method may further include contacting the second effluent with the third reactor bed to maintain a third temperature of the third reactor bed within a third temperature range of about 300°C to 550°C and to produce a third reaction mixture.

[0091] In some respects, a multistage reactor assembly may include two or more reactors, wherein the first and second stages may be carried out in a first reactor and the third stage may be carried out in a second reactor.

[0092] In some aspects, a multistage reactor assembly may include two or more reactors, wherein a first reactor bed may be located in a first reactor and a second reactor bed may be located in a second reactor. In other aspects, a third reactor bed may be located in a third reactor.

[0093] In the case of an adiabatic multistage reactor containing only two reactor beds, the output of the adiabatic multistage reactor is a second reaction mixture. The components of the second reaction mixture may include oxygen-containing compounds (e.g., alcohols and / or ethers), olefins (e.g., C5+ olefins), water, and co-products (e.g., saturated compounds). In some respects, alcohols include ethanol, propanol, butanol, etc.

[0094] In the case of an adiabatic multistage reactor comprising three reactor beds, the output of the adiabatic multistage reactor is a third reaction mixture. The components of the third reaction mixture may include oxygen-containing compounds (e.g., alcohols and / or ethers), olefins (e.g., C5+ olefins), water, and co-products (e.g., saturated compounds). In some respects, alcohols include ethanol, propanol, butanol, etc.

[0095] The system of the present invention for the conversion of oxygen-containing compounds may include additional elements. For example, in addition to an adiabatic multistage reactor, the system of the present invention may also include one or more of the following elements: a single-stage reactor, one or more heat exchanger units, a condenser, a separation subsystem (e.g., a distillation system), one or more furnaces, or any combination thereof. Although not discussed in detail herein, it should be noted that other elements within the system of the present invention are also contemplated.

[0096] In some aspects, the system may include a single-stage reactor comprising a reactor bed having one or more catalysts. In use, the output of an adiabatic multistage reactor (e.g., a second or third reaction mixture) may be introduced into the single-stage reactor and contacted with the one or more catalysts to produce an output stream comprising one or more product olefins. The one or more product olefins may comprise C2-C7 olefins, such as ethylene, propylene, butene, pentene, etc., or any combination thereof. In one aspect, the one or more product olefins may at least comprise ethylene.

[0097] In the case of an adiabatic multistage reactor containing only two reactor beds, the temperature of the second reaction mixture can be reduced before introducing it into the single-stage reactor. In the case of an adiabatic multistage reactor containing only three reactor beds, the temperature of the third reaction mixture can be reduced before introducing it into the single-stage reactor. In either case, this temperature reduction can be achieved, for example, by a heat exchanger unit.

[0098] In some respects, the output stream can be introduced into the separation subsystem to produce a first stream and a second stream. In other respects, the output stream can be condensed into a condensed output stream before being introduced into the separation subsystem, and the condensed output stream can be introduced into the separation subsystem. The separation subsystem may include various separation units, such as distillation systems, liquid-liquid separation systems, liquid extraction systems, membrane separation systems, and adsorbent systems, to perform separation processes to produce the first stream and the second stream.

[0099] The first stream may contain ethylene, propylene, butane, or any combination thereof. In one aspect, the first stream may contain a primary olefin, such as ethylene. The weight percentage of the “primary olefin” as used herein may be greater than that of any other single olefin in the first stream, for example, it may be present in an amount of at least 50 wt%, at least 75 wt%, or at least 95 wt% of the olefins in the first stream. In some aspects, the primary olefin may be present in an amount of 25 wt% to 99 wt% of the olefins in the first stream, 25 wt% to 90 wt% of the olefins in the first stream, 35 wt% to 90 wt% of the olefins in the first stream, 40 wt% to 90 wt% of the olefins in the first stream, 45 wt% to 90 wt% of the olefins in the first stream, 50 wt% to 99 wt% of the olefins in the first stream, 55 wt% to 99 wt% of the olefins in the first stream, 60 wt% to 99 wt% of the olefins in the first stream, or 75 wt% to 99 wt% of the olefins in the first stream. In some aspects, the primary olefin may be present in an amount of 35 wt% to 65 wt% of the olefins in the first stream. Furthermore, the main olefin can exist in amounts ranging from any of these stated ranges.

[0100] The second stream may contain C3+ olefins, such as at least one C3 to C7 olefin. Furthermore, in some aspects, the second stream may contain co-products, such as aromatic compounds and saturated compounds.

[0101] In the case of an olefin cycle integrated within the system, the first stream can be combined with one or more first oxygen-containing compounds to produce a first input feed. In some aspects, the one or more first oxygen-containing compounds can be heated to temperatures such as about 200°C to 500°C, about 200°C to 500°C, about 375°C to 500°C, about 360°C to 550°C, or about 400°C to 500°C before the first input stream is introduced into the adiabatic multistage reactor. Alternatively or additionally, the one or more second oxygen-containing compounds can be heated to temperatures such as about 200°C to 500°C, about 200°C to 500°C, about 375°C to 500°C, about 360°C to 550°C, or about 400°C to 500°C before the second input stream is introduced into the adiabatic multistage reactor. Alternatively or additionally, the one or more second oxygen-containing compounds may be heated to, for example, about 200°C to 500°C, about 200°C to 500°C, about 375°C to 500°C, about 360°C to 550°C, or about 400°C to 500°C before the third input stream is introduced into the adiabatic multistage reactor. In some aspects, the one or more first oxygen-containing compounds, the one or more second oxygen-containing compounds, and / or the one or more third oxygen-containing compounds may be heated by a heat exchanger (e.g., a single furnace). In other aspects, the one or more first oxygen-containing compounds, the one or more second oxygen-containing compounds, and / or the one or more third oxygen-containing compounds may be heated by two or more heat exchangers (e.g., corresponding furnaces).

[0102] In some respects, the weight space-time velocity (WHSV) of an adiabatic multistage reactor can be from about 0.25 to 15. As used herein, “weight space-time velocity” is defined as the weight of hydrocarbons flowing through per hour per total weight of catalyst in a multistage reactor.

[0103] It should be understood that the net thermodynamics of the oxygen-containing compound to olefin conversion process depends at least on the characteristics of the oxygen-containing compound, the desired olefin product mixture, and the presence of any side reactions. For example, in some aspects, especially at higher lower olefin recycling rates, the net process may be exothermic and require heat removal from the system. This cooling can be achieved in several ways. For example, a heat exchanger can be used to lower the temperature of the output of the adiabatic multistage reactor before one or more final stages of olefin oligomerization and cracking. This heat exchanger can be separate from the adiabatic multistage reactor or integrated within it. The one or more final stages of the reaction can be carried out in separate vessels, such as in a single reactor downstream of the adiabatic multistage reactor, or the side stream from the adiabatic multistage reactor can be cooled and then reintroduced into the adiabatic multistage reactor. Another approach is to cool the corresponding reactor bed using a lower-temperature second and third oxygen-containing compound feed.

[0104] In some respects, particularly when the recycling rate of lower olefins is as low as zero, or when the first input feed contains a low amount of methanol or lower olefins, the net process may be endothermic and require the addition of heat to the system. This heating can be achieved in several ways. One approach is to heat the one or more first oxygenated compounds to a temperature above the temperature of the first reactor bed. A certain amount of the one or more olefins (e.g., lower olefin recycling) may be required to maintain the process temperature of one or more initial stages of the adiabatic multistage reactor. The one or more oxygenated compounds subsequently added (e.g., the one or more second oxygenated compounds and / or the one or more third oxygenated compounds) can be heated to a temperature above the highest desired temperature of the adiabatic multistage reactor so that the total process temperature before each reaction stage is sufficiently high to continue simultaneously dehydrating the one or more oxygenated compounds and oligomerizing the olefins present in the reaction mixtures (e.g., the first reaction mixture, the second reaction mixture, and / or the third reaction mixture). By increasing the number of reaction stages, the net lower olefin recycling can be reduced, in some cases to a negligible value, although olefin selectivity may decrease as the olefins are exposed to the catalyst for longer periods.

[0105] Figure 1 An exemplary schematic diagram of a system 100 for the conversion of oxygen-containing compounds is shown. For simplicity only, this exemplary system 100 is discussed with respect to one or more first, second, and third oxygen-containing compounds being ethanol and one or more olefins being ethylene. Those skilled in the art will understand that this exemplary system can be used for other oxygen-containing compounds and olefins, and is therefore not limited to ethanol or ethylene.

[0106] In the illustrated system 100, system 100 includes an ethanol source 102, an optionally present thermally integrated subsystem 104, and an adiabatic multistage reactor 106. While the adiabatic multistage reactor 106 may have two or more reaction stages, in this illustrated example, the adiabatic multistage reactor comprises three reaction stages. The first reaction stage includes a first reactor bed 108, the second reaction stage includes a second reactor bed 110, and the third reaction stage includes a third reactor bed 112. Each reactor bed 108, 110, 112 contains one or more catalysts. As will be described in more detail below, in this illustrated system, heated ethanol is supplied to the adiabatic multistage reactor 106 in three portions. While the thermally integrated subsystem can have various configurations, in this illustrated system, the thermally integrated subsystem includes a preheater configured to preheat the ethanol to a temperature, for example, about 450°C, and a condenser configured to condense the output stream (e.g., the output stream of a single-stage reactor) into a condensate output stream.

[0107] In use, ethanol 102 is introduced into a preheater (not shown) and heated. A first portion 102a of the heated ethanol is then combined with an ethylene recirculation stream 114 (e.g., a first stream) to generate a first input feed 116, which is then introduced into a first end 118 (e.g., a first inlet) of an adiabatic multistage reactor 106. The first input feed 116 is then contacted with a first reactor bed 108, thereby maintaining a first temperature of the first reactor bed 108 within a first temperature range and generating a first reaction mixture (not shown). The first reactor bed 108 is designed such that the heat expected to be generated by the exothermic olefin oligomerization reaction is substantially or completely balanced with the heat absorbed by the dehydration of ethanol.

[0108] A second portion of heated ethanol is introduced as a second input feed 102b into an adiabatic multistage reactor 106. After leaving the first reaction stage, the first reaction mixture (not shown) is mixed with the second input feed 102b within the adiabatic multistage reactor 106 to produce a first effluent (not shown). The first effluent is then contacted with a second reactor bed 110, thereby maintaining a second temperature of the second reactor bed 110 within a second temperature range and producing a second reaction mixture (not shown). The second reactor bed 110 is designed such that the heat expected to be generated by the exothermic oligomerization of olefins is substantially or completely balanced with the heat absorbed by the dehydration of ethanol to produce ethylene.

[0109] A third portion of heated ethanol is introduced as a third input feed 102c into the adiabatic multistage reactor 106. After leaving the second reaction stage, the second reaction mixture (not shown) is mixed with the second input feed 102c within the adiabatic multistage reactor 106 to produce a second effluent (not shown). The second effluent then contacts a third reactor bed 112, thereby maintaining a second temperature of the third reactor bed 112 within a third temperature range and producing a third reaction mixture 120. The third reactor bed 112 is designed such that the heat expected to be generated by the exothermic oligomerization of olefins is substantially or completely balanced with the heat absorbed by the dehydration of ethanol to produce ethylene. The third reaction mixture 120 then exits the adiabatic multistage reactor 106 at a second end 122 (e.g., an outlet) opposite the first end 118. Those skilled in the art will understand that the first end 118 and the second end 122 can be located at different positions on the adiabatic multistage reactor, and are therefore not limited to this. Figure 1 The location shown.

[0110] like Figure 1As further shown, system 100 includes a first heat exchanger 124, a single-stage reactor 126, a separation subsystem 128, and a second heat exchanger 130. In use, a third reaction mixture 120 is first introduced into the first heat exchanger 124 to lower its temperature. The resulting cooled third reaction mixture 121 is then introduced as input feed into the single-stage reactor 126. The single-stage reactor 126 includes a reactor bed 132 with one or more catalysts, such that at least a portion of the ethylene in the third reaction mixture 120 is converted into higher carbon olefins (e.g., C3 to C5 olefins). In other words, when the third reaction mixture 120 is contacted with the reactor bed 132 of the single-stage reactor 126, an output stream 134 is generated. The output stream 134 includes one or more product olefins (e.g., C3 to C5 olefins) and ethylene.

[0111] Optionally, the output stream 134 can then be introduced first into the condenser of the thermal integration subsystem 104. Subsequently, the condensate output stream 136 can be introduced into the separation subsystem 128, which produces a first stream 138 and a second stream 140 (C3+ olefins). The first stream 138 contains ethylene, and the second stream contains C3-C5 olefins, water, and co-products (e.g., aromatic compounds and / or saturated compounds). In the illustrated system, the first stream 138 is then introduced into a second heat exchanger 130 to raise the temperature of the ethylene, and then mixed with a first portion of ethanol 102a to form a first input stream 116. Thus, at the start of the process, the first input feed 116 comprises only the first portion of ethanol 102a, but as the process continues, the first stream 138 (e.g., the generated ethylene recycle) is combined with the first portion of ethanol 102a upstream of the multistage reactor 106, such that the first input stream 116 then comprises a combination of ethanol 102a and the generated ethylene recycle 138.

[0112] In some cases, most of the ethylene is extracted from the system rather than recycled back, thus recycling it back to the multistage reactor. Therefore, where most of the ethylene is extracted from the output stream, it may be necessary to heat the first input feed to, for example, a temperature of about 450°C before partially introducing the ethanol into the multistage reactor. Heating of the ethanol can be achieved, for example, by using a furnace, electric heater, or other heat source installed in the system.

[0113] As described above, in some aspects, the first stream 138 may be ethylene (e.g., ethylene is the component with the highest concentration in the first stream). In other aspects, it may be necessary to limit or avoid the separation of olefins. In these aspects, the first stream may contain a mixture of various olefins. For example, in some aspects, the first stream may contain ethylene and propylene (e.g., ethylene and propylene are the components with the highest concentration in the first stream). In other aspects, the first stream may contain C2-C4 olefins (e.g., C2-C4 olefins are the components with the highest concentration). In other aspects, the first stream may contain C2-C5 olefins. In some aspects, a portion of the condensate output stream may be added to the first stream before separation by the separation subsystem.

[0114] In some respects, the one or more olefins can be directly generated from C2+ alcohols in a separate reactor using a dehydration-specific catalyst and subsequently used as part of the first input feed, without separation from unconverted alcohols, the resulting water, or any co-products.

[0115] In some respects, the reactor may have an additional stream introduced into the reactor, wherein the first input feed may also include methanol and / or dimethyl ether. Figure 2 An exemplary schematic diagram of an ethanol feed and methanol and / or dimethyl ether feed system for the conversion of oxygen-containing compounds is shown. For simplicity only, this exemplary system 200 is discussed in relation to only two streams combined to form a first input stream introduced into an adiabatic reactor. More specifically, the first stream is ethanol, and the second stream is methanol and / or dimethyl ether. Those skilled in the art will understand that this exemplary system can be used for other oxygen-containing compounds and olefins, and is therefore not limited to methanol, dimethyl ether, or ethanol.

[0116] In the illustrated system 200, system 200 includes a methanol source 201, an optional first heat exchanger 203, an ethanol source 202, an optional thermally integrated subsystem 204, and an adiabatic multistage reactor 206. While the adiabatic multistage reactor 206 may have two or more reaction stages, in the illustrated embodiment, the adiabatic multistage reactor comprises three reaction stages. The first reaction stage includes a first reactor bed 208, the second reaction stage includes a second reactor bed 210, and the third reaction stage includes a third reactor bed 212. Each reactor bed 208, 210, 212 contains one or more catalysts. As will be described in more detail below, in this illustrated system, heated methanol is supplied to the adiabatic multistage reactor 206 in a single pass, and heated ethanol is supplied to the adiabatic multistage reactor 206 in three separate passes. Alternatively, additional portions of heated methanol may be supplied to the adiabatic multistage reactor, for example, downstream of the first reactor bed. While the first heat exchanger 203 can have various configurations, in the system shown, the first heat exchanger is configured to preheat methanol to a temperature of, for example, about 450°C to 550°C (e.g., about 450°C). Furthermore, while the thermal integration subsystem 204 can have various configurations, the second thermal integration subsystem includes a preheater configured to preheat ethanol to a temperature of, for example, about 450°C, and a condenser configured to condense the output stream (e.g., the output stream of a single-stage reactor) into a condensate output stream.

[0117] In operation, methanol 201 is introduced into a preheater (not shown) and heated, and ethanol 102 is introduced into a preheater (not shown) and heated. A first portion 102a of the heated ethanol is then combined with a heated methanol stream 205 (e.g., a first stream) to generate a first input feed 216, which is then introduced into a first end 218 (e.g., a first inlet) of an adiabatic multistage reactor 206. In other respects, the first portion 202a of the heated ethanol and the heated methanol stream 205 are not necessarily introduced as a combined stream into the adiabatic multistage reactor 106, but rather as two separate streams. The first input feed 216 then contacts a first reactor bed 208, thereby maintaining a first temperature in the first reactor bed 208 within a first temperature range and generating a first reaction mixture (not shown). The first reactor bed 208 is designed such that the heat expected from the exothermic conversion of methanol to dimethyl ether, the conversion of methanol and dimethyl ether to olefins, and the oligomerization of olefins is substantially or completely balanced with the heat absorbed by the dehydration of ethanol.

[0118] A second portion of heated ethanol is introduced as a second input feed 202b into an adiabatic multistage reactor 206. After leaving the first reaction stage, a first reaction mixture (not shown) is mixed with the second input feed 202b within the adiabatic multistage reactor 206 to produce a first effluent (not shown). The first effluent is then contacted with a second reactor bed 210, thereby maintaining a second temperature of the second reactor bed 210 within a second temperature range and producing a second reaction mixture (not shown). The second reactor bed 210 is designed such that the heat generated by the exothermic conversion of methanol to dimethyl ether, the conversion of methanol and dimethyl ether to olefins, and the oligomerization of olefins is substantially or completely balanced with the heat absorbed by the dehydration of ethanol to produce ethylene.

[0119] A third portion of heated ethanol is introduced as a third input feed 202c into an adiabatic multistage reactor 206. After exiting the second reaction stage, a second reaction mixture (not shown) is mixed with the second input feed 202c within the adiabatic multistage reactor 206 to produce a second effluent (not shown). The second effluent is then contacted with a third reactor bed 212, thereby maintaining a second temperature of the third reactor bed 212 within a third temperature range and producing a third reaction mixture 220. The third reactor bed 212 is designed such that the heat expected to be generated by the exothermic olefin oligomerization reaction is substantially or completely balanced with the heat absorbed by the dehydration of ethanol to produce ethylene. The third reaction mixture 220 then exits the adiabatic multistage reactor 206 at a second end 222 (e.g., an outlet) opposite the first end 218. Those skilled in the art will understand that the first end 218 and the second end 222 can be located at various positions within the adiabatic multistage reactor, and are therefore not limited to them. Figure 2 The location shown.

[0120] like Figure 2 As further shown, system 200 includes a second heat exchanger 224 and a single-stage reactor 226. In use, a third reaction mixture 220 is first introduced into the second heat exchanger 224, causing the temperature of the third reaction mixture 220 to decrease. The cooled third reaction mixture 221 is then introduced as input feed into the single-stage reactor 226. The single-stage reactor 226 includes a reactor bed 232 having one or more catalysts, such that at least a portion of the ethylene in the third reaction mixture 220 is converted into higher carbon olefins (e.g., C3 to C5 olefins). In other words, when the third reaction mixture 220 is contacted with the reactor bed 232 of the single-stage reactor 226, an output stream 234 is generated. The output stream 234 contains one or more product olefins (e.g., C3 to C5 olefins) and ethylene.

[0121] Optionally, the output stream 234 can then be first introduced into the condenser of the thermal integration subsystem 204. Afterwards, the condensate output stream 236 can be introduced into the separation subsystem. Although not shown, the separation subsystem can be similar to separation subsystem 128. Furthermore, although not shown, the ethanol circulation stream (e.g.) Figure 1 114) can be seen in the above text regarding Figure 1 The adiabatic reactor 206 is generated and introduced into the system 200.

[0122] An exemplary method for converting one or more oxygen-containing compounds into one or more olefins may include: introducing a first input feed comprising ethanol, water, methanol, and / or olefins into an adiabatic multistage reactor, wherein the temperature of the first input feed may be about 400°C to 480°C. In this exemplary method, ethanol may be present in the first input feed in an amount of about 20-25% by weight, while methanol, ethylene, or other mixed olefins may be present in the first input feed in an amount of about 60-70% by weight, the balance of the first input feed being water. The temperature of the first reactor bed may be greater than or equal to about 350°C and less than or equal to about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the first reaction mixture is formed, it may be combined with a second input feed of ethanol to form a first effluent, wherein another portion of the ethanol is at a temperature above about 300°C. The ethanol present in the first effluent is about 15-30% by weight of the first effluent. Water may optionally be added to the second input feed such that the total water in the first effluent does not exceed about 60% by weight. The temperature of the second reactor bed can be equal to or greater than about 350°C and equal to or less than about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the second reaction mixture is formed, it can be combined with a third ethanol feed to form a second effluent, wherein the temperature of the ethanol is above about 300°C. The ethanol present in the second effluent is about 10-25% by weight. Water can optionally be added to the third feed such that the total water in the second effluent does not exceed about 60% by weight. The temperature of the third reactor bed can be equal to or greater than about 350°C and equal to or less than about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the third reaction mixture is formed, it can exit the adiabatic multistage reactor as an effluent stream.

[0123] In the case of an additional downstream reactor bed in the multi-stage reactor, the method may further include: after the formation of the third reaction mixture, it may be combined with a fourth ethanol input feed to form a third effluent, wherein the temperature of the ethanol is above about 300°C. The ethanol present in the second effluent is about 8-22% by weight of the third effluent. Water may optionally be added to the fourth input feed such that the total water in the third effluent does not exceed about 60% by weight. The temperature of the fourth reactor bed may be equal to or greater than about 350°C and equal to or less than about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the formation of the fourth reaction mixture, it may exit the multi-stage reactor as output vapor. Optionally, the output stream may be cooled by a heat exchanger and fed as a fifth input feed to the fifth reactor bed of the multi-stage reactor at a given input temperature (e.g., about 350°C to 400°C). Optionally, water may be added to the fifth input stream such that the total water in the fifth input feed does not exceed about 60% by weight.

[0124] Another exemplary method for converting one or more oxygen-containing compounds into one or more olefins may include: introducing a first input feed comprising ethanol, water, methanol, and / or olefins into an adiabatic multistage reactor, wherein the temperature of the first input feed may be about 400°C to 480°C. In this exemplary method, the content of ethanol in the first input feed may be about 25-30% by weight, while the content of methanol, ethylene, or other mixed olefins in the first input feed may be about 50-60% by weight, with the remainder being water. The temperature of the first reactor bed may be greater than or equal to about 350°C and less than or equal to about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the first reaction mixture is formed, it may be combined with a second input feed of ethanol to form a first effluent, wherein another portion of the ethanol is at a temperature above 300°C. The ethanol present in the first effluent is about 20-30% by weight. Water may optionally be added to the second input feed such that the total water in the first effluent does not exceed about 50% by weight. The temperature of the second reactor bed can be equal to or greater than about 350°C and equal to or less than about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the second reaction mixture is formed, it can be combined with a third ethanol feed to form a second effluent, wherein the temperature of the ethanol is above about 300°C. The ethanol present in the second effluent is about 15-25% by weight. Water can optionally be added to the third feed such that the total water in the second effluent does not exceed about 50% by weight. The temperature of the third reactor bed can be equal to or greater than about 350°C and equal to or less than about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the third reaction mixture is formed, it can exit the adiabatic multistage reactor as an effluent stream.

[0125] In the case of an additional downstream reactor bed in the multi-stage reactor, the method may further include: after the formation of the third reaction mixture, it may be combined with a fourth ethanol input feed to form a third effluent, wherein the temperature of the ethanol is above about 300°C. The ethanol present in the second effluent is about 15-25% by weight of the third effluent. Water may optionally be added to the fourth input feed such that the total water in the third effluent does not exceed about 50% by weight. The temperature of the fourth reactor bed may be equal to or greater than about 350°C and equal to or less than about 480°C (350°C ≥ first reactor bed temperature ≤ 480°C). After the fourth reactor bed is formed, it may exit the multi-stage reactor as output vapor. Optionally, the output stream may be cooled by a heat exchanger and fed as a fifth input feed to the fifth reactor bed of the multi-stage reactor at a certain input temperature (e.g., about 350°C to 400°C). Optionally, water may be added to the fifth input feed such that the total water in the fifth input feed does not exceed about 60% by weight.

[0126] In any of the above exemplary methods, where the first input stream contains at least one or more first oxygen-containing compounds and one or more first olefins, the net molar ratio of ethylene to ethanol fed to all reaction stages can, for example, be 1:1. This molar ratio can be increased or decreased depending on the number of reactor beds in the adiabatic multistage reactor. For example, in some cases where the multistage reactor has more than five reactor beds, the net molar ratio of ethylene to ethanol fed to all reaction stages can, for example, be 1:5 or 1:9.

[0127] The terminology used herein is for the purpose of describing specific implementation schemes and methods only and is not intended to be limiting. For example, unless the context clearly indicates otherwise, the singular forms “a,” “an,” and “the” used herein also include the plural forms.

[0128] In the foregoing description and claims, phrases such as “at least one of…” or “one or more of…” may appear after a list of connecting elements or features. The term “and / or” may also appear in a list of two or more elements or features. Unless the context in which they are applied explicitly or implicitly contradicts this, such phrases are intended to mean either one of the listed elements or features, or a combination of a listed element or feature with any other stated element or feature. For example, the phrases “at least one of A and B,” “one or more of A and B,” and “A and / or B” are each intended to mean “A alone, B alone, or A and B together.” A similar interpretation is intended for lists containing three or more items. For example, the phrases “at least one of A, B, and C,” “one or more of A, B, and C,” and “A, B, and / or C” are each intended to mean “A alone, B alone, C alone, A and B together, A and C together, B and C together, or A and B and C together.” The term “based on” as used above and in the claims is intended to mean “at least partially based on,” and therefore unstated features or elements are also permitted.

[0129] Although the terms “first” and “second” may be used in this document to describe various features / elements (including steps), these features / elements should not be limited by these terms unless the context otherwise requires. These terms are used to distinguish one feature / element from another. Thus, the first feature / element discussed below may be referred to as the second feature / element, and similarly, the second feature / element discussed below may be referred to as the first feature / element, without departing from the teachings provided herein.

[0130] Unless otherwise expressly stated, all figures used in this specification and claims (including those used in the embodiments) are to be understood to begin with the word “about” or “approximately”, even if such terms do not explicitly appear. When used to describe values ​​and / or locations, the phrase “about” or “approximately” may indicate that the value and / or location is within a reasonably expected range of those values ​​and / or locations. When the word “about” or “approximately” immediately precedes a numerical value, it indicates a range of ±10% of that value; for example, “about 50” means 45 to 55, “about 25000” means 22500 to 27500, and so on. Furthermore, the phrase “less than about a value” or “greater than about a value” should be understood in light of the definition of the term “about” provided herein. It should also be understood that when a value is disclosed, “less than or equal to” that value, “greater than or equal to” that value, and possible ranges between values ​​as understood by those skilled in the art are also disclosed. For example, if the value “X” is disclosed, “less than or equal to X” and “greater than or equal to X” (e.g., where X is a numerical value) are also disclosed. It should also be understood that throughout the application, data is provided in a variety of different formats, and these data represent endpoints and starting points, as well as ranges for any combination of data points. For example, if specific data point "10" and specific data point "15" are disclosed, it should be understood that numbers greater than, greater than or equal to, less than, less than or equal to, and equal to 10 and 15, as well as numbers between 10 and 15, are disclosed. It should also be understood that each unit between two specific units is also disclosed. For example, if 10 and 15 are disclosed, then 11, 12, 13, and 14 are also disclosed.

[0131] While various exemplary embodiments have been described above, numerous changes may be made to these embodiments without departing from the teachings herein. For example, in alternative embodiments, the order of execution of the various method steps may typically be altered, while in other alternative embodiments, one or more method steps may be skipped entirely. Optional features of various device and system embodiments may be included in some embodiments but not in others. Therefore, the foregoing description is provided primarily for illustrative purposes and should not be construed as limiting the scope of the claims.

[0132] The embodiments and illustrations contained herein are shown by way of example, not limitation, of specific implementations of the subject matter. As described, other implementations can be derived from and utilized from these embodiments, allowing for structural and logical substitutions and changes without departing from the scope of this disclosure. For convenience only, The term "invention" may be used herein to refer specifically or collectively to these embodiments of the subject matter of the invention, and is not intended to limit the scope of this application to any single invention or inventive concept (if multiple inventions or inventive concepts are actually disclosed). Therefore, although specific embodiments have been illustrated and described herein, any arrangement aimed at achieving the same purpose may be substituted for the specific embodiments shown. This disclosure is intended to cover all adjustments or variations of the various embodiments. Those skilled in the art, upon reading the foregoing description, will be able to understand combinations of the above embodiments as well as other embodiments not specifically described herein. The term "based on" as used herein and in the claims is intended to mean "at least partially based on," and therefore features or elements not listed are also permitted.

[0133] The subject matter described herein can be embodied in systems, apparatus, methods, and / or articles as required. The embodiments set forth in the above description do not represent all embodiments consistent with the subject matter described herein. Rather, they are merely some examples consistent with aspects related to the subject matter. Although some variations have been described in detail herein, other modifications or additions are possible. Specifically, other features and / or variations may be provided in addition to the features and / or variations described herein. For example, the embodiments described herein may be for various combinations and sub-combinations of the disclosed features, and / or combinations and sub-combinations of several other features disclosed herein. Furthermore, the logical flows depicted in the drawings and / or described herein do not necessarily require the specific order or sequential order shown to achieve the desired results. Other embodiments may be within the scope of the following claims.

Claims

1. A method for converting one or more oxygenates to one or more olefins, the method comprising: introducing a first input feed to a first end of an adiabatic multi-stage reactor, the first input feed comprising one or more first oxygenates and one or more first olefins, the multi-stage reactor having at least a first reaction stage and a second reaction stage, wherein the first reaction stage is upstream of the second reaction stage, and the first reaction stage has a first reactor bed and the second reaction stage has a second reactor bed; contacting the first input feed with the first reactor bed, thereby maintaining a first temperature of the first reactor bed within a first temperature range of about 300°C to 550°C, and producing a first reaction mixture; introducing a second input feed downstream of the first reaction stage of the multi-stage reactor, such that upon exiting the first reaction stage, the first reaction mixture is mixed with the second input feed to produce a first effluent having a different composition relative to the first reaction mixture, the second input feed comprising one or more second oxygenates; and contacting the first effluent with the second reactor bed, thereby maintaining a second temperature of the second reactor bed within a second temperature range of about 300°C to 550°C and producing a second reaction mixture.

2. The method of claim 1, wherein the multi-stage reactor has a third reaction stage having a third reactor bed, the method further comprising, introducing a third input feed downstream of the second reaction stage of the multi-stage reactor, such that upon exiting the second reaction stage, the second reaction mixture is mixed with the third input feed to produce a second effluent having a different composition relative to the second reaction mixture, the third input feed comprising one or more third oxygenates; and contacting the second effluent with the third reactor bed, thereby maintaining a third temperature of the third reactor bed within a third temperature range of about 300°C to 550°C and producing a third reaction mixture. No external heat is added to the multi-stage reactor during each reaction stage and between reaction stages.

3. The method of claim 1 or 2, wherein, No heat is removed from the multi-stage reactor during each reaction stage and between reaction stages.

4. The method of claim 1 or 2, wherein, 5. The method of any one of claims 1 to 4, wherein the first effluent is not removed from the multi-stage reactor.

6. The method of any one of claims 1 to 5, wherein the second effluent is not removed from the multi-stage reactor.

7. The method of any one of claims 1, 2, 5, and 6, wherein heat is not removed from the first reaction mixture prior to mixing with the second input feed.

8. The method of any one of claims 1, 2, 5, 6, and 7, wherein heat is not removed from the second reaction mixture prior to removal from the multi-stage reactor or then mixing with the third input feed.

9. The method of any one of claims 2, 5, 6, 7, and 8, wherein heat is not removed from the third reaction mixture prior to removal from the multi-stage reactor or then mixing with the fourth input feed. ​ 10. The method of any one of claims 1 to 9, wherein the one or more first oxygenates comprises a primary first oxygenate and the one or more first olefins comprises a primary first olefin, wherein the primary first oxygenate is ethanol and the primary first olefin is ethylene.

11. The method of claim 10, wherein the molar ratio of ethylene to ethanol in the first input feed is about 0.25 to 10.

12. The method of claim 11, wherein the molar ratio of ethylene to ethanol in the first input feed is about 0.25 to 5.

13. The method of any one of claims 1 to 12, wherein the first temperature range is about 350 °C to 500 °C.

14. The method of any one of claims 1 to 13, wherein the second temperature range is about 350 °C to 500 °C.

15. The method of any one of claims 2 to 14, wherein the third temperature range is about 350 °C to 500 °C.

16. The method of any one of claims 1 to 15, wherein at least one of the first reactor bed or the second reactor bed is a fixed bed.

17. The method of any one of claims 2 to 16, wherein the third reactor bed is a fixed bed.

18. The method of any one of claims 1 to 15, wherein at least one of the first reactor bed or the second reactor bed is a fluidized bed.

19. The method of any one of claims 2 to 15, wherein the third reactor bed is a fluidized bed.

20. The method of any one of claims 1 to 15, wherein at least one of the first reactor bed or the second reactor bed is a moving bed.

21. The method of any one of claims 2 to 15, wherein the third reactor bed is a moving bed.

22. The method of any one of claims 1 to 21, wherein the one or more first oxygenates and the one or more second oxygenates are the same.

23. The method of any one of claims 2 to 22, wherein the one or more first oxygenates, the one or more second oxygenates, and the one or more third oxygenates are the same.

24. The method of any one of claims 1 to 23, wherein the one or more first oxygenates comprises one or more C2+ alcohols.

25. The method of any one of claims 1 to 24, wherein the one or more second oxygenates comprises one or more C2+ alcohols.

26. The method of any one of claims 2 to 25, wherein the one or more third oxygenates comprises one or more C2+ alcohols.

27. The method of any one of claims 1 to 26, wherein the one or more first oxygenates comprises a primary first oxygenate, wherein the primary oxygenate is ethanol.

28. The method of any one of claims 1 to 27, wherein the one or more second oxygenates comprises a second primary oxygenate, wherein the primary oxygenate is ethanol.

29. The method of any one of claims 2-28, wherein the one or more third oxygenate compounds comprise a primary third oxygenate compound, wherein the primary oxygenate compound is ethanol.

30. The method of any one of claims 1, 3-22, 24, 25, 27, and 28, further comprising introducing a second reaction mixture into a single-stage reactor comprising one or more catalysts and contacting the second reaction mixture with the one or more catalysts to produce an output stream comprising one or more product olefins.

31. The method of claim 30, further comprising reducing a temperature of the second reaction mixture prior to introducing the second reaction mixture into the single-stage reactor.

32. The method of claim 30 or 31, further comprising introducing the output stream into a separation sub-system to produce a first stream and a second stream.

33. The method of claim 31, wherein the second stream comprises at least one C3+ olefin.

34. The method of claim 33, combining the first stream with the one or more first oxygenate compounds to produce a first input feed.

35. The method of any one of claims 32-34, wherein the first stream comprises a primary olefin, wherein the primary olefin is ethylene.

36. The method of claim 30 or 31, further comprising condensing the output stream into a condensed output stream and introducing the condensed output stream into a separation sub-system to produce a first stream and a second stream.

37. The method of claim 36, combining the first stream with the one or more first oxygenate compounds to produce a first input feed.

38. The method of claim 36 or 37, wherein the first stream comprises a primary olefin, wherein the primary olefin is ethylene.

39. The method of any one of claims 36-38, wherein the second stream comprises at least one C3+ olefin.

40. The method of any one of claims 2-29, further comprising introducing a third reaction mixture into a single-stage reactor comprising one or more catalysts and contacting the third reaction mixture with the one or more catalysts to produce an output stream comprising one or more product olefins.

41. The method of claim 40, further comprising reducing a temperature of the third reaction mixture prior to introducing the third reaction mixture into the single-stage reactor.

42. The method of claim 40 or 41, further comprising introducing the output stream into a separation system to produce a first stream and a second stream.

43. The method of claim 34, combining the first stream with the one or more first oxygenate compounds to produce a first input feed.

44. The method of claim 42 or 43, wherein the first stream comprises a primary olefin, wherein the primary olefin is ethylene.

45. The method of any one of claims 42-44, wherein the second stream comprises at least one C3+ olefin.

46. The method of claim 40 or 41, further comprising condensing the output stream into a condensed output stream and introducing the condensed reaction mixture into a separation subsystem to produce a first stream and a second stream.

47. The method of claim 47, combining the first stream with the one or more first oxygenates to produce a first input feed.

48. The method of claim 46 or 47, wherein the first stream comprises a primary olefin, wherein the primary olefin is ethylene.

49. The method of any one of claims 46 to 48, wherein the second stream comprises at least one C3+ olefin.

50. The method of any one of claims 1 to 49, further comprising heating the one or more first oxygenates prior to introducing the first input stream into the adiabatic multistage reactor.

51. The method of any one of claims 1 to 50, further comprising heating the one or more second oxygenates prior to introducing the second input stream into the adiabatic multistage reactor.

52. The method of any one of claims 2 to 51, further comprising heating the one or more third oxygenates prior to introducing the third input stream into the adiabatic multistage reactor.

53. The method of any one of claims 1 to 52, wherein the multistage reactor has a gauge pressure of from 0 to about 30 bar.

54. The method of any one of claims 1 to 53, wherein the multistage reactor has a weight hourly space velocity (WHSV) of from about 0.25 to 15.

55. The method of any one of claims 1 to 54, wherein at least one of the first reactor bed or the second reactor bed comprises a catalyst mixture.

56. The method of claim 55, wherein the catalyst mixture comprises a zeolite and an alcohol dehydration catalyst.

57. The method of any one of claims 2 to 56, wherein the third reactor bed comprises a catalyst mixture.

58. The method of claim 57, wherein the catalyst mixture of the third reactor bed comprises a zeolite and an alcohol dehydration catalyst.

59. The method of any one of claims 1 to 58, wherein the second input feed is introduced into the adiabatic multistage reactor at a temperature higher than the first reaction mixture temperature.

60. The method of any one of claims 2 to 58, wherein the third input feed is introduced into the adiabatic multistage reactor at a temperature higher than the second reaction mixture temperature.

61. The method of any one of claims 2 to 60, wherein the multistage reactor includes one or more additional reaction stages downstream of the third reaction stage, each of the one or more additional reaction stages having a respective reactor bed, the method further comprising, introducing a subsequent input feed downstream of a previous reaction stage of the multistage reactor, such that upon exiting the previous reaction stage, a previous reaction mixture is mixed with the subsequent input feed to produce an additional effluent having a different composition than the previous reaction mixture, the subsequent input feed comprising one or more additional oxygenates; and contacting the previous effluent with the respective reactor bed of one of the one or more additional reaction stages, thereby maintaining the temperature of the respective reactor bed in a temperature range of about 300°C to 550°C, and producing an additional reaction mixture downstream of the previous reaction stage.

62. The method of any preceding claim, wherein the one or more first oxygenates comprise ethanol and methanol.

63. The method of any of claims 1-9, 13-34, 36, 37, 39-43, 45-47, and 49-62, wherein the one or more first olefins comprise ethylene, propylene, butylene, or any combination thereof.

64. The method of any of claims 1-61 and 63, wherein the one or more first oxygenates are free of methanol.

65. The method of any preceding claim, wherein the one or more second oxygenates are free of methanol.

66. The method of any preceding claim, wherein the one or more third oxygenates are free of methanol.

67. A method for converting one or more oxygenates to one or more olefins, the method comprising: introducing a first input feed to a first end of an adiabatic multi-stage reactor, the first input feed comprising one or more first oxygenates, the one or more first oxygenates comprising ethanol, and at least one of methanol or dimethyl ether, the multi-stage reactor having at least a first reaction stage and a second reaction stage, wherein the first reaction stage is upstream of the second reaction stage, and the first reaction stage has a first reactor bed, the second reaction stage has a second reactor bed; contacting the first input feed with the first reactor bed, thereby maintaining a first temperature of the first reactor bed in a first temperature range of about 300°C to 550°C, and producing a first reaction mixture; introducing a second input feed downstream of the first reaction stage of the multi-stage reactor, such that upon exiting the first reaction stage, the first reaction mixture mixes with the second input feed to produce a first effluent having a different composition relative to the first reaction mixture, the second input feed comprising one or more second oxygenates; and contacting the first effluent with the second reactor bed, thereby maintaining a second temperature of the second reactor bed in a second temperature range of about 300°C to 550°C, and producing a second reaction mixture.

68. The method of claim 67, wherein the multi-stage reactor has a third reaction stage, the third reaction stage having a third reactor bed, the method further comprising, introducing a third input feed downstream of the second reaction stage of the multi-stage reactor, such that upon exiting the second reaction stage, the second reaction mixture mixes with the third input feed to produce a second effluent having a different composition relative to the second reaction mixture, the third input feed comprising one or more third oxygenates; and contacting the second effluent with the third reactor bed, thereby maintaining a third temperature of the third reactor bed in a third temperature range of about 300°C to 550°C, and producing a third reaction mixture.

69. The method of claim 67 or 68, wherein the one or more first oxygenates comprise ethanol and methanol.

70. The method of claim 67 or 68, wherein the one or more first oxygenates comprise ethanol or dimethyl ether.

71. The method of claim 70, wherein the one or more first oxygenates further comprise methanol.

72. The method of any one of claims 67 to 71, wherein the one or more second oxygenates comprise ethanol, methanol, or a combination thereof.

73. The method of any one of claims 67 to 72, wherein the one or more second oxygenates are free of methanol.

74. The method of any one of claims 67 to 73, wherein the one or more third oxygenates comprise ethanol, methanol, or a combination thereof.

75. The method of any one of claims 67 to 74, wherein the one or more third oxygenates are free of methanol.

76. A system comprising the adiabatic multi-stage reactor of any one of claims 1 to 75.

77. A method for converting one or more oxygenates to one or more olefins, the method comprising: introducing a first input feed to a first end of an adiabatic multi-stage reactor assembly, the first input feed comprising one or more first oxygenates and at least one or more first olefins and methanol, the multi-stage reactor assembly having at least a first reaction stage and a second reaction stage, wherein the first reaction stage is upstream of the second reaction stage, and the first reaction stage has a first reactor bed and the second reaction stage has a second reactor bed; contacting the first input feed with the first reactor bed, thereby maintaining a first temperature of the first reactor bed within a first temperature range of about 300°C to 550°C and producing a first reaction mixture; introducing a second input feed downstream of the first reaction stage of the multi-stage reactor assembly, such that upon exiting the first reaction stage, the first reaction mixture mixes with the second input feed to produce a first effluent having a different composition relative to the first reaction mixture, the second input feed comprising one or more second oxygenates; and contacting the first effluent with the second reactor bed, thereby maintaining a second temperature of the second reactor bed within a second temperature range of about 300°C to 550°C and producing a second reaction mixture.

78. The method of claim 77, wherein the multi-stage reactor assembly has a third reaction stage having a third reactor bed, the method further comprising, introducing a third input feed downstream of the second reaction stage of the multi-stage reactor assembly, such that upon exiting the second reaction stage, the second reaction mixture mixes with the third input feed to produce a second effluent having a different composition relative to the second reaction mixture, the third input feed comprising one or more third oxygenates; and contacting the second effluent with the third reactor bed, thereby maintaining a third temperature of the third reactor bed within a third temperature range of about 300°C to 550°C and producing a third reaction mixture. ​ 79. The method of claim 77 or 78, wherein the multi-stage reactor assembly comprises two or more reactors, wherein the first stage and the second stage are conducted in a first reactor and the third stage is conducted in a second reactor.

80. The method of claim 77 or claim 78, wherein the multi-stage reactor assembly comprises two or more reactors, wherein a first reactor bed is located in a first reactor and a second reactor bed is located in a second reactor.

81. The method of claim 80, wherein a third reactor bed is located in a third reactor.

82. The method of any one of claims 77 to 81, wherein the first input feed comprises one or more first oxygenates, one or more first olefins, and methanol.

83. The method of any one of claims 77 to 81, wherein the first input feed comprises one or more first oxygenates and methanol.

84. The method of any one of claims 77 to 81, wherein the first input feed comprises one or more first oxygenates and one or more first olefins.

85. The method of any one of claims 77 to 84, wherein the one or more second oxygenates are free of methanol.

86. The method of any one of claims 78 to 85, wherein the one or more third oxygenates are free of methanol.

87. The method of any one of the preceding claims, wherein the one or more first olefins comprise one or more recycled olefins, wherein the one or more recycled olefins comprise ethylene, propylene, butylene, pentene, or any combination thereof.

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