CORE IN KETTLE REACTOR, METHODS FOR USING, AND METHODS FOR MAKING

FIELD OF THE INVENTION

This invention relates to heat exchange chemical reactors. REFERENCE TO AN EARLIER APPLICATION

This application is based on and claims priority to US Provisional Application Serial No.

61 /561 ,643, filed November 18, 201 1 , the entire contents of which being hereby incorporated by reference.

BACKGROUND

The Fischer-Tropsch synthesis reaction involves converting a reactant composition comprising H ₂ and CO in the presence of a catalyst to aliphatic hydrocarbon products. The reactant composition may comprise the product stream from another reaction process such as steam reforming (product stream H ₂ /CO~3), partial oxidation (product stream H ₂ /CO~2), autothermal reforming (product stream H ₂ /CO~2.5), C0 ₂ reforming (H ₂ /CO~1 ), coal gasification (product stream H ₂ /CO~1 ), and combinations thereof. The aliphatic hydrocarbon products may range from methane to paraffinic waxes of up to 100 carbon atoms or more.

Conventional reactors such as tubular fixed bed reactors and slurry reactors have various problems in heat and mass transfer resulting in limitations of choice of process conditions for Fischer-Tropsch synthesis reactions. Hot spots in the fixed bed reactors significantly promote methane formation, reduce the heavy hydrocarbon selectivity and deactivate the catalyst. On the other hand, strong mass transfer resistance inherent in a catalyst suspended in a slurry system generally reduces the effective reaction rate and also causes difficulty in separation of catalysts from the products.

Processes have been described in which methane is reacted with steam, to generate carbon monoxide and hydrogen in a first catalytic reactor; the resulting gas mixture is then used to perform Fischer-Tropsch synthesis in a second catalytic reactor. The overall result is to convert methane to hydrocarbons of higher molecular weight, which are usually liquid under ambient conditions. The two stages of the process, steam/methane reforming and Fischer- Tropsch synthesis, require different catalysts, and heat to be transferred to or from the reacting gases, respectively, as the reactions are respectively endothermic and exothermic. The reactors for the two different stages must comply with somewhat different requirements: Fischer-Tropsch synthesis is usually carried out at a higher pressure but a lower temperature than

steam/methane reforming; and in the heat transfer channels of the Fischer-Tropsch reactor only a coolant fluid is required, whereas the heat required for steam/methane reforming would typically be provided by catalytic combustion, and so would require a suitable catalyst.

In each case the reactor is preferably formed as a stack of plates, with flow channels defined between the plates, the flow channels for the different fluids alternating in the stack. In those channels that require a catalyst, this is preferably in the form of a corrugated metal substrate carrying the catalyst in a ceramic coating, such corrugated structures being removable from the channels when the catalyst is spent. However, where there is a large pressure difference between the two fluids, this will tend to cause the plates to bend, so heat transfer between the catalyst structure and the plates is impeded, and it may be difficult to remove or replace the catalyst structure; yet if the plates are to be strong enough to resist the pressure difference, then the plates will have to be thicker and/or the channels narrower, and the flow volume as a proportion of the total volume of the reactor will tend to be less.

Previous systems used plate-fin technology in which the process flow runs at right angles to the utility stream. These systems have problems such as poor heat transfer and stress across the reaction block.

Other complex reactors have been developed in which the pressurized fluid is separate from the reactants in order to provide a positive gauge pressure on at least part of a reaction core. Such pressure vessels partially enclose microchannel reactors, but such systems undesirably use stainless steel for the reactors, which are difficult and expensive to fabricate. In addition, the heat transfer of steels such as stainless steel is poor.

The embodiments described herein solve the aforementioned problems and others.

DESCRIPTION OF THE SEVERAL EMBODIMENTS

One embodiment relates to a reactor, comprising:

(A) a pressure vessel having a pressure bearing wall surrounding a pressurizable interior region;

(B) a process fluid inlet extending through the wall in fluid communication with the interior region; and (C) a heat exchange reactor enclosed within the pressure vessel; the heat exchange reactor having an exterior in fluid communication with the interior region; the heat exchange reactor further comprising:

(C1 ) a core section having a top end, a bottom end, and an interior comprising a plurality of thermally conductive, parallel parting plates extending vertically between the top and bottom ends; the parting plates separating and defining a plurality of alternating process and utility channels; the process channels extending vertically between the top and bottom ends; and

(C2) a bottom header defining an interior product region; the bottom header sealingly attached to and extending downward from the bottom end;

wherein the process channels are open at the top and bottom ends such that the interior region of the pressure vessel is in fluid communication with the interior product region of the bottom header through the process channels.

The parting plates may be suitably made from flat metal, the type of which is not particularly limited. For example, the parting plates may be suitably made from one or more of aluminum, 3000 series aluminum, 3003 aluminum, 5000 series aluminum, 5085 aluminum, 6000 series aluminum, 6061 aluminum, stainless steel, copper, titanium, monel, inconel, nickel, platinum, rhodium, chromium, brass, alloys thereof, or combination thereof.

So long as the parting plates are thermally conductive and provide heat transfer between adjacent process and utility channels, they can have any thickness, which is not particularly limited. For example, the parting plates may have a thickness ranging from 5/1000 inch to 2 mm, which range includes all values and subranges therebetween, including 5, 6, 7, 8, 9, 10, 1 1 , 12, 13, 14, 15, 16, 17, 18, 19, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, and 75/1000/inch, and 2 mm, or any combination thereof.

In one embodiment, the heat exchange reactor is substantially wholly enclosed by the pressure vessel such that the pressure within the heat exchange reactor is balanced by the pressure in the interior region of the pressure vessel. Generally, in one embodiment, the heat exchange reactor has top and bottom ends, a bottom header, and process channels open at the top end such that the process channels fluidly communicate with both the interior region of the pressure vessel and the interior product region in the bottom header. Put another way, the interior region of the pressure vessel is in fluid communication with the interior product region of the bottom header by way of the process channels. In this way, in one embodiment, one may inject a process fluid, e.g., reactant fluid, or the like, into the interior region, such that it exists in the space between the vessel's pressure bearing wall and the heat exchange reactor's exterior surfaces. Sufficiently pressurizing the vessel's interior region drives the process fluid down into the process channels from the open top end, through the process channels, and into the interior product region in the bottom header. Along the way, part of the process fluid may suitably undergo reaction in the process channels and be converted to product, which also flows into the interior product region together with unreacted process fluid. It generally follows that the heat exchange reactor is sealed on its sides, with the exception that side headers may be present to inject and remove a utility fluid into and from the utility channels. It is most preferred that the utility and process channels are configured to provide for co-current or countercurrent flow of the utility and process streams. Put another way, it is preferred that the process and utility channels are configured such that their respective streams run parallel or antiparallel to one another, and not at right angles to one another.

Using a stacked design of alternating utility and process channels separated from one another by thermally-conductive parting plates, the heat exchanger can be configured to separate and direct the respective utility and process streams in a low cost manner.

Such a design gives rise to unexpected advantages, including ease of access and manufacture, excellent temperature and pressure control, low cost, and advantageous use of materials. By the embodiments described herein, mass transfer is enhanced, reaction rate is improved, productivity is improved, yield is increased, and/or selectivity is increased. The pressure vessel can be made of steel or steel alloy, and the heat exchange reactor may be made of aluminum or aluminum alloy. Other advantages, which are not apparent and could not have been foreseen, arise from the design, as will be shown herein.

The parting plates are spaced apart from one another, and the spaces therebetween define the respective process and utility channels. The spacing is not particularly limited. For example, the parting plates may be spaced apart from one another by a distance ranging from 0.1 -20 mm, which range includes all values and subranges therebetween, including 0.1 , 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, and 20 mm, or any combination thereof.

The parting plates may have different spacing depending on whether two adjacent plates define a process channel or a utility channel therebetween. For example, two adjacent plates defining a process channel may have a greater or lesser spacing between them than do two adjacent plates defining a utility channel. The spacing between adjacent parting plates may be suitably adjusted according to considerations of structural support, reaction conditions, heat removal, fin height, catalyst type, fluid flow, and the like. In a direction normal to the plane of the parting plates, i.e., the direction along the "stack" of parting plates, process channels and utility channels, the parting plate spacing may be constant, i.e., it may be the same for each of the process channels, utility channels, or both. Alternatively, the parting plate spacing for one or both of the process and utility channels may vary along the stack direction. In one embodiment, each of the process channels is defined by parting plates having the same spacing. In another embodiment, each of the utility channels is defined by parting plates having the same spacing. In one embodiment, the spacing for process channels is greater than the spacing for the utility channels. It should follow that since the parting plates are parallel, the spacing defining a particular channel between parting plates will be the same for whole of that channel.

In one embodiment, the pressure vessel is adapted to contain a pressurized process fluid in the interior region at a pressure sufficient to force the process fluid into the process channels at the top end and downward through the bottom end into the interior product region.

In one embodiment, the bottom header is sealingly attached to the bottom end by a weld or with a flanged connection. The flanged connection may allow for easier removal and insertion of catalyst from or into the process channels. The bottom header may suitably be made from metal, the type of which is not particularly limited. For example, the bottom header may independently include or be made from one or more metal such as aluminum, 3000 series aluminum, 3003 aluminum, 5000 series aluminum, 5085 aluminum, 6000 series aluminum, 6061 aluminum, stainless steel, copper, titanium, monel, inconel, nickel, platinum, rhodium, chromium, brass, alloys thereof, or combination thereof.

In one embodiment, the reactor includes a process fluid outlet extending from the bottom header through the pressure bearing wall and in fluid communication with the interior product region. Reaction product, unreacted process fluid, and the like may suitably collected in the interior product region and sent downstream, for example to a second reactor or heat exchange reactor. In one embodiment, the reactor may include more than one heat exchanger enclosed therein, and the process fluid outlets of each may be collected into a single process fluid outlet, which may suitably exit the reactor through a single outlet extending through the pressure bearing wall. If desired, the reaction product may be separated from the unreacted process fluid components, whereupon the separated reaction product may be sent downstream, and the unreacted process fluid may be returned to the reactor for further reaction.

The process fluid outlet may suitably include a flanged connection between the bottom header and the pressure bearing wall.

If desired, one or more of the process channels, utility channels, or both contain one or more fins, catalysts, or a combination thereof. If present, the fins may be independently and suitably chosen from one or more of corrugated, castellated, herringbone, perforated, straight, or serrated materials, or a combination thereof.

The fins may be suitably optimized in consideration of structure and/or heat transfer. For example, the fins may provide structural support to adjacent parting plates or improve heat transfer between process and utility fluids.

In one embodiment, the structure and/or arrangement of the may be considered to form one or more "mini-channels", which may direct the flow or contribute to directing the flow of a fluid such as a process fluid or utility fluid as it travels through the channel. In one embodiment, the mini-channels run in the machine or process direction, such that the process fluid therein flows straight through from the top end to the bottom end of the heat exchange reactor.

Similarly, wherein co-current or countercurrent flow between the process and utility fluids are desired, the process and utility channels may each have fins arranged to have respective mini- channels which are parallel or substantially so. In another embodiment, the mini-channels run in a direction other than the process direction, for example wherein a cross-flow is desired between the process and utility channels is desired, the mini-channels in the respective channels may be aligned in a direction other than parallel, for example, 90 degrees to one another.

In one embodiment, both the process and utility channels contain fins. In another embodiment, one contains fins and the other does not. The same or different fin arrangements and/or types may be used in a particular individual channel. Similarly, the same or different fin arrangements and/or types may be used among the channels of the same type. For example, all of the process (or utility) channels may have the same arrangement and/or type of fins, or they may have a different arrangement and/or type.

The material forming the fins is not particularly limited. Typically, however, the fins may be independently and suitably be made from metal, metal foil, thin metal sheet, extruded metal, combinations thereof, or the like by any process such as stamping, folding, bending, extruding, or a combination thereof. Extruding may be particularly suitable for making fins having larger dimensions, e.g., up to 20 mm in height and/or width.

The fins may be independently and suitably made from metal, the type of which is not particularly limited. For example, the one or more of the process channel and/or utility channel fins may independently include or be made from one or more metal such as aluminum, 3000 series aluminum, 3003 aluminum, 5000 series aluminum, 5085 aluminum, 6000 series aluminum, 6061 aluminum, stainless steel, copper, titanium, monel, inconel, nickel, platinum, rhodium, chromium, brass, alloys thereof, or combination thereof. The height of the process channel fins is not particularly limited. For example, the process channel fins, if present, may have a height ranging from 0.1 - 20 mm, the height being measured as the distance between adjacent vertical parting plates, e.g. the separation distance between adjacent parting plates defining that channel. This height range includes all values and subranges therebetween, including 0.1 , 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, and 20 mm, or any combination thereof.

The width of the process channel fins is not particularly limited. For example, the width of the process channel fins, e.g., the distance between two fins, may suitably range from 0.1 - 20 mm, the width being measured normal to the process channel fin height, i.e., parallel to the plane of an adjacent parting plate.. This width range includes all values and subranges therebetween, including 0.1 , 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, and 20 mm, or any combination thereof. In one embodiment, there are two fins per inch.

The thickness of the process channel fin is not particularly limited. In one embodiment, the fin metal thickness may suitably range from 3/1000 inch to 100/1000 inch. This range includes all values and subranges therebetween, including 3, 4, 5, 6, 7, 8, 9, 10, 1 1 , 12, 13, 14, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, and 100/1000 inch, or any combination thereof.

If desired, the process channel fins may suitably have a catalyst coating, for example, a washcoated catalyst.

The height of the utility channel fins is not particularly limited. For example, the utility channel fins, if present, may have a height ranging from 0.5 - 20 mm, the height being measured as the distance between adjacent vertical parting plates, e.g. the separation distance between adjacent parting plates defining that channel. This height range includes all values and subranges therebetween, including 0.5, 0.6, 0.7, 0.8, 0.9, 1 , 1 .1 , 1 .2, 1 .3, 1 .4, 1 .5, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, and 20 mm, or any combination thereof.

The width of the utility channel fins is not particularly limited. For example, the width of the utility channel fins, e.g., the distance between two fins, may suitably range from 0.1 - 20 mm, the width being measured normal to the process channel fin height, i.e., parallel to the plane of an adjacent parting plate.. This width range includes all values and subranges therebetween, including 0.1 , 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, and 20 mm, or any combination thereof. In one embodiment, there are two fins per inch.

The thickness of the utility channel fin is not particularly limited. In one embodiment, the fin metal thickness may suitably range from 3/1000 inch to 100/1000 inch. This range includes all values and subranges therebetween, including 3, 4, 5, 6, 7, 8, 9, 10, 1 1 , 12, 13, 14, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, and 100/1000 inch, or any combination thereof.

In one embodiment, the fins are adapted to direct the flow of utility fluid in the utility channels and/or process fluid in the process channels.

As mentioned above, in one embodiment, the sides of the heat exchange reactor, e.g., the side edges of the process channels, are suitably sealed such that the only way for the process fluid to enter the process channels is through the top end, wherein the process channels fluidly communicate with the interior region of the pressure vessel.

In one embodiment, the sides may be sealed by the inclusion of one or more process channel side bars. The process channel side bars seal the side edges of the process channels between adjacent parting plates and extend vertically between the top and bottom ends such that they prevent fluid communication between the side regions of the process channels and the interior region of the pressure vessel. The process channel side bars may be suitably disposed within the process channels at the outer edges thereof and define the height of the process channels between adjacent parting plates, or they may be sealingly attached to the outside edges of the process channels. In the case wherein the process channel side bars are disposed within the process channels, they may help provide structural support between adjacent parting plates, and particularly at the outer edges of the process channels. For example, these side bars may resist compression or expansion damage of the process channel during manufacturing, use, or both. The process channel side bars may be made from metal, the type of which is not particularly limited. For example, the process channel side bars may be made from or include one or more of aluminum, 3000 series aluminum, 3003 aluminum, 5000 series aluminum, 5085 aluminum, 6000 series aluminum, 6061 aluminum, stainless steel, copper, titanium, monel, inconel, nickel, platinum, rhodium, chromium, brass, alloys thereof, or combination thereof.

The heat exchange reactor may suitably include one or more process channel support bars disposed within the process channels between adjacent parting plates and extending vertically between the top and bottom ends. When present, these support bars may help provide structural support between adjacent parting plates, or further direct the flow along the process channel. For example, these support bars may resist compression or expansion damage of the process channel during manufacturing, use, or both. The process channel support bars may be made from the same or different metal as the process channel side bars.

Turning to the utility channels, they are suitably closed at the top and bottom ends of the heat exchange reactor such that the utility channels are not in fluid communication with any of the interior region of the vessel, the process channels, or the interior product region at the bottom header.

In one embodiment, to prevent fluid communication between the interior region of the pressure vessel, the utility channels, and the interior product region in the bottom header, the heat exchange reactor may suitably include utility channel top and bottom bars at the top and bottom ends. The utility channel top and bottom bars suitably seal the top and bottom edges of the utility channels between adjacent parting plates and prevent fluid communication between the utility channels and both the interior region of the pressure vessel and the interior product region of the bottom header.

As mentioned above, the sides of the heat exchange reactor may be suitably sealed to prevent fluid communication between the interior fluid region and the sides or side edges of both the utility channels and process channels.

Accordingly, in one embodiment, the heat exchange reactor may include utility channel side bars; the utility channel side bars sealing the side edges of the utility channels between adjacent parting plates and preventing fluid communication between the interior region and the utility channels. In the case wherein the utility channel side bars are disposed within the utility channels, they may help provide structural support between adjacent parting plates, and particularly at the outer edges of the utility channels. For example, these side bars may resist compression or expansion damage of the utility channel during manufacturing, use, or both. The utility channel side bars may be made from metal, the type of which is not particularly limited. For example, the utility channel side bars may be made from or include one or more of aluminum, 3000 series aluminum, 3003 aluminum, 5000 series aluminum, 5085 aluminum, 6000 series aluminum, 6061 aluminum, stainless steel, copper, titanium, monel, inconel, nickel, platinum, rhodium, chromium, brass, alloys thereof, or combination thereof.

In one embodiment, the heat exchange reactor may include utility channel support bars disposed within the utility channels between adjacent parting plates; the support bars providing structural support between adjacent parting plates. When present, these support bars may help provide structural support between adjacent parting plates, or further direct the flow along the utility channel. For example, these support bars may resist compression or expansion damage of the utility channel during manufacturing, use, or both. The utility channel support bars may be made from the same or different metal as the process channel side bars.

When disposed between adjacent parting plates, the utility channel side bars and/or support bars may define the spacing of utility channels between adjacent parting plates. In one embodiment, the heat exchange reactor may include first and second side headers to provide for a flow of a utility fluid through the utility channels. The first and second side headers define respective interior utility fluid regions and are sealingly attached to the core section such that the first side header interior utility fluid region is in fluid communication with the second side header interior utility fluid region through one or more of the utility channels. The side headers may be placed along one or more of the sides of the core section such that they communicate with the side edges of one or more of the utility channels. For example, the first and second side headers may be placed on opposite sides of the core section such that their respective interior utility fluid regions are in fluid communication with each other (and the utility channels) through opposing side edges of the utility channels. Alternatively, the first and second side headers may be placed on the same side of the core section such that their respective interior utility fluid regions are in fluid communication with each other (and the utility channels) through the same-side edges of the utility channels. Any combination is

contemplated, including one in which the first and second side headers are placed at upper and lower portions (upper defined as nearer the top end, and lower defined as nearer the bottom end) of the core section. In one embodiment, the utility fluid enters and exits the core section through upper and lower side portions thereof, while the process fluid enters the core section from the upper end and exits into the bottom header at the lower end. The side headers may be made from the same or different material as the side bars or support bars.

In one embodiment, the reactor may include a utility fluid inlet extending through the pressure bearing wall into the first side header and in fluid communication with the first side header interior utility fluid region; and a utility fluid outlet extending through the pressure bearing wall into the second side header and in fluid communication with the second side header interior utility fluid region. In one embodiment, the utility fluid inlet and outlet may each include a flanged connection between the side headers and the pressure bearing wall.

It follows that when the heat exchange reactor includes utility channel side bars, the utility channel side bars do not seal the side edges at the interior utility fluid regions, in consideration of allowing fluid communication between the interior utility fluid regions and utility channels.

In one embodiment, one or more of the utility channels may additionally include directional fins; the fins adapted to direct the flow of a utility fluid between one or more of the interior utility fluid regions and the utility channels. For example, when the utility channels are adapted to provide for a vertical flow of a utility stream therein (i.e., co-current or countercurrent flow with a vertical flow of the process stream) but the utility stream flow enters and exits the utility channel at side headers, one or more directional fins may be included in those areas of the utility channel near the side headers/interior utility fluid region to help transition the flow of the utility stream between the vertical direction and the interior utility fluid regions of the side headers. The directional fins may be one or more of corrugated, castellated, herringbone, perforated, straight, serrated, or a combination thereof.

The directional fins may be independently and suitably made from metal, the type of which is not particularly limited. For example, they may include or be made from one or more metal such as aluminum, 3000 series aluminum, 3003 aluminum, 5000 series aluminum, 5085 aluminum, 6000 series aluminum, 6061 aluminum, stainless steel, copper, titanium, monel, inconel, nickel, platinum, rhodium, chromium, brass, alloys thereof, or combination thereof.

The height, width and thickness of the directional fins may be suitably and independently selected from those given for the utility channel fins.

In one embodiment, one or more portions of the utility channels may be substantially parallel with the process channels to provide for co-current or countercurrent flow of a utility fluid and a process fluid. Alternatively, the utility channels are not parallel with the process channels to provide for crosscurrent flow of a utility fluid and a process fluid. Generally speaking, the flow of a process stream within the process channel is vertical, and more preferably flows from the top end to the bottom end. The directional flow may be assisted using fins or mini-channels along the vertical direction. Similarly, in one embodiment, the flow of a utility stream in the utility channel may be directed in whole or part by the flow between the interior utility fluid regions, the locations of side headers and their respective utility fluid inlets and outlet, and/or the flow direction of a utility stream in the utility channel may be directed in whole or in part by using fins or mini-channels along the desired flow direction for the utility stream.

In one embodiment, the utility stream may be driven by a pump, thermosyphon or a combination thereof.

The pressure vessel may be made from any suitable pressure-bearing material, the type of which is not particularly limited. For example, all or part of the pressure vessel may be made from or include one or more of steel, stainless steel, carbon steel, nickel steel, chromium, hastalloy, Haynes metal, alloys thereof, or combination thereof.

The heat exchange reactor may be made from any suitable material, the type of which is not paryticularly limted. For example, all or part of the heat exchange reactor may include or be made from one or more of aluminum, 3000 series, 3003 aluminum, 5000 series, 5085 aluminum, 6000 series, 6061 aluminum, stainless steel, copper, titanium, monel, inconel, nickel, platinum, rhodium, chromium, brass, alloys thereof, or combination thereof. In one embodiment, the core section may uses the FINTEC line of heat exchangers and/or reactors such as available from Chart Energy & Chemicals, Inc., of LaCrosse, Wl. In one embodiment, the core uses the SHIMTEC™ line of heat exchangers and/or reactors such as available from Chart Energy & Chemicals, Inc., of LaCrosse, Wl. In this regard, the entire contents of each of U.S. Patent Nos. 7,998,345; 7,989,920; 6,736,201 ; 6,695,044; 6,510,894; and 5,193,61 1 are independently hereby incorporated by reference.

Given the teachings herein, the heat exchange reactor may be suitably made according to known methods, for example using one or more of brazing, bonding, diffusion bonding, diffusion brazing, laser welding, hot isostatic pressing, clamping, welding, or combination thereof.

In one embodiment, one or more additional heat exchange reactors may be enclosed within the pressure vessel.

In one embodiment, the pressure shell may include a flange sealingly attached thereto; the flange having a surface facing the interior region and forming part of the pressure bearing wall; the flange being removable to provide access to the heat exchange reactor.

In one embodiment, the heat exchange reactor includes more utility channels than process channels.

In one embodiment, the core section of the heat exchange reactor has height (H), width (W), and length (L) dimensions, which dimensions independently range from 6"H x 1 "W x 6"L to 5Ή x 6'W x 30'L; the height being measured in a vertical direction between the top and bottom ends, the width being measured in a horizontal direction normal to the parting plates, and the length being measured in a horizontal direction parallel to the parting plates. These H, W, and L ranges independently include all values and subranges therebetween, including: for the height range, 6, 7, 8, 9, 10, 1 1 , 12 inches, 1 Ί ", 1 '2", 1 '3", 1 '4", 1 '5", 1 '6", 2", 3", 4" and 5", and any combination thereof; for the width range, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 1 1 , 12 inches, 1 Ί ", 1 '2", 1 '3", 1 '4", 1 '5", 1 '6", 2', 3', 4', 5', and 6', and any combination thereof; and for the length range, 6, 7, 8, 9, 10, 1 1 , 12 inches, 1 Ί ", 1 '2", 1 '3", 1 '4", 1 '5", 1 '6", 2', 3', 4', 5', 6', 7', 8', 9', 10', 1 1 ', 12', 15', 20', 22', 24', 26', 28', and 30' and any combination thereof

Various fluid passageways or pipes may connect the core through the kettle wall to a corresponding passageway or pipe outside the kettle. For example, one or more feed gas lines, drain lines, process stream lines, utility stream lines, injection stream lines, may connect through the kettle to the core. See, for example, attached Dwg. Nos. 17687Z and 17582Z.

In one embodiment, the core is aluminum.

In one embodiment, the pressure vessel is steel or stainless steel. In one embodiment, one or more transition joints may be used to connect the aluminum core side to the steel or stainless steel pressure vessel side. Suitable transition joints include the type obtainable from Dynamic Materials Corporation in Boulder, Colorado. In one embodiment, explosion-welded clad metal transition joints may be used.

In one embodiment, the transition joint may include a corrosion resistant coating. In one embodiment, the coating resists penetration by hydrogen gas or other gas.

In one embodiment, one or more bellows may be used to connect part of the aluminum core side to the steel or stainless steel kettle side. Suitable bellows include the type obtainable from U.S. Bellows, Inc., in Houston, Texas.

As used herein, referring to the core section, H is a measure of the length of the process channel, W is a measure of the thickness of the stack of channels and parting plates, and L is a measure of the width of the process channel, e.g., a measure of the side-to-side distance process channel side bar to opposing process channel side bar.

In one embodiment, the HWL of the core section is 5'x6'x28'.

In one embodiment, the reactor may be suitably adapted to operate at a differential pressure of < 20 barg between the interior region and the interior product region at a

temperature ranging from -100 to 750 °F. A differential pressure may be defined as the absolute value of the difference between the referenced regions' pressures. The

aforementioned pressure range independently include all values and subranges therebetween, including 0, .1 , .2, .3, .4, .5, .6, .7, .8, .9, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 12.5, 15, 17.5, and 20 barg, and any combination thereof.

In one embodiment, the reactor may be adapted to operate at a differential pressure of < 140 barg between the process channels and the utility channels at a temperature of ranging from -100 to 750°F. This pressure range includes all values and subranges therebetween, including 0, .1 , .2, .3, .4, .5, .6, .7, .8, .9, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 12.5, 15, 17.5, 20, 25, 50, 75, 100, 1 10, 120, 130, and 140 barg, and any combination thereof.

In one embodiment, the reactor may be adapted to operate at a pressure of < 150 barg in the interior region at a temperature ranging from -100 to 750°F. This pressure range includes all values and subranges therebetween, including 0, .1 , .2, .3, .4, .5, .6, .7, .8, .9, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 12.5, 15, 17.5, 20, 25, 50, 75, 100, 1 10, 120, 130, 140, and 150 barg, and any combination thereof.

The aforementioned ranges for temperatures independently include all values and subranges therebetween, including -100, -90, -80, -70, -60, -50, -40, -30, -20, -10, -9, -8, -7, -6, - 5, -4, -3, -2, -1 , 0, 1 , 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, 20, 25, 50, 75, 100, 200, 300, 400, 500, 600, 700, and 750 °F.

Another embodiment relates to a method for making the reactor described herein, which includes:

assembling the parting plates, process channels, and utility channels, to form the core section;

sealingly attaching the bottom header to the bottom end of the core section; to form a core section having the bottom header;

assembling a portion of the pressure vessel and process fluid inlet, to form a partially completed pressure vessel having an opening;

inserting the core section having the bottom header into the opening; and

sealing the opening, to form the reactor.

The reactor is particularly suitable for carrying out an exothermic reaction or an endothermic reaction. Other examples of suitable reactions include out one or more of the following reactions: catalytic reaction, endothermic reaction, exothermic reaction, acetylation, addition reaction, alkylation, dealkylation, hydrodealkylation, reductive alkylation, amination, aromatization, arylation, autothermal reforming, carbonylation, decarbonylation, reductive carbonylation, carboxylation, reductive carboxylation, reductive coupling, condensation, cracking, hydrocracking, cyclization, cyclooligomerization, dehalogenation, dimerization, epoxidation, esterification, exchange, Fischer-Tropsch, halogenation, hydrohalogenation, homologation, hydration, dehydration, hydrogenation, dehydrogenation, hydrocarboxylation, hydroformylation, hydrogenolysis, hydrometallation, hydrosilation, hydrolysis, hydrotreating, hydrodesulferization/hydrodenitrogenation, isomerization, methanation, methanol synthesis, methylation, demethylation, metathesis, nitration, oxidation, partial oxidation, polymerization, reduction, Sabatier reaction, steam reforming, carbon dioxide reforming, sulfonation, telomerization, transesterification, trimerization, water gas shift, reverse water gas shift, phase change reaction, gas to liquid reaction, evaporation, absorption, adsorption, or a combination thereof.

In one embodiment, the reactor is suitable for carrying out one or more hydrogenation reaction, dehydrogenation reaction, oxidation reaction, Fischer-Tropsch reaction, gas to liquid reaction, steam reformation, or a combination thereof. In one embodiment, the reaction is a Fischer-Tropsch reaction.

Another embodiment relates to a process, carried out in the reactor, which process includes: heating or cooling the utility channels with a utility stream; and

injecting a process fluid through the process fluid inlet into the interior region, the process fluid comprising a reactant fluid;

pressurizing the interior region to force the process fluid into the process channels at the top end and downward through the process channels into the interior product region;

converting at least a portion of the process fluid to product fluid by a reaction in the process channels;

flowing the product fluid downward through the process channels into the interior product region.

In one embodiment, the process additionally includes injecting a cooling process fluid into the interior region before, after, or during the injecting of the process fluid, or a combination thereof, in consideration of controlling one or more of reaction rate, temperature, or pressure, to remove heat from the reaction, to limit, prevent or stop runaway reaction, or to control reaction startup, or to wind down and/or stop the reaction, the cooling process fluid being one or more of a liquid, gas, or liquid / gas mixture, vapor, liquid droplets, liquid water, cooling fluid, inert gas, nitrogen, argon, aliphatic hydrocarbon, hydrocarbon, C ₁ -C ₁₀₀ hydrocarbon, vaporizable liquid having a vaporization temperature at or below that of a reaction to be carried out in the reactor, air, carbon monoxide, carbon dioxide, oil, mineral oil, methane, ethane, ethylene, propane, butane, isobutane, pentane, isopentane, hexane, mixed refrigerant, vapor compression refrigeration fluid, ammonia, methylenechloride, chlorofluorocarbon, fluorochloromethane, dichlordiflouromethane, dichloromethane, hydrocarbon derived from fractionation of natural gas, product fluid, utility fluid, diluent fluid, injection fluid, or a combination thereof.

In another embodiment, the process includes increasing or decreasing the amount of process fluid relative to the amount of process cooling fluid in the interior region. Alternatively, the process may include increasing or decreasing the amount of cooling process fluid relative to the amount of process fluid in the interior region. By amount, one can easily measure injection rate, partial pressure, mass, space velocity of each fluid.

In one embodiment, of the process, the reaction is one or more of catalytic reaction, endothermic reaction, exothermic reaction, acetylation, addition reaction, alkylation,

dealkylation, hydrodealkylation, reductive alkylation, amination, aromatization, arylation, autothermal reforming, carbonylation, decarbonylation, reductive carbonylation, carboxylation, reductive carboxylation, reductive coupling, condensation, cracking, hydrocracking, cyclization, cyclooligomerization, dehalogenation, dimerization, epoxidation, esterification, exchange, Fischer-Tropsch, halogenation, hydrohalogenation, homologation, hydration, dehydration, hydrogenation, dehydrogenation, hydrocarboxylation, hydroformylation, hydrogenolysis, hydrometallation, hydrosilation, hydrolysis, hydrotreating,

hydrodesulferization/hydrodenitrogenation, isomerization, methanation, methanol synthesis, methylation, demethylation, metathesis, nitration, oxidation, partial oxidation, polymerization, reduction, Sabatier reaction, steam reforming, carbon dioxide reforming, sulfonation, telomerization, transesterification, trimerization, water gas shift, reverse water gas shift, phase change reaction, evaporation, absorption, adsorption, or a combination thereof.

As noted herein, the reaction may be an endothermic reaction, exothermic reaction, Fisher-Tropsch reaction, or combination thereof.

In one embodiment, the pressure vessel is adapted to contain a pressurized process fluid in the interior region, the process fluid being one or more of a liquid, gas, or liquid / gas mixture, vapor, liquid droplets, liquid water, steam, synthesis gas, carbon monoxide, carbon dioxide, hydrogen gas, nitrogen gas, oxygen gas, aliphatic hydrocarbon, hydrocarbon, methane, ethane, propane, butane, isobutane, pentane, Ci-Ci ₀₀ hydrocarbon, wax, unsaturated hydrocarbon, coal gasification product, desulfurized reactant or product, catalytic reaction product or reactant, endothermic reaction product or reactant, exothermic reaction product or reactant, acetylation product or reactant, addition reaction product or reactant, alkylation product or reactant, dealkylation product or reactant, hydrodealkylation product or reactant, reductive alkylation product or reactant, amination product or reactant, aromatization product or reactant, arylation product or reactant, autothermal reforming product or reactant, carbonylation product or reactant, decarbonylation product or reactant, reductive carbonylation product or reactant, carboxylation product or reactant, reductive carboxylation product or reactant, reductive coupling product or reactant, condensation product or reactant, cracking product or reactant, hydrocracking product or reactant, cyclization product or reactant, cyclooligomerization product or reactant, dehalogenation product or reactant, dimerization product or reactant, epoxidation product or reactant, esterification product or reactant, exchange product or reactant, Fischer- Tropsch product or reactant, halogenation product or reactant, hydrohalogenation product or reactant, homologation product or reactant, hydration product or reactant, dehydration product or reactant, hydrogenation product or reactant, dehydrogenation product or reactant, hydrocarboxylation product or reactant, hydroformylation product or reactant, hydrogenolysis product or reactant, hydrometallation product or reactant, hydrosilation product or reactant, hydrolysis product or reactant, hydrotreating product or reactant,

hydrodesulferization/hydrodenitrogenation product or reactant, isomerization product or reactant, methanation product or reactant, methanol synthesis product or reactant, methylation product or reactant, demethylation product or reactant, metathesis product or reactant, nitration product or reactant, oxidation product or reactant, partial oxidation product or reactant, polymerization product or reactant, reduction product or reactant, Sabatier reaction product or reactant, steam reforming product or reactant, carbon dioxide reforming product or reactant, sulfonation product or reactant, telomerization product or reactant, transesterification product or reactant, trimerization product or reactant, water gas shift product or reactant, reverse water gas shift product or reactant, phase change reaction product or reactant, evaporation product or reactant, absorption product or reactant, adsorption product or reactant, reactant fluid, product fluid, diluent fluid, injection fluid, catalyst regeneration fluid, scrubbing fluid, catalyst, liquid catalyst, gaseous catalyst, cooling process fluid, or a combination thereof.

In one embodiment, the process fluid may be one or more of a liquid, gas, or liquid / gas mixture, vapor, liquid droplets, liquid water, steam, synthesis gas, carbon monoxide, carbon dioxide, hydrogen gas, nitrogen gas, oxygen gas, aliphatic hydrocarbon, hydrocarbon, methane, ethane, propane, butane, isobutane, pentane, Ci-Ci ₀₀ hydrocarbon, wax, unsaturated hydrocarbon, steam reformation product stream, partial oxidation product stream, autothermal reforming product stream, C0 ₂ reforming product stream, coal gasification product stream, desulfurized reactant stream, reactant fluid, product fluid, diluent fluid, injection fluid, catalyst regeneration fluid, scrubbing fluid, catalyst, liquid catalyst, gaseous catalyst, or any combination thereof.

As used herein, the term reactant fluid may suitably refer to a process fluid which contains one or more reactants intended for the subject invention.

In one embodiment, the utility channels are adapted to contain a utility fluid, the utility fluid being one or more of a heating fluid, cooling fluid, liquid, gas, or liquid / gas mixture, vapor, liquid droplets, air, steam, liquid water, nitrogen, argon, carbon monoxide, carbon dioxide, molten salt, oil, mineral oil, aliphatic hydrocarbon, hydrocarbon, methane, ethane, ethylene, propane, butane, isobutane, pentane, isopentane, hexane, mixed refrigerant, vapor

compression refrigeration fluid, vaporizable liquid having a vaporization temperature at or below that of a reaction to be carried out in the reactor, ammonia, carbon dioxide, chlorofluorocarbon, methylenechloride, fluorochloromethane, dichlordiflouromethane, dicloromethane, hydrocarbon derived from fractionation of natural gas, or a combination thereof.

Another embodiment relates to a process, which is not limited to the reactor herein, and may be suitably carried out in other types of reactors. This embodiment relates to a process for controlling the rate or temperature or both of a catalyzed exothermic reaction, which process includes: contacting a cooling process fluid with one or more of a reactant for the exothermic reaction, a catalyst for the exothermic reaction, or a combination thereof;

wherein the cooling process fluid is one or more of a product of the exothermic reaction, a fluid having a vaporization temperature equal to or less than that of a reaction temperature of the exothermic reaction, or combination thereof.

In the aforementioned process, reaction may be one or more of catalytic reaction, acetylation, addition reaction, alkylation, dealkylation, hydrodealkylation, reductive alkylation, amination, aromatization, arylation, autothermal reforming, carbonylation, decarbonylation, reductive carbonylation, carboxylation, reductive carboxylation, reductive coupling,

condensation, cracking, hydrocracking, cyclization, cyclooligomerization, dehalogenation, dimerization, epoxidation, esterification, exchange, Fischer-Tropsch, halogenation,

hydrohalogenation, homologation, hydration, dehydration, hydrogenation, dehydrogenation, hydrocarboxylation, hydroformylation, hydrogenolysis, hydrometallation, hydrosilation, hydrolysis, hydrotreating, hydrodesulferization/hydrodenitrogenation, isomerization,

methanation, methanol synthesis, methylation, demethylation, metathesis, nitration, oxidation, partial oxidation, polymerization, reduction, Sabatier reaction, steam reforming, carbon dioxide reforming, sulfonation, telomerization, transesterification, trimerization, water gas shift, reverse water gas shift, phase change reaction, evaporation, absorption, adsorption, or a combination thereof.

In one embodiment, the catyalyzed exothermic reaction is a Fisher-Tropsch reaction.

In one embodiment, the cooling process fluid is one or more of a liquid, gas, or liquid / gas mixture, vapor, liquid droplets, liquid water, cooling fluid, inert gas, nitrogen, argon, aliphatic hydrocarbon, hydrocarbon, C ₁ -C ₁₀₀ hydrocarbon, air, carbon monoxide, carbon dioxide, oil, mineral oil, methane, ethane, ethylene, propane, butane, isobutane, pentane, isopentane, hexane, mixed refrigerant, vapor compression refrigeration fluid, ammonia, methylenechloride, chlorofluorocarbon, fluorochloromethane, dichlordiflouromethane, dichloromethane,

hydrocarbon derived from fractionation of natural gas, product fluid, utility fluid, diluent fluid, injection fluid, or a combination thereof.

In one embodiment, the process includes increasing or decreasing the amount of reactant or catalyst relative to the amount of cooling process fluid. In another embodiment, the process includes increasing or decreasing the amount of cooling process fluid relative to the amount of the reactant or catalyst.

Another embodiment relates to a method of starting up a catalyzed exothermal reaction, which includes the process of controlling the catalyzed exothermic reaction. Another embodiment relates to a method of stopping a catalyzed exothermal reaction, which includes the process of controlling the catalyzed exothermic reaction.

In one embodiment, a catalyst may be suitably used in the process channels, in the process liquid, or both. In one embodiment, The catalyst in the process channels is one or more of a packed catalyst, insertion catalyst, supported catalyst, washcoated catalyst, or a combination thereof.

In one embodiment, the catalyst is a Fischer-Tropsch catalyst. Fischer-Tropsch catalysts are known, and any type may be used herein. Suitable catalysts may be found in one or more of US Patents 7,749,466, 7,789,920, 7,084,180, and 6,491 ,880, the contents of each of which being hereby incorporated by reference.

In one embodiment, one of more of the process channels contain fins and catalyst, and if desired, the catalyst may be the same or different in the process channel from the top end to the bottom end.

In one embodiment, the heat exchange reactor includes one or more catalyst retention screens disposed between the bottom end and the bottom header in fluid communication with the process channels and the product interior region. In another embodiment, the heat exchange reactor includes one or more catalyst retention screens disposed between the top end and the interior region in fluid communication with the process channels and the interior region. Combinations of screens at the top and bottom may be used.

In one embodiment, the reactor may include a cooling process fluid inlet extending through the pressure bearing wall and in fluid communication with the interior region; the cooling process fluid inlet disposed over and directed towards the top end and adapted to inject a cooling process fluid towards the process channels at the top end.

In one embodiment, the cooling process fluid is one or more of a liquid, gas, or liquid / gas mixture, vapor, liquid droplets, liquid water, cooling fluid, inert gas, nitrogen, argon, aliphatic hydrocarbon, hydrocarbon, Ci-Ci ₀₀ hydrocarbon, vaporizable liquid having a vaporization temperature at or below that of a reaction to be carried out in the reactor, air, carbon monoxide, carbon dioxide, oil, mineral oil, methane, ethane, ethylene, propane, butane, isobutane, pentane, isopentane, hexane, mixed refrigerant, vapor compression refrigeration fluid, ammonia, methylenechloride, chlorofluorocarbon, fluorochloromethane, dichlordiflouromethane, dichloromethane, hydrocarbon derived from fractionation of natural gas, product fluid, utility fluid, diluent fluid, injection fluid, or a combination thereof. In one embodiment, the reactor may suitably include one or more second inlets extending through the pressure bearing wall and in fluid communication with the interior region; the one or more second inlets adapted to inject a second fluid into the interior region

In one embodiment, the the second fluid is one or more of a liquid, gas, liquid / gas mixture, vapor, liquid droplets, liquid water, steam, synthesis gas, carbon monoxide, carbon dioxide, hydrogen, nitrogen, oxygen, argon, air, aliphatic hydrocarbon, hydrocarbon, methane, ethane, propane, butane, isobutane, pentane, Ci-Ci ₀₀ hydrocarbon, wax, unsaturated hydrocarbon, coal gasification product, desulfurized reactant or product, catalytic reaction product or reactant, endothermic reaction product or reactant, exothermic reaction product or reactant, acetylation product or reactant, addition reaction product or reactant, alkylation product or reactant, dealkylation product or reactant, hydrodealkylation product or reactant, reductive alkylation product or reactant, amination product or reactant, aromatization product or reactant, arylation product or reactant, autothermal reforming product or reactant, carbonylation product or reactant, decarbonylation product or reactant, reductive carbonylation product or reactant, carboxylation product or reactant, reductive carboxylation product or reactant, reductive coupling product or reactant, condensation product or reactant, cracking product or reactant, hydrocracking product or reactant, cyclization product or reactant, cyclooligomerization product or reactant, dehalogenation product or reactant, dimerization product or reactant, epoxidation product or reactant, esterification product or reactant, exchange product or reactant, Fischer- Tropsch product or reactant, halogenation product or reactant, hydrohalogenation product or reactant, homologation product or reactant, hydration product or reactant, dehydration product or reactant, hydrogenation product or reactant, dehydrogenation product or reactant, hydrocarboxylation product or reactant, hydroformylation product or reactant, hydrogenolysis product or reactant, hydrometallation product or reactant, hydrosilation product or reactant, hydrolysis product or reactant, hydrotreating product or reactant,

hydrodesulferization/hydrodenitrogenation product or reactant, isomerization product or reactant, methanation product or reactant, methanol synthesis product or reactant, methylation product or reactant, demethylation product or reactant, metathesis product or reactant, nitration product or reactant, oxidation product or reactant, partial oxidation product or reactant, polymerization product or reactant, reduction product or reactant, Sabatier reaction product or reactant, steam reforming product or reactant, carbon dioxide reforming product or reactant, sulfonation product or reactant, telomerization product or reactant, transesterification product or reactant, trimerization product or reactant, water gas shift product or reactant, reverse water gas shift product or reactant, phase change reaction product or reactant, evaporation product or reactant, absorption product or reactant, adsorption product or reactant, reactant fluid, product fluid, cooling process fluid, diluent fluid, injection fluid, catalyst regeneration fluid, scrubbing fluid, catalyst, liquid catalyst, gaseous catalyst, or a combination thereof.