Conduit positioner

Abstract

A catalytic firebox reactor employing an exothermic catalytic reaction channel and multiple cooling conduits for creating a partially reacted fuel/oxidant mixture. An oxidation catalyst is deposited within an exothermic catalytic reaction channel. The catalyst is backside cooled. The heat of reaction is added to both the fluid in the exothermic catalytic reaction channel and the fluid passing through the cooling conduits. After discharge of the fluids from the exothermic catalytic reaction channel, the fluids mix to create a single combined flow.

Description

FIELD OF THE INVENTION

[0002] The present invention relates to catalytic reactor design. More specifically, the invention is a catalytic reactor for converting a fuel/oxidant mixture into a fuel/oxidant/product mixture and heat. The reactor employs an exothermic catalytic reaction channel cooled by numerous cooling channels, where the cooling fluid is a portion of the ultimate fuel/oxidant/product mixture. A further refinement in the invention incorporates geometric changes in the exothermic and/or cooling portions of the reactor to provide streamwise variation of the velocity of the fluids in the reactor.

BRIEF DESCRIPTION OF THE RELATED ART

[0003] Highly exothermic catalytic reactors with internal cooling are well known. While they have varying applications, the reactors are typified by exothermic reactions within the catalytic portion of the reactor and a cooling means to control the temperature within the catalytic portion to avoid a material failure, either of the substrate or the catalyst. Cooling in these reactors can be accomplished by a number of means, including placing the catalyst in a backside-cooled relationship with the cooling agent. A backside-cooling arrangement is particularly suitable for catalytic reactions that are both rapid and highly exothermic, such as catalytic combustion. In this arrangement, the catalyst substrate (typically a metal foil) is coated with an oxidation catalyst on only one side, the opposite side (or backside) remaining free of oxidation catalyst. The substrate is shaped and assembled, before or after catalyst coating, to create separate channels for exothermic reaction (in the channels coated with oxidation catalyst) or for cooling (in the channels free of oxidation catalyst). Fluid passing through the cooling channels removes a portion of the heat generated in the exothermic reaction channels.

[0004] An early example of a backside-cooled catalytic reactor for use in a catalytic combustion system is presented in U.S. Pat. No. 4,870,824 to Young et al. The '824 patent teaches the basic method of splitting a given fuel/air mixture flow into catalytic and non-catalytic passages. The '824 patent teaches the use of a ceramic substrate with multiple parallel channels, generally of the same shape and size, in which the walls which border and define each catalytic channel are coated with an oxidation catalyst on the sides facing the catalytic channel, but are not coated with an oxidation catalyst on the sides facing adjacent non-catalytic channels. By this method, the percentage of total reactants catalyzed in the reactor is no greater than the percentage of catalytic channels. The average temperature rise through the reactor is thus limited. In addition, the wall temperatures of catalytic channels bordering adjacent non-catalytic channels are controlled through the use of backside cooling.

[0005] Refinements of the basic structure taught by Young et al. are shown in U.S. Pat. Nos. 5,250,489 and 5,512,250 to Dalla Betta et al. In the '489 patent a metal substrate is used for improved heat conduction to the backside cooling fluid, and for greater resistance to thermal shock. Aluminum-containing steels are cited as being preferred. The '489 patent also teaches the use of non-similar shape and/or size channels, so that the flow split between catalytic and non-catalytic channels can be varied while retaining approximately half catalytic channels and half non-catalytic channels. Despite these changes, the fundamental structure claimed by Young et al., namely a multitude of catalytic channels and adjacent non-catalytic channels, is retained.

[0006] The '250 patent further refines the structure claimed by the '824 and '489 patents. In the '250 patent, Dalla Betta et al. teach a structure in which periodic alterations in channel shape provide different wall heat transfer rates in the catalytic channels and non-catalytic channels. Again, however, the fundamental structure claimed by Young et al., namely a multitude of catalytic channels and adjacent non-catalytic channels, is retained. Furthermore, while the '489 and '250 patents to Dalla Betta et al. teach catalytic and non-catalytic channels of different shape and tortuosity, the average channel properties (over some finite length) are not varied in the longitudinal direction, so that the catalytic reactors taught are effectively one- or two-dimensional in terms of channel flow properties such as bulk heat transfer coefficient, velocity, or average cross-sectional shape or area.

[0007] In general, the prior art backside-cooled catalytic reactors include a multitude of catalytic channels, where each individual catalytic channel is in essence a separate catalytic reactor. As a result, variations in fuel/air ratio from channel to channel (due to imperfect premixing, for example) can lead to different degrees of combustion and heat release in different channels. Likewise, variations in inlet temperature from channel to channel can also lead to variations in combustion behavior in different channels. Rate of reaction, catalyst light-off length, and maximum gas or surface temperature can all be affected by the temperature and fuel/air ratio at a channel inlet. In addition, manufacturing tolerances may result in unequal physical properties of different channels. Properties which may vary include channel size, wall thickness, catalyst or washcoat thickness, and catalyst loading; each of these may affect combustion behavior. In essence, multiple catalytic channels can produce widely varying degrees of catalytic combustion.

[0008] Because there is no mixing between separate catalytic channels in the prior-art backside-cooled reactors, the reactors suffer the above-mentioned disadvantages of sensitivity to premixing (fuel/air ratio) and sensitivity to inlet temperature uniformity. Given that all real systems have some level of gas-stream non-uniformity, these sensitivities translate to a narrowed operating range.

[0009] It has now been found that structures and methods that provide an un-partitioned exothermic catalytic reaction channel and multiple cooling channels offer superior performance. The un-partitioned exothermic catalytic reaction channel allows for continual mixing of the fuel/oxidant stream within the channel leading to a more uniform combustion and a wider operating range.

[0010] In addition, the structure of the present invention is more flexible, facilitating cross-stream area changes in the streamwise or longitudinal direction, since there is no constraint that walls contact each other to form multiple catalytic channels. Thus, the invention can be used to vary the bulk fluid properties in the streamwise or longitudinal direction via cross-stream area changes. In particular, it may be desirable to reduce the velocity of the fuel/air mixture after it has entered the exothermic catalytic reaction channel, to provide greater residence time for reaction within the reactor, while maintaining sufficient velocity at the reactor inlet to prevent flashback to the fuel/oxidant mixture upstream of the reactor.

SUMMARY OF THE INVENTION

[0011] The present invention, a catalytic firebox reactor, is a catalytic reactor employing an un-partitioned exothermic catalytic reaction channel and multiple cooling conduits passing through the exothermic catalytic reaction channel. An oxidation catalyst is deposited on the exterior surfaces of the conduits within the exothermic catalytic reaction channel. This placement of the catalyst allows the oxidation catalyst to be backside cooled by any fluid passing through the cooling conduits. Backside cooling means that at each location where an oxidation catalyst is deposited on one surface of a wall no oxidation catalyst is deposited on an adjacent or opposite surface in contact with the cooling fluid, and a portion of the heat generated by reaction on the oxidation catalyst is conducted through the substrate to the adjacent or opposite surface that is in direct contact with the cooling fluid.

[0012] The catalytic firebox reactor can be made in numerous configurations with the following common elements. A casing forms the outer boundary, which can be of any shape. The reactor casing can be a single fabricated component, or can consist of two or more components (such as a mixing duct and a conduit support duct) joined together. Two or more conduits are placed within the casing such that one fluid stream can traverse an un-partitioned channel, the exothermic catalytic reaction channel, defined by the interior surface of the casing and the exterior surfaces of the conduits, and a number of separate fluid streams can traverse the passages defined by the interior surfaces of the conduits, without mixing occurring between fluid in the exothermic catalytic reaction channel and fluid in the conduits' interior passages. A heat transfer relationship exists between the fluid in the exothermic catalytic reaction channel and the fluids in the conduits' interior passages.

[0013] In the first configuration, the exothermic catalytic reaction channel is the region between the conduits' exterior surfaces and the reactor casing's interior surface, beginning immediately downstream of the most downstream conduit inlet and ending immediately upstream of the most upstream conduit outlet (note that the most downstream conduit inlet is upstream of the most upstream conduit outlet). This region forms an un-partitioned channel because an intentional gap is made between adjacent conduits for some portion of the conduits' length, within the exothermic catalytic reaction channel. The term “un-partitioned” means that any two points within the channel can be connected by a path contained entirely within the channel. The terms “upstream” and “downstream” refer to the location of imaginary cross-stream surfaces, so that points which are not on the same streamline can have a definite upstream-downstream relationship. “Cross-stream” means perpendicular to the flow, so that streamlines of the flow always intersect a cross-stream surface perpendicularly. Thus, a first point is said to be upstream of a second point if the cross-stream surface on which the first point lies is upstream of the cross-stream surface on which the second point lies.

[0014] In the second configuration, the exothermic catalytic reaction channel begins downstream of the conduit entrance. Unlike in the first configuration, the separated inlets permit different fluids to enter and pass through the exothermic catalytic reaction channel and the conduits. Means to separate the flows includes baffle plates, manifolding and/or ducting. An example of manifolding would be having the conduits penetrating the reactor casing such that the conduit inlets are positioned outside the reactor casing such that if desired the conduits could be enclosed to receive a fluid from a common source. Ducting on the other hand refers to a scheme wherein additional structures defining flow paths are provided such that a fluid is directed into the conduits and/or the exothermic catalytic reaction channel.

[0015] The intentional gaps between adjacent conduits allow the exothermically catalyzed fluid to mix as the fluid catalytically reacts, so that nonuniformities in fluid velocity, fluid composition, and fluid temperature are ameliorated before the fluid exits the reactor. Incidental leakage of the exothermically catalyzed fluid between adjacent conduits is not considered an intentional gap. Rather, the intentional gaps must be of sufficient size that fluid may freely pass through the gaps. Specifically, this means that the sum of the flow areas through all of the gaps within the exothermic catalytic reaction channel must be greater than the channel's minimum cross-stream flow area. The cross-stream flow area of the exothermic catalytic channel, at any given streamwise location, is the area over which exothermically catalyzed fluid passes through an imaginary cross-stream surface within the channel. For flow through a gap between adjacent conduits, the flow area is defined as the minimum area within the exothermic catalytic reaction channel of an imaginary surface which passes through the axial (streamwise) centerlines of both conduits and which extends between a straight line connecting the two conduit inlets and a straight line connecting the two conduit outlets. While it is possible to have intermediate support structures within the exothermic catalytic reaction channel which locally close off one or more gaps between adjacent conduits, these support structures are open to the passage of fluid from the upstream portion of the reactor to the downstream portion of the reactor, and do not significantly reduce the continual mixing of fluid within the exothermic catalytic reaction channel.

[0016] Oxidation catalyst is deposited on at least a portion of the conduits' exterior surfaces within the exothermic catalytic reaction channel. The oxidation catalyst provides the exothermic reaction surface which supports the exothermic oxidation of fuel within the exothermic catalytic reaction channel. Catalyst coating may be applied to all of the conduits, or to only some of the conduits (leaving some of the conduits un-coated). In general, it is preferred that no oxidation catalyst is applied upstream of the most downstream conduit inlet, so that catalyzed fluid cannot enter any of the cooling conduits.

[0017] The conduits can be made in numerous configurations (cylindrical, fluted, externally finned, internally finned, internally partitioned, of round, lobed, polygonal, elliptical, or other cross-sectional shapes, straight or twisted, and so on), and can be arranged in numerous configurations within the casing (square-packed, close-packed, braided or spiraled, crisscrossed, and so on) using conduits of equal or unequal cross-sectional size, and of equal or unequal length. In all configurations, an intentional gap exists between adjacent conduits for some portion of the conduits' length, so that fluid in the exothermic catalytic reaction channel may pass between adjacent conduits, thereby allowing an un-partitioned exothermic catalytic reaction channel to exist within the reactor casing. A conduit may contain a single cooling passage, as in a simple tube for example, or a conduit may contain more than one cooling passage. For example, two parallel straight tubes may be joined to form a single conduit containing two cooling passages. Alternatively, a divider may; be inserted in a single tube to create a conduit containing two cooling passages. Three or more cooling passages may also be formed in a single conduit, if desired. In all configurations, however, oxidation catalyst is applied only to the conduitsí exterior surfaces, and the conduits must be configured with an intentional gap between adjacent conduits such that a single exothermic catalytic reaction channel is formed.

[0018] The present invention is also a method for using a backside-cooled catalyst structure, wherein the velocities of the exothermically catalyzed stream and the cooling stream may be separately varied as the streams pass through the reactor, and in particular where the velocity of the exothermically catalyzed stream is reduced, after the stream enters the exothermic catalytic reaction channel, by a streamwise increase in the cross-sectional (cross-stream) area of the exothermic catalytic reaction channel. The term “streamwise” means in the direction of the flow. The catalytic firebox structure can be configured to accomplish this variation of velocity by a streamwise reduction in the cross-stream area of the cooling conduits, resulting in a streamwise increase in the cross-stream area of the exothermic catalytic reaction channel, if the wall thickness between the cooling conduits and the exothermic catalytic reaction channel remains unchanged, and if the total cross-stream area of the reactor (including both the cooling conduits and the exothermic catalytic reaction channel) remains unchanged. Other means for reducing the velocity of the exothermically catalyzed stream area also possible, such as limiting the entrance flow area to the exothermic catalytic reaction channel by a baffle, plate, or other structure.

[0019] In the present invention, the cooling fluid and the exothermically catalyzed fluid comprise portions of an ultimate combustion mixture. As a fuel/oxidant mixture passes through the exothermic catalytic reaction channel it catalytically reacts. The heat of reaction is added to both the fluid in the exothermic catalytic reaction channel and the fluid passing through the cooling conduits. After discharge of the fluids from the exothermic catalytic reaction channel and from the cooling conduits, the fluids are allowed to mix such that a single combined flow is created.

BRIEF DESCRIPTION OF THE DRAWINGS

[0020] FIG. 1 illustrates the basic, or first configuration, catalytic firebox reactor.

[0021] FIG. 2 illustrates a second embodiment of a catalytic firebox reactor employing expanded conduit end-sections in conjunction with retainers.

[0022] FIG. 3 is a cross-sectional view of the catalytic firebox reactor of FIG. 2 taken immediately downstream of the conduit entrance looking upstream.

[0023] FIG. 4 is a cross-sectional view of the catalytic firebox of FIG. 2 taken in approximately the center of the reactor looking upstream.

[0024] FIG. 5 illustrates a catalytic firebox reactor employing a retainer strategy that does not require expanded conduit end sections.

[0025] FIG. 6 is a cross-section of the catalytic firebox reactor shown in FIG. 5 taken just downstream of the conduit entrances looking upstream.

[0026] FIG. 7 illustrates a catalytic firebox reactor using localized expansion of the conduits to retain the conduits within the reactor.

[0027] FIG. 8 illustrates a catalytic firebox reactor of close-packed configuration with expanded-end conduits.

[0028] FIG. 9 illustrates a close-packed configuration of a catalytic firebox reactor with intermediate conduit expansion.

[0029] FIG. 10 illustrates the second configuration of the catalytic fire box reactor employing a retainer positioning system.

[0030] FIG. 11 is an end view of the reactor of FIG. 10 with a grid support in lieu of a retainer.

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0031] As shown in FIG. 1, the catalytic firebox reactor is a structure comprised of an exothermic catalytic reaction channel 60 penetrated by multiple cooling conduits 20 for backside cooling of oxidation catalyst 50 supporting the reaction within the channel. In the operation of this reactor a portion of a fuel/oxidant mixture 80, 80a, enters the exothermic catalytic reaction channel 60 and is exothermically catalytically reacted on oxidation catalyst 50, while simultaneously a portion the fuel/oxidant mixture 80, 80b, enters the multiple cooling conduits 20 and cools the catalyst 50. The exothermically catalyzed fluid 80a then exits the exothermic catalytic reaction channel 60 and mixes with the cooling fluid 80b exiting the multiple cooling conduits, creating a heated combustible fuel/oxidant/product mixture.

[0032] FIG. 1 depicts a catalytic firebox reactor employing an exothermic catalytic reaction channel with an interstitial entrance and exit strategy. The reactor is comprised of a casing 10 into which conduits 20 are placed. An oxidation catalyst 50 is deposited on the exterior surfaces of the conduits 20 within the exothermic catalytic reaction channel 60. The conduits are expanded at their inlets and outlets. In the depiction shown in FIG. 2 the reactor is fabricated from a square-packed arrangement of parallel, equal-length, cylindrically-shaped conduits 20. In the configuration shown, the expanded sections 15 perform the dual function of creating a single un-partitioned exothermic catalytic reaction channel, by providing a gap between the conduits, and creating an entrance into (and exit from) the exothermic catalytic reaction channel by creating a series of interstices between adjacent expanded end-sections. A similar configuration could be created by expanding the conduits near, but not at, their inlets and outlets (an example of this is shown later, in FIG. 8). In the operation of this configuration a single fuel/air mixture stream enters the casing and is split between the exothermic catalytic reaction channel and the multiple conduits' cooling passages. At the exit of the reactor the catalyzed stream and the cooling streams mix to create a single heated, partially reacted, fuel/air/product mixture stream.

[0033] In the configuration shown in FIG. 1, the expanded sections 15 at the ends of each conduit are cylindrical (round), and are concentric with the conduit centerlines. Other cross-sectional shapes of the expanded sections are also possible, including ellipses, squares, hexagons, octagons, lobed shapes (“clover-leaf” ), and so on. In general, the term “expanded” means that at some axial location the maximum diameter of the conduit is greater than the maximum diameter of the conduit at other axial locations.

[0034] FIG. 2 shows another embodiment of a catalytic firebox reactor employing expanded conduit end-sections 15 in conjunction with a retainer strategy. In this embodiment the conduits 20 are expanded at the inlets and outlets and positioned within casing 10. The expanded sections position the conduits 20 laterally within the casing 10. A first retainer 33 is positioned at or near the conduit inlets and a second retainer 34 is positioned at or near the conduit outlets. The retainers, 33 and 34, longitudinally position conduits 20 within the casing. FIG. 3 is a cross-section of this reactor taken immediately downstream of the conduit entrances, looking upstream, showing that the expanded end-sections position the conduits 20 laterally within the casing 10 and provide interstices for fluid to enter the exothermic catalytic reaction channel. FIG. 4 is a cross-section of this reactor taken in the middle looking upstream and shows that the expanded sections create a single un-partitioned exothermic catalytic reaction channel by providing gaps between the conduits 20. The retainers 33 and 34 are shown as honeycombs. For this case, the cell size of the honeycomb is no larger than the expanded conduit ends, so that the conduits are not able to pass through the honeycomb cells. As in the configuration of FIG. 1, oxidation catalyst 50 is deposited on the exterior surfaces of the conduits 20 within the exothermic catalytic reaction channel 60.

[0035] FIG. 5 shows another configuration of the reactor employing a retainer strategy. In this reactor the conduits 20 are inserted in a first retainer 36 and a second retainer 37, and may or may not have expanded end-sections. The conduits may be attached to the first retainer 36, the second retainer 37, or both, by, for example, welding or brazing or press fit. If attachment at only one end is preferred, the conduits may slide freely through one of the retainers; for example, the conduits may be welded to the first retainer 36, but may slide freely through the second retainer 37. Like the honeycombs shown in FIG. 2, the retainers in FIG. 5 have passages that are open to the passage of fluid, as shown in FIG. 6. Passages 70a permit fluid to enter the exothermic catalytic reaction channel 60 while passages 70b (not shown) permit the fluid to exit. Passages 71a permit fluid to enter the conduits' 20 while passages 71b (not shown) permit the fluid to exit. Oxidation catalyst 50 is deposited on the exterior surfaces of conduits 20 within the exothermic catalytic reaction channel 60. A variation of the embodiment shown in FIG. 5 may incorporate only one retainer. In this case, the conduits pass through a single retainer 36, and may be attached to the retainer by, for example, welding or brazing or press fit.

[0036] FIG. 7 shows a similar configuration to that shown in FIG. 5, but shows a different method of retaining the conduits. In FIG. 7, the conduits 20 are inserted through a first retainer 36 and a second retainer 37, but are not attached to the retainers. Instead, each conduit passes through the retainers and is expanded at each end, to a size which does not permit the expanded conduit ends 15 to pass through the retainers. Thus, no attachment to the retainers is required, and the conduits may slide freely through the retainers until an expanded end contacts a retainer. The retainers are attached to the reactor casing 10. As in FIG. 5, the retainers in FIG. 7 have passage 70a and 70b that permit fluid to enter and exit the exothermic catalytic reaction channel 60, respectively. Oxidation catalyst 50 is deposited on the exterior surfaces of conduits 20 within the exothermic catalytic reaction channel 60.

[0037] The second retainer 37 defines passages 70b and 71b. Each passage 70b is sized to permit a conduit 20 to be positioned therein and positioned laterally, but not axially. In the preferred embodiment, each passage 71b is of equal size. The passages 70b and 71b are uniformly spaced. Uniformly spaced meaning that all passages 70b are spaced uniformly one to the other, as are passages 71b, and 70b and 71b are spaced uniformly as to each other. Retainer 37 may be in the form of a honeycomb structure with openings sized to accommodate the insertion of conduits 26 as well as in the form of the plate shown.

[0038] A close-packed configuration of expanded-end conduits is shown in FIG. 8. In this close-packed arrangement, the conduits 20 are arranged within casing 10 with the conduit centerlines lying on an imaginary grid consisting of adjacent equal-size equilateral triangles, so that each conduit is in direct contact with those adjacent at the expanded end-sections. The imaginary grid lines in this close-packed case consist of three sets of parallel, equally-spaced lines, each set of lines being oriented at a 60-degree angle from each other set of lines. In the example shown in FIG. 8 the conduits are attached to one another forming a bundle and conduits adjacent to the casing are attached to the casing by, for example, welding or brazing. Oxidation catalyst 50 is deposited on the exterior surfaces of conduits 20 within the exothermic catalytic reaction channel 60.

[0039] FIG. 9 illustrates another close-packed configuration of conduits 20. In this example, the expanded conduit sections 15 are located near, but not at, the tube ends. Thus, the conduits are supported and located laterally in the same manner as in FIG. 8, but the inlet face to the reactor differs between the two cases. In particular, since the conduits 20 are expanded at their inlets in FIG. 8 but are not expanded at their inlets in FIG. 9, the ratio of the inlet area of the conduits 20 to the total reactor cross-stream area (defined by the casing 10 size) is greater in FIG. 8 than in FIG. 9. In the example shown in FIG. 9, the conduits are attached to one another at their expanded sections, and conduits adjacent to the casing are attached to the casing at their expanded sections, by for example welding or brazing. Oxidation catalyst 50 is deposited on the exterior surfaces of conduits 20 within the exothermic catalytic reaction channel 60.

[0040] FIG. 10 depicts a reactor configuration of the second type. In this reactor a means for separating the flows 130 is positioned within reactor casing 10 such that the fluid 100 will only enter conduits 20. A second fluid 110 enters the exothermic catalytic channel 60 by at least one aperture 120 defined by housing 10. In the preferred embodiment, a plenum 115 is in fluid communication with the at least one apertures 120. While the plenum 115 can define one or more plenum openings 135, the plenum allows the second fluid 110 to enter the exothermic catalytic channel 60 through multiple apertures 120. Conduits 20 are positioned by retainer 37, shown as a plate with apertures.

[0041] FIG. 11 depicts an end view of the reactor depicted in FIG. 10 except that the retainer 37 has been replaced by a grid 125. The grid is comprised of a plurality of members 125 such as wires or ribbons attached to the housing 10 defining an opening 136 that secures conduits 20 laterally. It is preferred that the conduits 20 not be attached to the members 125 so the conduits 20 will not be fixed axially. Therefore, like the retainer, the conduit outlets will remain positioned relative to each other and the exothermic channel outlets will remain uniformly sized. Both serve as positioners. As an option, at the points of intersection of the members 125, the members can be attached one to the other.

[0042] Comparing the reactor configurations shown in FIGS. 1, 8, and 9, it is clear that in all cases shown a single fuel/air mixture stream enters the casing and is split between the exothermic catalytic reaction channel and the multiple conduits' cooling passages (note, however, that this is not required; separate fuel/air mixture streams may enter separate portions of the reactor, if proper manifolding is provided). The percentage of the initial fuel/air mixture stream which enters the exothermic catalytic reaction channel is approximately determined by the effective flow area of the cooling passages within the cooling conduits versus the effective flow area of the exothermic catalytic reaction channel, since the total pressure drop from reactor inlet to reactor exit is the same across each flow path. While there are many variables which determine the effective area of each flow path, the effective areas are in part determined by the cross-stream area at the entrance to a passage or channel. Thus, for similar size, shape, and length conduits, a greater percentage of the flow will enter the exothermic catalytic reaction channel in the configuration of FIG. 1 (square-packed) than in the configuration of FIG. 8 (close-packed), and a greater percentage of flow will enter the exothermic catalytic reaction channel in the configuration of FIG. 9 (expanded near, but not at, the conduit ends) than in the configuration of FIG. 8 (expanded at the conduit ends).

[0043] As stated above the invention requires that the fluid exiting the exothermic catalytic reaction channel exit and the fluid exiting the conduit outlets must come into contact to permit some degree of mixing to form the ultimate combustion mixture. To accomplish this, the exothermic catalytic reaction channel exit and the conduit outlets must be proximately located. Proximately located means that the exits are spatially located to permit the fluids exiting the exit and the outlets to come in contact so some degree of mixing is possible prior to ultimate combustion. FIGS. 1, 2, 5, 8, 9, and 10 show the closest possible streamwise proximate locations of the exothermic catalytic reaction channel exit and the conduit outlets, occurring essentially at the same streamwise location. FIG. 7 shows a configuration where the conduit outlets are downstream of the exothermic catalytic reaction channel.

[0044] FIGS. 1 through 11 illustrate several strategies for retaining the conduits 20 within casing 10. The invention does not require symmetry in securing the upstream and downstream ends of the conduits and the different securing structures illustrated could be combined in a single embodiment. For example, the conduits 20 could be secured at the upstream end by a retaining structure and at the downstream end by an expanded conduit structure. In addition, it must be realized that the casing and the conduits may operate at different temperatures, resulting in different amounts of thermal expansion. Thus, in the configuration shown in FIG. 2 for example, clearance may be provided between the conduits and the upstream or downstream retainers, to allow for thermal growth of the conduits. In the configuration shown in FIG. 1, the conduits may be secured (by welding, for example) to each other and to the casing only at one end, as for example at the inlet or upstream end, with the other end free to move longitudinally so that differential thermal growth of the conduits may be accommodated. If a clearance is allowed between the conduits and the retainer(s), or if differential thermal growth between adjacent conduits is expected, the conduits' expanded sections (if employed) should be of sufficient axial length that lateral support and positioning of the conduits is provided even when adjacent tubes move in opposite axial directions to the maximum extent allowed by the clearance space or the expected difference in thermal growth. If the conduits penetrate or pass through the retainers, as in FIGS. 5 and 7, respectively, and if they are laterally positioned by the retainers, the expanded sections need not provide lateral support to the conduits. In this case, it may also be advantageous to allow the conduits to slide freely through at least one of the retainers, to allow for thermal expansion of the conduits.

[0045] Conduits 20 can be fabricated from metal, preferably a high-temperature-tolerant alloy suitable for the application, which provides good heat transfer from the oxidation catalyst 50 to the cooling fluid contacting the interior surface of conduits 20. Conduits 20 may have any wall thickness. Generally, thinner walls will be weaker and less resistant to long-term oxidation, while thicker walls will result in increased pressure drop through the reactor. The preferred wall thickness is between 0.05 mm and 2 mm, with wall thicknesses between 0.1 mm and 1 mm being most preferred. If expanded sections are employed minor variations in wall thickness are acceptable. Casing 10 is also fabricated from high-temperature tolerant materials. Wall thickness is based upon the application.

[0046] Oxidation catalyst 50 is applied to the exterior of conduits 20 within the exothermic catalytic reaction channel. While the entire exterior of conduits 20 could be catalyst coated, as a practical matter catalyst coatings should not be applied where the channels touch one another or the casing 10. This allows close fabrication and assembly tolerances, without concern for variable coating thickness, and allows for welding or brazing of metal-to-metal contact points, if desired.

[0047] The reactor can also incorporate streamwise variation of the fluid velocities. Specifically, the velocity of the fluid in the exothermic catalytic reaction channel can be decreased after the fluid enters the channel by streamwise geometric changes in the reactor wherein the channel's entrance flow area is less than the channel's cross-stream flow area at some streamwise location where catalyst 50 is deposited. The channel's entrance flow area is defined as the channel's cross-stream flow area immediately downstream of the most downstream conduit inlet. If the conduit wall thicknesses are approximately constant, streamwise changes in flow velocity can be produced by providing, for example, either contracted sections of the conduits 20, expanded sections of the casing 10, or a combination of both. In a reactor employing expanded-end conduits 20 (or, equivalently, contracted center sections), as in FIGS. 1, 2, or 8, the cross-stream area of conduits 20 decreases just after the cooling flow enters the cooling passages, where the expanded conduit sections taper down to the nominal conduit size in the central portion of the reactor. As a result, the cooling flow velocity is increased to a value greater than its entrance velocity. Conversely, because the casing 10 is of constant cross-sectional size, the cross-stream flow area of the exothermic catalytic reaction channel increases just after the fuel/oxidant mixture enters. As a result, the flow velocity in the exothermic catalytic reaction channel is decreased to a value less than its entrance velocity.

[0048] The gas flow velocity entering the exothermic catalytic reaction channel should exceed the minimum required to prevent flashback into the fuel/oxidant stream upstream of the reactor if the fuel/oxidant mixture entering the exothermic catalytic reaction channel is within the limits of flammability. The laminar flame propagation velocity (velocity of a laminar deflagration wave) is typically less than 1 m/s for hydrocarbon fuels in air, but the turbulent flame propagation velocity may exceed 10 m/s and may approach 30 m/s for highly turbulent flow. To prevent flashback, the gas flow velocity should exceed 10 to 30 m/s at gas turbine engine conditions, or more if a safety margin is allowed. Because catalyst light-off becomes increasingly difficult with increasing velocity, it is desirable to reduce the velocity of the fuel/air stream once it has entered the exothermic catalytic reaction channel, by for example a streamwise variation of cross-stream area as discussed above. In the preferred embodiment of the present invention, the flow velocity of the fuel/air stream over the exothermic reaction surface (oxidation catalyst) in the exothermic catalytic reaction channel is nominally 30 m/s or less. This reduction in velocity is achieved by a streamwise increase in the cross-stream area for flow over the exothermic reaction surface. Streamwise changes in cross-stream area are fixed by the geometry of the reactor, and do not change in time.

[0049] The velocity of the cooling stream should exceed the maximum flame propagation velocity (nominally 10 to 30 m/s or more) at the exit of the cooling conduits, if the cooling fluid exiting the cooling passages is within the limits of flammability, to prevent flashback from a downstream combustion chamber. If expanded conduit outlets are employed, it is also very important that the downstream increase in cross-stream area of the cooling conduits 20 is sufficiently gradual that recirculation of the cooling flow does not occur, so that there is no possibility of flashback or flameholding in the downstream expanded conduit section. Typically the cone angle for an axi-symmetric diffuser section should not exceed approximately 8 to 10 degrees for good pressure recovery and minimal recirculation. If continued backside cooling is a consideration, the angle should be especially shallow (less than 4 or 5 degrees for an axi-symmetric section) to ensure that there is no local separation of the cooling flow and concurrent loss of cooling effectiveness.

[0050] Also, when the fuel/air ratio in the cooling channels is within the limits of flammability, it is preferred that the cross-stream area for flow through the cooling channels is not increased after the cooling stream enters conduits 20. The cross-stream area of the cooling passages may in fact be decreased to increase the cooling flow velocity for greater resistance to flashback or pre-ignition in the cooling portion of the reactor. The minimum residence time for pre-ignition to occur in conduits 20 is dependent upon fuel type, fuel/air ratio, temperature, and pressure, and can be measured experimentally or calculated on the basis of elementary chemical reaction rates, if known. Gas temperatures in the cooling portion of the reactor may rise to near the material limit of the catalyst and substrate (near 1200 Kelvin for precious metal catalysts), resulting in very short ignition delay times, possibly as short as 2 ms for natural gas in air at pressures near 10 atm. To prevent pre-ignition in the cooling portion of the reactor, the gas residence time in the cooling portion of the reactor should be less than the ignition delay time. Increasing the cooling flow velocity within the cooling passages reduces the residence time of the cooling fluid within the reactor, and reduces the cooling fluid's propensity for pre-ignition. Similarly, decreasing the velocity of the fluid in the exothermic catalytic reaction channel provides increased residence time for reaction in a given length reactor, while the cooling fluid's residence time within the same length reactor remains at a smaller value, allowing a reduced propensity for pre-ignition of the cooling fluid.

[0051] Regardless of the specific catalytic firebox reactor configuration, the reactor should be capable of providing good contact between the oxidation catalyst and the fuel/oxidant mixture in the exothermic catalytic reaction channel. For catalytic combustion applications, it is preferred that the reactor be sized such that the reaction of the fuel/oxidant mixture in the exothermic catalytic reaction channel should proceed more than 50% of the way to completion before exiting. This means that more than 50% of the limiting reactor fuel in the fuel-lean case and oxidant in the fuel-rich case entering the channel should be consumed. Most preferably, more than 75% entering the exothermic catalytic reaction channel should burn before exiting.

[0052] Both of these catalytic fire box reactors can operate fuel-lean or fuel-rich. Fuel lean is defined as having a stoichiometry less than 1.0, while fuel rich is defined as having a stoichiometry greater than or equal to 1.0. In operation, the uniformity of the size and spacing of the exits from the catalytic channel allows more uniform mixing of the catalyzed flow with the fluid exiting the conduits. This is especially important in fuel-rich operations.. Thus, the positioning of the conduit exits with respect to the plurality of exits from the catalytic channel should be fixed in a uniform pattern.

[0053] The percentage of reaction completed in the exothermic catalytic reaction channel depends both upon the flow rate of the fuel/oxidant mixture through the exothermic catalytic reaction channel and upon the physical characteristics of the catalytic firebox reactor. The chemical composition of the fuel/oxidant mixture may also affect the percentage of reaction completed, particularly if the rate of chemical reaction is significantly limiting when compared to the rate of mass transfer to the catalyst surface.

[0054] With regard to percentage of reaction completed, important physical characteristics within the exothermic catalytic reaction channel include the rate of mass transfer to the oxidation catalyst surface, the ratio of oxidation catalyst surface area to reaction channel volume, and the activity of the oxidation catalyst.

[0055] In a square-packed conduit configuration (parallel conduits bundled such that the conduit centerlines are arranged on an imaginary square grid), as shown in FIG. 5, the conduits are preferably between 2 mm and 8 mm in diameter, and between 75 mm and 400 mm in length, for a catalytic combustion application in which the average velocity of the fuel/air mixture entering the reactor is between 20 m/s and 100 m/s. A close-packed reactor would have conduits with dimensions in approximately the same ranges as those for the square-packed reactor.

[0056] The fuel may comprise C1 to C20 hydrocarbons, C1 to C20 hydrocarbon oxygenates, and blends thereof. Suitable gaseous fuels include natural gas, methane, and propane. Suitable liquid fuels include gasoline, kerosene, No. 1 heating oil, No. 2 heating oil, and conventional aviation turbine fuels such as Jet A, Jet B, JP-4, JP-5, JP-7, and JP-8. “Hydrocarbon” not only refers to organic compounds, including conventional liquid and gaseous fuels, but also to gas streams containing fuel values in the form of compounds such as carbon monoxide, organic compounds, or partial oxidation products of carbon containing compounds. If the fuel is a liquid, it should be vaporized or atomized before mixing with oxidant or while being mixed with oxidant.

[0057] The exothermic catalytic portion of the catalytic firebox reactor may have as an active ingredient precious metals, group VIII noble metals, base metals, metal oxides, or any combination thereof. Elements such as zirconium, vanadium, chromium, manganese, copper, platinum, palladium, osmium, iridium, rhodium, ruthenium, cerium, cobalt, nickel, iron, and the like may be used. Platinum and palladium are preferred, palladium being especially preferred for use with natural gas or methane fuels. The oxidation catalyst may be applied directly to the substrate of the reactor, or may be applied to an intermediate bond coat or washcoat composed of alumina, silica, zirconia, titania, magnesia, other refractory metal oxides, or any combination thereof. The washcoat may be stabilized by the addition of additives such as lanthanum, cerium, barium, chromium, or other materials. Alumina washcoats are preferred for use with natural gas or methane fuels.

[0058] The catalyst-coated substrate may be fabricated from any of various high temperature materials. High temperature metal alloys are preferred, particularly alloys composed of iron, nickel, and/or cobalt, in combination with aluminum, chromium, and/or other alloying materials. High temperature nickel alloys are especially preferred. Other materials which may be used include ceramics, metal oxides, intermetallic materials, carbides, and nitrides. Metallic substrates are most preferred due to their excellent thermal conductivity, allowing effective backside cooling of the catalyst.

Claims

1. A catalytic reactor comprising: a casing having an inlet and an outlet, and an interior surface and an exterior surface, the casing interior surface defining an interior chamber: at least two conduits, each conduit having an inlet and an outlet, and an interior surface and exterior surface, the conduit exterior surfaces and the casing interior surface forming an exothermic catalytic reaction channel having an exit, the exothermic catalytic reaction channel exit and the conduit outlets proximately located and laterally spaced by a positioner; and an oxidation catalyst deposited within the exothermic catalytic reaction channel on at least a portion of at least one of the conduit exterior surfaces.

2. The catalytic reactor of claim 1 wherein the positioner is a grid.

3. The reactor of claim 1 wherein the positioner is a honeycomb.

4. The method of supporting and positioning conduits within a catalytic reactor wherein a fuel and air mixture having a stoichometry equal to or greater than 1.0 is oxidized in the presence of the catalyst comprising: providing a catalytic reactor comprising conduits and an exothermic catalytic reaction channel, each conduit having an outlet; and positioning the conduit exits with respect to a plurality of exits from the exothermic catalytic channel in a fixed lateral relationship.

5. The method of claim 2 wherein the plurality of exits are uniformly spaced.

6. The method of supporting and positioning conduits within a catalytic reactor wherein a fuel and air mixture having a stoichometry greater than 1.0 is oxidized in the presence of the catalyst comprising: providing a catalytic reactor comprising conduits and an exothermic catalytic reaction channel, each conduit having an outlet; and positioning the conduit exits with respect to a plurality of exits from the exothermic catalytic channel in a fixed lateral relationship.

7. A catalytic reactor comprising: a casing having an inlet and an outlet, and an interior surface and an exterior surface, the casing interior surface defining an interior chamber: at least two conduits, each conduit having an inlet and an outlet, and an interior surface and exterior surface, the conduit exterior surfaces and the casing interior surface forming an exothermic catalytic reaction channel having an exit, the exothermic catalytic reaction channel exit and the conduit outlets proximately located and laterally spaced by a positioner; separated inlets to the conduits and to the exothermic reactor channel; and an oxidation catalyst deposited within the exothermic catalytic reaction channel on at least a portion of at least one of the conduit exterior surfaces.

8. The catalytic reactor of claim 7 further comprising a plenum in fluid communication with the exothermic catalytic reaction channel.

9. A catalytic reactor comprising: a casing having an inlet and an outlet, and an interior surface and an exterior surface, the casing interior surface defining an interior chamber; at least two conduits, each conduit having an inlet and an outlet, and an interior surface and exterior surface, the conduit exterior surfaces and the casing interior surface forming an exothermic catalytic reaction channel having an exit, the exothermic catalytic reaction channel exit and the conduit outlets proximately located and positioned by a retainer; separated inlets to the conduits and to the exothermic reaction channel; and an oxidation catalyst deposited within the exothermic catalytic reaction channel on at least a portion of at least one of the conduit exterior surfaces.

10. The catalytic reactor of claim 9 further comprising a plenum in fluid communication with the exothermic catalytic reaction channel.

11. The catalytic reactor of claim 9 wherein the retainer defines a plurality of passages, the passages being uniformly spaced.

12. The catalytic reactor of claim 11 further comprising a plenum in fluid communication with the exothermic catalytic reaction channel.