Sublimation reagent cartridge and reactor device

Abstract

A reagent cartridge (1000) and a reactor device for sublimating a solid reagent (1001) are disclosed. The reagent cartridge (1000) includes a reagent chamber (1200) for holding the solid reagent (1001) and at least one pressure sensor (1100) for measuring the pressure inside the reagent cartridge (1000).

Description

Technical Field

[0001] The present disclosure relates to chemical reactors and components thereof. In particular, the present disclosure relates to the sublimation of solid reagents to form reagent gases used in chemical reactors, such as flow reactors.

Background Art

[0002] In a flow reactor configured for floating-catalyst chemical vapor deposition (FCCVD) of carbon-based high-aspect-ratio molecular structures (HARMS), such as carbon nanotubes, e.g., single-walled carbon nanotubes and / or multi-walled carbon nanotubes; carbon nanobuds; and / or graphene nanoribbons, ferrocene is commonly used as a precursor for the in-situ formation of iron-containing catalyst nanoparticles that promote the formation of HARMS.

[0003] Generally, precise control of reagent concentration during a chemical reaction is of utmost importance. For example, in the case of FCCVD of carbon-based HARMS, the mass flow rate of ferrocene gas formed by sublimation of solid ferrocene must be accurately controlled to form catalyst nanoparticles having a precise target property range. Various solutions have been devised to control the sublimation of solid reagents, but due to certain factors such as non-uniform heating of the solid reagent and the formation of blockages due to condensation or deposition in the reactor, variations may occur in the reagent outflow rate from the reagent cartridge used for reagent sublimation.

[0004] In view of the above, it may be desirable to develop new solutions related to the control of sublimation of solid reagents.

Summary of the Invention

[0005] This summary is provided to introduce, in simplified form, a selection of concepts that are further described below in the detailed description. This summary is not intended to identify key features or essential features of the claimed subject matter, nor is it intended to be used to limit the scope of the claimed subject matter.

[0006] According to a first aspect, there is provided a reagent cartridge for sublimating a solid reagent to form a reagent gas and mixing the reagent gas with a flowing carrier gas to form a reagent carrier gas mixture. The reagent cartridge comprises a reagent chamber for holding the solid reagent and at least one pressure sensor for measuring the pressure within the reagent cartridge.

[0007] In an embodiment of the first aspect, the reagent cartridge is according to the third aspect or any embodiment thereof.

[0008] According to a second aspect, there is provided a reactor device comprising a reagent cartridge holder configured to hold a reagent cartridge according to the first aspect during operation of the reactor device. The reactor device is configured to receive from at least one pressure sensor of the reagent cartridge at least one cartridge pressure reading indicative of the pressure within the reagent cartridge.

[0009] In an embodiment of the second aspect, the reagent cartridge is according to the fourth aspect or any embodiment thereof.

[0010] According to a third aspect, there is provided a reagent cartridge for sublimating a solid reagent to form a reagent gas and mixing the reagent gas with a flowing carrier gas to form a reagent carrier gas mixture. The reagent cartridge comprises a reagent chamber for holding the solid reagent, a gas injection chamber upstream from the reagent chamber for injecting carrier gas into the reagent cartridge, a first temperature sensor configured to measure the temperature within the reagent chamber, and a second temperature sensor configured to measure the temperature within the gas injection chamber.

[0011] In an embodiment of the third aspect, the reagent cartridge follows the first aspect or any of its embodiments.

[0012] According to a fourth aspect, there is provided a reactor device comprising a reagent cartridge holder configured to hold a reagent cartridge according to the third aspect during operation of the reactor device. The reactor device is configured to receive a first temperature reading indicating the temperature within the reagent cartridge from a first temperature sensor and a second temperature reading indicating the temperature within the gas injection chamber from a second temperature sensor.

[0013] In an embodiment of the fourth aspect, the reagent cartridge follows the second aspect or any of its embodiments.

Brief Description of the Drawings

[0014] The present disclosure will be better understood from the following detailed description read in conjunction with the accompanying drawings.

[0015]

Figure 1

Figure 2

Figure 3

[0016] Unless otherwise specified, any of the foregoing drawings may not be drawn to scale, such that any element in the drawing may be drawn at an inaccurate ratio relative to other elements in the drawing to emphasize a particular structural aspect of the embodiment of the drawing.

[0017] Furthermore, corresponding elements in the embodiments of any two of the foregoing drawings may be disproportionate to each other in the two drawings to emphasize a particular structural aspect of the embodiments of the two drawings.

Modes for Carrying Out the Invention

[0018] Regarding the reagent cartridge and reactor device discussed in this detailed description, please note the following.

[0019] Throughout this specification, "high aspect ratio molecular structure" or "HARMS" may refer to a nanostructure, i.e., a structure having one or more characteristic dimensions on the nanoscale, e.g., 0.1 nanometer (nm) or more and about 100 nm or less. Additionally or alternatively, HARMS may refer to a structure having two perpendicular dimensions with significantly different orders of magnitude. For example, HARMS may have a length that is tens or hundreds of times its thickness and / or width. Examples of HARMS include nanotubes, e.g., carbon nanotubes and boron nitride nanotubes; nanoribbons, e.g., graphene nanoribbons, graphite nanoribbons, and boron nitride nanoribbons; nanowires, e.g., tungsten nanowires, copper nanowires, aluminum nanowires, nickel nanowires, and silver nanowires; nanofibers, e.g., carbon nanofibers and silicon carbide nanofibers; and nanoplatelets, e.g., graphene nanoplatelets, borophene nanoplatelets, and boron nitride nanoplatelets.

[0020] Furthermore, "carbon-based" HARMS may refer to HARMS mainly composed of carbon (C). Additionally or alternatively, carbon-based HARMS may refer to HARMS containing at least 50 atomic percent (at.%), or at least 60 at.%, or at least 70 at.%, or at least 80 at.%, or at least 90 at.%, or at least 95 at.% carbon. Generally, carbon-based HARMS may be doped with non-carbon dopants, e.g., to change their electrical and / or thermal properties. Examples of carbon-based HARMS include carbon nanotubes, carbon nanobuds, graphene nanoribbons, carbon nanofibers, graphene nanoplatelets, and combinations thereof.

[0021] In the present disclosure, the "high aspect ratio molecular structure network" or "HARMS network" may refer to a plurality of HARMs interconnected with each other. Generally, the HARMS network may form a solid and / or monolithic material on a macroscopic scale, and the individual HARMs are non-directional, that is, they are substantially randomly oriented, or randomly oriented, or oriented. Typically, the HARMS network may be arranged in various macroscopic forms, such as as a film, which may or may not be optically transparent, and / or may have high electrical conductivity.

[0022] FIG. 1 shows a schematic cross-sectional view of a reagent cartridge 1000 for sublimating a solid reagent 1001 to form a reagent gas 1002 and mixing the reagent gas 1002 with a flowing carrier gas 1003 to form a reagent carrier gas mixture 1004 according to one embodiment.

[0023] The reagent cartridge 1000 of the embodiment of FIG. 1 complies with both the first aspect and the third aspect. In other embodiments, the reagent cartridge may comply with the first aspect and / or the third aspect.

[0024] The reagent cartridge 1000 of the embodiment of FIG. 1 is configured for sublimation of the solid reagent 1001. In other embodiments according to the first aspect and / or the third aspect, the reagent cartridge for sublimation of the solid reagent may be suitable or configured for sublimation of the solid reagent.

[0025] In the embodiment of FIG. 1, the reagent cartridge 1000 includes a reagent chamber 1200 for holding a solid reagent 1001 and at least one pressure sensor 1100 for measuring the pressure within the reagent cartridge 1000. Generally, a reagent cartridge having at least one pressure sensor for measuring the pressure within the reagent cartridge may facilitate maintaining the pressure in the vicinity of the solid reagent held within the reagent cartridge within a predefined pressure range and may enable limiting variations in the reagent output mass flow rate from the reagent cartridge. Additionally or alternatively, a reagent cartridge having at least one pressure sensor for measuring the pressure within the reagent cartridge may enable compensating for the influence of changes in reactor pressure on the pressure within the reagent cartridge. Additionally or alternatively, a reagent cartridge having at least one pressure sensor for measuring the pressure within the reagent cartridge may enable detecting the formation of an obstruction downstream from the reagent cartridge. In other embodiments according to a third aspect, the reagent cartridge may or may not include at least one pressure sensor for measuring the pressure within the reagent cartridge.

[0026] In the embodiment of FIG. 1, the at least one pressure sensor 1100 includes a first pressure sensor 1110 configured to measure the pressure within the reagent chamber 1200. Generally, at least one pressure sensor of a reagent cartridge having a first pressure sensor configured to measure the pressure within a reagent chamber for holding a solid reagent can enhance the accuracy or fidelity of the pressure reading interpreted as being related to the pressure in the vicinity of the solid reagent. In other embodiments according to the first aspect and / or the third aspect, the at least one pressure sensor of the reagent cartridge may or may not include a first pressure sensor configured to measure the pressure within the reagent chamber of the reagent cartridge.

[0027] The reagent cartridge 1000 includes a gas discharge chamber 1400 downstream from the reagent chamber 1200 for discharging the reagent carrier gas mixture 1004 from the reagent cartridge 1000, and at least one pressure sensor 1100 includes a second pressure sensor 1120 configured to measure the pressure within the gas discharge chamber 1400. Generally, at least one pressure sensor of a reagent cartridge that includes a second pressure sensor configured to measure the pressure within a gas discharge chamber for discharging a reagent carrier gas mixture from the reagent cartridge may be capable of enhancing the effectiveness of a blockage formation detection algorithm based on detecting an increase in at least one cartridge pressure reading indicative of the pressure within the reagent cartridge. In other embodiments according to the first and / or third aspects, at least one pressure sensor of the reagent cartridge may or may not include a second pressure sensor configured to measure the pressure within a gas discharge chamber for discharging a reagent carrier gas mixture from the reagent cartridge.

[0028] In the embodiment of FIG. 1, the reagent cartridge 1000 includes, in addition to a reagent chamber 1200 for holding a solid reagent 1001, a gas injection chamber 1300 upstream from the reagent chamber 1200 for injecting a carrier gas 1003 into the reagent cartridge 1000, a first temperature sensor 1510 configured to measure the temperature within the reagent chamber 1200, and a second temperature sensor 1520 configured to measure the temperature within the gas injection chamber 1300.

[0029] Generally, a reagent cartridge comprising a first temperature sensor configured to measure the temperature within a reagent chamber and a second temperature sensor configured to measure the temperature within a gas injection chamber may be capable of more accurately maintaining a solid reagent at a predetermined solid reagent temperature across the extent of the reagent chamber. Additionally or alternatively, if the reagent cartridge comprises at least one pressure sensor for measuring the pressure within the reagent cartridge, a reagent cartridge comprising a first temperature sensor configured to measure the temperature within a reagent chamber and a second temperature sensor configured to measure the temperature within a gas injection chamber may be capable of more accurately controlling the thermodynamic state of the solid reagent across the extent of the reagent chamber, and may be capable of forming a reagent carrier gas mixture having more clearly defined characteristics, and / or may be capable of more accurately adjusting the carrier gas mass flow rate in order to maintain a predetermined reagent output mass flow rate.

[0030] In other embodiments according to the first aspect, the reagent cartridge may or may not comprise a gas injection chamber upstream from a reagent chamber for injecting carrier gas into the reagent cartridge, a first temperature sensor configured to measure the temperature within the reagent chamber, and / or a second temperature sensor configured to measure the temperature within the gas injection chamber.

[0031] The reagent cartridge 1000 of the embodiment of FIG. 3 further comprises a third temperature sensor 1530 configured to measure the temperature within the gas discharge chamber 1400. In other embodiments according to the first aspect and / or the third aspect, the reagent cartridge may or may not comprise such a third temperature sensor.

[0032] In the embodiment of FIG. 1, each of the first temperature sensor 1510, the second temperature sensor 1520, and the third temperature sensor 1530 includes a resistance thermometer element, specifically a platinum resistance thermometer (PRT) element such as a Pt100 resistance thermometer element, and each of the first temperature sensor 1510, the second temperature sensor 1520, and the third temperature sensor 1530 is configured for a three-wire or four-wire electrical output connection in accordance with the IEC 60751:2008 standard. In other embodiments according to the first aspect and / or the third aspect, one or more of the first temperature sensor, the second temperature sensor, and the third temperature sensor may or may not include one or more PRTs, such as one or more Pt100 resistance thermometer elements or one or more Pt1000 resistance thermometer elements. In other embodiments according to the first aspect and / or the third aspect, at least one of the first temperature sensor, the second temperature sensor, and the third temperature sensor includes a PRT element, and at least a part of the at least one sensor may or may not be configured for a three-wire or four-wire electrical output connection in accordance with the IEC 60751:2008 standard.

[0033] In the embodiment of FIG. 1, at least one pressure sensor 1100 further includes a third pressure sensor 1130 configured to measure the pressure within the gas injection chamber 1300. In other embodiments according to the first aspect and / or the third aspect, at least one pressure sensor of the reagent cartridge may or may not include such a third pressure sensor.

[0034] Each of the at least one pressure sensor 1100, namely the first pressure sensor 1110, the second pressure sensor 1120, and the third pressure sensor 1130, includes a flush-mounted diaphragm. In other embodiments according to the first aspect and / or the third aspect, one or more of the at least one pressure sensor, for example, each, may include a flush-mounted diaphragm.

[0035] In the embodiment of FIG. 1, the reagent chamber 1200 contains solid ferrocene (Fe(C5H2)2). In other embodiments according to the first aspect and / or the third aspect, the reagent chamber of the reagent cartridge may or may not be provided with any suitable sublimable solid reagent such as solid ferrocene (Fe(C5H2)2).

[0036] In the embodiment of FIG. 1, the reagent chamber 1200 and the gas injection chamber 1300 are separated from each other by a sintered filter 1210, i.e., a porous disk formed of stainless steel configured to block the passage of fine particles. On the other hand, the reagent chamber 1200 and the gas discharge chamber 1400 are separated from each other by a perforated wall, particularly a stainless steel mesh screen 1220. In other embodiments according to the first aspect and / or the third aspect, the reagent chamber may be separated from the gas injection chamber and / or the gas discharge chamber in any suitable manner, for example, by a filter, such as a sintered filter, and / or a perforated wall, such as a mesh screen. In such other embodiments, any such separation structure may be formed of any suitable material(s), such as stainless steel and / or titanium.

[0037] The reagent chamber 1200 of the embodiment of FIG. 1 has a width (W rc ) of the reagent chamber of about 5 centimeters (cm) as measured perpendicular to the flow direction 1005 of the carrier gas in the reagent chamber 1200. In other embodiments according to the first aspect and / or the third aspect, the reagent chamber has a width of any suitable reagent chamber as measured perpendicular to the flow direction of the carrier gas in the reagent chamber, for example, a width of 1 cm or more, 2 cm or more, 3 cm or more, 4 cm or more, and / or 20 cm or less, 15 cm or less, 10 cm or less, 7 cm or less.

[0038] The reagent chamber 1200 of the embodiment of FIG. 1 has a length (L rc) It has. In other embodiments according to the first aspect and / or the third aspect, the reagent chamber is measured parallel to the flow direction of the carrier gas in the reagent chamber, and the length of any suitable reagent chamber, for example, 3 cm or more, 5 cm or more, 8 cm or more, 10 cm or more, 12 cm or more, and / or 50 cm or less, 40 cm or less, 30 cm or less, 25 cm or less, 20 cm or less.

[0039] In the embodiment of FIG. 1, the reagent cartridge 1000 is configured to pass the carrier gas 1003 through the reagent chamber 1200 to cause fluidization of the particulate material disposed within the reagent chamber 1200. Generally, a reagent cartridge configured to pass a carrier gas through a reagent chamber to cause fluidization of the particulate material disposed within the reagent chamber can facilitate reducing local temperature differences within the reagent chamber. In other embodiments according to the first aspect and / or the third aspect, the reagent cartridge may or may not be configured in such a manner.

[0040] The reagent cartridge 1000 of the embodiment of FIG. 1 includes a carrier gas inlet 1310 for supplying the carrier gas 1003 to the reagent cartridge 1000 and a reagent carrier gas mixture outlet 1410 for discharging the reagent carrier gas mixture 1004 from the reagent cartridge 1000. In other embodiments according to the first aspect and / or the third aspect, the reagent cartridge may include any suitable type(s) of carrier gas inlet(s) and reagent carrier gas mixture outlet(s).

[0041] It should be understood that the embodiments of the first aspect and / or the third aspect described above may be used in combination with each other. Some embodiments may be combined together to form further embodiments of the first aspect and / or the third aspect.

[0042] In the above, the features of the reagent cartridge have been mainly described. In the following, emphasis will be placed on the features of the reactor device. What has been described above regarding the implementation method, definition, details, and advantages of the reagent cartridge is applicable to the reactor device described below with necessary modifications. The reverse is also equally applicable.

[0043] FIG. 2 schematically shows a reactor device 2000 according to an embodiment.

[0044] The reactor device 2000 of the embodiment of FIG. 2 complies with both the second aspect and the fourth aspect. In other embodiments, the reactor device may comply with the second aspect and / or the fourth aspect.

[0045] In the embodiment of FIG. 2, the reactor device 2000 includes a reagent cartridge holder 2100 configured to hold a reagent cartridge 2200 according to the first aspect and the third aspect during the operation of the reactor device 2000. The reactor device 2000 further includes a reagent cartridge 2200 according to the first aspect and the third aspect held by the reagent cartridge holder 2100. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may include a reagent cartridge holder configured to hold or be configured to hold a reagent cartridge according to the first aspect and / or the third aspect during the operation of the reactor device. In such embodiments, the reactor device may or may not include the reagent cartridge.

[0046] The reagent cartridge 2200 of the embodiment of FIG. 2 may be the same as the reagent cartridge 1000 of the embodiment of FIG. 1. In other embodiments according to the second aspect and / or the fourth aspect, any suitable reagent cartridge, for example, a reagent cartridge different from, similar to, or the same as the reagent cartridge 1000 of the embodiment of FIG. 1 can be used.

[0047] The reactor device 2000 of the embodiment of FIG. 2 is configured to receive at least one cartridge pressure reading value 2310 indicating the pressure within the reagent cartridge 2200 from at least one pressure sensor 1100 of the reagent cartridge 2200. In other embodiments according to the fourth aspect, the reactor device may or may not be configured to receive at least one cartridge pressure reading value indicating the pressure within the reagent cartridge from at least one pressure sensor of the reagent cartridge.

[0048] In the embodiment of FIG. 2, the reactor device 2000 is configured to produce carbon-based HARMS, particularly carbon nanobuds, by floating catalyst chemical vapor deposition (FCCVD). In other embodiments according to the second and / or fourth aspects, the reactor device may or may not be configured to produce carbon-based HARMS such as carbon nanotubes, e.g., single-walled carbon nanotubes and / or multi-walled carbon nanotubes; carbon nanobuds; and / or graphene nanoribbons, e.g., by FCCVD.

[0049] Even if not explicitly shown in FIG. 2, the reactor device 2000 of the embodiment of FIG. 2 can include any features and / or elements necessary or beneficial for producing carbon-based HARMS, e.g., a carbon source reservoir where one or more heaters and / or pressure sensors may be provided; a carbon source conduit where one or more heaters and / or one or more flow controllers may be provided.

[0050] The reactor device 2000 of the embodiment of FIG. 2 may be implemented as a continuous flow reactor device. In other embodiments according to the second and / or fourth aspects, the reactor device may or may not be implemented as a continuous flow reactor device. For example, in some such embodiments, the reactor device may be implemented as a batch reactor device.

[0051] In the embodiment of FIG. 2, the reactor apparatus 2000 comprises a flow reactor 2900. In other embodiments according to the second and / or fourth aspects, the reactor apparatus may comprise any suitable type(s) of reactor(s), for example, one or more flow reactors.

[0052] As used herein, a "flow reactor" may refer to a chemical reactor into which one or more reagents, such as one or more catalyst particle precursors and / or one or more reactants, such as a carbon source, and / or one or more auxiliary substances, such as a catalyst and / or a growth promoter, such as sulfur (S); phosphorus (P); nitrogen (N); one or more sulfur-containing compounds, such as hydrogen sulfide (H2S), carbon disulfide (CS2), and / or thiophene (C4H4S); one or more phosphorus-containing compounds, such as phosphine (PH3); one or more nitrogen-containing compounds, such as ammonia (NH3) and / or nitric oxide (NO); and / or an oxidizing or reducing agent, such as oxygen (O2), water (H2O), carbon dioxide (CO2), and / or hydrogen (H2) are introduced, for example, continuously, and from which one or more products are recovered, for example, continuously. Additionally or alternatively, a flow reactor may refer to a reactor through which one or more reagents pass and in which a catalytic reaction proceeds. Typically, a flow reactor may be formed from any suitable material(s), such as stainless steel, fused silica, or fused quartz.

[0053] In the embodiment of FIG. 2, the reactor device 2000 includes a carrier gas conduit 2800 for providing a flow of carrier gas through the reagent cartridge 2200, and a reagent gas conduit 2700 for directing a reagent carrier gas mixture formed within the reagent cartridge 2200 to the flow reactor 2900. In other embodiments according to the second aspect and / or the fourth aspect, the flow of carrier gas may be provided through the reagent cartridge by any suitable means, e.g., via a carrier gas conduit, and the reagent carrier gas mixture formed within the reagent cartridge may be directed by any suitable means, e.g., via a reagent gas conduit, to any suitable destination, e.g., a chemical reactor.

[0054] The reagent cartridge 2200 in the embodiment of FIG. 2 is configured to form a reagent carrier gas mixture containing ferrocene (Fe(C5H2)2) gas as the reagent gas and nitrogen (N2) gas as the carrier gas. In other embodiments according to the second aspect and / or the fourth aspect, any suitable reagent gas(es), e.g., one or more catalyst particle precursors (e.g., iron-containing organometallic or metal-organic compounds such as ferrocene (Fe(C5H2)2), iron pentacarbonyl (Fe(CO)5), and / or iron(II) phthalocyanine (C 32 H 16 FeN8); and / or one or more nickel-containing organometallic or metal-organic compounds such as nickelocene (Ni(C5H5)2); and / or one or more cobalt-containing organometallic or metal-organic compounds such as cobaltocene (Co(C5H5)2)), and carrier gas(es), e.g., argon (Ar), helium (He), nitrogen (N2), carbon monoxide (CO), and / or hydrogen (H2) can be used.

[0055] In the embodiment of FIG. 2, the reactor device 2000 is configured to decompose the reagent gas to form catalyst particles, particularly iron-containing nanoparticles. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not be configured in such a manner.

[0056] Throughout this specification, the "catalyst particles" may refer to a part of a particulate material suitable for increasing the reaction rate through catalysis. Additionally or alternatively, the catalyst particles may refer to particles suitable for heterogeneous catalysis. Additionally or alternatively, the catalyst particles may refer to a part of a particulate catalyst material suitable for the catalysis in the production of carbon-based HARMS, for example, by chemical vapor deposition, such as floating catalyst chemical vapor deposition (FCCVD). Generally, the catalyst particles may contain, consist essentially of, or consist of one or more transition metals such as iron (Fe), cobalt (Co), and / or nickel (Ni). Typically, the catalyst particles may have a diameter in any suitable range, for example, in the range of 0.1 nm to 300 nm, or 1 nm to 200 nm, or 5 nm to 100 nm, or 10 nm to 50 nm.

[0057] In the embodiment of FIG. 2, the reactor device 2000 is configured to adjust the carrier gas mass flow rate based on at least a part of at least one cartridge pressure reading value 2310 in order to maintain a predetermined reagent output mass flow rate from the reagent cartridge 2200.

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[0058] ​ The reactor device "configured to" execute a process may refer to the ability and suitability of the reactor device for such a process. This can be achieved in various ways. For example, the reactor device or its control unit can include at least one processor and at least one memory coupled to the at least one processor, and the memory stores program code instructions that cause the processor to execute the process(es) in question when executed on the at least one processor. Additionally or alternatively, any functionally described feature of the reactor device may be executed, at least in part, by one or more hardware logic components. For example, without limitation, suitable types of hardware logic components include field-programmable gate arrays (FPGAs), application-specific integrated circuits (ASICs), application-specific standard products (ASSPs), system-on-a-chip systems (SOCs), complex programmable logic devices (CPLDs), and the like. The reactor device can generally be operated by any suitable circuit and / or signal known in the art according to any suitable principle.

[0059] In the embodiment of FIG. 2, the reagent cartridge 2200 contains solid ferrocene as a solid reagent, and an increase in pressure decreases the sublimation rate of ferrocene. As a result, the reactor device 2000 of the embodiment of FIG. 2 increases in response to an increase in pressure within the reagent cartridge 2200

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[0060] The reactor device 2000 of the embodiment of FIG. 2 is specifically based on a first pressure reading 2311 indicating the pressure within the reagent chamber 1200 of the reagent cartridge 2200.

Number

[0061] In other embodiments according to the second and / or fourth aspects, the reactor device is configured to adjust the carrier gas mass flow rate based on at least a portion of at least one cartridge pressure reading to maintain a predetermined reagent output mass flow rate from the reagent cartridge, and the reactor device may be configured to adjust the carrier gas mass flow rate based on any one or more of at least one cartridge pressure reading, for example, at least a first pressure reading indicating the pressure within the reagent chamber of the reagent cartridge.

[0062] In the embodiment of FIG. 2, the reactor device 2000 is also configured to detect the formation of an obstruction 2001 downstream from the reagent cartridge 2200 based on at least a portion of at least one cartridge pressure reading 2310. Such an obstruction may typically be formed downstream from the reagent cartridge due to condensation or deposition of the reagent gas, which may result, for example, from insufficient heating of the reagent gas conduit used to direct the reagent carrier gas mixture from the reagent cartridge towards the reactor of the reactor device. The formation of the obstruction may generally be detected based on a relatively rapid increase in at least a portion of at least one cartridge pressure reading. Generally, a reactor device configured to detect the formation of an obstruction downstream from the reagent cartridge based on at least a portion of at least one cartridge pressure reading can facilitate the maintenance of the reactor device. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not be configured to detect the formation of an obstruction downstream from the reagent cartridge based on at least a portion of at least one cartridge pressure reading.

[0063] Specifically, the reactor device 2000 of the embodiment of FIG. 2 is configured to detect the formation of the obstruction 2001 based on a second pressure reading 2312 indicating the pressure within the gas discharge chamber of the reagent cartridge 2200. Generally, a reactor device configured to detect the formation of an obstruction based on at least a second pressure reading indicating the pressure within the gas discharge chamber of the reagent cartridge can increase the accuracy or veracity of such detection, for example, by reducing the probability of false positive detection results. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device is configured to detect the formation of an obstruction downstream from the reagent cartridge based on at least a portion of at least one cartridge pressure reading, and the reactor device may or may not be configured to detect the formation of the obstruction based on at least a second pressure reading indicating the pressure within the gas discharge chamber of the reagent cartridge.

[0064] The reactor device 2000 includes a reagent conduit mass flow meter 2720 for measuring the mass flow through the reagent gas conduit 2700,

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[0065] As used herein, "control unit" may refer to a device, such as an electronic device, having at least one specific function related to determining and / or influencing operating conditions, status, or parameters related to another device, unit, or element. The control unit may or may not form part of a multi-functional control system.

[0066] Furthermore, a control unit that is "operably coupled" to a device, unit, or element may refer to a control unit having at least one specific function related to the determination and / or influence of operating conditions, status, or parameters associated with the device, unit, or element.

[0067] In the embodiment of FIG. 2, the reactor device 2000 may be further configured to compensate for changes in pressure within the flow reactor 2900 in order to stabilize the pressure within the reagent cartridge 2200. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not be configured in such a manner.

[0068] In the embodiment of FIG. 2, the reactor device 2000 is further configured to receive a first temperature reading 2410 indicating the temperature within the reagent chamber 1200 from a first temperature sensor of the reagent cartridge 2200 and a second temperature reading 2420 indicating the temperature within the gas injection chamber 1300 from a second temperature sensor of the reagent cartridge 2200. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not be configured to receive a first temperature reading indicating the temperature within the reagent chamber from the first temperature sensor and a second temperature reading indicating the temperature within the gas injection chamber from the second temperature sensor.

[0069] The reactor device 2000 of the embodiment of FIG. 2 is based on at least the first temperature reading 2410 and the second temperature reading 2420 to a predetermined solid reagent temperature (T r) is configured to maintain. Generally, a reactor device configured to maintain a predetermined solid reagent temperature based on at least a first temperature reading and a second temperature reading can facilitate maintaining a narrower solid reagent temperature distribution across the range of the reagent chamber. Additionally or alternatively, a reactor device configured to maintain a predetermined solid reagent temperature based on at least a first temperature reading and a second temperature reading may be able to mitigate or avoid temporary variations in the solid reagent temperature caused, for example, by delays in temperature control due to the time-consuming heat conduction of the solid reagent. In other embodiments according to the second and / or fourth aspects, the reactor device is configured to receive a first temperature reading indicative of the temperature within the reagent chamber and a second temperature reading indicative of the temperature within the gas injection chamber, and the reactor device may or may not be configured to maintain a predetermined solid reagent temperature based on at least the first temperature reading and the second temperature reading.

[0070] In the embodiment of FIG. 2, the reactor device 2000 includes a cartridge heater 2500 for heating the reagent cartridge 2200 and a preheater 2600 for heating the carrier gas upstream of the reagent cartridge 2200. During operation of the reactor device 2000, the reactor device 2000 adjusts the temperature (T r ) of the preheater based on a comparison between a predetermined solid reagent temperature (T ph ) and the second temperature reading 2420, and adjusts the temperature (T r ) of the cartridge heater based on a comparison between the solid reagent temperature (T ch) is configured to adjust. Generally, a reactor device configured to adjust the temperature of a preheater based on a comparison between a predetermined (target) solid reagent temperature and a second temperature reading, and to adjust the temperature of a cartridge heater based on a comparison between the solid reagent temperature and a first temperature reading, may enable the utilization of heat provided by the preheater to reduce variations in the solid reagent temperature across the range of the reagent chamber. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not be configured to adjust the temperature of the preheater based on a comparison between a predetermined (target) solid reagent temperature and a second temperature reading, and / or to adjust the temperature of the cartridge heater based on a comparison between the solid reagent temperature and a first temperature reading.

[0071] The reactor device 2000 is operably coupled to a first temperature sensor and a second temperature sensor of the reagent cartridge 2200 for receiving a first temperature reading 2410 and a second temperature reading 2420, respectively, and further includes a temperature control unit 2400 operably coupled to a cartridge heater 2500 and a preheater 2600 for heating the reagent cartridge 2200 and the carrier gas 1003 upstream of the reagent cartridge 2200, respectively.

[0072] In the embodiment of FIG. 2, the reactor device 2000 is configured to maintain a predetermined solid reagent temperature (T r ) by utilizing closed-loop control, particularly multi-loop closed-loop control. Typically, closed-loop control may be achieved, for example, by utilizing proportional (P) control, which may optionally be supplemented by integral (I) and / or derivative (D) control terms. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not be configured to maintain a predetermined solid reagent temperature by utilizing closed-loop control, such as multi-loop closed-loop control.

[0073] In the embodiment of FIG. 2, T rIt may be about 35°C. In other embodiments according to the second aspect and / or the fourth aspect, any suitable solid reagent temperature can be used, for example, a solid reagent temperature in the range of 20°C to 100°C, or 25°C to 80°C, or 30°C to 50°C.

[0074] The cartridge heater 2500 of the embodiment of FIG. 2 is implemented as an electrical side heater, specifically, as a silicone heating mat surrounding the reagent chamber of the reagent cartridge 2200. The cartridge heater 2500 may be fixed to the reagent cartridge 2200 using fixing means such as an adhesive, whereby the cartridge heater 2500 can form part of the reagent cartridge 2200. In other embodiments according to the second aspect and / or the fourth aspect, the cartridge heater may be implemented in any suitable manner, for example, as an electrical side heater such as a heating mat surrounding the reagent chamber. In any embodiment according to the first aspect and / or the third aspect, the cartridge heater may be implemented as part of the reagent cartridge.

[0075] The reactor device 2000 of the embodiment of FIG. 2 further includes a reagent conduit heater 2710, and the temperature control unit 2400 is operably coupled to the reagent conduit heater 2710 for heating the reagent gas conduit 2700. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not include a reagent conduit heater, and the temperature control unit may or may not be operably coupled to a reagent conduit heater for heating the reagent gas conduit.

[0076] In the embodiment of FIG. 2, the temperature control unit 2400 is configured to maintain the temperature of the reagent gas conduit 2700 at about 50° C. In other embodiments according to the second aspect and / or the fourth aspect, the temperature control unit is operably coupled to a reagent conduit heater for heating the reagent gas conduit and can use any suitable reagent gas conduit temperature(s). For example, in some such embodiments, the temperature control unit may be configured to maintain the temperature of the reagent gas conduit in the range of 30° C. to 200° C., or in the range of 50° C. to 190° C., or in the range of 100° C. to 180° C.

[0077] The reactor device 2000 of the embodiment of FIG. 2 forms an example of a reactor device comprising a reagent gas conduit for extracting a reagent carrier gas mixture from a reagent cartridge and a reagent conduit heater for heating the reagent gas conduit. In other embodiments according to the second aspect and / or the fourth aspect, the reactor device may or may not comprise a reagent gas conduit for extracting a reagent carrier gas mixture from a reagent cartridge and a reagent conduit heater for heating the reagent gas conduit.

[0078] FIG. 3 shows a simplified proportional closed-loop temperature control algorithm 3000 by which a predetermined T may be maintained based on a first temperature reading and a second temperature reading by a reactor device such as the reactor device 2000 of the embodiment of FIG. 2. Of course, the reactor device according to the second and / or fourth aspects can utilize any suitable temperature control algorithm(s), which may be the same as, similar to, or different from the temperature control algorithm 3000 of FIG. 3. r

[0079] The temperature control algorithm 3000 of FIG. 3 comprises an initialization step 3100 for initializing the temperature (T ph ) of the preheater and the temperature (T ch ) of the cartridge heater, a preheater control step 3200, and a cartridge heater control step 3300.

[0080] During preheater control step 3200, a second temperature reading indicating the temperature within the gas injection chamber is compared to a predetermined solid reagent temperature (T r ). On the other hand, if the second temperature reading is higher than T r , T ph is decreased and the temperature control algorithm 3000 returns to the start of preheater control step 3200. On the other hand, if the second temperature reading is lower than T r , T ph is increased and the temperature control algorithm 3000 returns to the start of preheater control step 3200.

[0081] During cartridge heater control step 3300, a first temperature reading indicating the temperature within the reagent chamber is compared to T r . On the other hand, if the first temperature reading is higher than T r , T ch is decreased and the temperature control algorithm 3000 returns to the start of preheater control step 3200. On the other hand, if the first temperature reading is lower than T r , T ch is increased and the temperature control algorithm 3000 returns to the start of preheater control step 3200.

[0082] It will be apparent to those skilled in the art that, as technology advances, the basic concepts of the present invention may be implemented in various ways. Accordingly, the present invention and its embodiments are not limited to the examples described above, but may instead be modified within the scope of the claims.

[0083] It will be understood that any benefits and advantages described above may relate to one embodiment or to multiple embodiments. Embodiments are not limited to those that solve any or all of the problems described or have any or all of the benefits and advantages described.

[0084] In this specification, the term "comprising" is used to mean that the feature(s) or act(s) preceding the term include, without excluding the presence of one or more additional features or acts. Further, reference to "a(n)" item is understood to refer to one or more of those items.

Explanation of Signs

[0085]

Number

Number

Claims

1. A reagent cartridge (1000) for sublimating a solid reagent (1001) to form a reagent gas (1002) and mixing the reagent gas (1002) with a flowing carrier gas (1003) to form a reagent carrier gas mixture (1004), comprising: the reagent cartridge (1000) includes a reagent chamber (1200) for holding the solid reagent (1001) and at least one pressure sensor (1100) for measuring the pressure inside the reagent cartridge (1000); the reagent cartridge (1000) includes a gas discharge chamber (1400) downstream of the reagent chamber (1200) for discharging the reagent carrier gas mixture (1004) from the reagent cartridge (1000), and the at least one pressure sensor (1100) includes a second pressure sensor (1120) configured to measure the pressure inside the gas discharge chamber (1400). The reagent cartridge (1000) is characterized by this.

2. The reagent cartridge (1000) according to claim 1, wherein the at least one pressure sensor (1100) includes a first pressure sensor (1110) configured to measure the pressure inside the reagent chamber (1200).

3. The reagent cartridge (1000) according to claim 1 or 2, further comprising a gas injection chamber (1300) upstream of the reagent chamber (1200) for injecting a carrier gas (1003) into the reagent cartridge (1000), a first temperature sensor (1510) configured to measure the temperature inside the reagent chamber (1200), and a second temperature sensor (1520) configured to measure the temperature inside the gas injection chamber (1300).

4. A reactor device (2000) comprising a reagent cartridge holder (2100) for holding the reagent cartridge (2200) according to any one of claims 1 to 3 during operation of the reactor device (2000), wherein the reactor device (2000) is configured to receive from the at least one pressure sensor (1100) of the reagent cartridge (2200) at least one cartridge pressure reading (2310) indicating the pressure inside the reagent cartridge (2200).

5. The reactor device (2000) adjusts the carrier gas mass flow rate based on at least a part of the at least one cartridge pressure reading value (2310) 【Number 1】 to maintain a predetermined reagent output mass flow rate from the reagent cartridge (2200). 【Number 2】 The reactor device (2000) according to claim 4. **Claim 6** The reactor device (2000) is configured to adjust the carrier gas mass flow rate based on at least a first pressure reading value (2311) indicating the pressure within the reagent chamber (1200) of the reagent cartridge (2200). [Number 3] The reactor device (2000) according to claim 5. **Claim 7** The reactor device (2000) according to any one of claims 4 to 6, is configured to detect the formation of an occlusion (2001) downstream from the reagent cartridge (2200) based on at least a part of the at least one cartridge pressure reading value (2310). **Claim 8** The reactor device (2000) according to claim 7, is configured to detect the formation of the occlusion (2001) based on at least a second pressure reading value (2312) indicating the pressure within the gas discharge chamber (1400) of the reagent cartridge (2200). **Claim 9** The reactor device (2000) according to any one of claims 4 to 8, is configured to produce a carbon-based high aspect ratio molecular structure, HARS, such as carbon nanotubes, such as single-walled carbon nanotubes and / or multi-walled carbon nanotubes; and / or carbon nanobuds; and / or graphene nanoribbons; and / or graphite nanoribbons; and / or carbon nanofibers; and / or graphene nanoplatelets. **Claim 10** The reagent cartridge (2200) forms a reagent carrier gas mixture (1004) as the reagent gas (1002) that includes one or more catalyst particle precursors, such as an iron-containing organometallic or metal-organic compound, such as ferrocene (Fe(C ５ H ２ )2), iron pentacarbonyl (Fe(CO) ５ ), and / or iron(II) phthalocyanine (C ３２ H １６ FeN ８ ); and / or one or more nickel-containing organometallic or metal-organic compounds, such as nickelocene (Ni(C ５ H ５ ) ２ ); and / or one or more cobalt-containing organometallic or metal-organic compounds, such as cobaltocene (Co(C ５ H ５ ) ２ ), the reactor device (2000) according to any one of claims 4 to 9. **Claim 11** When dependent on claim 3, the reactor device (2000) is configured to receive a first temperature reading value (2410) indicating the temperature within the reagent chamber (1200) from the first temperature sensor (1510) and a second temperature reading value (2420) indicating the temperature within the gas injection chamber (1300) from the second temperature sensor (1520). The reactor device (2000) according to any one of claims 4 to 10. **Claim 12** The reactor device (2000) is configured to maintain a predetermined solid reagent temperature T based on at least the first temperature reading (2410) and the second temperature reading (2420). ｒ The reactor device (2000) according to claim 11, which is configured to maintain the temperature. **Claim 13** The reactor device (2000) includes a cartridge heater (2500) for heating the reagent cartridge (2200) and a preheater (2600) for heating the carrier gas (1003) upstream of the reagent cartridge (2200), and the reactor device (2000) is a) the temperature T of the solid reagent ｒ Based on the comparison between the temperature T of the preheater and the second temperature reading value (2420), ｐｈ adjust the temperature T b) the temperature T of the solid reagent ｒ Based on the comparison between the temperature reading (2410) of the first temperature sensor and the temperature T of the solid reagent, adjust the temperature T ｃｈ of the cartridge heater configured as such, the reactor device (2000) according to claim 12.

14. The reactor device (2000) according to any one of claims 11 to 13, comprising a reagent gas conduit (2700) for extracting a reagent carrier gas mixture (1004) from the reagent cartridge (2200) and a reagent conduit heater (2710) for heating the reagent gas conduit (2700).

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