Kit for sublimation and reaction device

Abstract

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

Description

Technical Field

[0001] The present disclosure relates to chemical reactors and components thereof. In particular, the present disclosure relates to sublimation of solid reagents to form reagent gases for use 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, such as single-walled carbon nanotubes and / or multi-walled carbon nanotubes; carbon nanobuds; and / or graphene nanoribbons, ferrocene is typically used as a precursor for the in situ formation of iron-containing catalyst nanoparticles, which promote the formation of HARMS.

[0003] In general, it is extremely important to precisely control the concentration of reagents during chemical reactions. For example, in the case of FCCVD of carbon-based HARMS, the mass inflow rate of ferrocene gas formed by sublimation of solid ferrocene must be precisely controlled to form catalyst nanoparticles with a strict target performance range. Although various solutions have been designed to control the sublimation of solid reagents, certain factors, such as uneven heating of the solid reagents and the formation of blockages caused by condensation or deposition within the reactor, may result in variations in the outflow rate of the reagents from the reagent chamber used for reagent sublimation.

[0004] In view of the foregoing, it may be desirable to develop new solutions related to controlling the sublimation of solid reagents. Summary of the invention

[0005] This Summary is provided to introduce some concepts in a simplified form 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, a reagent kit is provided for sublimating a solid reagent to form a reagent gas and for mixing the reagent gas with a flowing carrier gas to form a reagent-carrier gas mixture. The reagent kit includes a reagent chamber for holding the solid reagent and at least one pressure sensor for measuring the pressure within the reagent kit.

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

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

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

[0010] According to a third aspect, a reagent kit is provided for sublimating a solid reagent to form a reagent gas, and for mixing the reagent gas with a flowing carrier gas to form a reagent-carrier gas mixture. The reagent kit includes a reagent chamber for holding the solid reagent, a gas injection chamber upstream of the reagent chamber for injecting the carrier gas into the reagent kit, a first temperature sensor configured to measure the temperature in the reagent chamber, and a second temperature sensor configured to measure the temperature in the gas injection chamber.

[0011] In an embodiment of the third aspect, the kit is a kit according to the first aspect or any embodiment thereof.

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

[0013] In an embodiment of the fourth aspect, the kit is a kit according to the second aspect or any embodiment thereof. BRIEF DESCRIPTION OF THE DRAWINGS

[0014] The present disclosure will be better understood from the following detailed description when read in light of the accompanying drawings, in which:

[0015] Figure 1 A kit is shown,

[0016] Figure 2 A reaction apparatus is described, and

[0017] Figure 3 The temperature control algorithm is shown.

[0018] Unless specifically stated to the contrary, any of the foregoing figures may not be drawn to scale, such that any element in the figure may be drawn in inaccurate proportion relative to other elements in the figure in order to emphasize certain structural aspects of the embodiments of the figure.

[0019] Furthermore, corresponding elements in the embodiments of any two of the aforementioned figures may be out of scale with respect to each other in the two figures in order to emphasize certain structural aspects of the embodiments of the two figures. DETAILED DESCRIPTION

[0020] With respect to the kits and reaction apparatus discussed in this detailed description, the following should be noted.

[0021] In this description, "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., greater than or equal to 0.1 nanometers (nm) and less than or equal to about 100 nm. Additionally or alternatively, HARMS may refer to a structure having dimensions in two perpendicular directions of significantly different orders of magnitude. For example, a HARMS may have a length that is tens or hundreds of times greater than its thickness and / or width. Embodiments of HARMS include nanotubes, such as carbon nanotubes and boron nitride nanotubes; nanoribbons, such as graphene nanoribbons, graphite nanoribbons, and boron nitride nanoribbons; nanowires, such as tungsten nanowires, copper nanowires, aluminum nanowires, nickel nanowires, and silver nanowires; nanofibers, such as carbon nanofibers and silicon carbide nanofibers; and nanosheets, such as graphene nanosheets, polyborane nanosheets, and boron nitride nanosheets.

[0022] In addition, "carbon-based" HARMS may refer to HARMS that are primarily composed of carbon (C). Additionally or alternatively, carbon-based HARMS may refer to HARMS that contain 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. Typically, carbon-based HARMS may be doped with non-carbon dopants, for example to change their electrical and / or thermal properties. Embodiments of carbon-based HARMS include carbon nanotubes, carbon nanobuds, graphene nanoribbons, carbon nanofibers, graphene nanosheets, and combinations thereof.

[0023] In the present disclosure, a "high aspect ratio molecular structure network" or "HARMS network" may refer to a plurality of interconnected HARMS. Typically, the HARMS network may form a solid and / or monolithic material on a macroscopic scale, wherein the individual HARMS are non-oriented, i.e., substantially randomly oriented or randomly oriented, or oriented. Typically, the HARMS network may be arranged in various macroscopic forms, for example, as a film, which may or may not be optically transparent and / or have high electrical conductivity.

[0024] Figure 1 is a schematic cross-sectional view of a kit 1000 for sublimating a solid reagent 1001 to form a reagent gas 1002 and for mixing the reagent gas 1002 with a flowing carrier gas 1003 to form a reagent-carrier gas mixture 1004 according to one embodiment.

[0025] Figure 1 The kit 1000 of the embodiment is consistent with the first aspect and the third aspect. In other embodiments, the kit can be a kit according to the first aspect and / or the third aspect.

[0026] Figure 1 The kit 1000 of the illustrated embodiment is configured for sublimation of a solid reagent 1001. In other embodiments according to the first aspect and / or the third aspect, the kit for sublimation of a solid reagent may be suitable for or configured for sublimation of a solid reagent.

[0027] exist Figure 1 In the embodiment of the present invention, the test kit 1000 includes a reagent chamber 1200 and at least one pressure sensor 1100, the reagent chamber 1200 is used to store the solid reagent 1001, and the pressure sensor 1100 is used to measure the pressure inside the test kit 1000. Generally, the test kit including at least one pressure sensor for measuring the pressure in the test kit can facilitate the pressure near the solid reagent kept in the test kit to be kept within a predetermined pressure range, which in turn can make it possible to limit the change of the reagent output mass flow rate from the test kit. Additionally or alternatively, the test kit including at least one pressure sensor for measuring the pressure in the test kit can make it possible to compensate for the influence of the change of the reactor pressure on the pressure in the test kit. Additionally or alternatively, the test kit including at least one pressure sensor for measuring the pressure inside the test kit can make it possible to detect the formation of a plug in the downstream of the test kit. In other embodiments according to the third aspect, the test kit may include or not include at least one pressure sensor for measuring the pressure inside the test kit.

[0028] exist Figure 1 In an embodiment, at least one pressure sensor 1100 includes a first pressure sensor 1110, which is configured to measure the pressure inside the reagent chamber 1200. Generally, at least one pressure sensor of the test kit including a first pressure sensor can increase the accuracy or authenticity of the pressure reading interpreted as being related to the pressure near the solid reagent, wherein the first pressure sensor is configured to measure the pressure inside the reagent chamber for holding the solid reagent. In other embodiments according to the first aspect and / or the third aspect, at least one pressure sensor of the test kit may or may not include a first pressure sensor configured to measure the pressure inside the reagent chamber of the test kit.

[0029] The test kit 1000 includes a gas injection chamber 1400, which is located downstream of the reagent chamber 1200 for ejecting the reagent-carrier gas mixture 1004 out of the test kit 1000, and the at least one pressure sensor 1100 includes a second pressure sensor 1120, which is configured to measure the pressure within the gas injection chamber 1400. In general, the at least one pressure sensor of the test kit including the second pressure sensor can enable the effectiveness of the blockage formation detection algorithm to be increased based on detecting an increase in at least one box pressure reading indicating the pressure inside the test kit, the second pressure sensor being configured to measure the pressure inside the gas injection chamber for ejecting the reagent-carrier gas mixture out of the test kit. In other embodiments according to the first aspect and / or the third aspect, the at least one pressure sensor of the test kit may or may not include a second pressure sensor configured to measure the pressure inside the gas injection chamber so as to eject the reagent-carrier gas mixture from the test kit.

[0030] exist Figure 1 In an embodiment, in addition to the reagent chamber 1200 for holding the solid reagent 1001, the reagent kit 1000 also includes a gas injection chamber 1300 upstream of the reagent chamber 1200 for injecting a carrier gas 1003 into the reagent kit 1000, a first temperature sensor 1510 configured to measure the internal temperature of the reagent chamber 1200, and a second temperature sensor 1520 configured to measure the internal temperature of the gas injection chamber 1300.

[0031] Typically, a test kit comprising a first temperature sensor configured to measure the temperature inside the reagent chamber and a second temperature sensor configured to measure the temperature inside the gas injection chamber can enable more accurate maintenance of the solid reagent at a predetermined solid reagent temperature throughout the reagent chamber. Additionally or alternatively, when the test kit comprises at least one pressure sensor for measuring the pressure inside the test kit, a test kit comprising a first temperature sensor configured to measure the temperature inside the reagent chamber and a second temperature sensor configured to measure the temperature inside the gas injection chamber can enable more accurate control of the thermodynamic state of the solid reagent throughout the reagent chamber, which in turn enables the formation of a reagent-carrier gas mixture having more clearly defined properties, and / or enables more accurate regulation of the carrier gas mass flow rate to maintain a predetermined reagent output mass flow rate.

[0032] In other embodiments according to the first aspect, the reagent kit may or may not include a gas injection chamber upstream of a reagent chamber for injecting a carrier gas into the reagent kit, a first temperature sensor configured to measure the temperature within the reagent chamber, and / or a second temperature sensor configured to measure the temperature inside the gas injection chamber.

[0033] Figure 3 The kit 1000 of the illustrated embodiment further comprises a third temperature sensor 1530 configured to measure the temperature within the gas injection chamber 1400. In other embodiments according to the first and / or third aspects, the kit may or may not comprise such a third temperature sensor.

[0034] exist Figure 1 In an embodiment of the present invention, 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 3-wire or 4-wire electrical output connection according to 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 resistance thermometer elements, such as one or more PRTs, for example, 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, wherein at least one of the first temperature sensor, the second temperature sensor and the third temperature sensor includes a PRT element, at least a portion of the at least one sensor may or may not be configured for a 3-wire or 4-wire electrical output connection according to the IEC 60751:2008 standard.

[0035] exist Figure 1 In an embodiment, the 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, the at least one pressure sensor of the kit may or may not include such a third pressure sensor.

[0036] At least one pressure sensor 1100, i.e., each of the first pressure sensor 1110, the second pressure sensor 1120, and the third pressure sensor 1130, comprises a flush-mounted diaphragm. In other embodiments according to the first aspect and / or the third aspect, one or more, e.g., each, of the at least one pressure sensor may comprise a flush-mounted diaphragm.

[0037] exist Figure 1In the embodiment of the present invention, the reagent chamber 1200 includes solid ferrocene (Fe(C5H2)2). In other embodiments according to the first aspect and / or the third aspect, the reagent chamber of the kit may or may not include any suitable sublimable solid reagent, such as solid ferrocene (Fe(C5H2)2).

[0038] exist Figure 1 In an embodiment, 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, which is configured to block the passage of particles, while the reagent chamber 1200 and the gas injection chamber 1400 are separated from each other by a perforated wall, in particular a stainless steel mesh 1220. In other embodiments according to the first aspect and / or the third aspect, the reagent chamber can be separated from the gas injection chamber and / or the gas injection chamber in any suitable manner, for example by a filter, such as a sintered filter, and / or a perforated wall, such as a mesh. In such other embodiments, any such separation structure can be formed of any suitable material, such as stainless steel and / or titanium.

[0039] Figure 1 The reagent chamber 1200 of the embodiment of the present invention has a reagent chamber width (W) of approximately 5 centimeters (cm) measured perpendicular to the direction 1005 of carrier gas flow within the reagent chamber 1200. rc ). In other embodiments according to the first aspect and / or the third aspect, the reagent chamber may have any suitable reagent chamber width measured perpendicular to the direction of carrier gas flow in the reagent chamber, for example, a reagent chamber width greater than or equal to 1 cm, or 2 cm, or 3 cm, or 4 cm and / or less than or equal to 20 cm, or 15 cm, or 10 cm, or 7 cm.

[0040] Figure 1 The reagent chamber 1200 of the embodiment of the present invention has a reagent chamber length (L) of approximately 15 centimeters (cm) measured parallel to the direction 1005 of carrier gas flow within the reagent chamber 1200. rc ). In other embodiments according to the first aspect and / or the third aspect, the reagent chamber may have any suitable reagent chamber length measured parallel to the direction of carrier gas flow in the reagent chamber, for example, a reagent chamber length greater than or equal to 3 cm, or 5 cm, or 8 cm, or 10 cm, or 12 cm and / or less than or equal to 50 cm, or 40 cm, or 30 cm, or 25 cm, or 20 cm.

[0041] exist Figure 1In an embodiment of the present invention, the reagent kit 1000 is configured to pass a carrier gas 1003 through the reagent chamber 1200 to cause fluidization of the granular material disposed in the reagent chamber 1200. Generally, a reagent kit configured to pass a carrier gas through the reagent chamber to cause fluidization of the granular material disposed in the reagent chamber can help reduce local temperature differences within the reagent chamber. In other embodiments according to the first aspect and / or the third aspect, the reagent kit may or may not be configured in this manner.

[0042] Figure 1 The reagent kit 1000 of the illustrated embodiment includes a carrier gas inlet 1310 for delivering a carrier gas 1003 into the reagent kit 1000 and a reagent-carrier gas mixture outlet 1410 for discharging a reagent-carrier gas mixture 1004 from the reagent kit 1000. In other embodiments according to the first aspect and / or the third aspect, the reagent kit may include any suitable type of carrier gas inlet and reagent-carrier gas mixture outlet.

[0043] It should be understood that the embodiments of the first aspect and / or the third aspect described above can be used in combination with each other. Several embodiments can be combined together to form further embodiments of the first aspect and / or the third aspect.

[0044] The main features of the kit are discussed above. In the following, more emphasis is placed on the features of the reaction device. The above description of the embodiments, definitions, details and advantages related to the kit applies mutatis mutandis to the reaction device discussed below. The same applies vice versa.

[0045] Figure 2 A reaction device 2000 according to one embodiment is schematically shown.

[0046] Figure 2 The reaction device 2000 of the embodiment is consistent with the second aspect and the fourth aspect. In other embodiments, the reaction device can be a device according to the second aspect and / or the fourth aspect.

[0047] exist Figure 2 In an embodiment of the present invention, the reaction device 2000 includes a reagent kit holder 2100 configured to hold a reagent kit 2200 according to the first aspect and the third aspect during operation of the reaction device 2000. The reaction device 2000 also includes a reagent kit 2200 according to the first aspect and the third aspect held by the reagent kit holder 2100. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may include a reagent kit holder for holding or configured to hold, respectively, the reagent kit according to the first aspect and / or the third aspect during operation of the reaction device. In such an embodiment, the reaction device may or may not include the reagent kit.

[0048] Figure 2 The kit 2200 of the illustrated embodiment can be used with Figure 1 The kit 1000 of the embodiment shown is the same. In other embodiments according to the second aspect and / or the fourth aspect, any suitable kit can be used, such as Figure 1 The kit 1000 of the illustrated embodiment is different, similar or the same as a kit.

[0049] Figure 2 The reaction device 2000 of the embodiment of the present invention is configured to receive at least one cartridge pressure reading 2310 indicating the internal pressure of 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 reaction device may or may not be configured to receive at least one cartridge pressure reading indicating the internal pressure of the reagent cartridge from at least one pressure sensor of the reagent cartridge.

[0050] exist Figure 2 In an embodiment of the invention, the reaction device 2000 is configured for producing carbon-based HARMS, in particular carbon nanobuds, by floating catalyst chemical vapor deposition (FCCVD). In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be configured for producing carbon-based HARMS, such as carbon nanotubes, for example single-walled carbon nanotubes and / or multi-walled carbon nanotubes; carbon nanobuds; and / or graphene nanoribbons, for example by FCCVD.

[0051] Even if not Figure 2 It is clearly stated that Figure 2 The reaction device 2000 of the embodiment may include any features and / or elements necessary or beneficial for producing carbon-based HARMS, such as a carbon source storage, which may be provided with one or more heaters and / or pressure sensors; a carbon source conduit, which may have one or more heaters and / or one or more flow controllers, etc.

[0052] Figure 2 The reaction device 2000 of the embodiment of the present invention can be implemented as a continuous flow reaction device. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be implemented as a continuous flow reaction device. For example, in some such embodiments, the reaction device may be implemented as an intermittent reaction device.

[0053] exist Figure 2 In the embodiment of the present invention, the reaction device 2000 includes a flow reactor 2900. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may include any suitable type of reactor, such as one or more flow reactors.

[0054] 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, are added (e.g., continuously added), and / or one or more auxiliary substances, such as catalysts and / or growth promoters, 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 redox agents, such as oxygen (O2), water (H2O), carbon dioxide (CO2) and / or hydrogen (H2), are added (e.g., continuously added), and one or more products are collected (e.g., continuously collected). Additionally or alternatively, a flow reactor may refer to a reactor through which one or more reagents pass and in which catalysis is ongoing. Typically, a flow reactor may be formed of any suitable material (one or more), such as stainless steel, fused silica or fused quartz.

[0055] exist Figure 2 In the embodiment of the present invention, the reaction device 2000 includes a carrier gas conduit 2800 for providing a carrier gas flow through the reagent kit 2200 and a reagent gas conduit 2700 for guiding the reagent-carrier gas mixture formed in the reagent kit 2200 to the flow reactor 2900. In other embodiments according to the second aspect and / or the fourth aspect, the carrier gas flow through the reagent kit can be provided by any suitable means, such as via a carrier gas conduit, and the reagent-carrier gas mixture formed in the reagent kit can be guided to any suitable destination, such as a chemical reactor, by any suitable means, such as via a reagent gas conduit.

[0056] Figure 2 The reagent kit 2200 of the embodiment is configured to form a reagent-carrier gas mixture, which includes ferrocene (Fe(C5H2)2) gas as a reagent gas and nitrogen (N2) as a carrier gas. In other embodiments according to the second aspect and / or the fourth aspect, any suitable reagent gas can be used, such as one or more catalyst particle precursors (e.g., iron-containing organic metals or metal organic compounds, such as ferrocene (Fe(C5H2)2), pentacarbonyl iron (Fe(CO)5) and / or iron (II) phthalocyanine (C5H2)2). 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 a carrier gas), such as argon (Ar), helium (He), nitrogen (N2), carbon monoxide (CO) and / or hydrogen (H2).

[0057] exist Figure 2 In the embodiment of the invention, the reaction device 2000 is configured to decompose the reagent gas to form catalyst particles, in particular iron-containing nanoparticles. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be configured in this manner.

[0058] Throughout the specification, "catalyst particles" may refer to particles of materials suitable for increasing reaction rate by catalysis. Additionally or alternatively, catalyst particles may refer to particles suitable for heterogeneous catalysis. Additionally or alternatively, catalyst particles may refer to a particle catalyst material block suitable for catalyzing the production of carbon-based HARMS, such as by chemical vapor deposition, such as floating catalyst chemical vapor deposition (FCCVD). Typically, catalyst particles may include one or more transition metals, such as iron (Fe), cobalt (Co) and / or nickel (Ni), are substantially composed of one or more transition metals, or are composed of one or more transition metals. Typically, catalyst particles may have any suitable diameter, for example, 0.1nm to 300nm, or 1nm to 200nm, or 5nm to 100nm, or a diameter in the range of 10nm to 50nm.

[0059] exist Figure 2 In an embodiment, the reaction device 2000 is configured to adjust the carrier gas mass flow rate based on at least a portion of at least one cartridge pressure reading 2310. To maintain a predetermined reagent output mass flow rate from reagent cartridge 2200 Typically, a reaction device 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 can facilitate feeding a constant amount of reagent gas into the reaction device. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be 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.

[0060] A reaction device that is "configured to" perform a process may refer to the ability and suitability of the reaction device for such a process. This may be achieved in various ways. For example, the reaction device or its control unit may include at least one processor and at least one memory coupled to the at least one processor, the memory storing program code instructions, and when the program code instructions are executed on the at least one processor, the program code instructions cause the processor to perform the (one or more) processes discussed. Additionally or alternatively, any functionally described features of the reaction device may be at least partially performed by one or more hardware logic components. For example, but not limited to, suitable hardware logic components of illustrative types include field programmable gate arrays (FPGAs), application specific integrated circuits (ASICs), application specific standard products (ASSPs), systems on chips (SOCs), complex programmable logic devices (CPLDs), etc. The reaction device may generally be operated according to any appropriate principle and by any appropriate circuits and / or signals known in the art.

[0061] exist Figure 2 In an embodiment, the kit 2200 includes solid ferrocene as a solid reagent, and the increase in pressure reduces the rate at which ferrocene sublimates. Figure 2 The reaction device 2000 of the embodiment is configured to increase in response to an increase in the internal pressure of the reagent chamber 2200. and decreases in response to a decrease in the internal pressure of the reagent cartridge 2200. In other embodiments according to the second aspect and / or the fourth aspect, wherein the reaction device is configured to adjust the carrier gas mass flow rate based on at least a portion of at least one box pressure reading to maintain a predetermined reagent output mass flow rate from the reagent cartridge, the reaction device may be configured to increase or decrease the carrier gas mass flow rate in response to an increase in at least a portion of at least one box pressure reading.

[0062] Figure 2 The reaction device 2000 of the embodiment of the present invention is specifically configured to adjust based on the first pressure reading 2311 indicating the pressure inside the reagent chamber 1200 of the reagent cartridge 2200. In general, a reaction device configured to adjust the carrier gas mass flow rate based on at least the first pressure reading indicating the pressure inside the reagent chamber of the reagent cartridge can increase the accuracy or authenticity of the pressure reading interpreted as being related to the pressure near the solid reagent, which in turn can achieve more accurate control of the carrier gas mass flow rate.

[0063] In other embodiments according to the second aspect and / or the fourth aspect, wherein the reaction device is configured to adjust the carrier gas mass flow rate based on at least a portion of at least one box pressure reading to maintain a predetermined reagent output mass flow rate from the reagent kit, the reaction device can be configured to adjust the carrier gas mass flow rate based on any one or more of the at least one box pressure reading, for example, at least the first pressure reading indicates the pressure inside the reagent chamber of the reagent kit.

[0064] exist Figure 2 In the embodiment of the present invention, the reaction device 2000 is also configured to detect the formation of a blockage 2001 downstream of the test kit 2200 based on at least a portion of at least one box pressure reading 2310. Such a blockage may usually be formed downstream of the test kit due to condensation or deposition of reagent gas, which may be caused by insufficient heating of the reagent gas conduit used to guide the reagent-carrier gas mixture from the test kit to the reactor of the reaction device, and the formation of the blockage can usually be detected based on a relatively sudden increase of at least a portion of at least one box pressure reading. Typically, a reaction device configured to detect the formation of a blockage downstream of the test kit based on at least a portion of at least one box pressure reading can facilitate the maintenance of the reaction device. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be configured to detect the formation of a blockage downstream of the test kit based on at least a portion of at least one box pressure reading.

[0065] Figure 2 The reaction device 2000 of the embodiment is specifically configured to detect the formation of the blockage 2001 based on the second pressure reading 2312 indicating the pressure within the gas injection chamber of the reagent kit 2200. In general, a reaction device configured to detect the formation of a blockage based on at least the second pressure reading indicating the pressure within the gas injection chamber of the reagent kit can increase the accuracy or authenticity of such detection, for example by reducing the probability of a false positive detection result. In other embodiments according to the second aspect and / or the fourth aspect, in which the reaction device is configured to detect the formation of a blockage downstream of the reagent kit based on at least a portion of at least one cartridge pressure reading, the reaction device may or may not be configured to detect the formation of a blockage based on at least the second pressure reading indicating the pressure within the gas injection chamber of the reagent kit.

[0066] The reaction device 2000 includes a reagent conduit mass flow meter 2720 for measuring the mass flow rate through the reagent gas conduit 2700; and a pressure control unit 2300, which is operably connected to at least one pressure sensor of the reagent cartridge 2200 for receiving at least one cartridge pressure reading 2310, and connected to the reagent conduit mass flow meter 2720 and the carrier gas flow controller 2810 for use based on adjust In other embodiments according to the second aspect and / or the fourth aspect, the pressure control unit may or may not be operatively connected with at least one pressure sensor, a reagent conduit mass flow meter and a carrier gas flow controller in this manner. For example, in some such embodiments, a predetermined reagent output mass flow rate can be maintained by adjusting the carrier gas mass flow rate based on at least one box pressure reading and a known phenomenon model describing the relationship between at least one box pressure reading and the reagent sublimation rate. In this case, a specific reagent conduit mass flow meter can be omitted.

[0067] In this specification, a "control unit" may refer to a device, such as an electronic device, having at least one designated function, the at least one designated function involving determining and / or influencing an operating condition, state or parameter associated with another device, unit or element. A control unit may or may not form part of a multifunctional control system.

[0068] Furthermore, a control unit "operatively coupled" to a device, unit or element may refer to a control unit having at least one designated function associated with determining and / or influencing an operating condition, state or parameter associated with the device, unit or element.

[0069] exist Figure 2 In the embodiment of the present invention, the reaction device 2000 can also be configured to compensate for the pressure changes inside the flow reactor 2900 to stabilize the pressure inside the reagent box 2200. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be configured in this way.

[0070] exist Figure 2 In the embodiment of the present invention, the reaction device 2000 is further configured to receive a first temperature reading 2410 indicating the temperature in the reagent chamber 1200 from the first temperature sensor of the reagent cartridge 2200 and to receive a second temperature reading 2420 indicating the temperature in the gas injection chamber 1300 from the second temperature sensor of the reagent cartridge 2200. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be configured to receive a first temperature reading indicating the temperature in the reagent chamber from the first temperature sensor and to receive a second temperature reading indicating the temperature in the gas injection chamber from the second temperature sensor.

[0071] Figure 2 The reaction device 2000 of the embodiment of the present invention is configured to maintain a predetermined solid reagent temperature (T r). Typically, a reaction 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 narrow solid reagent temperature distribution throughout the reagent chamber. Additionally or alternatively, a reaction device configured to maintain a predetermined solid reagent temperature based on at least a first temperature reading and a second temperature reading can enable mitigation or avoidance of temporary solid reagent temperature fluctuations caused by, for example, temperature control lags caused by time-consuming heat transfer in the solid reagent. In other embodiments according to the second aspect and / or the fourth aspect, wherein the reaction device is configured to receive a first temperature reading indicating a temperature within the reagent chamber and a second temperature reading indicating a temperature within the gas injection chamber, the reaction 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.

[0072] exist Figure 2 In an embodiment, the reaction device 2000 includes a cartridge heater 2500 for heating the reagent cartridge 2200 and a preheater 2600 for heating a carrier gas upstream of the reagent cartridge 2200. During operation of the reaction device 2000, the reaction device 2000 is configured to heat the solid reagent based on a predetermined solid reagent temperature (T r ) and the second temperature reading 2420 to adjust the preheater temperature (T ph ), and based on the solid reagent temperature (T r ) and the first temperature reading 2410 to adjust the box heater temperature (T ch ). Typically, a reaction device configured to adjust the preheater temperature based on a comparison between a predetermined (target) solid reagent temperature and a second temperature reading and to adjust the box heater temperature based on a comparison between the solid reagent temperature and a first temperature reading can enable the use of heat provided by the preheater to reduce solid reagent temperature variations throughout the reagent chamber. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not be configured to adjust the preheater temperature based on a comparison between a predetermined (target) solid reagent temperature and a second temperature reading, and / or to adjust the box heater temperature based on a comparison between the solid reagent temperature and the first temperature reading.

[0073] The reaction device 2000 includes a temperature control unit 2400, which is operably coupled to a first temperature sensor and a second temperature sensor of the reagent box 2200 for receiving a first temperature reading 2410 and a second temperature reading 2420, respectively, and is also coupled to a box heater 2500 and a preheater 2600 for heating the reagent box 2200 and the carrier gas 1003 upstream of the reagent box 2200, respectively.

[0074] exist Figure 2In the embodiment, the reaction device 2000 is configured to maintain a predetermined solid reagent temperature (T r ). Typically, closed-loop control can be achieved, for example, using proportional (P) control, which can be optionally supplemented with integral (I) and / or differential (D) control terms. In other embodiments according to the second aspect and / or the fourth aspect, the reaction 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.

[0075] exist Figure 2 In the embodiment, T r It may be about 35° C. In other embodiments according to the second aspect and / or the fourth aspect, any suitable solid reagent temperature may 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.

[0076] Figure 2 The cartridge heater 2500 of the embodiment is implemented as a transverse electric heater, specifically as a silicone heating pad surrounding the reagent chamber of the reagent cartridge 2200. The cartridge heater 2500 can be fastened to the reagent cartridge 2200 using a fastening means such as an adhesive, whereby the cartridge heater 2500 can form a part of the reagent cartridge 2200. In other embodiments according to the second aspect and / or the fourth aspect, the cartridge heater can be implemented in any suitable manner, for example, as a transverse electric heater, such as a heating pad surrounding the reagent chamber. In any embodiment according to the first aspect and / or the third aspect, the cartridge heater can be implemented as part of the reagent cartridge.

[0077] Figure 2 The reaction device 2000 of the embodiment further includes a reagent conduit heater 2710, and the temperature control unit 2400 is operatively connected to the reagent conduit heater 2710 to heat the reagent gas conduit 2700. In other embodiments according to the second aspect and / or the fourth aspect, the reaction device may or may not include a reagent conduit heater, and the temperature control unit may or may not be operatively connected to the reagent conduit heater to heat the reagent gas conduit.

[0078] exist Figure 2In an embodiment of the present invention, 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, wherein the temperature control unit is operatively coupled to a reagent conduit heater to heat the reagent gas conduit, any suitable reagent gas conduit temperature may be used. For example, in some such embodiments, the temperature control unit may be configured to maintain the temperature of the reagent gas conduit in a range from 30°C to 200°C, or from 50°C to 190°C, or from 100°C to 180°C.

[0079] Figure 2 The reaction device 2000 of the embodiment forms an embodiment of a reaction device, which includes a reagent gas conduit for extracting a reagent-carrier gas mixture from a reagent test kit 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 reaction device may include or not include a reagent gas conduit for extracting a reagent-carrier gas mixture from a reagent test kit and a reagent conduit heater for heating the reagent gas conduit.

[0080] Figure 3 A simplified proportional closed-loop temperature control algorithm 3000 is shown, according to which a reaction device, such as Figure 2 The reaction device 2000 of the embodiment maintains a predetermined temperature T based on the first temperature reading and the second temperature reading. r Naturally, the reaction apparatus according to the second and / or fourth aspects may utilize any suitable temperature control algorithm, which may be used in conjunction with Figure 3 The temperature control algorithm 3000 may be the same, similar or different.

[0081] Figure 3 The temperature control algorithm 3000 includes a method for initializing the preheater temperature (T ph ) and the box heater temperature (T ch )'s initialization step 3100, preheater control step 3200 and box heater control step 3300.

[0082] During the preheater control step 3200, a second temperature reading indicative of the temperature within the gas injection chamber is compared to a predetermined solid reagent temperature (T r On the one hand, if the second temperature reading is higher than T r , then T ph decreases, and the temperature control algorithm 3000 returns to the beginning of the preheater control step 3200. On the other hand, if the second temperature reading is below T r , then T ph increases, and the temperature control algorithm 3000 returns to the beginning of the preheater control step 3200.

[0083] During the cartridge heater control step 3300, a first temperature reading indicative of the temperature inside the reagent chamber is compared to T r On the one hand, if the first temperature reading is higher than T r , then T ch decreases, and the temperature control algorithm 3000 returns to the beginning of the preheater control step 3200. On the other hand, if the first temperature reading is below T r , then T ch increases, and the temperature control algorithm 3000 returns to the beginning of the preheater control step 3200.

[0084] It is obvious to those skilled in the art that the basic idea of ​​the invention can be implemented in various ways as technology advances. Therefore, the present invention and its embodiments are not limited to the above-described embodiments, but they can be varied within the scope of the claims.

[0085] It should be understood that any benefits and advantages described above may relate to one embodiment or may relate to several embodiments. The embodiments are not limited to those that solve any or all of the problems described, or those that have any or all of the benefits and advantages described.

[0086] The term "comprising" is used in this specification to indicate including the features or actions that follow, without excluding the existence of one or more additional features or actions. It will also be understood that references to "an" item refer to one or more of these items.

[0087] Reference Mark

[0088] Carrier gas mass flow rate

[0089] Reagent output mass flow rate

[0090] T r Solid reagent temperature

[0091] T ph Preheater temperature

[0092] T ch Cartridge heater temperature

[0093] W rc Reagent chamber width

[0094] L rc Reagent chamber length

[0095] 1000 Kit 1510 First Temperature Sensor

[0096] 1001 solid reagent

[0097] 1002 reagent gas 1520 second temperature sensor

[0098] 1003 carrier gas 1530 third temperature sensor

[0099] 1004 Reagent-Carrier Gas Mixture 2000 Reaction Device

[0100] 1005 Carrier gas flow direction 2001 Blockage

[0101] 1100 at least one pressure sensor 2100 reagent kit holder

[0102] 1110 First Pressure Sensor 2200 Kit

[0103] 1120 second pressure sensor 2300 pressure control unit

[0104] 1130 Third pressure sensor 2310 At least one box pressure reading

[0105] 1200 reagent chamber

[0106] 1210 Sintered filter 2311 First pressure reading

[0107] 1220 mesh screen 2312 second pressure reading

[0108] 1300 Gas injection chamber

[0109] 1310 Carrier gas inlet 2400 Temperature control unit

[0110] 1400 Gas injection chamber

[0111] 1410 Reagent-carrier gas mixture outlet 2410 First temperature reading

[0112] 2420 Second temperature reading 2810 Carrier gas flow controller

[0113] 2500 Cartridge Heater 2900 Flow Reactor

[0114] 2600 Preheater 3000 Temperature Control Algorithm

[0115] 2700 Reagent Gas Tube

[0116] 2710 Reagent Tube Heater 3100 Initialization Steps

[0117] 2720 ​​reagent catheter mass flow meter 3200 preheater control steps

[0118] 2800 Carrier Gas Tube 3300 Box Heater Control Procedure

Claims

1. A reagent kit (1000) for sublimating a solid reagent (1001) to form a reagent gas (1002), and for mixing the reagent gas (1002) with a flowing carrier gas (1003) to form a reagent-carrier gas mixture (1004), the reagent kit (1000) comprising a reagent chamber (1200) for storing the solid reagent (1001) and at least one pressure sensor (1100) for measuring the internal pressure of the reagent kit (1000); It is characterized in that The reagent kit (1000) includes a gas injection chamber (1400), which is located downstream of the reagent chamber (1200) and is used to spray the reagent-carrier gas mixture (1004) out of the reagent kit (1000), and the at least one pressure sensor (1100) includes a second pressure sensor (1120), which is configured to measure the pressure within the gas injection chamber (1400).

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

3. The test kit (1000) according to any one of the preceding claims, comprises a gas injection chamber (1300), a first temperature sensor (1510) and a second temperature sensor (1520), wherein the gas injection chamber (1300) is located upstream of the reagent chamber (1200) and is used to inject a carrier gas (1003) into the test kit (1000), the first temperature sensor (1510) is configured to measure the temperature inside the reagent chamber (1200), and the second temperature sensor (1520) is configured to measure the temperature inside the gas injection chamber (1300).

4. A reaction device (2000), comprising a reagent kit holder (2100), wherein the reagent kit holder (2100) is used to hold a reagent kit (2200) according to any one of the preceding claims during operation of the reaction device (2000), and the reaction device (2000) is configured to receive at least one box pressure reading (2310) indicating the internal pressure of the reagent kit (2200) from the at least one pressure sensor (1100) of the reagent kit (2200).

5. The reaction device (2000) according to claim 4, wherein: The reaction device (2000) is configured to adjust the carrier gas mass flow rate based on at least a portion of the at least one cartridge pressure reading (2310). To maintain a predetermined reagent output mass flow rate from the reagent cartridge (2200) 6. The reaction device (2000) according to claim 5, wherein: The reaction device (2000) is configured to adjust the carrier gas mass flow rate based on at least a first pressure reading (2311) indicating the internal pressure of the reagent chamber (1200) of the reagent cartridge (2200).

7. The reaction device (2000) according to any one of claims 4 to 6, wherein: The reaction device (2000) is configured to detect the formation of a blockage (2001) downstream of the reagent cartridge (2200) based on at least a portion of the at least one cartridge pressure reading (2310).

8. The reaction device (2000) according to claim 7, wherein: The reaction device (2000) is configured to detect the formation of the blockage (2001) based on at least a second pressure reading (2312) indicating the internal pressure of the gas injection chamber (1400) of the reagent cartridge (2200).

9. The reaction device (2000) according to any one of claims 4 to 8, wherein: The reaction device (2000) is configured to produce carbon-based high-aspect ratio molecular structure HARMS, 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 nanosheets.

10. The reaction device (2000) according to any one of claims 4 to 9, wherein: The kit (2200) is configured to form a reagent-carrier gas mixture (1004) comprising one or more catalyst particle precursors, such as an iron-containing organometallic or metal-organic compound, 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 organic metals or metal-organic compounds, such as nickelocene (Ni(C5H5)2); and / or one or more cobalt-containing organic metals or metal-organic compounds, such as cobaltocene (Co(C5H5)2), as the reagent gas (1002).

11. A reaction device (2000) according to any one of claims 4 to 10, when dependent on claim 3, the reaction device (2000) is configured to receive a first temperature reading (2410) indicating the internal temperature of the reagent chamber (1200) from the first temperature sensor (1510) and to receive a second temperature reading (2420) indicating the internal temperature of the gas injection chamber (1300) from the second temperature sensor (1520).

12. The reaction device (2000) according to claim 11, wherein: The reaction 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 .

13. The reaction device (2000) according to claim 12, wherein: The reaction device (2000) comprises 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 reaction device (2000) is configured as follows: a) Based on the solid reagent temperature T r The preheater temperature T is adjusted by comparing the second temperature reading (2420) with the ph ; as well as b) Based on the solid reagent temperature T r The box heater temperature T is adjusted by comparing with the first temperature reading (2410). ch .

14. The reaction device (2000) according to any one of claims 11 to 13, wherein: The reaction device (2000) includes 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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