Apparatus and method for producing catalyst particles

Abstract

The present disclosure relates to an apparatus and method for producing catalyst particles and high aspect ratio molecular structure networks. The apparatus 1000 includes a flow reactor 1100 and a laminar flow injector 1200 configured to introduce a catalyst particle precursor 1201 into the flow reactor 1100. The laminar flow injector 1200 includes a temperature controlled flow straightener 1210 disposed upstream of the flow reactor 1100.

Description

[Technical field]

[0001] The present disclosure relates to the production of catalyst particles. Additionally, the present disclosure relates to the synthesis of carbon-based high aspect ratio molecular structures, particularly by floating catalyst chemical vapor deposition. [Background technology]

[0002] Films containing networks of carbon-based High-Aspect-Ratio Molecular Structures (HARMS), such as carbon nanotubes and carbon nanobuds, can be used in a variety of applications where high electrical conductivity and optical transmittance films are required.

[0003] Various methods have been developed to synthesize HARMS. One of the most promising synthetic methods for industrial-scale production of HARMS is the so-called Floating-Catalyst Chemical Vapor Deposition (FCCVD) due to its low cost, high throughput, and high degree of control achievable by FCCVD over various structural parameters of the synthesized HARMS, such as length, diameter, and / or functional group density.

[0004] In FCCVD, catalyst composition and size are crucial processing parameters that greatly affect the morphology and properties of the synthesized HARMS. Although FCCVD synthesis methods have already been utilized to form HARMS films with low sheet resistances of about 100 Ω / sq at optical transmittances of over 95%, improved control of catalyst composition and size may lead to further improvements in the properties of FCCVD grown HARMS networks.

[0005] In light of the above, it may be desirable to develop new solutions related to methods for producing catalyst particles. Summary of the Invention

[0006] This Summary is provided to introduce a selection of 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.

[0007] According to a first aspect, there is provided an apparatus for producing catalyst particles, the apparatus comprising a flow reactor and a laminar flow injector configured to introduce a catalyst particle precursor into the flow reactor, the laminar flow injector including a temperature controlled flow straightener disposed upstream of the flow reactor.

[0008] According to a second aspect, there is provided a method for producing catalyst particles, the method comprising introducing a catalyst particle precursor into a flow reactor through a temperature controlled flow straightener disposed upstream of the flow reactor.

[0009] It should be specifically understood that catalyst particles may be produced according to any method according to the second aspect using the apparatus according to the first aspect. Similarly, the apparatus according to the first aspect may be provided with means for producing catalyst particles according to any method according to the second aspect.

[0010] In one embodiment, the apparatus for producing catalyst particles and / or the method for producing catalyst particles is implemented as an apparatus for producing high aspect ratio molecular structures (HARMS) and / or a method for producing HARMS.

[0011] According to a third aspect, there is provided a HARMS network comprising carbon-based HARMS obtained by the apparatus and method according to the previous embodiment.

[0012] It should be specifically understood that the apparatus for producing HARMS according to the first aspect and / or the method for producing HARMS according to the second aspect may be used to produce a HARMS network according to the third aspect.

[0013] The present disclosure will be further understood from the following detailed description read in light of the accompanying drawings. [Brief description of the drawings]

[0014] [Figure 1] FIG. 1 shows an apparatus for producing catalyst particles. [Diagram 2] FIG. 2 shows a partial cross-sectional view of the device of FIG. [Diagram 3] FIG. 1 illustrates a method for producing catalyst particles. [Figure 4] FIG. 1 illustrates a HARMS network. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0015] Unless specifically stated to the contrary, any of the foregoing drawings may not be drawn to scale, such that any element in said drawing may be drawn inaccurately in proportion to other elements in said drawing to emphasize certain structural aspects of said drawing embodiments.

[0016] Furthermore, corresponding elements in any two of the aforementioned drawing embodiments may be out of proportion to each other in the two drawings to highlight certain structural aspects of the two drawing embodiments.

[0017] Detailed Description With respect to the apparatus and methods discussed in this detailed description, please note the following.

[0018] Throughout this specification, "high aspect ratio molecular structures" or "HARMS" may refer to nanostructures, i.e., structures 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 structures having dimensions in two perpendicular directions that are orders of magnitude significantly different. For example, HARMS may have a length that is tens or hundreds of times greater than its thickness and / or width.

[0019] Further, "carbon-based" HARMS may refer to HARMS that are composed primarily of carbon (C). Additionally or alternatively, carbon-based HARMS may refer to HARMS that include 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% carbon. In general, carbon-based HARMS may be doped, for example, with non-carbon dopants, to alter their electrical and / or thermal properties. Examples of carbon-based HARMS include carbon nanotubes, carbon nanobuds, graphene nanoribbons, and combinations thereof.

[0020] In the present disclosure, a "high aspect ratio molecular structure network" or "HARMS network" may refer to a plurality of interconnected HARMS. In general, the HARMS network may form a solid and / or monolithic material on a macroscopic scale, and 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 may or may not have high electrical conductivity.

[0021] As used herein, a "film" may refer to a structure having a lateral dimension substantially greater than its thickness. In general, a film may have any suitable shape, for example, a flat and / or smooth shape or a curved and / or uneven shape.

[0022] Throughout this specification, "catalyst particles" may refer to particulate bodies suitable for enhancing the rate of catalytically mediated reactions. Additionally or alternatively, catalyst particles may refer to particles suitable for heterogeneous catalysis. Additionally or alternatively, catalyst particles may refer to pieces of particulate catalyst material suitable for catalyzing the production of carbon-based HARMS, for example, by chemical vapor deposition, e.g., floating catalyst chemical vapor deposition (FCCVD). Generally, catalyst particles may comprise, consist essentially of, or consist of one or more transition metals, such as iron (Fe), cobalt (Co), and / or nickel (Ni). Typically, catalyst particles may have any suitable diameter, for example, a diameter ranging from 0.1 nm to 300 nm, or from 1 nm to 200 nm, or from 5 nm to 100 nm, or from 10 nm to 50 nm.

[0023] FIG. 1 shows a schematic representation of an apparatus 1000 for producing catalyst particles, and FIG. 2 shows a partial cross-sectional view of the apparatus 1000 along the plane II-II shown in FIG.

[0024] In the embodiment of FIGS. 1 and 2, the apparatus 1000 includes a flow reactor 1100 .

[0025] As used herein, a "flow reactor" may refer to a reactor into which one or more catalyst particle precursors, optionally one or more reactants such as a carbon source, and / or one or more auxiliary substances, e.g., catalysts and / or growth promoters, e.g., sulfur (S), phosphorus (P), nitrogen (N), one or more sulfur-containing compounds, e.g., hydrogen sulfide (HS), carbon disulfide (CS), and / or thiophenes (CHS), one or more phosphorus-containing compounds, e.g., phosphanes (PH), one or more nitrogen-containing compounds, e.g., ammonia (NH) and / or nitric oxide (NO), and / or redox agents, e.g., oxygen (O), water (H0), carbon dioxide (CO), and / or hydrogen (H), are introduced, e.g., continuously introduced, and from which 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 reactants are passed and in which a catalytic reaction takes place. Typically, a flow reactor may be formed from any suitable material, for example, stainless steel, fused silica, or fused quartz.

[0026] In the embodiment of FIGS. 1 and 2, the apparatus 1000 further includes a laminar flow injector 1200 configured to introduce a catalyst particle precursor 1201 into the flow reactor 1100 .

[0027] Throughout this disclosure, a "precursor" may refer to a chemical from which another chemical or other product may be formed. In general, a precursor may be used in any suitable state of matter, e.g., solid, gas, or liquid state. Of course, a "catalyst particle precursor" may therefore refer to a precursor for forming a catalyst particle. Additionally or alternatively, the catalyst particle precursor may comprise one or more iron-containing organometallic or organometallic compounds, such as ferrocene (Fe(CH)), iron pentacarbonyl (Fe(CO)), and / or iron(II) phthalocyanine (C 32 H 16FeN8), and / or one or more nickel-containing organometallic or organometallic compounds, such as nickelocene (Ni(C5H5)2), and / or one or more cobalt-containing organometallic or organometallic compounds, such as cobaltocene (Co(C5H5)2).

[0028] As used herein, a "laminar flow injector" or "laminar flow gas distributor" may refer to a device configured to introduce one or more catalyst particle precursors, and optionally one or more reactants and / or one or more further auxiliary materials, e.g., catalysts, into a flow reactor. Additionally or alternatively, a laminar flow injector may refer to a device suitable or configured to introduce one or more fluids, e.g., gases and / or aerosols, into a flow reactor such that a laminar flow profile is maintained at the upstream end of said flow reactor.

[0029] As used herein, a "laminar flow profile" maintained at a particular location in a flow reactor may refer to maintaining a Reynolds number (Re) at said location of 2300 or less, or 2100 or less, or 2000 or less.

[0030] In the embodiment of Figures 1 and 2, the laminar flow injector 1200 includes a temperature controlled flow straightener 1210 disposed upstream of the flow reactor 1100. In general, a laminar flow injector including a temperature controlled flow straightener upstream of a flow reactor of an apparatus for producing catalyst particles may provide improved control of both flow characteristics and temperature of catalyst particle precursors in said flow reactor, which in turn may result in increased control over nucleation of catalyst nanoparticles in said flow reactor. Additionally or alternatively, a laminar flow injector including a temperature controlled flow straightener upstream of a flow reactor of an apparatus for producing carbon-based HARMS may enable production of HARMS networks with a predetermined optical transmittance and reduced sheet resistance.

[0031] Throughout this disclosure, a "flow straightener" or "honeycomb" may refer to a device or structure suitable or configured to reduce, minimize, or eliminate swirl from a flow of one or more fluids and / or one or more aerosols. Additionally or alternatively, a "flow straightener" or "honeycomb" may refer to a device suitable or configured to reduce, minimize, or eliminate asymmetry in such flows.

[0032] Further, a flow straightener being disposed "upstream" of a flow reactor may refer to the flow reactor including an upstream end, and the flow straightener being disposed in a counter-flow direction from the upstream end. Additionally or alternatively, a flow straightener being disposed upstream of a flow reactor may refer to the flow straightener being configured to discharge catalyst particle precursors in a jetting direction, and the flow reactor including an upstream end from the flow straightener in the jetting direction. Additionally or alternatively, a flow straightener being disposed upstream of a flow reactor may refer to the flow reactor being disposed outside of the flow reactor.

[0033] As used herein, a device or structure of an apparatus or part thereof is "temperature controlled" may refer to the temperature of said device or structure being maintained within a predetermined temperature range during operation of said apparatus. Typically, a temperature within such a predetermined temperature range may be different from the ambient temperature at the location of said apparatus and / or part thereof. In general, a temperature-controlled device or structure of an apparatus or part thereof may or may not be thermally coupled to one or more heating elements for heating said temperature-controlled device or structure.

[0034] The apparatus 1000 of the embodiments of Figures 1 and 2 may be implemented as a continuous flow apparatus. In other embodiments, the apparatus for producing catalyst particles may or may not be implemented as a continuous flow apparatus. For example, in some embodiments, the apparatus for producing catalyst particles may be implemented as a batch apparatus.

[0035] 1 and 2, the flow reactor 1100 has an upstream end 1101 and the laminar flow injector 1200 is configured to introduce catalyst particle precursor 1201 into the flow reactor 1100 such that a Re at the upstream end 1101 is maintained at or below 2300. In other embodiments, the laminar flow injector may or may not be configured in this manner. For example, in some embodiments, the laminar flow injector may be configured to maintain a Re at or below 2300, or below 2100, or below 2000 at the upstream end of the flow reactor.

[0036] 1 and 2 may be Fe(C5H2)2. In other embodiments, any suitable catalyst particle precursor may be used.

[0037] 1 and 2, the flow reactor 1100 is tubular. In particular, the flow reactor 1100 includes a right cylindrical first section 1103 and a tapered second section 1104 extending from the first section 1103. In general, a tubular flow reactor may provide improved control of flow characteristics of catalyst particle precursors in the flow reactor. In other embodiments, the flow reactor may have any suitable shape, e.g., tubular.

[0038] Throughout this disclosure, the term "tubular" should be interpreted broadly. Thus, the term tubular may refer to any elongated hollow shape that may have any suitable cross-sectional shape. An element having a tubular shape may or may not have a circular, substantially circular, elliptical, or polygonal cross-sectional shape. Additionally or alternatively, a tubular element may or may not be at least partially tapered, cylindrical, and / or curvilinear.

[0039] 1 and 2 includes fused silica. In other embodiments, the flow reactor may include, consist essentially of, or consist of any suitable material, such as fused silica or quartz.

[0040] In the embodiment of FIG. 1 and FIG. 2, the flow straightener 1210 includes a flow straightener body 1211 that defines a plurality of flow paths 1212 that extend parallel to one another. In general, a flow straightener including a flow straightener body that defines a plurality of flow paths may facilitate maintaining a laminar flow profile at the upstream end of the flow reactor. Additionally or alternatively, a flow straightener including a flow straightener body that defines a plurality of flow paths may facilitate uniform transfer of heat from at least one heating element through the flow straightener into the catalyst particle precursor introduced into the flow reactor by the laminar flow injector, which in turn may enable the formation of catalyst particles with a narrower size distribution. In other embodiments, the flow straightener may be implemented in any suitable manner. For example, in some embodiments, the flow straightener may include a flow straightener body that defines a plurality of flow paths that extend parallel to one another.

[0041] The flow straightener body 1211 of the embodiment of Figures 1 and 2 comprises stainless steel. In general, a flow straightener body formed from a material having a higher thermal conductivity may further facilitate uniform heat distribution to the catalyst particle precursor introduced into the flow reactor by the laminar flow injector. In other embodiments, the flow straightener body may comprise, consist essentially of, or consist of any suitable material, for example, a metal such as stainless steel and / or titanium.

[0042] In the embodiment of FIG. 1 and FIG. 2, the plurality of channels 1212 are configured to guide the catalyst particle precursor 1201 toward the jetting direction 1213, and the flow straightener body 1211 has a thickness (h) measured along the jetting direction 1213 of about 20 centimeters (cm). fs In other embodiments, the rectifier body may have any suitable thickness, such as, for example, a thickness of 2 cm or more, or 5 cm or more, or 10 cm or more, and / or a thickness of 100 cm or less, or 50 cm or less, or 30 cm or less.

[0043] 1 and 2, the laminar flow injector 1200 includes at least one heating element 1220 for heating the flow straightener 1210. In particular, the at least one heating element 1220 in the embodiment of Figures 1 and 2 includes an electric lateral heating element 1221 and an electric internal heating element 1222. In general, a laminar flow injector that includes at least one heating element for heating the flow straightener may facilitate maintaining the temperature of the flow straightener above ambient temperature.

[0044] In other embodiments, the laminar flow injector may or may not include at least one heating element for heating the flow straightener, e.g., a lateral heating element such as a band heater and / or an internal heating element, one or more of which may be an electric heating element. In some embodiments, the laminar flow injector may include a radiant heater, e.g., a laser source, and / or an induction heater in addition to or as an alternative to the electric heating element.

[0045] In the embodiment of FIGS. 1 and 2, the lateral heating element 1221 is specifically embodied as a band heater surrounding the rectifier 1210 , and the internal heating element 1222 is disposed within the rectifier body 1211 .

[0046] In other embodiments where the at least one heating element includes a lateral heating element and / or an internal heating element, the lateral heating element may or may not surround the rectifier and / or the internal heating element may be disposed at least partially within the rectifier body. For example, in some embodiments, the lateral heating element may extend only partially around the periphery of the rectifier, and the at least one heating element may optionally include two or more such lateral heating elements.

[0047] The laminar flow injector 1200 of the embodiment of FIG. 1 and FIG. 2 is fs ) and the device 1000 has a T of about 275° C. fs and an injector temperature control unit 1300 operatively coupled to each of the temperature sensor 1230 and the lateral heating element 1221 and the electrical internal heating element 1222 to maintain a temperature within a suitable temperature range of the flow straightener of a laminar flow injector of an apparatus for producing catalyst particles.

[0048] In other embodiments in which the laminar flow injector of the apparatus for producing catalyst particles includes a temperature sensor for measuring the temperature of the flow straightener, the apparatus may or may not include an injector temperature control unit operably coupled to the temperature sensor and at least one heating element to maintain the temperature within any suitable temperature range, e.g., 100°C to 700°C, or 200°C to 600°C, or 250°C to 400°C.

[0049] As used herein, a "control unit" may refer to a device, e.g., an electronic device, having at least one specified function related to determining and / or influencing an operating condition, status or parameter associated with another device, unit or element. A control unit may or may not form part of a multi-function control system.

[0050] Furthermore, a control unit "operably coupled" to a device, unit or element may refer to a control unit having at least one specified function related to determining and / or influencing an operating condition, status or parameter associated with said device, unit or element.

[0051] A control unit "configured" to execute a process may refer to the capability and suitability of the control unit for such a process. This may be accomplished in various ways. For example, a 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 that, when executed in the at least one processor, cause the processor to execute the process. Additionally or alternatively, any functionally described features of the control unit may be implemented, at least in part, by one or more hardware logic components. For example, without limitation, exemplary types of suitable 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 control unit may generally be operated according to any suitable principles and by any suitable circuits and / or signals known in the art.

[0052] In the embodiment of FIGS. 1 and 2, the laminar flow injector 1200 includes at least one gas inlet 1240, and the apparatus 1000 includes an injector flow control unit 1400 configured to control the volumetric flow rate through the at least one gas inlet 1240, thereby controlling the residence time (t cat) is about 1620 milliseconds (ms). In general, a longer residence time of the catalyst particle precursor in a temperature controlled straightener can reduce temperature variations in the catalyst particle precursor introduced into a flow reactor, whereas a shorter residence time can reduce thermal decomposition of the catalyst particle precursor in the straightener.

[0053] In other embodiments in which the laminar flow injector of the apparatus for producing catalyst particles has at least one gas inlet, the apparatus may or may not include an injector flow control unit configured to control the volumetric flow rate through the at least one gas inlet such that any suitable residence time of the catalyst particle precursor in the flow straightener is maintained. For example, in some such embodiments, the residence time of the catalyst particle precursor in the flow straightener may be 150 ms or more, or 400 ms or more, or 800 ms or more, and / or 8500 ms or less, or 4000 ms or less, or 2500 ms or less.

[0054] The apparatus 1000 of the embodiment of Figures 1 and 2 may be implemented as an apparatus for producing carbon-based HARMS. In particular, the apparatus 1000 of the embodiment of Figures 1 and 2 may include a means for introducing a carbon source 1202 into the flow reactor 1100. In other embodiments where the apparatus for producing catalyst particles is implemented as an apparatus for producing carbon-based HARMS, the apparatus may or may not include a means for introducing a carbon source into the flow reactor into which the catalyst particle precursor is introduced. For example, in some embodiments, the apparatus for producing carbon-based HARMS may include a first flow reactor for producing catalyst particles and an additional flow reactor for producing carbon-based HARMS, disposed downstream of the first flow reactor and configured to receive catalyst particles from the first flow reactor.

[0055] 1 and 2 may consist essentially of carbon monoxide (CO). In other embodiments, the carbon source may consist essentially of CO and / or one or more hydrocarbons, such as one or more aliphatic hydrocarbons, such as methane (CH), ethene (C2H4), and / or ethyne (C2H2), one or more aromatic hydrocarbons, such as benzene (C6H6), toluene (C6H5CH3), dimethylbenzene (C6H4(CH3)2), and / or trimethylbenzene (C6H3(CH3)3), one or more alcohols, such as methanol (CH3OH), ethanol (C2H5OH), and / or octanol (C8H 17 The composition may comprise, consist essentially of, or consist of any suitable chemical compound, such as dimethylaminoethyl ether (DMSO) or dimethylaminoethyl ether (DMSO) (OH).

[0056] In the embodiment of Figures 1 and 2, the laminar flow injector 1200 of the embodiment of Figures 1 and 2 is configured to introduce a carbon source 1202 into the flow reactor 1100. In other embodiments in which the apparatus includes a means for introducing a carbon source into a flow reactor into which a catalyst particle precursor is introduced, the laminar flow injector may or may not be configured to introduce said carbon source into said flow reactor. In some embodiments, the apparatus for producing catalyst particles may include a carbon source inlet separate from said laminar flow injector for supplying a carbon source to the flow reactor, as an alternative or in addition to a laminar flow injector.

[0057] To mix the catalyst particle precursor 1201 and the carbon source 1202 prior to injection into the flow reactor 1100, the laminar flow injector 1200 includes a mixing chamber 1250 upstream of the flow straightener 1210 and a pre-mix chamber 1260 upstream of the mixing chamber 1250. In general, a laminar flow injector that includes both a mixing chamber upstream of the flow straightener and a pre-mix chamber upstream of said mixing chamber may enhance mixing of the catalyst particle precursor and the carbon source, which in turn may facilitate enhanced uniformity of carbon-based HARMS produced by an apparatus including such a laminar flow injector.

[0058] In other embodiments where a laminar flow injector is configured to introduce a catalyst particle precursor and a carbon source into a flow reactor, the laminar flow injector may or may not include a mixing chamber upstream of a flow straightener and a pre-mix chamber upstream of the mixing chamber for mixing the catalyst particle precursor and the carbon source. For example, in some such embodiments, the laminar flow injector may include a mixing chamber upstream of a flow straightener without the presence of a pre-mix chamber.

[0059] 1 and 2, the apparatus 1000 includes a precursor conduit 1510 for supplying a catalyst particle precursor 1201 into the laminar flow injector 1200. The precursor conduit 1510 is configured to control the temperature of the precursor conduit 1510 (T pc ) and a precursor conduit heating element 1512 for heating the precursor conduit 1510. The apparatus 1000 has a T pc The precursor conduit further includes a conduit temperature control unit 1600 operably coupled to the precursor conduit temperature sensor 1511 and the precursor conduit heating element 1512 to maintain

[0060] In general, maintaining the temperature of the precursor conduit at an appropriate predetermined temperature may further reduce temperature variations in the catalyst particle precursor introduced into the flow reactor.

[0061] In other embodiments where an apparatus for producing catalyst particles includes a precursor conduit for delivering catalyst particle precursor into a laminar flow injector, the precursor conduit may or may not include a precursor conduit temperature sensor for measuring a temperature of the precursor conduit and a precursor conduit heating element for heating the precursor conduit, and the apparatus may or may not further include a conduit temperature control unit operatively coupled to the precursor conduit temperature sensor and the precursor conduit heating element for maintaining the temperature within any suitable temperature range, for example, between 30° C. and 200° C., or between 50° C. and 190° C., or between 100° C. and 180° C. For example, in some embodiments, a precursor conduit heating element having a constant heating power per unit length of conduit may be used, such that a particular conduit temperature control unit may be omitted.

[0062] The apparatus 1000 of the embodiment of FIG. 1 and FIG. 2 further includes a carbon source conduit 1520 for feeding the carbon source 1202 into the laminar flow injector 1200, the carbon source conduit 1520 controlling the temperature of the carbon source conduit 1520 (T CC ) and a carbon source conduit heating element 1522 for heating the carbon source conduit 1520. The conduit temperature control unit 1600 is configured to regulate a T CC The carbon source conduit is operably coupled to a carbon source conduit temperature sensor 1521 and a carbon source conduit heating element 1522 to maintain

[0063] In other embodiments in which the apparatus for producing catalyst particles includes a carbon source conduit for feeding a carbon source into a laminar flow injector, the carbon source conduit may or may not include a carbon source conduit temperature sensor for measuring a temperature of the carbon source conduit and a carbon source conduit heating element for heating the carbon source conduit, and a conduit temperature control unit may or may not be operatively coupled to the carbon source conduit temperature sensor and the carbon source conduit heating element to maintain the temperature within any suitable temperature range, for example, between 30°C and 200°C, or between 50°C and 190°C, or between 100°C and 180°C.

[0064] Although not explicitly shown in Figure 1, the catalyst particle precursor and / or carbon source may be introduced into the flow reactor using one or more carrier gases, such as argon (Ar), helium (He), nitrogen (N2), carbon monoxide (CO), and / or hydrogen (H2). For example, in the embodiments of Figures 1 and 2, H2 may be used as the carrier gas.

[0065] In the embodiment of FIGS. 1 and 2, the apparatus 1000 includes a tube furnace 1700 for holding the flow reactor 1100 such that the upstream portion 1102 of the flow reactor 1100 extends from the tube furnace 1700, and a temperature (T up and a ventilation collar 1800 configured to surround the upstream portion 1102 to adjust the temperature distribution in the flow reactor. In general, an apparatus for producing catalyst particles including such a ventilation collar may enable optimizing the temperature distribution in the flow reactor in a robust and efficient manner.

[0066] In other embodiments in which a flow reactor of an apparatus for producing catalyst particles has an upstream portion and the apparatus includes a tube furnace for holding the flow reactor such that the upstream portion extends from the tube furnace, the apparatus may or may not include a ventilation collar configured to surround at least a portion of the upstream portion to regulate the temperature of the upstream portion during operation of the apparatus.

[0067] 1 and 2 is configured to passively cool the upstream portion 1102 by exposing the upstream portion 1102 to ambient air. In other embodiments, the ventilated collar may or may not be configured to passively cool the upstream portion by exposing the upstream portion to ambient air. For example, in some embodiments, an actively ventilated collar may be used to cool the upstream portion and / or the upstream portion may be exposed to one or more fluids other than air, such as nitrogen, argon, and / or water.

[0068] 1 and 2 is configured to heat the flow reactor 1100 such that the maximum temperature in the flow reactor 1100 is about 1100° C. In other embodiments, the tube furnace may be configured to heat the flow reactor to any suitable maximum temperature, such as a maximum temperature of 700° C. or more, or 800° C. or more, and / or 1300° C. or less, or 1200° C. or less.

[0069] 1 and 2, the tube furnace 1700 is configured to hold the flow reactor 1100 in an upright position. In other embodiments, the tube furnace of the apparatus for producing catalyst particles may be configured to hold the flow reactor in any suitable orientation relative to gravity at the location of the apparatus, such as upright, e.g., (substantially) vertical, or lateral, e.g., (substantially) horizontal.

[0070] It should be understood that the embodiments of the first aspect described above may be used in combination with each other. Some embodiments may be combined with each other to form further embodiments.

[0071] Above, the structural features of the apparatus for producing catalyst particles and its parts are mainly described. Below, more emphasis is placed on the features related to the method for producing catalyst particles. What has been said above about the implementation, definitions, details and advantages related to the apparatus applies mutatis mutandis to the method described below, and vice versa.

[0072] Figure 3 illustrates a method 3000 for producing catalyst particles according to one embodiment. In other embodiments, the method for producing catalyst particles may be the same as, similar to, or different from the method 3000 of the embodiment of Figure 3. In general, the method for producing catalyst particles may include any number of additional processes and / or steps not disclosed herein with respect to the method 3000 of the embodiment of Figure 3.

[0073] The embodiment of the method 3000 of Figure 3 may specifically be performed as a continuous flow process. In other embodiments, the method for producing catalyst particles may or may not be performed as a continuous flow process. For example, in some embodiments, the method for producing catalyst particles may be performed as a batch process.

[0074] As used herein, a "process" may refer to one or more series of steps leading to an end result. Thus, a process may be a single-step or multi-step process. In addition, a process may be divisible into multiple sub-processes, the individual sub-processes of which may or may not share common steps. As used herein, a "step" may refer to measures taken to achieve a given result.

[0075] In the embodiment of FIG. 3, the method 3000 includes introducing 3100 a catalyst particle precursor into a flow reactor through a temperature controlled flow straightener disposed upstream of the flow reactor.

[0076] As shown in Figure 3 using dashed lines, the method 3000 of the embodiment of Figure 3 may optionally further include heating the rectifier (3200). The process of heating the rectifier (3200) of the embodiment of Figure 3 may include maintaining the temperature of the rectifier at about 275°C (3210). In other embodiments, the process of heating the rectifier may include maintaining the temperature of the rectifier (3210) at any suitable temperature, for example, in the range of 100°C to 700°C, or 200°C to 600°C, or 250°C to 400°C.

[0077] In the embodiment of Figure 3, the residence time of the catalyst particle precursor in the flow straightener may be about 1620 milliseconds (ms). In other embodiments, any suitable residence time may be used, such as, for example, a residence time of 150 ms or more, or 400 ms or more, or 800 ms or more, and / or 8500 ms or less, or 4000 ms or less, or 2500 ms or less.

[0078] 3 may alternatively be implemented as a method for producing carbon-based HARMS. In other embodiments, the method for producing catalyst particles may or may not be implemented as a method for producing carbon-based HARMS.

[0079] As shown in Figure 3 using dashed lines, the embodiment method 3000 of Figure 3 may optionally further include the process of introducing a carbon source into the flow reactor (3300). In other embodiments, the method for producing catalyst particles may or may not include the process of introducing a carbon source into the flow reactor.

[0080] The process of introducing a carbon source into a flow reactor (3300) in the embodiment of Figure 3 includes mixing a catalyst particle precursor and a carbon source upstream of a flow straightener (3310). In other embodiments in which the method for producing catalyst particles includes introducing a carbon source into a flow reactor, the process of introducing a carbon source into a flow reactor may or may not include mixing a catalyst particle precursor and a carbon source upstream of a flow straightener.

[0081] As shown in FIG. 3 using dashed lines, the process of mixing the catalyst particle precursor and the carbon source (3310) of the embodiment of FIG. 3 may optionally include a step of premixing the catalyst particle precursor and the carbon source in a premix chamber (3311) and a step of mixing the catalyst particle precursor and the carbon source in a mixing chamber located downstream of the premix chamber (3312).

[0082] In other embodiments, where the method for producing catalyst particles includes introducing a carbon source into a flow reactor, and the process of introducing the carbon source into the flow reactor includes mixing the catalyst particle precursor and the carbon source upstream of a flow straightener, the process of mixing the catalyst particle precursor and the carbon source may or may not include the steps of premixing and mixing the catalyst particle precursor and the carbon source in a premix chamber and a mixing chamber located downstream of the premix chamber, respectively.

[0083] As shown in Figure 3 using dashed lines, the method 3000 of the embodiment of Figure 3 may optionally further include feeding the catalyst particle precursor into the laminar flow injector via a precursor conduit (3400), where the process of feeding the catalyst particle precursor through the precursor conduit includes maintaining a temperature of the precursor conduit at about 50°C (3410). In other embodiments where the method for producing catalyst particles includes feeding the catalyst particle precursor into the laminar flow injector via a precursor conduit, the process of feeding the catalyst particle precursor through the precursor conduit may or may not include maintaining a temperature of the precursor conduit at any suitable predetermined temperature, for example, in the range of 30°C to 200°C, or 50°C to 190°C, or 100°C to 180°C.

[0084] As shown in Figure 3 using dashed lines, the embodiment method 3000 of Figure 3 may optionally further include supporting the flow reactor in a tube furnace such that an upstream portion of the flow reactor extends from the tube furnace (3500). In other embodiments, the method for producing catalyst particles may or may not include supporting the flow reactor in a tube furnace in this manner.

[0085] As shown in Figure 3 using dashed lines, the process of retaining the flow reactor in the tube furnace of the embodiment of Figure 3 (3500) may optionally include providing a ventilation collar surrounding the upstream portion (3510). In other embodiments in which the method for producing catalyst particles includes retaining the flow reactor in the tube furnace such that the upstream portion of the flow reactor extends from the tube furnace, the process of retaining the flow reactor in the tube furnace may or may not include providing a ventilation collar surrounding the upstream portion.

[0086] It should be understood that the embodiments of the second aspect described above may be used in combination with each other. Some embodiments may be combined with each other to form further embodiments.

[0087] 4 shows a HARMS network 4000 consisting essentially of HARMS 4010 obtained by an apparatus for producing carbon-based HARMS according to a first embodiment and a method for producing carbon-based HARMS according to a second embodiment. In other embodiments, the HARMS network may comprise, consist essentially of, or consist of HARMS obtained by an apparatus for producing carbon-based HARMS according to a first embodiment and a method for producing carbon-based HARMS according to a second embodiment. For example, in some embodiments, the HARMS network may include HARMS obtained by an apparatus for producing carbon-based HARMS according to a first embodiment and a method for producing carbon-based HARMS according to a second embodiment, and one or more types of non-carbon-based HARMS, such as metal nanowires, e.g., silver nanowires.

[0088] 4 is disposed as a film 4100 extending over a substrate 4200. In other embodiments, the HARMS network may be disposed in any suitable form, such as a film extending over a substrate or as a free-standing film.

[0089] The example film 4100 of FIG. 4 has a thickness (h f In other embodiments in which the HARMS network is disposed as a film, the film may have any suitable thickness, for example, a thickness of 1 nm or more, or 10 nm or more, or 50 nm or more, or 100 nm or more, and / or a thickness of 1000 nm or less, or 800 nm or less, or 500 nm or less.

[0090] 4, HARMS 4010 comprises a carbon nanotube backbone 4011 covalently bonded to carbon based fullerene-like protuberances 4012 extending from the carbon nanotube backbone 4011. In other embodiments, the HARMS obtained by the apparatus for producing carbon based HARMS according to the first embodiment and the method for producing carbon based HARMS according to the second embodiment may or may not comprise single-wall and / or multi-wall carbon nanotube backbones covalently bonded to carbon based fullerene-like protuberances extending from said carbon nanotube backbone.

[0091] It is obvious to a person skilled in the art that due to the development of technology, the basic concept of the invention can be implemented in various ways. The invention and its embodiments are therefore not limited to the above-mentioned examples, but instead may vary within the scope of the claims.

[0092] It should be understood that any benefits and advantages described above may relate to one embodiment or to several embodiments, and the embodiments are not limited to those that solve any or all of the stated problems or have any or all of the stated benefits and advantages.

[0093] The term "comprising" is used herein to mean including the features or acts that follow the term without excluding the presence of one or more additional features or acts. Further, reference to "an" thing should be understood to refer to one or more of those things. [Explanation of symbols]

[0094] HARMS High aspect ratio molecular structure FCCVD Floating Catalyst Chemical Vapor Deposition Re: Reynolds number T fs Rectifier Temperature T pc Precursor conduit temperature T cc Carbon source conduit temperature T up Upstream temperature t cat Residence time h f Film Thickness h fs Rectifier body thickness 1000 devices 1100 Flow Reactor 1101 Upstream end 1102 Upstream part 1103 First Section 1104 Second Section 1200 Laminar Flow Injector 1201 Catalyst particle precursor 1202 Carbon source 1210 rectifier 1211 Rectifier body 1212 Multiple channels 1213 Injection direction 1220 At least one heating element 1221 Lateral heating element 1222 Internal Heating Element 1230 Temperature Sensor 1240 at least one gas inlet 1250 Mixing Chamber 1260 Premix Chamber 1300 Injector Temperature Control Unit 1400 Injector Flow Control Unit 1510 Precursor Conduit 1511 Precursor conduit temperature sensor 1512 Precursor conduit heating element 1520 Carbon source conduit 1521 Carbon source conduit temperature sensor 1522 Carbon source conduit heating element 1600 Conduit Temperature Control Unit 1700 Tube Furnace 1800 Ventilation Color 3000 ways 3100 Introduce the catalyst particle precursor into the flow reactor through a temperature-controlled flow straightener. 3200 Heating the Rectifier Maintaining the temperature of the 3210 rectifier 3300 Introduce the carbon source into the flow reactor 3310 Mixing the catalyst particle precursor with the carbon source 3311 Premix 3312 Mix 3400 Supplying catalyst particle precursor through precursor conduit 3410 Maintaining the temperature of the precursor conduit Hold the flow reactor in a 3500 tube furnace 3510 Provides ventilation collar 4000 HARMS Network 4010 HARMS 4011 Carbon nanotube main chain 4012 Protrusion 4100 Film 4200 Board

Claims

1. a flow reactor (1100); a laminar flow injector (1200) configured to introduce catalyst particle precursors (1201) into the flow reactor (1100), The laminar flow injector (1200) includes a temperature-controlled flow rectifier (1210) located upstream of the flow reactor (1100). An apparatus (1000) for producing catalyst particles, comprising:

12. An apparatus (1000) for producing catalyst particles, wherein the laminar flow injector (1200) comprises at least one heating element (1220) for heating the flow rectifier (1210).

2. The apparatus (1000) of claim 1, wherein the flow reactor (1100) is tubular.

3. 3. The apparatus (1000) of claim 1 or 2, wherein the flow straightener (1210) comprises a flow straightener body (1211) defining a plurality of flow paths (1212) extending parallel to one another.

4. 3. The apparatus (1000) of claim 1 or 2, wherein the at least one heating element (1220) comprises a lateral heating element (1221) and / or an internal heating element (1222) for heating the rectifier (1210).

5. The laminar flow injector (1200) is configured to ｆｓ and the device (1000) includes a temperature sensor (1230) for measuring the temperature T of the rectifier (1210). ｆｓ 5. The apparatus of claim 4, further comprising an injector temperature control unit operatively coupled to the temperature sensor and the at least one heating element to maintain a temperature in the range of 100°C to 700°C, or 200°C to 600°C, or 250°C to 400°C.

6. The laminar flow injector (1200) includes at least one gas inlet (1240), and the apparatus (1000) is configured to adjust the residence time t of the catalyst particle precursor (1201) in the flow straightener (1210). ｃａｔ 3. The apparatus (1000) of claim 1, comprising an injector flow control unit (1400) configured to control a volumetric flow rate through the at least one gas inlet (1240) such that is 150 ms or more, or 400 ms or more, or 800 ms or more, and / or 8500 ms or less, or 4000 ms or less, or 2500 ms or less.

7. 3. The apparatus according to claim 1, wherein the laminar flow injector is configured to introduce a carbon source into the flow reactor, and the laminar flow injector comprises a mixing chamber upstream of the flow rectifier and a pre-mixing chamber upstream of the mixing chamber for mixing the catalyst particle precursor and the carbon source.

8. The apparatus (1000) includes a precursor conduit (1510) for supplying the catalyst particle precursor (1201) into the laminar flow injector (1200), the precursor conduit (1510) having a temperature T ｐｃ and a precursor conduit heating element (1512) for heating said precursor conduit (1510), and said apparatus (1000) is adapted to measure the temperature T ｐｃ 3. The apparatus (1000) of claim 1 or 2, further comprising a conduit temperature control unit (1600) operatively coupled to the precursor conduit temperature sensor (1511) and the precursor conduit heating element (1512) to maintain a temperature in the range of 30°C to 200°C, or 50°C to 190°C, or 100°C to 180°C.

9. The flow reactor (1100) has an upstream portion (1102), and the apparatus (1000) includes a tube furnace (1700) for holding the flow reactor (1100) such that the upstream portion (1102) extends from the tube furnace (1700), and a temperature T ｕｐ and a ventilation collar configured to surround at least a portion of the upstream portion to regulate a flow rate of the upstream portion.

10. 1. A method (3000) for producing catalyst particles, comprising: Introducing a catalyst particle precursor into the flow reactor through a temperature-controlled flow rectifier located upstream of the flow reactor (3100); and heating a flow straightener (3200) comprising a laminar flow injector configured to introduce the catalyst particle precursor into the flow reactor.

11. 11. The method of claim 10, wherein the process of heating the rectifier comprises maintaining the temperature of the rectifier in the range of 100°C to 700°C, or 200°C to 600°C, or 250°C to 400°C.

12. 12. The method (3000) of claim 10 or 11, wherein the residence time of the catalyst particle precursor in the flow straightener is 150 ms or more, or 400 ms or more, or 800 ms or more, and / or 8500 ms or less, or 4000 ms or less, or 2500 ms or less.

13. 12. The method according to claim 10 or 11, wherein the method comprises introducing a carbon source into the flow reactor, the process of introducing the carbon source into the flow reactor comprising mixing the catalyst particle precursor and the carbon source upstream of the flow straightener, the process of mixing the catalyst particle precursor and the carbon source comprising premixing the catalyst particle precursor and the carbon source in a premixing chamber and a mixing chamber downstream of the premixing chamber, respectively.

14. 12. The method (3000) of claim 10 or 11, wherein the method (3000) comprises supplying (3400) the catalyst particle precursor into the laminar flow injector via a precursor conduit, and wherein the process (3400) of supplying the catalyst particle precursor via a precursor conduit comprises maintaining (3410) a temperature of the precursor conduit in a range of 30°C to 200°C, or 50°C to 190°C, or 100°C to 180°C.

15. 12. The method (3000) of claim 10 or 11, wherein the method (3000) includes holding the flow reactor in a tube furnace (3500) so that an upstream portion of the flow reactor extends from the tube furnace, and the process (3500) of holding the flow reactor in the tube furnace includes providing a ventilation collar (3510) surrounding the upstream portion.

16. 12. The method (3000) of claim 10 or 11, wherein the method (3000) is performed as a method for producing 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.

17. A HARMS network (4000) comprising carbon-based HARMS (4010) obtained by the method (3000) of claim 16.

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