Mold for manufacturing ceramic filling members

Abstract

A mold for producing a filler member from a liquid ceramic composition, the mold comprising a first portion and a second portion, the first portion and / or the second portion having an open mold cavity, the first and second portions operable to engage to form a closed mold cavity, the mold further comprising a reservoir-forming member, the mold operable to be moved from an open position in which the first and second portions are at least partially spaced apart so that the reservoir member forms the reservoir cavity and the mold cavity is open, to a partially closed position in which the position of the reservoir cavity moves relative to the mold cavity and / or the volume of the reservoir cavity is reduced, and further to a closed position in which the first and second portions engage to close the mold cavity.

Description

[Technical field]

[0001] The present invention relates to moulds for use in the manufacture of packing elements for packed beds, in particular supports for catalysts, and supported catalysts. More particularly, the present invention relates to moulds for use in the manufacture of ceramic catalyst supports and supported catalysts for use in processes such as steam reforming and the production of direct-reduced iron. [Background technology]

[0002] Metal catalysts used in industrial processes such as steam reforming and the production of direct reduced iron are more active when finely divided into small particles to increase the metal surface area. A large metal surface area can be maintained during such reactions by spreading the metal particles over a refractory support. Another advantage of using catalyst supports in such processes is that only small amounts of the more expensive catalytic metal are required to be spread over large amounts of inexpensive support material, thereby significantly reducing the cost of catalyst material required on a commercial scale.

[0003] In many such processes, the reactions requiring the catalyst are very fast and are confined to the pellet surface. The reactions are therefore dependent on the geometric surface area of ​​the supported catalyst. Furthermore, supported catalysts with low internal surface area (BET) and very small internal pore volume generally suffer from low activity in such processes. The strength of the support is also important, as damage during loading, operation and discharge of the supported catalyst can reduce activity and increase delays and costs. For example, in the Midrex process for direct reduced iron (DRI), the catalyst is a steam reforming catalyst and can therefore be subjected to high levels of mechanical handling and thermal cycling. Furthermore, the supported catalyst should provide good heat transfer properties while maintaining low pressure drop.

[0004] Supports for catalysts in such industrial processes are typically made by extrusion, pelletizing or granulating ceramic powders, followed by firing of the green bodies.

[0005] However, such methods have been found to provide only limited support geometries and physical characteristics, for example such supports can achieve high strength, but only at the expense of low geometric surface area and poor porosity. Summary of the Invention [Problem to be solved by the invention]

[0006] Thus, there is a need for improved supports for catalysts that have a better combination of desirable properties that can be economically produced. Accordingly, it is an object of embodiments of the present invention to address one or more of the above-mentioned problems or other issues. [Means for solving the problem]

[0007] According to a first aspect of the present invention there is provided a mould for producing a filler member from a liquid ceramic composition, the mould comprising a first part and a second part, the first part and / or the second part comprising an open mould cavity, the first part and the second part being operable to engage to form a closed mould cavity, the mould further comprising a reservoir forming member, the mould being operable to be moved from an open position in which the reservoir member forms the reservoir cavity and the first and second parts are at least partially spaced apart so that the mould cavity is open, to a partially closed position in which the position of the reservoir cavity is moved relative to the mould cavity and / or in which the volume of the reservoir cavity is reduced, and further to a closed position in which the first and second parts are engaged so that the mould cavity is closed.

[0008] According to a second aspect of the present invention there is provided a process for manufacturing packing elements for use in a packed bed comprising the steps of: a. placing a mould comprising a first portion and a second portion, the first portion and / or the second portion comprising an open mould cavity, the mould further comprising a reservoir-forming member, in an open position in which the first and second portions are at least partially spaced apart such that the reservoir member forms a reservoir cavity and the mould cavity is open; b. at least partially filling a reservoir cavity of the mold with a liquid ceramic composition; c. moving the mold to a partially closed position such that the location of the reservoir cavity changes relative to the mold cavity and / or the volume of the reservoir cavity decreases to transfer a portion of the liquid ceramic composition from the reservoir cavity to the open mold cavity; d. moving the mold to a closed position, in which the first and second portions are engaged to close the mold cavity and a portion of the liquid ceramic composition is retained within the closed mold cavity to produce a green body; e. Optionally, heating the green body; f. Removing the green body from the mold; and g. Optionally, firing the green body to produce a filler member.

[0009] According to a third aspect of the present invention there is provided a moulding apparatus for use in producing a filler member from a liquid ceramic composition, suitably for use in the process of the second aspect of the present invention, the moulding apparatus comprising a mould according to the first aspect of the present invention and a guide member operable to position the mould in an open position.

[0010] According to a fourth aspect of the present invention there is provided a packing element for use in a packed bed, preferably for use as a catalyst support in a packed bed reactor, obtainable by a process according to the second aspect of the invention and / or by moulding a liquid ceramic composition according to the first aspect of the invention in a moulding apparatus according to the third aspect of the invention.

[0011] The first and second parts may each comprise an open mold cavity. Suitably, the mold cavities of the first and second parts may be open partial mold cavities, and the first and second parts of the mold are operable to engage such that the partial mold cavity of the first part aligns with the partial mold cavity of the second part to form a closed enlarged mold cavity. As used herein, an "open" mold cavity may mean that the filler member or green body, or a portion thereof, is operable to be removed from the mold cavity through the same aperture through which the liquid ceramic composition is introduced into the mold cavity. As used herein, a "closed" mold cavity may mean that the liquid ceramic composition is held within the mold cavity such that it cannot exit the mold cavity.

[0012] The first and / or second part may include a plurality of open mould cavities. Suitably, each of the first and / or second part may comprise a plurality of open part mould cavities.

[0013] The mould cavity may include texturing operable to form a surface structure on the filler member. Preferably, a surface of the mould cavity operable to contact the liquid ceramic composition during moulding may include texturing.

[0014] The mould cavity may include a pin operable to form a bore in the filler member, such as a bore extending through the filler member. Suitably, the mould cavity may include at least two pins, for example at least three or at least four pins. The pin may be located on a bottom surface of the mould cavity and extend upwardly towards an opening of the mould cavity. The pin may be substantially centrally located on the bottom surface of the mould cavity. The pin may be cylindrical.

[0015] The reservoir member can be operable to form a reservoir cavity capable of receiving and holding the liquid ceramic composition. The reservoir cavity may not be a mold cavity such that in the closed position, the reservoir cavity is not substantially operable to hold a portion of the composition or to form a molded article.

[0016] The reservoir member may comprise a first reservoir member disposed on the first mould part and a second reservoir member disposed on the second mould part, the first and second reservoir members operable to cooperatively engage to form a reservoir cavity. Preferably, the first and second reservoir members may be male and female reservoir members, such that the male reservoir member is operable to be received within the female reservoir member to form the reservoir cavity. The male reservoir member may be in the form of a tongue and the female reservoir member may be in the form of a groove. Preferably, the male and female reservoir members may be operable to form an interference fit when engaged. As used herein, "interference fit" refers to a fit operable to prevent the liquid ceramic composition from passing through the engaged reservoir members.

[0017] The first and / or second mould section may include a reservoir member, preferably a tongue or groove, preferably a longitudinally extending reservoir member, extending along opposite sides of the mould cavity of the mould section. Preferably, the first and second mould sections may each comprise a mould cavity, the first reservoir member comprising a tongue extending along opposite sides of the mould cavity of the mould section and the second reservoir member comprising a groove extending along opposite sides of the mould cavity of the mould section. The reservoir member of the mould section may further comprise a base reservoir member extending between the side reservoir members. The base reservoir member may extend laterally along the mould section. The base member may be located below the mould cavity of the mould section. Suitably, the first reservoir member may comprise a base tongue extending between the opposing side tongues and / or the second reservoir member may comprise a base groove extending between the opposing side grooves. Such a reservoir member configuration may be in the form of a U-shape, with the side reservoir members extending longitudinally along the mould portion and the base reservoir member extending laterally along the mould portion between the side reservoir members. The base reservoir member may provide a bottom inner surface, i.e. a base, of the reservoir cavity in use. The side reservoir members may provide sides of the reservoir cavity in use. The surfaces of the mould portions extending between the side reservoir members may comprise the mould cavity and may provide front and rear surfaces of the reservoir cavity. Typically, the reservoir cavity comprises an opening. The opening may extend between the ends of the side reservoir members that are not connected to the base reservoir member. Suitably, the opening of the reservoir cavity may extend laterally across the mould portion, typically substantially parallel to the base reservoir member.

[0018] Suitably, the first and / or second mould sections may comprise a plurality of mould cavities arranged in groups. The side reservoir members may be arranged to extend along opposite sides of the groups. The base member may be arranged to extend below the groups.

[0019] The reservoir member of the mold part may be disposed in the same plane as the mold cavity. The reservoir member of the mold part may be disposed such that engagement of the reservoir member is operable to align the part mold cavity on the mold part to form an enlarged mold cavity in the closed position.

[0020] As such, when the mold is in the open position, the reservoir members may be operable to receive the liquid ceramic composition through the openings of the reservoir cavities and then engage to form a reservoir cavity operable to hold the liquid ceramic composition within the reservoir cavity. Preferably, the mold cavity may be located within the initial reservoir cavity when the mold is in the open position. The mold cavity may be located outside the initial reservoir cavity when the mold is in the open position. As the mold is moved from the open position to the partially closed position and then to the closed position, the reservoir members of the mold parts may be operable to further engage such that the reservoir cavities move along the group of mold cavities to close the now filled mold cavities of the initial reservoir cavities and transfer the remaining composition to the relocated reservoir cavities and new mold cavities. This movement may continue until the reservoir members are fully engaged such that the mold cavities are closed by the engagement between the mold parts, preferably spanning the entire mold cavities. Typically, the reservoir cavity has a volume that is less than the total volume of the mold cavities of the mold.

[0021] The first and / or second mold parts may be elastically deformable. The mold may be operable to move from an open position, in which the first and second parts are partially spaced apart, by deforming the mold parts, to a partially closed position by reducing deformation of the mold parts, and to a closed position by further reducing deformation of the mold parts.

[0022] Suitably, the first and / or second mould parts may be formed from a polymeric material such as silicone, which may be formed from a two-part silicone composition comprising a silicone resin and a hardener or catalyst.

[0023] The material forming the first and / or second mould part may have a Shore hardness of at least 5, such as at least 10, or at least 15, such as at least 20. The material forming the first and / or second mould part may have a Shore hardness of up to 40, such as up to 35, or up to 32, such as up to 30. The material forming the first and / or second mould part may have a Shore hardness of 5 to 40, such as 10 to 35, or 15 to 32, such as 20 to 30. Advantageously, it has been found that materials having a Shore hardness within the above ranges provide moulds with flexibility allowing effective moulding according to the invention whilst retaining sufficient shape and rigidity. As described herein, Shore hardness was measured using ASTM D2240 Type A.

[0024] The material forming the first and / or second mold parts may have a shrinkage rate of up to 1%, such as up to 0.5%, or up to 0.4%, such as up to 0.3%. Advantageously, materials having shrinkage rates within the above ranges have been found to provide molds with improved alignment between the mold parts. As described herein, shrinkage rate may refer to the amount of dimensional change, preferably over a period of one week, such as one month or three months.

[0025] The mould parts may comprise a retaining member operable to assist in maintaining alignment of the mould parts. The mould parts may comprise a retaining member operable to assist in maintaining alignment of the mould parts during delivery of the liquid ceramic composition to the mould. The feed retaining member may be spaced from the reservoir cavity, e.g. may not provide an inner surface of the reservoir cavity. Typically, the feed retaining member is not directly attached to the reservoir member. The feed retaining member may comprise cooperating members disposed on the first and second mould parts. Suitably, the cooperating feed retaining members may be male and female, such that the male member may be received within the female member to assist in alignment of the mould parts. The male retaining member may be a tongue and the female alignment member may be a groove. The mould part retaining member may be disposed below a base of the reservoir cavity. The retaining member may extend laterally along the mould parts, substantially parallel to the base of the reservoir cavity or the base reservoir member. Advantageously, the use of a supply retention member allows for a larger initial reservoir cavity to be formed while still maintaining good alignment of the mold sections.

[0026] The mould parts may comprise post-dispense retention members operable to assist in maintaining alignment of the mould cavities after dispensing of the liquid ceramic composition. The post-dispense retention members may be arranged outside the reservoir cavity, e.g. so as not to provide an inner surface of the reservoir cavity. The post-dispense retention members may comprise cooperating members arranged on the first and second mould parts. Preferably, the cooperating post-dispense retention members may be male and female such that the male retention member may be received within the female retention member to assist in maintaining alignment of the mould parts. The male retention member may be a tongue and the female alignment member may be a groove. The post-dispense retention members may be arranged laterally adjacent to the mould cavity or group of mould cavities. The retention members may extend laterally along the mould parts. The post-dispense retention members may comprise a set of retention members arranged on either side of the mould cavity or group of mould cavities, preferably arranged laterally adjacent to the mould cavity or group of mould cavities. Each set of retention members may comprise at least two retention members spaced longitudinally along the mould sections, such as at least three retention members. Advantageously, the use of post-dispense retention members allows for improved retention of alignment between the mould sections after dispensing of the composition.

[0027] The mould part may comprise a recess located above the mould cavity, preferably above the opening of the reservoir cavity. Typically the recess may be elongate and extend substantially parallel to the base of the reservoir cavity or the base reservoir member. The recess may be operable to receive any excess composition contained in the reservoir cavity when the mould part reaches the closed position.

[0028] The mould section may comprise a guide member. Preferably, the guide member extends outwardly from the mould section. The mould section may comprise a guide member disposed on each of two opposing faces of the mould section, preferably on two opposing side faces of the mould section. The mould section may comprise at least three guide members, for example at least four, at least five or at least six guide members, on each of the two opposing faces of the mould section. The faces of the mould section may comprise a guide member disposed towards an opposite end of the face and an intermediate guide member disposed between the end guide members.

[0029] The mould section may comprise a reinforcing member, preferably the reinforcing member may be more rigid than the body of the mould section. The reinforcing member may be at least partially disposed within the mould section body. The reinforcing member may extend substantially from one end of the mould section body to another end, for example the opposite end. The reinforcing member may protrude from the mould section to provide a guide member. Preferably the reinforcing member may protrude on an opposite side of the mould section to provide a guide member on an opposite side of the mould section. In this way the guide member may be provided by the protruding reinforcing member.

[0030] The filling member may be formed from a casting composition or slip, such as a clay or non-clay castable composition, a liquid cement or a gel cast composition. Thus, the liquid ceramic composition may be a gel cast composition, and preferably the composition may comprise a ceramic material, an organic binder component and optionally a pore forming component.

[0031] The organic binder component may be operable to be substantially removed from the filler member after shaping of the filler member, preferably by heat treatment, more preferably during firing of the filler member.

[0032] The organic binder component may comprise a polymerizable component, preferably the polymerizable component may comprise a polymerizable monomer and a cross-linking member, where the binder component is operable to polymerize to form a (co)polymer.

[0033] The polymerizable monomer may comprise one or more ethylenically unsaturated monomers, such as acrylic monomers or derivatives thereof, such as acrylamide monomers, and / or vinyl monomers, such as monomers selected from one or more of methacrylamide (MAM), N-(hydroxymethyl)acrylamide (hMAM), hydroxyethylacrylamide (hEAM) and / or N-vinyl-2-pyrrolidinone (NVP). Preferably, the polymerizable monomer comprises one or more acrylamide monomers, more preferably monomers selected from one or more of methacrylamide (MAM), N-(hydroxymethyl)acrylamide (hMAM) and hydroxyethylacrylamide (hEAM). Most preferably, the polymerizable monomer comprises a MAM.

[0034] The cross-linking member may be selected from one or more of diethylenically unsaturated monomers, such as diacryl monomers or derivatives thereof, such as diacrylamide monomers, acrylic salts, and / or polyethylene glycol substituted acrylic monomers. The cross-linking member may be selected from one or more of poly(ethylene glycol) dimethacrylate (PEGDMA), N,N'-methylene bis(acrylamide) (BIS), ammonium acrylate, and PEG methylethyl methacrylate (PEGMEM), preferably one or more of poly(ethylene glycol) dimethacrylate (PEGDMA), and N,N'-methylene bis(acrylamide) (BIS).

[0035] The organic binder component may be formed from 40 to 95 wt % polymerizable monomer and 60 to 5 wt % crosslinker, for example 50 to 90 wt % polymerizable monomer and 50 to 10 wt % crosslinker, or 55 to 85 wt % polymerizable monomer and 45 to 15 wt % crosslinker, or 60 to 80 wt % polymerizable monomer and 40 to 20 wt % crosslinker, for example 65 to 75 wt % polymerizable monomer and 35 to 25 wt % crosslinker.

[0036] The composition may further include a polymerization accelerator operable to accelerate polymerization of the binder components. The polymerization accelerator may be any suitable accelerator. For example, the accelerator may be tetramethylethylenediamine (TEMED).

[0037] The composition may further include an initiator operable to initiate polymerization of the binder components. The initiator may be any suitable initiator. The initiator may be a free radical initiator. For example, the initiator may be ammonium persulfate and / or potassium persulfate.

[0038] The pore-forming material may be operable to be removed from the filler member after shaping of the filler member, preferably by heat treatment, more preferably during firing of the filler member. The pore-forming material may be selected from one or more of microbeads, starch, seeds and / or cellulose.

[0039] The pore forming material is D 10 The particle size distribution of the pore-forming material may be 5 to 100 μm, preferably 10 to 75 μm, more preferably 15 to 50 μm, and most preferably 20 to 40 μm. 50 The diameter of the pore-forming material may be 50 to 200 μm, preferably 75 to 175 μm, more preferably 90 to 160 μm, and most preferably 100 to 150 μm. 90 The thickness may be 120 to 300 μm, preferably 150 to 270 μm, more preferably 170 to 250 μm, and most preferably 185 to 235 μm.

[0040] The ceramic material may be a refractory ceramic material. The ceramic material may include aluminum oxide, aluminum silicate, magnesium aluminate, calcium aluminate, zirconia, silica, titanate, carbon and / or magnesium oxide.

[0041] Ceramic materials are D 10The pore-forming material may have a particle size distribution of 0.1 to 20 μm, preferably 0.5 to 10 μm, more preferably 1 to 5 μm, and most preferably 1.5 to 3 μm. 50 The diameter of the pore-forming material may be 0.5 to 30 μm, preferably 1 to 25 μm, more preferably 1.5 to 20 μm, and most preferably 2 to 15 μm. 90 The thickness may be 10 to 100 μm, preferably 15 to 80 μm, more preferably 20 to 70 μm, and most preferably 25 to 60 μm.

[0042] The ceramic material may be a ceramic powder. The ceramic powder may be ball milled or spray dried. Advantageously, it has been found that ball milled or spray dried ceramic powders exhibit easier casting behavior.

[0043] The composition or packing member may include a promoter operable to increase the reactivity of the main reaction and / or suppress undesirable side reactions. The promoter may be selected from one or more of oxides of lanthanum, copper, magnesium, manganese, potassium, calcium, zirconium, barium, cerium, sodium, lithium, molybdenum, yttrium, cobalt, and chromium.

[0044] The composition may further comprise a carrier, such as an aqueous carrier. Suitably, the composition may be an aqueous ceramic slurry.

[0045] The composition may include further additives.For example, the composition may include a dispersant such as a polymer salt, for example a polyacrylic salt, preferably an ammonium polyacrylic salt.Suitable dispersants may be selected from one or more of Ecodis P90, Narlex LD42 and Dispex A40.

[0046] The composition may comprise 0.1-10% polymerizable monomer by dry weight of the composition, preferably 0.5-8 wt%, more preferably 1-6 wt%, for example 1.5-5 wt%, most preferably 2-4 wt% polymerizable monomer.

[0047] The composition may comprise 0.1-10% crosslinking member by dry weight of the composition, preferably 0.5-8 wt%, more preferably 0.75-6 wt%, for example 1-5 wt%, most preferably 1-4 wt% crosslinking member.

[0048] The composition may comprise from 50 to 95 wt% ceramic material, preferably from 50 to 90 wt%, more preferably from 55 to 85 wt%, most preferably from 60 to 80 wt% ceramic material by dry weight of the composition. The filler member may comprise at least 75 wt% ceramic material, preferably at least 85 wt%, more preferably at least 90 wt%, such as at least 95 wt%, most preferably at least 97 wt% ceramic material by dry weight of the composition.

[0049] The composition may comprise >0-40% pore former by dry weight of the composition, preferably 0.5-30wt%, more preferably 2-25wt%, for example 3-20wt%, most preferably 4-15wt% pore former.

[0050] The composition may contain 0.1 to 5% by weight of the initiator, preferably 0.5 to 4% by weight, more preferably 0.75 to 3.5% by weight, and most preferably 1 to 3% by weight of the initiator, based on the dry weight of the composition.

[0051] The composition may comprise up to 5% accelerator by dry weight of the composition, preferably up to 3 wt%, more preferably up to 2 wt%, most preferably up to 1.5 wt% accelerator.

[0052] The composition may contain 0.1 to 10% by weight of dispersant, preferably 0.5 to 8% by weight, more preferably 0.75 to 6% by weight, and most preferably 1 to 5% by weight of dispersant, based on the dry weight of the composition.

[0053] The composition may have a solids content of 45 to 99% by weight of the total composition, for example 50 to 95 wt%, preferably 55 to 90 wt%, most preferably 60 to 85 wt%.

[0054] The composition may be formed by combining a preformed aqueous binder component with the ceramic composition. Suitably, the aqueous binder component may include a polymerizable monomer, a crosslinking member, and water.

[0055] Prior to contacting the liquid ceramic composition with the form, the composition may be contacted with an initiator and, optionally, a polymerization accelerator.

[0056] The packing elements of the present invention may be inert packing elements. As such, the inert packing elements may be substantially free of catalytic material. Advantageously, the use of inert packing elements according to the present invention in the catalyst bed improves heat transfer and gas flow turbulence, which helps the reaction medium further along the reactor to be at a suitable temperature for the desired reaction.

[0057] The packing member, or support, of the present invention may be a supported catalyst comprising a catalytic material that may be operable to provide catalytic activity in a desired process in which the supported catalyst is applied.

[0058] The catalytic material may comprise a metal selected from one or more of a transition metal, preferably a transition metal oxide, and / or a noble metal, preferably an alloy thereof. The catalytic material may comprise a metal selected from one or more of iron, nickel, silver, gold, platinum, ruthenium, vanadium, molybdenum, and cobalt.

[0059] The composition may be mixed prior to placement in a mold to form a homogenous slurry, preferably prior to addition of the initiator and optional accelerator. The composition may be mixed after addition of the initiator and optional accelerator to form a homogenous slurry.

[0060] The mould is preferably a template. The mould may be operable to form a surface structure on the green body.

[0061] The green body produced by step (c) may be dried by baking the green body at at least 40° C., such as at least 50° C. or at least 55° C. or at least 60° C. Suitably the green body may be baked for at least 10 hours, such as at least 15 hours or at least 20 hours, such as at least 24 hours.

[0062] The green bodies may be fired at above 1000° C., preferably above 1200° C., more preferably above 1400° C., most preferably above 1500° C. Suitably, the green bodies may be sintered until substantially all of the binder and pore forming components are removed from the support or supported catalyst.

[0063] The packing members may be impregnated with the catalytic material by immersing the packing members in a solution of the catalytic material. The impregnated packing members may be dried after immersion.

[0064] Advantageously, the present invention allows the green support or supported catalyst body to be removed from the mold while it is still in a relatively rubbery form, allowing for easier handling, which leads to lower scrap rates than other types of casting techniques.

[0065] The guide member of the apparatus of the present invention may suitably be operable to guide the mould into the open configuration by receiving the guide member on the mould. Suitably the guide member may include a portion operable to position the mould in a closed or at least partially closed position and a portion operable to position the mould in a position where the mould portions are at least partially spaced in the open position. The mould may be operable to move within the guide member from the closed portion of the guide member to the spaced portion of the guide member. Typically the guide member is operable to position the mould in an open position where parts of the mould portions abut and parts of the mould portions are spaced, suitably in a position where the supply retention member may be engaged while the mould cavity is opened to form the reservoir cavity. The guide member may be operable to position the mold in a position where the supply retaining member engages and / or abuts a portion of the mold portion while the mold cavity is open and the reservoir cavity is being formed, where the open mold cavity and / or reservoir cavity is positioned over the engaged supply retaining member and / or over the abutting portion of the mold portion. The guide member may further comprise a drive member operable to move the mold through the guide portion of the guide member.

[0066] The molding apparatus may further comprise a supply member operable to dispense the liquid ceramic composition into the mold. Suitably, the supply member may be disposed above the guide portion of the guide member.

[0067] The packing member may be a catalyst support, preferably a ceramic catalyst support. The packing member may be a supported catalyst.

[0068] The packing member of the present invention may be a cast packing member, such as a gel cast packing member.

[0069] The filling material is 0.7 cm 2 / cm 3 Geometric surface area (GSA) per volume of 1 cm or more and side crushing strength of 250 kgf or more, e.g. 2 / cm3 GSA of at least 1.2 cm 2 / cm 3 GSA of 1.3cm or more, preferably 1.3cm 2 / cm 3 GSA of at least 1.4 cm 2 / cm 3 The filling member may have a GSA of 275 kgf or more, preferably 300 kgf or more, more preferably 325 kgf or more, and most preferably 350 kgf or more.

[0070] The filling material is 1.5 cm 2 / cm 3 GSA or more and side breaking strength of 150kgf or more, for example, 1.7cm 2 / cm 3 GSA of at least 1.9 cm 2 / cm 3 GSA of 2.1cm or more, preferably 2.1cm 2 / cm 3 GSA of at least 2.3 cm, most preferably 2 / cm 3 The filling member may have a GSA of 170 kgf or more, preferably 185 kgf or more, more preferably 200 kgf or more, and most preferably 215 kgf or more.

[0071] The filling material is 3cm 2 / cm 3 GSA or more and side breaking strength of 60kgf or more, for example 3.3cm 2 / cm 3 GSA of at least 3.6 cm 2 / cm 3 GSA of 3.9cm or more, preferably 3.9cm 2 / cm 3 GSA of at least 4.2 cm, most preferably 2 / cm 3 The filling member may have a GSA of 70 kgf or more, preferably 80 kgf or more, more preferably 90 kgf or more, and most preferably 100 kgf or more.

[0072] The GSA herein is calculated by measuring the outer dimensions of the filler member, including all macro-structural and surface structural features, and calculating the surface area. The calculated surface area is then divided by the calculated volume of the filler member. Suitable 3D modeling software can be used to provide these calculations quickly and accurately.

[0073] Side breaking strength in this specification is given by a value expressed in kgf. It is the maximum load recorded at which the specimen breaks when pressed between two parallel flat hardened steel plates of a minimum diameter of 80 mm. One plate is fixed to a load cell and recording device, the other is attached to a ram moving at a controlled speed of 5 mm / min. Initial trial tests are performed to determine the dimension in which the filler member is weakest. A side breaking test is then performed in the weakest direction.

[0074] The packing member may have a porosity of 6% or more, preferably 15% or more, more preferably 20% or more, and most preferably 25% or more. The packing member may have a porosity of 6 to 50%, preferably 15 to 40%, more preferably 20 to 35%, and most preferably 25 to 30%. Suitably, the carrier may have a porosity of 15% or more, more preferably 20% or more, and most preferably 25% or more. The carrier may have a porosity of 15 to 50%, more preferably 20 to 40%, and most preferably 25 to 35%.

[0075] Porosity herein is measured by mercury intrusion porosimetry using ASTM D4284-12(2017)e1, Standard Test Method for Determining Pore Volume Distribution of Catalysts and Catalyst Carriers by Mercury Intrusion Porosimetry.

[0076] The filler member may have a macrostructure and a surface structure on an outer surface of the macrostructure. Typically, the surface structure of the filler member is formed during the molding step of the filler member, i.e. the step in which the green body of the filler member is formed, preferably by suitable texturing in the mould cavity. Thus, preferably, the surface structure is not post-processed after the shaping of the green body of the filler member.

[0077] The macrostructures may be in the form of multiple lobes, for example trilobes, tetralobes or pentlobes, rings, spheres, cubes, cuboids, cylinders, or gears.

[0078] The gear macrostructure includes a plurality of castellations extending radially outwardly. The gear macrostructure may have a transverse cross-section, excluding the castellations, that is substantially circular, triangular, square, or rectangular, among others. At least some, and preferably all, of the castellations may be tapered along the depth and / or width of the castellation, and preferably each castellation tapers in the same direction as the other castellations of the gear, suitably with the maximum width and depth points of the castellation towards the same end of the castellation.

[0079] The macrostructure may have a concave upper and / or lower surface, suitably at least 30% of the upper and / or lower surface is concave, such as at least 40% or at least 50%. It will be appreciated that a bore extending through the macrostructure is not a recess in the upper and / or lower surface according to the present invention.

[0080] Advantageously, it has been found that gear macrostructures having tapered castellations and / or recessed upper or lower surfaces provide improved packing density in combination with reduced interlocking.

[0081] The spherical macrostructure may comprise at least one linear depression on the outer surface of the macrostructure, for example at least two, at least three, or at least four linear depressions. Preferably, the spherical macrostructure comprises at least two, for example at least three or at least four linear parallel depressions. Preferably, the depressions are substantially hemispherical in transverse cross section.

[0082] The macrostructure may be integral or may include one or more bores extending through the macrostructure. Preferably, the filler member includes at least one bore extending through the macrostructure, and more preferably, the macrostructure includes at least three bores. The macrostructure may be a honeycomb structure. The bores of the macrostructure may be straight cut or faceted.

[0083] The packing member may comprise a plurality of surface structures, suitably a plurality of repeating surface structures. Preferably the packing member comprises at least 5 surface structures, suitably repeating surface structure portions, more preferably at least 10, such as at least 15, or at least 20, most preferably at least 25.

[0084] By surface structure is meant ridges and / or depressions on the carrier, the height of which is significantly smaller than the width / diameter of the macrostructure of the filler member. Such a surface structure may be considered as a roughened surface finish on the macrostructure of the filler member. The surface structure may be considered as not including microscopic surface roughness. For example, the filler member may consist of a cubic macrostructure having a width of 32 mm and a length of 50 mm. The outer surface of this filler member may include a plurality of surface structures in the form of a plurality of repeating identical discrete mounds, each mound having a height of 2 mm. It will be understood that standard features of the macrostructure, such as multiple castellations or multi-lobed leaves of a gear wheel, are not considered to be surface structures according to the present invention.

[0085] The surface structures may be in the form of ridges and / or mounds.

[0086] The ridge may be in the form of an annular ridge, said annular ridge being not limited to a circular shape. The annular ridge may be substantially circular in shape or in the form of a regular convex polygon, such as a triangle, a square, a pentagon, a hexagon, a heptagon, an octagon, a nonagon or a decagon. Preferably, the annular ridge is in the form of a regular convex polygon, more preferably a pentagon, a hexagon or a heptagon, most preferably a hexagon. The portion of the surface structure extending between the annular ridges may be flat, inclined and / or curved. For example, the portion of the surface structure extending between the annular ridges may be in the form of an inverted pyramid. The surface structure may comprise a plurality of attached annular ridge structures, suitably interconnected annular ridge structures such that a ridge of at least a first annular surface structure forms part of a second annular surface structure.

[0087] The surface structures in the form of mounds may be recessed into the macrostructure or protrude outwardly from the macrostructure. The mounds may be curved, pyramidal and / or stepped. The stepped mounds may include 2 to 10 steps, for example 3 to 8 steps. The mounds may be interconnected such that adjacent mounds abut or fuse together.

[0088] The mean average height of the surface structures of the filler member may be up to 10mm, preferably up to 7mm, more preferably up to 6mm, most preferably up to 5mm.

[0089] The mean average height of the surface structures of the filler member may be at least 0.1 mm, such as at least 0.3 mm, preferably at least 0.5 mm, more preferably at least 0.7 mm, and most preferably at least 0.8 mm. The height of the surface structures herein is measured using a vernier caliper with depth measuring capability.

[0090] The packing element may have a maximum dimension of up to 1000mm, such as up to 750mm or up to 500mm, preferably up to 400mm. The packing element may comprise a width / diameter of up to 500mm, such as up to 300mm or up to 200mm, preferably up to 150mm, more preferably up to 100mm, most preferably up to 50mm.

[0091] The mean average height of the surface structures of the packing member may be up to 40% of the width / diameter of the packing member, such as up to 30%, preferably up to 25%, more preferably up to 20%, and most preferably up to 15%.

[0092] The surface structure may extend on at least two surfaces of the filler member, for example at least one side and one top and / or bottom surface.

[0093] The surface structure may extend over at least 50%, such as at least 60%, preferably at least 70%, more preferably at least 80%, and most preferably at least 85% of the side of the filler member. The surface structure may extend over at least 50%, such as at least 60%, preferably at least 70%, more preferably at least 80%, and most preferably at least 85% of the outer surface of the filler member. Where the surface structure comprises a repeating series of ridges, such as annular ridges, the surfaces extending between the ridges are included as part of the surface structure for this calculation even when the surface is substantially flat or the ridges are not interconnected.

[0094] Advantageously, the molds and processes of the present invention allow for commercially viable production of packing members that have improved geometric surface area while still providing excellent strength. Furthermore, the strength and / or porosity of packing members that can be effectively produced using the present invention may be modified while keeping the same shape, thereby reducing the need and cost of redesign. Furthermore, the packing members may provide a highly porous carrier while still providing excellent strength. Most advantageously, the packing members may provide improved geometric surface area in combination with excellent strength and high levels of porosity. The improved geometric surface area of ​​the packing members is particularly advantageous for applications where catalytic reactions are surface-based.

[0095] The packing member may also provide a high heat transfer coefficient in combination with other improved properties such as improved packing.

[0096] The packing members may also be used to provide superior packing characteristics with low pressure drop. The packing members may provide improved packing density while maintaining optimal airflow.

[0097] According to a fifth aspect of the present invention there is provided a method for producing a mould according to any of the first to third aspects of the present invention, the method comprising the steps of: a. Optionally, creating a digital model of a negative of the mold; b. Creating a negative mold according to the model using additive manufacturing, preferably printing with a 3D printer; and c. Forming a mold from the negative mold.

[0098] According to a sixth aspect of the present invention there is provided a method for manufacturing a packing element, such as a support for a catalyst, or a supported catalyst, the packing element may be a packing element according to the fourth aspect of the present invention, the method comprising the steps of: a. Optionally, creating a digital model of a negative of the mould according to any of the first to third aspects of the invention; b. Creating a negative mold according to the model using additive manufacturing, preferably printing with a 3D printer; c. forming a mold from the negative mold; and d. Casting the moulding composition, which may suitably be a moulding composition as defined in relation to the fourth aspect of the invention, to form a packing member or a supported catalyst, suitably according to the process of the second aspect of the invention.

[0099] According to a seventh aspect of the present invention there is provided a reactor comprising a catalyst bed, the catalyst bed comprising packing elements according to the fourth aspect of the present invention.

[0100] According to an eighth aspect of the present invention there is provided a reaction medium comprising a catalyst bed, the catalyst bed comprising packing elements according to the fourth aspect of the present invention.

[0101] Suitably, the reactor or reaction medium may be for the production of synthesis gas such as ammonia, methanol, hydrogen, hydrogen peroxide and / or oxoalcohols, direct reduction of iron (DRI), endothermic gas generation, catalytic partial oxidation, or autothermal reforming.

[0102] According to a ninth aspect of the present invention there is provided the use of a packing element according to the fourth aspect of the present invention as a catalyst support.

[0103] According to a tenth aspect of the present invention there is provided a process for producing synthesis gas, such as ammonia, methanol, hydrogen, hydrogen peroxide and / or oxo alcohols, comprising producing synthesis gas using a reactor in which a catalyst bed is provided with packing elements according to the fourth aspect of the present invention.

[0104] According to an eleventh aspect of the present invention there is provided a method for producing direct reduced iron comprising using a reactor in which a catalyst bed is provided with packing elements according to the fourth aspect of the present invention.

[0105] According to a twelfth aspect of the present invention there is provided an endothermic gas production method comprising using a reactor in which a catalyst bed is provided with packing elements according to the fourth aspect of the present invention.

[0106] According to a thirteenth aspect of the present invention there is provided a method for catalytic partial oxidation comprising using a reactor in which the catalyst bed is provided with a packing element according to the fourth aspect of the present invention.

[0107] According to a fourteenth aspect of the present invention there is provided a method of autothermal reforming comprising using a reactor in which a catalyst bed is provided with a packing element according to the fourth aspect of the present invention.

[0108] Any numerical range described herein is intended to include all subranges subsumed therein. The singular includes the plural and vice versa. For example, although the present specification refers to "a" first portion and "a" second portion, "an" open mold cavity, "a" reservoir-forming member, etc., one or more of each of these and any other components may be used. As used herein, the term "polymer" refers to oligomers and both homopolymers and copolymers, and the prefix "poly" refers to more than one.

[0109] The use of "mold" herein is intended to refer to a container having a hollow portion that is used to impart shape to a liquid composition upon hardening into a solid form. A mold may be, for example, a casting mold, a die, or a former.

[0110] The use of "longitudinal" and "lateral" in this specification refers to the reservoir cavity, with longitudinal referring to an axis extending substantially through the opening and bottom of the cavity, and "lateral" referring to an axis extending substantially perpendicular to the longitudinal axis.

[0111] All of the features contained herein can be combined with any of the above aspects in any combination.

[0112] For a better understanding of the present invention and to show how embodiments thereof may be carried into effect, reference is now made, by way of example, to the following figures:

[0113] The invention will now be described, by way of example only, with reference to the accompanying drawings, in which: [Brief description of the drawings]

[0114] [Figure 1] 1 shows a top perspective view of a first embodiment of a mold according to the present invention; [Diagram 2] 2 shows a top view of a second embodiment of a mold according to the invention. [Figure 3A] FIG. 2 shows a top perspective view of a first embodiment of a molding apparatus formed with a mold according to a second embodiment in an open position. [Figure 3B] FIG. 3B shows a top view of the molding apparatus of FIG. 3A. [Figure 4A] 3B shows a top perspective view of the molding apparatus of FIG. 3A with the mold in a partially closed position. [Figure 4B] FIG. 4B shows a top view of the molding apparatus of FIG. 4A. [Diagram 5] 1 shows a perspective view of a filling member according to the present invention; DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0115] 1 shows a mould 10 according to a first embodiment of the present invention. The mould 10 is substantially cubic and is formed of a first mould part 100 and a second mould part 200. The first part 100 and the second part 200 each comprise approximately half the mass of the mould and are each formed of an elastically deformable two-component silicone-based rubber.

[0116] The first mold part 100 is formed of a substantially cubical body 102. The body 102 has a rectangular inner surface and a rectangular outer surface. The inner surface forms the inner surface of the mold and the outer surface forms the outer surface of the mold when the mold parts are engaged. The body 102 also has a rectangular front surface, a rear surface, and two side surfaces.

[0117] The inner surface of the body 102 has a group of twelve discrete, generally hemispherical, partial mold cavities 104 that include surface texturing on the molding surface of the cavities. The mold cavities are arranged in four rows of groups with three cavities 104 per row. The partial cavities 104 are equally spaced from adjacent mold cavities to form a grid-like group arrangement that is laterally centered on the inner surface. A first row is adjacent to, parallel to, but spaced from an edge of the inner surface adjacent the front surface of the body 102, and a last (fourth) row is adjacent to, parallel to, but spaced from an edge of the inner surface adjacent the rear surface. The first row is closer to its said edge than the last row is to its respective said edge. Side reservoir member tongues 106a and 106b project, extending along either side of the grid-like group of partial cavities 104. The side reservoir member tongues 106a, 106b are generally cuboidal in shape with a convex upper surface and extend longitudinally along the inner surface from the edge adjacent the front surface to just after the last row of partial cavities 104. The side reservoir members 106a, 106b are connected at their bottom ends (i.e., the end adjacent the rear surface of the body 102) via the base reservoir member tongue 106c. The base reservoir member 106c is the same height as the side reservoir members 106a and 106b and it extends laterally across the inner surface to connect the reservoir members 106a and 106b. The reservoir members 106a, 106b are integrally connected at each end of the base reservoir member 106c to form a generally U-shaped enclosure that encloses the grid-like grouping of partial cavities 104 at both sides and the bottom (i.e., the end adjacent the rear surface of the body 102). The enclosure forms part of a reservoir cavity 108 in which the partial cavities 104 are disposed. The reservoir cavity has a laterally extending opening in the form of an open end extending between the ends of the side reservoir members that are not connected to the base reservoir member. Thus, the opening is disposed between the first row of partial cavities and the end of the inner surface adjacent the front surface of the body 102.

[0118] The mould section 100 further comprises two sets of three post-feed cube-shaped retaining members 110a,b integrally formed on two sides with the inner surface and the side reservoir member. Each of the post-feed retaining members extends outwardly from the inner surface and the side reservoir member. The first set of retaining members 110a is disposed along the outer surface (relative to the reservoir cavity) of the side reservoir member 106a, and the second set of retaining members 110b is disposed opposite the first set on the outer surface of the side reservoir member 106b. The three retaining members of each set 110a and b are equally spaced longitudinally down the inner surface from adjacent retaining members of the set, with each retaining member diametrically opposite a corresponding retaining member on the opposing side reservoir member.

[0119] The inner surface of the body 102 is formed with a supply retention tongue 112 spaced from, underlying and extending parallel to the base reservoir member 106c and adjacent to, extending parallel to but spaced from an edge of the inner surface adjacent the rear surface. The supply retention member 112 is a generally cuboidal protrusion that extends laterally across the body 102 and is spaced from the side edge.

[0120] An elongated recess 114 is disposed on the inner surface between an edge of the inner surface adjacent the front surface of the body 102 and the opening of the reservoir cavity 108, proximate to but spaced from said edge. The recess 114 is relatively laterally centrally located on the inner surface between the side edges of the body 102 and spaced from the side edges of the body 102. The recess 114 is generally oval in shape. The recess 114 is generally coterminous with the width of the opening of the reservoir cavity.

[0121] The first mold section 100 also has three cylindrical, spaced apart reinforcing rods 116 that extend laterally through the central mass of the body 102 from one side to the other at three different points along the body 102. The rods 116 protrude from both sides such that there are three protrusions on each side of the first mold section 100 that act as guide members. The rods 116 are equally spaced along the longitudinal length of the body 102.

[0122] The second mold part 200 (not shown) is similar to the first mold part 100, but has a female equivalent that extends inwardly of the reservoir member and retaining member. Thus, the second mold part 200 has a corresponding female reservoir member 206 (not shown) that is a cubical groove in the body 202 (not shown) suitable for receiving the reservoir member of the first mold part 100, and female retaining members 210 (not shown) and 212 (not shown) that fit inside for mating with the male retaining members 110, 112, allowing the first and second mold parts 100, 200 to be held in alignment. When the first mold cavity 100 and the second mold cavity 200 are mated together, the part cavities 104, 204 form a closed, enlarged, generally spherical mold cavity 304 (not shown).

[0123] In use, the mold 10 is placed in an open position in which the first mold part 100 and the second mold part 200 are partially spaced apart such that the supply retention members 112, 212 cooperatively engage to hold the first and second mold parts 100, 200 in alignment and the reservoir members 106, 206 (not shown) are fully engaged to form reservoir cavities with the base reservoir member forming the base of the cavities and all of the mold cavities being open. In this configuration, the front faces of the mold parts are spaced apart and the rear faces of the mold parts are not spaced apart.

[0124] In this initial a configuration, the initial reservoir cavity 108 can be filled with liquid ceramic composition by dropping the liquid composition from above the spaced apart front faces of the mold parts into the openings of the reservoir cavity 108. The received liquid composition is retained within the cavity 108 and also enters and fills the mold cavities 104, 204 located within the initial reservoir cavity.

[0125] The mold 10 can then be moved to a partially closed position by incrementally further engaging the side reservoir members 106, 206 upward from the base reservoir members toward the openings of the reservoir cavities. This action results in the closure of the initial reservoir cavities, thereby closing off some of the currently filled mold cavities, but by further engaging the side reservoir members, the reservoir cavities are moved further up the mold 10 toward the front face of the mold portion. The relocated reservoir cavities carry the remaining composition not captured by the initially filled mold cavities. This has the effect of transferring a portion of the liquid ceramic composition to a higher position in the group of cavity members, thereby allowing composition to move from the relocated reservoir cavities 108 to the previously empty open mold cavities now contained within the relocated reservoir cavities 108.

[0126] Mold parts 100, 200 can then be moved to a closed position in which reservoir members 106, 206 and post-dispense retention members are fully engaged, thereby closing the reservoir cavities and also closing all of the mold cavities so that the liquid ceramic composition is retained within closed mold cavity 304. Any excess composition is captured in recess 114.

[0127] The composition is retained in mold cavity 304 until the green body is produced, optionally by heating the green body.

[0128] The green body can then be removed from the mold and fired to produce the filler member.

[0129] Figures 2A and 2B show a second embodiment of a mold 20 according to the present invention. The mold 20, as shown in Figures 2A and 2B, is substantially cubic and has a first mold part 300 and a second mold part 400. The first mold part 300 and the second mold part 400 are structurally similar to the first mold part 100 and the second mold part 200 of the first embodiment. The mold 20 has all the features as described in the first embodiment, unless otherwise noted below.

[0130] The first mold part 300 and the second mold part 400 contain more partial cavities, 305 and 405, respectively. There are eleven straight, end-aligned, parallel rows of partial cavities 305, 405, with 15 cavities per row.

[0131] Side reservoir member tongues 306a and 306b are located on the first mold part 300 and extend longitudinally along the inner surface from just after the last row of partial cavities 305 to an edge of the inner surface adjacent the front surface of the body 302. The side reservoir member tongues 306a and 306b, as well as the base reservoir member tongue 306c, thereby surround the partial cavities 305 and the elongated recess 314 located on the inner surface of the body 302. Side reservoir members 406a and 406b are similarly located on the second mold part 400.

[0132] The number of post-dispense cube-shaped retaining members 310a,b integrally formed with the inner surface and two side surfaces of the side reservoir members 306a,b has been increased to seven on each side as compared to the first embodiment. Also, the second mould section 400 is provided with seven corresponding female retaining members 410a,b. There are eight equally spaced reinforcing rods 316 extending laterally through the central mass of each mould section as in the first embodiment.

[0133] Figures 3 and 4 show a first embodiment of a mould device 30 according to the invention. The mould device 30 is formed by a mould 20 according to the second embodiment described above and two guide members 450. The guide members 450 are fixed in a vertical orientation. Each guide member 450 has two cuboid-shaped grooves 452 running downwards in the longitudinal direction of the guide member at a slight incline such that the distance between the two grooves 452 is smaller at the bottom than at the top of the guide member 450. The grooves of each guide member are arranged so that they face towards and are diametrically opposite the corresponding grooves of the other guide member.

[0134] The reinforcing rods 316, 416 can fit into grooves 452 on each side of the mold halves, allowing the mold 20 to move along the grooves and be held vertically with the front faces of the mold halves 300, 400 facing up and the rear faces facing down.

[0135] In use, the mold 20 is placed in an open position by moving the mold over the guide member 450 until the rods 316 and 416 enter the grooves 452 at the bottom of the guide member and the front faces of the mold parts 300 and 400 are toward the top of the guide member 450 (FIG. 3A). As the mold parts 300 and 400 are moved over the guide member 450, the grooves 452 are angled outwardly so that the mold parts 300 and 400 are spaced apart at their upper ends, providing an open position in which an initial reservoir cavity is formed in the space between the mold parts. In this position, the supply retaining members 312, 412 are cooperatively engaged at the lower end of the mold to hold the first and second mold parts 300, 400 in alignment and to allow the base reservoir member to form the base of the cavity and form a large reservoir cavity in which all of the mold cavities are open.

[0136] In the open position, the initial reservoir cavity 308 is capable of receiving liquid ceramic compact composition by dropping the liquid composition into an opening 454 in the reservoir cavity 308 from a supply member disposed above the spaced-apart front faces of the mold portions. The received liquid composition is retained within the initial reservoir cavity 308 and fills any mold cavities 305, 405 located within the initial reservoir cavity.

[0137] The mold 20 can then be moved to a partially closed position by moving the mold along the grooves and under the guide members to incrementally further engage the side reservoir members 306, 406 and the inner surfaces of the mold portion upward from the base reservoir member toward the opening of the reservoir cavity, as shown in Figures 4A and 4B. In the partially closed position, the side reservoir members and the inner surfaces of the mold are further engaged to move the reservoir cavity further up the mold 20 toward the front face of the mold portion. This action closes the initial reservoir cavity, thereby also closing the filled mold cavity that was located in the initial reservoir cavity. The repositioned reservoir cavity carries the remaining composition not captured by the originally filled mold cavity. This has the effect of transferring a portion of the liquid ceramic composition to a higher position in the group of cavity members, thereby allowing composition to move from the relocated reservoir cavity 308 to the previously empty open mold cavity that is now in the relocated reservoir cavity 308. The relocated reservoir cavity can also receive additional composition from the supply member. In the partially closed position, the base of the reservoir cavity is ultimately formed by the abutment of the inner surfaces of the mold parts.

[0138] The mold sections 300, 400 can then be moved to a closed position in which the reservoir members 306, 406 and the post-dispense retention members 310 are fully engaged, thereby closing the reservoir cavity 308 and also closing all of the mold cavities to retain the liquid ceramic composition within the closed mold cavities. Any excess composition is captured in the recesses 314, 414.

[0139] By way of example, supported catalysts were prepared using mold apparatus 30 and mold compositions formed by mixing the ingredients provided below in the following manner.

[0140] Alumina powder, a pore former, and a dispersant were mixed to form a powder mixture. An aqueous monomer solution containing a chain forming monomer, a chain linking monomer, and water was added to the powder mixture to form an aqueous slurry. A catalyst and an initiator were then added to the aqueous slurry. The amounts of each component in the resulting slurry were as follows: amount Alumina Powder 475 Pore ​​former 60g Dispersant 12.25g Polymerizable monomer 16.3g Crosslinker 8.2 Catalyst 3ml Initiator 8ml 135g water

[0141] The resulting aqueous slurry was then poured into the reservoir cavity of the mold 20 from a supply member positioned above the mold 20 while the mold 20 was in an open position. The mold 20 was then moved gradually from the open position to a partially closed position while additional aqueous slurry was added. The mold 20 was then placed in a closed position. Once the slurry had gelled into a plurality of solid green bodies within the closed and enlarged mold cavity, the green bodies were then removed from the mold. At this point, the green bodies had a rubbery, jelly-like consistency. The green bodies were then left to dry at room temperature for 24 hours. The dried green bodies were then sintered at 1450° C., at which point the binder and pore formers had burned off leaving solid porous filler members.

[0142] Next, this filling material is treated with the catalytic material Ni(NO3) 2 After immersion in an aqueous solution containing , it was dried at 500 ° C. This impregnation step of the catalyst material was repeated two more times to produce a supported catalyst.

[0143] The supported catalyst produced had a macrostructure and surface structure as shown in supported catalyst 500 in FIG. 5. Supported catalyst 500 has a cylindrical gear-shaped macrostructure with a plurality of bores (five total) extending through the longitudinal length of the support and a plurality of spaced, longitudinally oriented castellations (ten total) projecting radially outward from the support. The supported catalyst 500 macrostructure further includes a recess 502 in the top surface of the support 500. Each castellation of the gear tapers in depth such that supported catalyst 500 has a maximum outer width F (38.0 mm) at the base to a minimum outer width E (35.1 mm) at the top surface of supported catalyst 500. Each castellation further tapers in width from its widest point at the base of supported catalyst 500 to its narrowest width at the top surface of supported catalyst 500.

[0144] The supported catalyst 500 has a surface structure that extends across substantially the entire exterior surface of the supported catalyst 500. The surface structure is generally in the form of interconnected hexagonal shaped ridges 502.

[0145] In this manner, packing members having improved properties can be manufactured using the large volumes of open vertical packing required in the time required to achieve commercially viable production.

[0146] Attention is directed to all articles and documents filed contemporaneously or prior to this application in connection with this application and published herewith, and the contents of all such articles and documents are incorporated herein by reference.

[0147] All of the features disclosed in this specification (including the accompanying claims, abstract and drawings), and / or all of the steps of any method or process so disclosed, may be combined in any combination, except where at least some of such features and / or steps are mutually exclusive.

[0148] Each feature disclosed in this specification (including the accompanying claims, abstract and drawings), unless expressly stated otherwise, may be replaced by alternative features serving the same, equivalent or similar purpose. Thus, unless expressly stated otherwise, each feature disclosed is only an example of a generic series of equivalent or similar features.

[0149] The invention is not limited to the details of the foregoing embodiments, and extends to any novel one or any novel combination of features disclosed in this specification (including the accompanying claims, abstract and drawings), or any novel one or any novel combination of steps of any method or process so disclosed.

Claims

1. 1. A mold for producing a filler member from a liquid ceramic composition, comprising a first part and a second part, the first part and / or the second part comprising an open mold cavity, the first part and the second part being operable to engage to form a closed mold cavity, the mold further comprising a reservoir forming member, the mold being operable to be moved from an open position in which the reservoir member defines a reservoir cavity and the first and second parts are at least partially spaced apart such that the mold cavity is open, to a partially closed position in which a volume of the reservoir cavity is reduced, and further to a closed position in which the first and second parts are engaged such that the mold cavity is closed.

2. The mold of claim 1 , wherein the first and second portions each comprise an open mold cavity.

3. 3. The mold of claim 2, wherein the mold cavities of the first and second portions are open half mold cavities, and the first and second portions of the mold are operable to engage such that the half mold cavity of the first portion aligns with the half mold cavity of the second portion to form a closed enlarged mold cavity.

4. A mould according to any one of claims 1 to 3, wherein the first and / or second part comprises a plurality of open mould cavities.

5. The mold described in claim 4, wherein each of the first and / or second portions has a plurality of open partial mold cavities.

6. A mould according to any preceding claim, wherein the mould cavity comprises texturing operable to form a surface structure on the filler member.

7. 7. The mold of claim 1, wherein the reservoir member comprises a first reservoir member disposed on the first mold part and a second reservoir member disposed on the second mold part, the first and second reservoir members being operable to cooperatively engage to form a reservoir cavity.

8. The mold of claim 7 , wherein the first and second reservoir members comprise male and female reservoir members.

9. A mould according to any preceding claim, wherein the first and / or second mould sections comprise side reservoir members extending along opposite sides of the mould cavity of the mould sections.

10. A mould according to any preceding claim, wherein the first and / or second mould parts comprise a base reservoir member.

11. The mold of claim 10, wherein the base reservoir member extends between the side reservoir members.

12. A mould according to any one of the preceding claims, wherein the first and / or second mould parts are elastically deformable.

13. A mould according to any one of the preceding claims, wherein the material forming the first and / or second mould parts has a shrinkage of up to 1%.

14. A mould according to any preceding claim, wherein the mould parts include cooperating retaining members operable to assist in maintaining alignment of the mould parts.

15. A mould according to any preceding claim, wherein the mould portion comprises a reinforcing member.

16. The mold of claim 15 , wherein the reinforcing members protrude from the mold portions to provide guide members.

17. A moulding apparatus for use in producing a filler member from a liquid ceramic composition, the moulding apparatus comprising a mould according to any one of claims 1 to 16 and a guide member operable to position the mould in an open position.

18. 18. The molding apparatus of claim 17, wherein the guide member is operable to position the mold in an open position with some of the mold portions abutting and some of the mold portions spaced apart.

19. The molding apparatus of claim 18, wherein in the open position, the mold is operable to receive a portion of the molding composition from a supply member disposed above the mold.

20. 1. A process for producing packing elements for use in a packed bed, comprising the steps of: placing a mould comprising a first part and a second part, said first part and / or second part comprising an open mould cavity, said mould further comprising a reservoir forming member, in an open position in which said first and second parts are at least partially spaced apart such that said reservoir member forms a reservoir cavity and said mould cavity is open, said mould may be as claimed in any one of claims 1 to 16, or may be a moulding apparatus as claimed in any one of claims 17 to 19; b. at least partially filling the reservoir cavity of the mold with a liquid ceramic composition; c) moving the mold to a partially closed position such that the position of the reservoir cavity changes relative to the mold cavity and / or the volume of the reservoir cavity decreases; d. moving the mold to a closed position, wherein the first and second portions are engaged to close the mold cavity and a portion of the liquid ceramic composition is retained within the closed mold cavity to produce a green body; e. Optionally, heating the green body; f. removing the green body from the mold; and g. Optionally, firing the green body to produce a filler member; A process including.

21. The process of claim 20, wherein step (b) at least partially fills the reservoir cavity of the mold with liquid ceramic composition by dispensing it from above the mold.

22. The process of claim 20 or 21, wherein step (c) further comprises transferring a portion of the liquid ceramic composition from the reservoir cavity to the open mold cavity.

23. 23. A packing element for use in a packed bed, the packing element being a cast packing element formed from molding a liquid ceramic composition in a mould according to any one of claims 1 to 16, in a forming apparatus according to any one of claims 17 to 19, or by the process according to any one of claims 20 to 22.

24. The packing member of claim 23, wherein the packing member is for use as a catalyst support in a packed bed reactor.

25. 25. The filler member of claim 23 or 24, wherein the filler member is formed from a casting molding composition or slip.

26. The filling member of claim 25, wherein the filling member is formed from a clay or non-clay castable composition, a liquid cement or a gel cast composition.

27. 27. The filling member of claim 25 or 26, wherein the filling member is formed from a gel cast composition.

28. 30. The filling member of claim 27, wherein the gel cast composition comprises a ceramic material, an organic binder component, and optionally a pore-forming component.

29. 30. The packing member of claim 28, wherein the organic binder component comprises a polymerizable component, the binder component being operable to polymerize to form a (co)polymer.

30. The filling member of claim 29, wherein the organic binder component comprises a polymerizable monomer and a cross-linking member.

31. 31. The filling member of claim 30, wherein the polymerizable monomer comprises one or more ethylenically unsaturated monomers and / or vinyl monomers.

32. The filling member of claim 31, wherein the polymerizable monomer comprises an acrylic monomer or a derivative thereof.

33. A filling member described in claim 31 or 32, wherein the polymerizable monomer comprises one or more acrylamide monomers.

34. A filling member according to any one of claims 31 to 33, wherein the polymerizable monomer comprises a monomer selected from one or more of methacrylamide (MAM), N-(hydroxymethyl)acrylamide (hMAM), hydroxyethylacrylamide (hEAM) and / or N-vinyl-2-pyrrolidinone (NVP).

35. A filling member according to any one of claims 30 to 34, wherein the cross-linking member is selected from one or more of diethylenically unsaturated monomers, acrylic salts and / or polyethylene glycol substituted acrylic monomers.

36. The filling member of claim 35, wherein the diethylenically unsaturated monomer comprises a diacryl monomer or a derivative thereof.

37. A filling member as described in claim 35 or 36, wherein the diethylenically unsaturated monomer comprises a diacrylamide monomer.

38. A packing member according to any one of claims 28 to 37, wherein the ceramic material comprises aluminium oxide, aluminium silicate, magnesium aluminate, calcium aluminate, zirconia, silica, titanate, carbon and / or magnesium oxide.

39. The process of any one of claims 20 to 22, wherein the filler member is formed from a casting composition or slip.

40. The process of claim 39, wherein the filling member is formed from a clay or non-clay castable composition, a liquid cement or a gel cast composition.

41. The process of claim 39 or 40, wherein the filling member is formed from a gel cast composition.

42. The process of claim 41, wherein the gel cast composition comprises a ceramic material, an organic binder component, and optionally a pore-forming component.

43. The process of claim 42, wherein the organic binder component comprises a polymerizable component, the binder component operable to polymerize to form a (co)polymer.

44. The process of claim 43, wherein the organic binder component comprises a polymerizable monomer and a cross-linking member.

45. The process of claim 44, wherein the polymerizable monomers comprise one or more ethylenically unsaturated monomers and / or vinyl monomers.

46. ​​The process of claim 45, wherein the polymerizable monomer comprises an acrylic monomer or a derivative thereof.

47. The process of claim 45 or 46, wherein the polymerizable monomer comprises one or more acrylamide monomers.

48. The process of any one of claims 45 to 47, wherein the polymerizable monomer comprises a monomer selected from one or more of methacrylamide (MAM), N-(hydroxymethyl)acrylamide (hMAM), hydroxyethylacrylamide (hEAM), and / or N-vinyl-2-pyrrolidinone (NVP).

49. The process of any one of claims 44 to 48, wherein the cross-linking member is selected from one or more of diethylenically unsaturated monomers, acrylic salts and / or polyethylene glycol substituted acrylic monomers.

50. The process of claim 49, wherein the diethylenically unsaturated monomer comprises a diacryl monomer or a derivative thereof.

51. The process of claim 49 or 50, wherein the diethylenically unsaturated monomer comprises a diacrylamide monomer.

52. The process of any one of claims 42 to 51, wherein the ceramic material comprises aluminum oxide, aluminum silicate, magnesium aluminate, calcium aluminate, zirconia, silica, titanate, carbon and / or magnesium oxide.

53. A reactor comprising a catalyst bed, said catalyst bed comprising a packing element according to any one of claims 18 to 38.

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