WO2021104166A1 - 氧铝联产电解用的电极结构 - Google Patents
氧铝联产电解用的电极结构 Download PDFInfo
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- WO2021104166A1 WO2021104166A1 PCT/CN2020/130415 CN2020130415W WO2021104166A1 WO 2021104166 A1 WO2021104166 A1 WO 2021104166A1 CN 2020130415 W CN2020130415 W CN 2020130415W WO 2021104166 A1 WO2021104166 A1 WO 2021104166A1
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- Prior art keywords
- cathode
- carbon
- conductive base
- aluminum
- tib
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- 238000005868 electrolysis reaction Methods 0.000 title claims abstract description 24
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 23
- CQBLUJRVOKGWCF-UHFFFAOYSA-N [O].[AlH3] Chemical compound [O].[AlH3] CQBLUJRVOKGWCF-UHFFFAOYSA-N 0.000 title abstract description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 43
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 33
- 238000000576 coating method Methods 0.000 claims abstract description 31
- 239000000463 material Substances 0.000 claims abstract description 26
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 23
- 239000011248 coating agent Substances 0.000 claims abstract description 23
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 21
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 15
- 239000010406 cathode material Substances 0.000 claims abstract description 6
- 239000007788 liquid Substances 0.000 claims abstract description 5
- 238000009434 installation Methods 0.000 claims description 20
- 239000000945 filler Substances 0.000 claims description 19
- 239000002131 composite material Substances 0.000 claims description 14
- 239000003575 carbonaceous material Substances 0.000 claims description 13
- 239000000835 fiber Substances 0.000 claims description 12
- 239000000919 ceramic Substances 0.000 claims description 11
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 8
- 239000004917 carbon fiber Substances 0.000 claims description 8
- 239000004744 fabric Substances 0.000 claims description 8
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical group C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 8
- 229910052760 oxygen Inorganic materials 0.000 claims description 8
- 239000001301 oxygen Substances 0.000 claims description 8
- 229910000831 Steel Inorganic materials 0.000 claims description 6
- 239000010959 steel Substances 0.000 claims description 6
- 239000004568 cement Substances 0.000 claims description 5
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 4
- 239000010439 graphite Substances 0.000 abstract description 10
- 229910002804 graphite Inorganic materials 0.000 abstract description 10
- 229910052700 potassium Inorganic materials 0.000 abstract description 10
- 229910052708 sodium Inorganic materials 0.000 abstract description 10
- 150000003839 salts Chemical class 0.000 abstract description 4
- 238000005266 casting Methods 0.000 abstract description 2
- QYEXBYZXHDUPRC-UHFFFAOYSA-N B#[Ti]#B Chemical compound B#[Ti]#B QYEXBYZXHDUPRC-UHFFFAOYSA-N 0.000 abstract 2
- 229910033181 TiB2 Inorganic materials 0.000 abstract 2
- 229910052581 Si3N4 Inorganic materials 0.000 abstract 1
- 230000015572 biosynthetic process Effects 0.000 abstract 1
- 150000001875 compounds Chemical class 0.000 abstract 1
- 229910052593 corundum Inorganic materials 0.000 abstract 1
- 230000002687 intercalation Effects 0.000 abstract 1
- 238000009830 intercalation Methods 0.000 abstract 1
- 229910001845 yogo sapphire Inorganic materials 0.000 abstract 1
- 238000000034 method Methods 0.000 description 20
- 239000011734 sodium Substances 0.000 description 9
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 8
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 8
- 239000011591 potassium Substances 0.000 description 8
- 238000010586 diagram Methods 0.000 description 6
- 230000035515 penetration Effects 0.000 description 5
- 239000011324 bead Substances 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- 239000003792 electrolyte Substances 0.000 description 2
- 238000005265 energy consumption Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000001125 extrusion Methods 0.000 description 2
- 239000005431 greenhouse gas Substances 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 229910016569 AlF 3 Inorganic materials 0.000 description 1
- 229910004261 CaF 2 Inorganic materials 0.000 description 1
- KRHYYFGTRYWZRS-UHFFFAOYSA-M Fluoride anion Chemical compound [F-] KRHYYFGTRYWZRS-UHFFFAOYSA-M 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 150000001491 aromatic compounds Chemical class 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002006 petroleum coke Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- SRVJKTDHMYAMHA-WUXMJOGZSA-N thioacetazone Chemical group CC(=O)NC1=CC=C(\C=N\NC(N)=S)C=C1 SRVJKTDHMYAMHA-WUXMJOGZSA-N 0.000 description 1
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
- C25C3/00—Electrolytic production, recovery or refining of metals by electrolysis of melts
- C25C3/06—Electrolytic production, recovery or refining of metals by electrolysis of melts of aluminium
- C25C3/08—Cell construction, e.g. bottoms, walls, cathodes
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
Definitions
- the present invention belongs to a wettable electrode structure for co-production of oxygen and aluminum or carbon-free aluminum electrolysis, and particularly relates to a so-called “inert” or “wettable” electrode structure.
- the current Hall-Herout aluminum electrolysis cell uses consumable carbon anodes, which not only consumes a large amount of high-quality petroleum coke as the main carbon material, but also emits a large amount of greenhouse gas CO 2 , strong greenhouse gas fluorocarbons (CF 4 , C 2 F 6 ) , SO 2 , and in the current aluminum electrolysis process, the pre-baked anode carbon block needs to be replaced frequently and frequently, which leads to unstable electrolysis production, and increases labor intensity, the personal risk of workers facing high-temperature melt, and the risk of fluoride.
- non-carbon anodes or inert anodes to achieve a new process of co-production of oxygen and primary aluminum electrolysis can solve the above-mentioned emission and pollution problems, and can improve production efficiency, reduce floor space, and reduce production costs. It has become the international aluminum industry and materials industry. The focus of attention and research hotspots.
- the use of non-carbon anodes in the electrolysis process of oxy-aluminum co-production has the following advantages: (1) The electrode is almost not consumed during the electrolysis process, and the material consumption is less than one percent of the carbon anode. No additional carbon processing plant and carbon anode assembly are required.
- the electrode is not consumed, the pole distance is stable, easy to control, the anode replacement frequency is reduced by more than ten times, labor intensity and occupational risks It is greatly reduced; (3) A higher current per unit volume can be used to increase the capacity of the electrolyzer; (4) The anode product is oxygen, which avoids environmental pollution, and oxygen can also be used as a by-product.
- the traditional horizontal arrangement of electrodes can no longer be used, but the vertical arrangement of electrodes must be adopted, so as to well maintain thermal balance, reduce cell voltage, and reduce energy consumption.
- the vertical installation method of the wettable cathode plays an important role in the realization of carbon-free aluminum electrolysis technology.
- the object of the present invention is to provide a method for installing, preventing and eliminating expansion of a vertical wettable cathode block or an inverted hollow cup cathode used in the electrolysis of co-production of aluminum oxide to improve the service life of the existing technology.
- Oxygen-aluminum co-production or non-carbon anode aluminum electrolysis cell consists of an electrolytic cell furnace, a cathode conductive base, an aluminum pool, and a high-temperature molten salt.
- the vertical non-carbon anode and the vertical cathode are arranged in parallel and opposite, and the anode and the cathode can be continuously spaced to the required capacity. until.
- the high-temperature molten salt is NaF-KF-CaF 2 -MgF 2 -LiF-AlF 3 -Al 2 O 3 melt at 750-950°C.
- the electrode structure for the electrolysis of co-production of aluminum and oxygen includes an anode group, a cathode group, and a cathode conductive base.
- the anode group and the cathode group are arranged perpendicularly and parallel to each other.
- the cathode is in the shape of a plate, block or rectangular parallelepiped deep cup installed in the electrolysis At the bottom of the slot, the cathode is on the conductive base.
- the cathode support base is arranged in a groove or groove on the cathode conductive base, and a filler is arranged between the cathode support base and the cathode conductive base, and the material of the cathode support base is TiB One of 2 -based materials, graphite-based materials, carbon materials, graphite-based materials with TiB 2 -based coatings on the surface, or carbon materials.
- the cathode conductive base material is one of graphite-based materials, carbon materials or TiB 2 -C composite materials; the cathode conductive base is provided with grooves or grooves to support the vertical cathode, and the cathode base has conductivity, which will come from the anode
- the current transmitted to the cathode through the electrolyte is then transmitted to the current collector iron rod or steel rod or alloy rod inside or below it to the cathode bus bar.
- the cathode is made of TiB 2 -C composite material.
- the cathode is plate-shaped or block-shaped, it is an integrated structure. Its shape is chamfered or the long side is straight, and the two sides are arcs.
- the cathode is made of TiB 2 -C composite material.
- the cathode is a cuboid deep cup shape, the periphery is chamfered or the long side is straight, and the two sides are arcs. When installed, it is connected to the battery and inserted into the deep cup. Inside, then the battery core is inserted into the groove or slot of the cathode conductive base.
- the battery core is one of TiB 2 -based materials, graphite-based materials, carbon materials, graphite-based materials with TiB 2 -based coatings on the surface, or carbon materials, and a filler is arranged between the battery core and the deep-cup cathode material .
- the filler is woven or pressed by one or a combination of graphite fiber, carbon fiber, carbon cloth, carbon paper, SiC fiber, and TiB 2 fiber.
- the filler is used as a buffer layer to adjust the verticality and prevent Thermal expansion at high temperatures squeezes the cathode material itself or the cathode substrate to maintain the stability of the vertical cathode.
- an insulating layer is also provided between the aluminum liquid level and the cathode conductive base to further stabilize the cathode and maintain its verticality.
- the insulating layer material is casted with amorphous high alumina material, or alumina ceramics, SiC ceramics , Si 3 N 4 ceramics, BN-TiB 2 composite ceramics or their composites.
- a coating is coated on the surface of the cathode conductive base, and the coating is one of high alumina cement, TiB 2 -based coating, SiC coating, Si 3 N 4 coating, or a combination of two or more of them. coating.
- the purpose is to reduce the penetration of Na and K in the electrolyte to the cathode conductive base causing sodium and potassium to expand.
- a cathode steel rod current collector is also provided under the cathode conductive base.
- Figure 1 is a schematic diagram of the arrangement of vertical anodes and vertical cathodes
- Figure 2 is a block or plate (a), deep cup (b) TiB 2 -based cathode material;
- Example 3 is a schematic diagram of the shape and installation of the vertical cathode of the non-electric core in Example 1;
- FIG. 4 is a schematic diagram of the shape and installation of the vertical cathode of the battery cell in the second embodiment
- Figure 5 is a schematic diagram of the shape and installation of the vertical cathode of the non-electric core in the third embodiment
- Fig. 6 is a schematic diagram of the vertical cathode plate without a battery and its installation in embodiment 4;
- Figure 7 is a schematic diagram of the shape and installation of two vertical cathodes without a battery in the fifth embodiment
- One of the shape and installation method of the vertical cathode a shape and installation method of a vertical cathode without a battery, as shown in Figure 3.
- the anode group and the cathode group are arranged vertically and parallel to each other.
- the cathode is a plate-shaped or block-shaped integrated structure.
- the cathode is directly inserted into the groove or groove on the cathode conductive base during installation. Insulation is also provided between the aluminum liquid level and the cathode conductive base.
- the layering is coated with a coating on the surface of the cathode conductive base, and a cathode steel rod current collector is arranged under the extremely conductive base.
- One of the shape and installation method of the vertical cathode a shape and installation method of a vertical cathode with a battery cell, as shown in Figure 4.
- the anode group and the cathode group are arranged vertically and parallel to each other.
- the cathode is a cuboid deep cup shape. When installed, it is connected to the battery core and inserted into the deep cup, and then the battery core is inserted into the cathode conductive base groove or slot, the battery core and the deep cup A filler is arranged between the shaped cathode materials, an insulating layer is also arranged between the aluminum liquid level and the cathode conductive base, and a cathode steel rod current collector is arranged under the extremely conductive base.
- FIG. 5 Another shape and installation method of the vertical cathode without a battery is shown in Figure 5.
- a filler is used to cover the cathode, and the cathode plate is pushed into the long slit reserved on the cathode base by extrusion, and the cathode is kept vertical.
- the filler is woven from carbon fiber or a Layers or layers of carbon cloth or carbon paper are made into bags.
- an insulating bead is used for supporting and positioning, and the insulating bead is prefabricated by one of high alumina ceramics, high alumina amorphous material casting, SiC ceramics, and Si 3 N 4 ceramics.
- a coating is applied on the surface of the cathode base (base) to reduce the penetration of sodium and potassium into the base (base).
- the coating can be SiC, high alumina cement, Si 3 N 4 , One of TiB 2 -C composite coatings.
- FIG. 6 Another shape and installation method of the vertical cathode without a battery is shown in Figure 6.
- a filler is used to cover the cathode, and the cathode plate is pushed into the long slit reserved on the cathode conductive base by squeezing, and the cathode is kept vertical.
- the filler is woven by carbon fiber or used One or several layers of carbon cloth or carbon paper are made into bags.
- a coating is applied on the surface of the cathode base (base) to reduce the penetration of sodium and potassium into the base (base).
- the coating can be SiC, high alumina cement, Si 3 N 4 , One of TiB 2 -C composite coatings.
- One of the shape and installation method of the vertical cathode a shape and installation method of a two-section vertical cathode without a battery, as shown in Figure 7.
- a filler is used to hold the cathode, and the cathode plate is pushed into the long slit reserved on the cathode support base by extrusion, and the cathode is kept vertical.
- the filler is woven by carbon fiber or used One or several layers of carbon cloth or carbon paper are made into bags.
- the cathode support base can be TiB 2 -C composite material, graphite-based material, carbon material, graphite-based material coated with TiB 2 -C coating on the surface, or carbon material.
- the cathode support base is then pushed into the pit reserved for the cathode conductive base.
- a coating is applied on the surface of the cathode base (base) to reduce the penetration of sodium and potassium into the base (base).
- the coating can be SiC, high alumina cement, Si 3 N 4 , One of TiB 2 -C composite coatings.
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Electrolytic Production Of Metals (AREA)
Abstract
Description
Claims (7)
- 氧铝联产电解用的电极结构,其特征在于,包括阳极组、阴极组、阴极导电底座,所述阳极组与阴极组垂直平行相对排列,所述阴极呈板状、块状或长方体深杯状安装在电解槽槽底阴极导电底座上;所述阴极由TiB 2-C复合材料构成;当所述阴极为板状或块状时,为一体化的结构,其形状周边为倒角或长边为直边,两侧为圆弧,安装时直接插入阴极导电底座上的沟或槽,或先镶嵌在阴极支撑基座上再插入阴极导电底座上的沟槽;且阴极与阴极支撑基座间设有填充物;所述填充物为碳纤维、碳布、碳纸、SiC纤维、TiB 2纤维中的一种或几种组合编织或压制而成;当所述阴极为长方体深杯状时,周边为倒角或长边为直边,两侧为圆弧,安装时与电芯连接,倒插入深杯内部,然后电芯再插入阴极导电底座沟或槽中;所述电芯是TiB 2基材料、碳材料、表面有TiB 2基涂层的碳材料中的一种,电芯与深杯状阴极材料之间设有填充物,所述填充物为碳纤维、碳布、碳纸、SiC纤维、TiB 2纤维中的一种或几种组合编织或压制而成。
- 如权利要求1所述的氧铝联产电解用的电极结构,其特征在于,还包括阴极支撑基座,所述阴极支撑基座设于阴极导电底座上的沟或槽内,且阴极支撑基座和阴极导电底座间设有填充物,阴极支撑基座材料是TiB 2基材料、碳材料、表面有TiB 2基涂层的碳材料中的一种。
- 如权利要求1所述的氧铝联产电解用的电极结构,其特征在于,所述阴极导电底座材料是碳材料或TiB 2-C复合材料中的一种;所述阴极导电底座上设有沟或槽,支撑垂直阴极,阴极底座具备导电性。
- 如权利要求2所述的氧铝联产电解用的电极结构,其特征在于,所述填充物为碳纤维、碳布、碳纸、SiC纤维、TiB 2纤维中的一种或几种组合编织或压制而成。
- 如权利要求1所述的氧铝联产电解用的电极结构,其特征在于,铝液水平面和阴极导电底座之间还设有绝缘压条,所述绝缘压条材料采用无定形高氧化铝材料浇注,或采用氧化铝陶瓷、SiC陶瓷、Si 3N 4陶瓷、BN-TiB 2复合陶瓷中的一种或其复合物制成。
- 如权利要求1所述的氧铝联产电解用的电极结构,其特征在于,在阴极导电底座表面涂覆有涂层,所述涂层为高氧化铝水泥、TiB 2基涂层、SiC涂层、Si 3N 4涂层中的一种或其两种以上复合涂层。
- 如权利要求1所述的氧铝联产电解用的电极结构,其特征在于,阴极导电底座下方还设有阴极钢棒集流体。
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CN111979562B (zh) * | 2020-08-18 | 2023-03-10 | 天津大学 | 一种插拔式胶囊阴极及可扩展高效合成h2o2反应器装置 |
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