CN218561125U - Preparation device of high-purity trisilylamine - Google Patents
Preparation device of high-purity trisilylamine Download PDFInfo
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- CN218561125U CN218561125U CN202222906337.1U CN202222906337U CN218561125U CN 218561125 U CN218561125 U CN 218561125U CN 202222906337 U CN202222906337 U CN 202222906337U CN 218561125 U CN218561125 U CN 218561125U
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- VOSJXMPCFODQAR-UHFFFAOYSA-N ac1l3fa4 Chemical compound [SiH3]N([SiH3])[SiH3] VOSJXMPCFODQAR-UHFFFAOYSA-N 0.000 title claims abstract description 62
- 238000002360 preparation method Methods 0.000 title claims abstract description 19
- 239000000463 material Substances 0.000 claims abstract description 86
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims abstract description 40
- 238000003756 stirring Methods 0.000 claims abstract description 38
- KOPOQZFJUQMUML-UHFFFAOYSA-N chlorosilane Chemical compound Cl[SiH3] KOPOQZFJUQMUML-UHFFFAOYSA-N 0.000 claims abstract description 37
- 238000010438 heat treatment Methods 0.000 claims abstract description 31
- 239000002904 solvent Substances 0.000 claims abstract description 29
- 150000001335 aliphatic alkanes Chemical class 0.000 claims abstract description 27
- 238000001914 filtration Methods 0.000 claims abstract description 27
- 239000012295 chemical reaction liquid Substances 0.000 claims abstract description 25
- 238000006243 chemical reaction Methods 0.000 claims abstract description 22
- 238000003860 storage Methods 0.000 claims abstract description 20
- 239000012065 filter cake Substances 0.000 claims abstract description 12
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 40
- 238000002156 mixing Methods 0.000 claims description 18
- 229910052757 nitrogen Inorganic materials 0.000 claims description 18
- 238000012856 packing Methods 0.000 claims description 16
- 239000002808 molecular sieve Substances 0.000 claims description 10
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 10
- 238000010926 purge Methods 0.000 claims description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 7
- 239000007788 liquid Substances 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- 239000011521 glass Substances 0.000 claims description 4
- 229910001220 stainless steel Inorganic materials 0.000 claims description 4
- 239000010935 stainless steel Substances 0.000 claims description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 4
- 229910021536 Zeolite Inorganic materials 0.000 claims description 3
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 3
- 239000000945 filler Substances 0.000 claims description 3
- 239000010457 zeolite Substances 0.000 claims description 3
- 229910001873 dinitrogen Inorganic materials 0.000 claims 4
- 238000000034 method Methods 0.000 abstract description 14
- 239000000126 substance Substances 0.000 abstract description 8
- 239000005046 Chlorosilane Substances 0.000 abstract description 4
- 230000008901 benefit Effects 0.000 abstract description 3
- 239000000047 product Substances 0.000 abstract description 3
- 238000004904 shortening Methods 0.000 abstract 1
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 40
- 239000013067 intermediate product Substances 0.000 description 12
- 239000007791 liquid phase Substances 0.000 description 11
- OFBQJSOFQDEBGM-UHFFFAOYSA-N Pentane Chemical compound CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 10
- 239000000243 solution Substances 0.000 description 8
- 238000009825 accumulation Methods 0.000 description 7
- 150000003863 ammonium salts Chemical class 0.000 description 7
- 230000005587 bubbling Effects 0.000 description 6
- 238000007086 side reaction Methods 0.000 description 6
- 230000015572 biosynthetic process Effects 0.000 description 5
- 238000009835 boiling Methods 0.000 description 5
- 230000007613 environmental effect Effects 0.000 description 5
- 238000003786 synthesis reaction Methods 0.000 description 5
- 150000003973 alkyl amines Chemical class 0.000 description 4
- 239000012535 impurity Substances 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- 239000010963 304 stainless steel Substances 0.000 description 3
- 229910000589 SAE 304 stainless steel Inorganic materials 0.000 description 3
- 229910021529 ammonia Inorganic materials 0.000 description 3
- 239000007795 chemical reaction product Substances 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 238000010907 mechanical stirring Methods 0.000 description 3
- FZHAPNGMFPVSLP-UHFFFAOYSA-N silanamine Chemical class [SiH3]N FZHAPNGMFPVSLP-UHFFFAOYSA-N 0.000 description 3
- 238000005406 washing Methods 0.000 description 3
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 2
- 238000000231 atomic layer deposition Methods 0.000 description 2
- 238000005229 chemical vapour deposition Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
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- 238000010574 gas phase reaction Methods 0.000 description 2
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- 239000004065 semiconductor Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- 229910052581 Si3N4 Inorganic materials 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- KOOADCGQJDGAGA-UHFFFAOYSA-N [amino(dimethyl)silyl]methane Chemical compound C[Si](C)(C)N KOOADCGQJDGAGA-UHFFFAOYSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 238000013019 agitation Methods 0.000 description 1
- 235000019270 ammonium chloride Nutrition 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000007810 chemical reaction solvent Substances 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 238000013329 compounding Methods 0.000 description 1
- 230000006837 decompression Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 238000005137 deposition process Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000004821 distillation Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 238000002290 gas chromatography-mass spectrometry Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 229920001709 polysilazane Polymers 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 239000012713 reactive precursor Substances 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
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Abstract
The utility model provides a preparation device of high-purity trisilylamine, which belongs to the technical field of chemical industry and comprises a low-temperature mixer, a four-in-one reactor and a rectifying tower group which are connected in sequence; the input end of the low-temperature mixer is communicated with the alkane solvent storage tank and the chlorosilane storage tank; the four-in-one reactor comprises an intelligent temperature control unit for controlling the reaction temperature, a stirring unit for mechanically stirring the mixed material and the liquid ammonia to obtain a reaction liquid, a heating unit for heating the reaction liquid under reduced pressure to obtain a volatile material and a residual material, and a closed filtering unit for filtering the residual material to form a filter cake; the volatile material output end of the four-in-one reactor is communicated with the rectifying tower group through a condenser and a receiver. The method has the advantages of shortening the preparation process, reducing the equipment cost and investment, and improving the product preparation efficiency, operability and safety.
Description
Technical Field
The utility model relates to a chemical industry technical field specifically says, relates to a preparation facilities of high-purity trisilylamine.
Background
Organic aminosilanes can be used in a variety of deposition processes including Atomic Layer Deposition (ALD), chemical Vapor Deposition (CVD), and are layer precursors that can be used in the semiconductor industry as silicon nitride or silicon oxynitride layers in chip fabrication. Among them, trisilylamine is a liquid organic aminosilane with good fluidity, colorless, and easy to hydrolyze, can be used for depositing a high-purity silicon oxide film used as a filling gap in a semiconductor process, and is a reactive precursor for film growth without direct plasma excitation.
The trisilylamine is produced by a gas phase reaction method and a liquid phase reaction method; the gas phase reaction method is to react monochlorosilane and ammonia in gaseous form at different temperatures and different pressures according to different feed ratios, and to obtain trisilylamine by collecting reaction products and separating the reaction products in a certain way. The liquid phase reaction method is that monochlorosilane reacts with ammonia in various forms of liquid, and the reaction product is filtered and separated to prepare trisilylamine. Although the preparation of trisilylamine is achieved, it still has the following disadvantages: 1) The synthesis side reaction is more, because the reaction is an exothermic reaction, although a reaction solvent exists, the solution still has local heat accumulation; 2) Because the filter is replaced by a filter and a distillation link of the filtrate exists, the preparation process is longer, and the equipment investment cost is higher; 3) Because the materials are required to be transferred among all links, the risk of introducing impurities in the transferring process is increased; 4) In a large-scale production scene, the filter is difficult to disassemble, and certain safety and environmental protection risks exist.
Therefore, an apparatus for preparing trisilylamine that avoids the occurrence of heat accumulation reaction is desired.
Disclosure of Invention
The utility model aims to provide a preparation facilities of high-purity trisilylamine to solve at least one problem that exists among the prior art.
In order to achieve the aim, the utility model provides a preparation device of high-purity trisilylamine, which comprises a low-temperature mixer, a four-in-one reactor and a rectifying tower group which are connected in sequence; the low-temperature mixer is used for fully mixing monochlorosilane and alkane solvent to form a mixed material; the output end of the low-temperature mixer and the output end of the liquid nitrogen storage tank are communicated with the input end of the four-in-one reactor; wherein, the input end of the low-temperature mixer is communicated with the alkane solvent storage tank and the monochlorosilane storage tank;
the four-in-one reactor comprises an intelligent temperature control unit for controlling the reaction temperature, a stirring unit for mechanically stirring the mixed material and the liquid ammonia to obtain a reaction liquid, a heating unit for heating the reaction liquid under reduced pressure to obtain a volatile material and a residual material, and a closed filtering unit for filtering the residual material to form a filter cake;
the volatile material output end of the four-in-one reactor is communicated with the rectifying tower group through a condenser and a receiver.
Further, the preferable structure comprises that the rectifying tower group comprises a light component removing rectifying tower and a heavy component removing rectifying tower;
the output end of the receiver is connected with the input end of the light component removal rectifying tower; the tower kettle of the light component removing rectifying tower is connected with the input end of the heavy component removing rectifying tower;
the top of the de-heavy rectifying tower is a high-purity trisilylamine output end.
Further, the preferable structure comprises that the light component removal rectifying tower and the heavy component removal rectifying tower are both packed towers, and the packing of the packed towers is one of stainless steel theta ring packing, triangular spiral packing or glass spring packing.
Further, a preferred structure includes a dryer provided between the input end of the low-temperature mixer and the alkane solvent storage tank.
Further, the preferable structure includes that the filler of the dryer is one of 4A molecular sieve, 5A molecular sieve, activated carbon or artificial zeolite.
Further, the preferred structure includes that a nitrogen conveying device used for purging and replacing the mixed material by nitrogen is arranged between the output end of the low-temperature mixer and the four-in-one reactor, and the nitrogen conveying device is communicated with a nitrogen input port of the four-in-one reactor.
Further, the preferable structure comprises that the intelligent temperature control unit of the four-in-one reactor is a jacket wrapped on the outer side of the reactor.
Further, a preferred structure includes that the stirring unit of the four-in-one reactor is a stirring blade provided in the reactor.
Further, the preferable structure comprises that a filter is arranged between the receiver and the rectifying tower group, and the filter is a T-shaped filter or a Y-shaped filter.
Further, the preferable structure includes that the heating medium of the rectifying tower kettle of the rectifying tower group is hot water or heat conducting oil.
As mentioned above, the utility model discloses a preparation facilities of high-purity trisilyl amine, through carrying out the low temperature mixture with chlorosilane and alkane solvent earlier after, adopt and control the temperature with intelligence, stirring, heating and closed filtration carry out the integrated four-in-one reactor and react and obtain thick trisilyl amine, utilize the rectifying column to carry out the rectification under reduced pressure and obtain high-purity trisilyl amine at last. The beneficial effects are as follows:
1) Compared with the prior liquid phase reaction method for preparing trisilylamine, the utility model firstly utilizes the low-temperature mixer to mix monochlorosilane and alkane solvent at low temperature, and then carries out low-temperature stirring reaction in the four-in-one reactor, thereby effectively avoiding local heat accumulation and reducing more synthesis side reactions;
2) The closed filter unit is one part of the four-in-one reactor, so that the transfer link of materials in the air is reduced, and the risk of introducing impurities is reduced;
3) Through adopting and carrying out the four unification reactors that integrate with intelligent accuse temperature, stirring, heating and closed filtration, effectively shorten the preparation flow, reduced safe risk and environmental protection risk.
4) The method has the characteristics of simple process technology and device structure and reliable operation, and realizes higher economic benefit and environmental protection benefit.
Drawings
FIG. 1 is a schematic diagram illustrating the structural principle of an apparatus for preparing high-purity trisilylamine according to an embodiment of the present invention.
Detailed Description
It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the invention. The examples do not show specific techniques or conditions, and the reagents or apparatuses used are not shown in the specifications of the products, and the conventional products are available from normal distributors.
In the description of the present invention, it is to be understood that the terms "center", "longitudinal", "lateral", "length", "width", "thickness", "upper", "lower", "front", "rear", "left", "right", "vertical", "horizontal", "top", "bottom", "inner", "outer", "clockwise", "counterclockwise", "axial", "radial", "circumferential", and the like, indicate the orientation or positional relationship indicated based on the drawings, and are only for convenience of description and simplicity of description, and do not indicate or imply that the device or element referred to must have a particular orientation, be constructed and operated in a particular orientation, and therefore, should not be construed as limiting the present invention.
Furthermore, the terms "first", "second" and "first" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include at least one such feature. In the description of the present invention, "a plurality" means at least two, e.g., two, three, etc., unless expressly specified otherwise.
In the present invention, unless otherwise expressly stated or limited, the terms "mounted," "connected," and "fixed" are to be construed broadly and may, for example, be fixedly connected, detachably connected, or integrally formed; may be mechanically coupled, may be electrically coupled or may be in communication with each other; they may be directly connected or indirectly connected through intervening media, or they may be connected internally or in any other suitable relationship, unless expressly stated otherwise. The specific meaning of the above terms in the present invention can be understood according to specific situations by those skilled in the art.
In the present application, unless expressly stated or limited otherwise, the first feature may be directly on or directly under the second feature or indirectly via intermediate members. Also, a first feature "on," "over," and "above" a second feature may be directly or diagonally above the second feature, or may simply indicate that the first feature is at a higher level than the second feature. A first feature being "under," "below," and "beneath" a second feature may be directly under or obliquely under the first feature, or may simply mean that the first feature is at a lesser elevation than the second feature.
In the description of the present specification, reference to the description of "one embodiment," "some embodiments," "an example," "a specific example," or "some examples" or the like means that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the present invention. In this specification, the schematic representations of the terms used above are not necessarily intended to refer to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, various embodiments or examples and features of different embodiments or examples described in this specification can be combined and combined by one skilled in the art without contradiction.
Various embodiments of the present invention will be described in detail below with reference to the accompanying drawings.
FIG. 1 specifically illustrates the principle of an apparatus for preparing high purity trisilylamine according to an embodiment of the present invention. Specifically, fig. 1 is a schematic diagram of an apparatus for preparing high purity trisilylamine according to an embodiment of the present invention.
As shown in FIG. 1, the preparation device of high-purity trisilylamine comprises a low-temperature mixer, a four-in-one reactor and a rectifying tower set which are connected in sequence; the low-temperature mixer is used for fully mixing Monochlorosilane (MCS) and alkane solvent to form a mixed material; the output end of the low-temperature mixer and the output end of the liquid ammonia storage tank are communicated with the input end of the four-in-one reactor; wherein, the input end of the low-temperature mixer is communicated with the alkane solvent storage tank and the monochlorosilane storage tank; the four-in-one reactor comprises an intelligent temperature control unit for controlling the reaction temperature, a stirring unit for mechanically stirring the mixed material and the liquid ammonia to obtain reaction liquid, a heating unit for heating the reaction liquid under reduced pressure to obtain volatile materials and residual materials, and a closed filtering unit for filtering the residual materials to form a filter cake; the volatile material output end of the four-in-one reactor is communicated with the rectifying tower group through a condenser and a receiver. Wherein, the intelligent temperature control unit of the four-in-one reactor is a heat exchange jacket wrapped outside the reactor. The stirring unit of the four-in-one reactor is a stirring blade arranged in the reactor. The utility model discloses compare with current liquid phase reaction method preparation trisilylamine, through carrying out the low temperature with chlorosilane and alkane solvent earlier and mixing the back, adopt to control the temperature with intelligence, stirring, heating and the closed four unification reactors that carry out the integration react and obtain thick trisilylamine, utilize the rectifying column to carry out the decompression rectification and obtain high-purity trisilylamine at last. Namely, the monochlorosilane and the alkane solvent are mixed at low temperature and then stirred at low temperature in the four-in-one reactor, so that the local heat accumulation is effectively avoided, and more synthesis side reactions are reduced.
The low-temperature mixer was made of 304 stainless steel and was electropolished inside. The four-in-one multifunctional reactor is a kettle type reaction kettle and is made of 304 stainless steel, and the stirring blades are made of 304 stainless steel; the temperature resistant range is from +200 ℃ to-40 ℃, and the working pressure is 1.0-2.0 Mpa. The reactor needs an intelligent temperature control unit to provide a heat exchange jacket for wrapping the reactor (the temperature is controlled to be-30-200 ℃), and a stirring unit is configured for mechanical stirring and a closed filtering unit is configured for closed filtering. A plurality of reserved ports at the top of the four-in-one reactor, including a nitrogen input port, a tail gas port, a feed inlet, an exhaust port, a liquid discharge port and the like. Wherein, the input end of the four-in-one reactor is a feed inlet; the tail gas outlet discharges uncondensed monochlorosilane; the exhaust port is communicated with the condenser and the receiver, and the exhaust port discharges the reacted ammonia, shan Jiagui alkylamine, disilylamine (DSA) and Trisilylamine (TSA).
Specifically, the exhaust port is connected to a vacuum pump, and the environment of the reactor can be pressurized and depressurized by providing the vacuum pump. Wherein, the charge door of four unification reactors directly communicates with the output of the last level's low temperature mixer and the output of liquid ammonia holding vessel, and the gas vent of four unification reactors directly communicates with heat exchanger and receiver directly, forms a confined reaction environment, has avoided the possible pollution that artifical application of sample brought. Moreover, the whole four-in-one reactor can be vacuumized and ventilated by a vacuum pump, and can be purged and replaced by a nitrogen input port. The above embodiments are all closed, can effectively avoid volatilization of the solution, ensure the atmosphere of the reactor, are particularly suitable for organic solvents, avoid pollution of external substances to the solution, and achieve the effects of improving the reaction efficiency and not polluting the environment.
In addition, compared with the prior art that the filter is difficult to disassemble and has certain safety and environmental protection risks, the four-in-one reactor can be disassembled in a closed manner by utilizing the detachable flange under normal pressure after the residual materials are filtered to form filter cakes, so that the disassembling action is quickly completed, and the condition that the interior of the four-in-one reactor is exposed in the air is effectively prevented; and after the filter cake is taken out, the four-in-one reactor is subjected to back loading and pressing by utilizing a detachable flange.
In a specific embodiment, the rectification column group comprises a light component removal rectification column and a heavy component removal rectification column; the output end of the receiver is connected with the input end of the light component removal rectifying tower; the tower kettle of the light component removal rectifying tower is connected with the input end of the heavy component removal rectifying tower; the top of the de-heavy rectifying tower is a high-purity trisilylamine output end. The light component removal rectifying tower and the heavy component removal rectifying tower are both packed towers, and the packing of the packed towers is one of stainless steel theta ring packing, triangular spiral packing or glass spring packing. The heating medium of the rectifying tower kettle of the rectifying tower group is hot water or heat conducting oil. The top of the rectifying tower group can be cooled by water with the temperature of 7 ℃; and the top of the light component removal rectifying tower outputs low-boiling substances, and the low-boiling substances comprise silylamine, disilylamine and other low-boiling substances. And the tower kettle of the heavy component removal rectifying tower outputs high-boiling substances and solid particles, wherein the high-boiling substances are n-hexane and the like with relatively high metal impurity content.
In a particular embodiment, a dryer is disposed between the input of the cryogenic mixer and the alkane solvent storage tank. The filler of the dryer is one of a 4A molecular sieve, a 5A molecular sieve, activated carbon or artificial zeolite.
In a specific embodiment, a nitrogen conveying device for purging and replacing the mixed material by using nitrogen is arranged between the output end of the low-temperature mixer and the four-in-one reactor, and the nitrogen conveying device is communicated with the nitrogen inlet of the four-in-one reactor.
In a specific embodiment, a filter is arranged between the receiver and the rectifying tower group, and the filter is a T-shaped filter or a Y-shaped filter.
The utility model also discloses a preparation method of the high-purity trisilylamine, which comprises the steps S110 to S160.
S110, fully mixing monochlorosilane and the dried alkane solvent in a low-temperature mixer at the working temperature of minus 30 ℃ to minus 20 ℃ and the working pressure of 1.0 to 3.0Mpa to form a mixed material.
In order to further avoid local heat accumulation and synthesis side reactions, besides low-temperature control and closed operation, the purity of monochlorosilane, alkane solvent and liquid ammonia needs to be limited; specifically, in the step of fully mixing the monochlorosilane material and the dried alkane solvent in a low-temperature mixer to form a mixed material, the alkane solvent is n-hexane solution with the purity of more than 99%, and the monochlorosilane material has the purity of more than 99.99%; the purity of the liquid ammonia is more than 99.99 percent; the working temperature of the low-temperature mixer is-20 ℃ to-10 ℃, and the working pressure is 1.0 to 1.5Mpa; wherein, the volume ratio of the alkane solvent to the monochlorosilane material is 2-10, and the mixing mode is bottom-sinking bubbling mixing. Wherein, the alkane solvent can be n-hexane or n-pentane.
To further ensure that the alkane solvent has as low a moisture content as possible (0-10 ppm), the alkane solvent needs to be dried by passing through a dryer before it reaches the low temperature mixer from the alkane solvent storage tank.
S120, adding the mixed materials into a four-in-one reactor, wherein the four-in-one reactor comprises an intelligent temperature control unit, a stirring unit, a heating unit and a closed filtering unit.
Before the mixed material is added into the four-in-one reactor, the method also comprises the following steps: the four-in-one reactor was purged with nitrogen to replace the dew point to acceptable (-60 ℃).
The step of adding the mixed material into the four-in-one reactor comprises S121, adding liquid ammonia into the four-in-one reactor in a liquid phase form; s122, adding the mixed material into liquid ammonia in a four-in-one reactor at a dropping speed of 0.3-1.5 g/min; wherein the mol ratio of the monochlorosilane to the liquid ammonia is as follows: 1.0 to 2.0. Through the mode of dropwise add the compounding in to liquid ammonia, further avoided the heat accumulation that exothermic reaction caused, further reduced the emergence of side reaction.
S130, controlling the temperature in the four-in-one reactor to be-20-10 ℃ through an intelligent temperature control unit, and mechanically stirring and reacting the mixed material and liquid ammonia for 10-60 min through a stirring unit to obtain a reaction liquid. It should be noted that, during the process of dropping the mixed solution, mechanical stirring is performed simultaneously, and after the dropping operation is completed, mechanical stirring is continued for 10 to 60min, so as to obtain the reaction solution. After obtaining the reaction liquid, the method also comprises the following steps: and adding an alkane solvent into the four-in-one reactor, and stirring and washing the four-in-one reactor by using the alkane solvent. The reactor is stirred and washed, so that the aim of removing ammonium salt attached inside the reactor is fulfilled. As an improvement of the embodiment, when the mixed material and liquid ammonia are mechanically stirred and reacted for 20-40 min, the reaction effect is better. It should be noted that the agitation washing step may be performed after the preparation of the highly pure trimethylsilylamine is completed. The solution obtained by washing the ammonium salt (solid ammonium chloride) adhered to the solution with a solvent is filtered, and the solvent is distilled off from the filtrate, whereby polysilazane can be obtained.
And S140, decompressing and heating the reaction liquid through a heating unit to obtain a volatile material and a residual material. Wherein the working pressure for decompressing and heating the reaction liquid by the heating unit is-30 to-10 Kpa, and the working temperature is 50 to 70 ℃.
S150, condensing the volatile materials through a condenser and then enabling the volatile materials to reach a receiver to obtain crude trisilylamine; simultaneously, the remaining material passes through a closed filtration unit to form a filter cake. Wherein the working temperature of the condenser is-10-0 ℃.
S160, feeding the crude trisilylamine into a light component removal rectifying tower after passing through a filter with the filtering precision of 1 mu m to obtain an intermediate product; and (3) conveying the intermediate product to a heavy component removal rectifying tower through a tower kettle of the light component removal rectifying tower, and obtaining high-purity trisilylamine through the tower top of the heavy component removal rectifying tower. Wherein the working pressure of the light component removing rectifying tower and the heavy component removing rectifying tower is-20 to 0Kpa, and the working temperature is 30 to 52 ℃.
The light component removal rectifying tower and the heavy component removal rectifying tower are both packed towers, and the packing of the packed towers is one of stainless steel theta ring packing, triangular spiral packing or glass spring packing. In a specific embodiment, the pressure of the light component removal rectifying tower is-10 Kpa, and the top temperature is 40 ℃; the tower pressure of the heavy component removal rectifying tower is-5 Kpa, and the top temperature is 42 ℃.
The following will describe in detail various examples of the process for preparing highly pure trisilylamine according to the present invention.
Example 1
S110, fully mixing normal hexane with the purity of 99% and monochlorosilane with the purity of 99.99% in a low-temperature mixer at the working temperature of minus 30 ℃ and the working pressure of 1.0Mpa, wherein the volume ratio of the normal hexane to the monochlorosilane is 2:1, and forming a mixed material. Wherein, n-hexane is dried by a 5A molecular sieve dryer in an n-hexane storage tank, then reaches a low-temperature mixer, and is subjected to bottom-sinking bubbling mixing.
S120, purging and replacing the four-in-one reactor by using nitrogen until the dew point is qualified (-60 ℃); adding liquid ammonia with the purity of 99.99 percent into a four-in-one reactor in a liquid phase form; adding the mixed material into liquid ammonia in a four-in-one reactor at a dropping speed of 0.3 g/min; wherein the mol ratio of the monochlorosilane to the liquid ammonia is as follows: 1.0:1.
S130, controlling the temperature in the four-in-one reactor to be-20 ℃, and mechanically stirring and reacting the mixed material and liquid ammonia for 10min through a stirring unit to obtain a reaction liquid.
After the reaction liquid is obtained, normal hexane is added into the four-in-one reactor, and the four-in-one reactor is stirred and washed by the normal hexane to remove ammonium salt attached to the interior of the reactor.
S140, decompressing and heating the reaction liquid through a heating unit under the conditions that the working pressure is-30 Kpa and the working temperature is 50 ℃ to obtain a volatile material and a residual material.
S150, condensing the volatile materials through a condenser with the working temperature of-10 ℃ and then enabling the volatile materials to reach a receiver to obtain crude trisilylamine; meanwhile, the residual materials pass through a closed filtering unit to form a filter cake. And a T-shaped filter is arranged between the receiver and the rectifying tower group.
S160, passing the crude trisilylamine through a filter with the filtering precision of 1 mu m, and then entering a light component removal rectifying tower with the working pressure of-20 Kpa and the working temperature of 30 ℃ to obtain an intermediate product; and (3) conveying the intermediate product to a heavy component removal rectifying tower with the working pressure of 0Kpa and the working temperature of 52 ℃ through a tower kettle of the light component removal rectifying tower, and obtaining high-purity trisilylamine through the tower top of the heavy component removal rectifying tower.
Example 2
S110, fully mixing normal hexane with the purity of 99% and monochlorosilane with the purity of 99.99% in a low-temperature mixer with the working temperature of-10 ℃ and the working pressure of 3.0Mpa, wherein the volume ratio of the normal hexane to the monochlorosilane is 10. Wherein, n-hexane is dried by a 4A molecular sieve dryer in an n-hexane storage tank, then reaches a low-temperature mixer, and is subjected to bottom-sinking bubbling mixing.
S120, purging and replacing the four-in-one reactor by using nitrogen until the dew point is qualified (-60 ℃); adding liquid ammonia with the purity of 99.99 percent into a four-in-one reactor in a liquid phase form; adding the mixed material into liquid ammonia in a four-in-one reactor at a dropping speed of 1.5 g/min; wherein the mol ratio of the monochlorosilane to the liquid ammonia is as follows: 2.0:1.
S130, controlling the temperature in the four-in-one reactor to be 10 ℃, and mechanically stirring and reacting the mixed material and liquid ammonia for 60min through a stirring unit to obtain a reaction liquid.
S140, decompressing and heating the reaction solution through a heating unit under the conditions that the working pressure is-10 Kpa and the working temperature is 70 ℃ to obtain a volatile material and a residual material.
S150, condensing the volatile materials through a condenser with the working temperature of 0 ℃ and then enabling the volatile materials to reach a receiver to obtain crude trisilylamine; simultaneously, the remaining material passes through a closed filtration unit to form a filter cake. And a Y-shaped filter is arranged between the receiver and the rectifying tower group.
S160, passing the crude trisilylamine through a filter with the filtering precision of 1 mu m, and then entering a light component removal rectifying tower with the working pressure of 0Kpa and the working temperature of 52 ℃ to obtain an intermediate product; and (3) conveying the intermediate product to a heavy component removal rectifying tower with the working pressure of-20 Kpa and the working temperature of 30 ℃ through a tower kettle of the light component removal rectifying tower, and obtaining the high-purity trisilylamine through the tower top of the heavy component removal rectifying tower. Normal hexane is added into the four-in-one reactor, and the four-in-one reactor is stirred and washed by the normal hexane to remove ammonium salt attached inside the reactor.
Example 3
S110, fully mixing n-pentane with the purity of 99% and monochlorosilane with the purity of 99.99% in a low-temperature mixer at the working temperature of-20 ℃ and the working pressure of 1.5Mpa, wherein the volume ratio of n-pentane to monochlorosilane is 5:1, and forming a mixed material. Wherein, the n-pentane is dried by an active carbon dryer in a n-pentane storage tank and then reaches a low-temperature mixer, and bottom-sinking bubbling mixing is carried out.
S120, purging and replacing the four-in-one reactor by using nitrogen until the dew point is qualified (-60 ℃); adding liquid ammonia with the purity of 99.99 percent into a four-in-one reactor in a liquid phase form; adding the mixed material into liquid ammonia in a four-in-one reactor at a dropping speed of 1.0 g/min; wherein the mol ratio of the monochlorosilane to the liquid ammonia is as follows: 1.5:1.
S130, controlling the temperature in the four-in-one reactor to be 0 ℃, and mechanically stirring the mixed material and liquid ammonia through a stirring unit to react for 20min to obtain reaction liquid.
After the reaction liquid is obtained, normal hexane is added into the four-in-one reactor, and the four-in-one reactor is stirred and washed by the normal hexane to remove ammonium salt attached to the interior of the reactor.
S140, decompressing and heating the reaction liquid through a heating unit under the conditions that the working pressure is-20 Kpa and the working temperature is 60 ℃ to obtain a volatile material and a residual material.
S150, condensing the volatile materials through a condenser with the working temperature of-5 ℃ and then enabling the volatile materials to reach a receiver to obtain crude trisilylamine; meanwhile, the residual materials pass through a closed filtering unit to form a filter cake. And a T-shaped filter is arranged between the receiver and the rectifying tower group.
S160, passing the crude trisilylamine through a filter with the filtering precision of 1 mu m, and then entering a light component removal rectifying tower with the working pressure of-10 Kpa and the working temperature of 40 ℃ to obtain an intermediate product; and (3) conveying the intermediate product to a heavy component removal rectifying tower with the working pressure of-5 Kpa and the working temperature of 42 ℃ through a tower kettle of the light component removal rectifying tower, and obtaining the high-purity trisilylamine through the tower top of the heavy component removal rectifying tower.
Example 4
S110, fully mixing normal hexane with the purity of 99% and monochlorosilane with the purity of 99.99% in a low-temperature mixer at the working temperature of-20 ℃ and the working pressure of 2Mpa, wherein the volume ratio of the normal hexane to the monochlorosilane is 4:1, and thus forming a mixed material. Wherein, n-hexane is dried by a 5A molecular sieve dryer in an n-hexane storage tank, then reaches a low-temperature mixer, and is subjected to bottom-sinking bubbling mixing.
S120, purging and replacing the four-in-one reactor by using nitrogen until the dew point is qualified (-60 ℃); adding liquid ammonia with the purity of 99.99 percent into a four-in-one reactor in a liquid phase form; adding the mixed material into liquid ammonia in a four-in-one reactor at a dropping speed of 0.5 g/min; wherein the mol ratio of the monochlorosilane to the liquid ammonia is as follows: 1.2:1.
S130, controlling the temperature in the four-in-one reactor to be-10 ℃, mechanically stirring the mixed material and liquid ammonia through a stirring unit for reaction for 30min, and controlling the stirring speed to be 400r/min to obtain a reaction liquid.
After the reaction liquid is obtained, normal hexane is added into the four-in-one reactor, and the four-in-one reactor is stirred and washed by the normal hexane to remove ammonium salt attached inside the reactor.
S140, decompressing and heating the reaction liquid through a heating unit under the conditions that the working pressure is-10 Kpa and the working temperature is 60 ℃ to obtain a volatile material and a residual material.
S150, condensing the volatile materials through a condenser with the working temperature of-10 ℃ and then enabling the volatile materials to reach a receiver to obtain crude trisilylamine; simultaneously, the remaining material passes through a closed filtration unit to form a filter cake. And a T-shaped filter is arranged between the receiver and the rectifying tower group.
S160, passing the crude trisilylamine through a filter with the filtering precision of 1 mu m, and then entering a light component removal rectifying tower with the working pressure of-10 Kpa and the working temperature of 40 ℃ to obtain an intermediate product; and (3) conveying the intermediate product to a heavy component removal rectifying tower with the working pressure of-5 Kpa and the working temperature of 42 ℃ through a tower kettle of the light component removal rectifying tower, and obtaining the high-purity trisilylamine through the tower top of the heavy component removal rectifying tower.
Example 5
S110, fully mixing normal hexane with the purity of 99% and monochlorosilane with the purity of 99.99% in a low-temperature mixer at the working temperature of-15 ℃ and the working pressure of 1.7Mpa, wherein the volume ratio of the normal hexane to the monochlorosilane is 6:1, and a mixed material is formed. Wherein, n-hexane is dried by a 5A molecular sieve dryer in an n-hexane storage tank, then reaches a low-temperature mixer, and is subjected to bottom-sinking bubbling mixing.
S120, purging and replacing the four-in-one reactor by using nitrogen until the dew point is qualified (-60 ℃); adding liquid ammonia with the purity of 99.99 percent into a four-in-one reactor in a liquid phase form; adding the mixed material into liquid ammonia in a four-in-one reactor at a dropping speed of 0.3 g/min; wherein the mol ratio of the monochlorosilane to the liquid ammonia is as follows: 1.0:1.
S130, controlling the temperature in the four-in-one reactor to be-5 ℃, and mechanically stirring and reacting the mixed material and liquid ammonia for 40min through a stirring unit to obtain a reaction liquid.
After the reaction liquid is obtained, normal hexane is added into the four-in-one reactor, and the four-in-one reactor is stirred and washed by the normal hexane to remove ammonium salt attached to the interior of the reactor.
S140, decompressing and heating the reaction liquid through a heating unit under the conditions that the working pressure is-15 Kpa and the working temperature is 55 ℃ to obtain a volatile material and a residual material.
S150, condensing the volatile materials through a condenser with the working temperature of-1 ℃ and then enabling the volatile materials to reach a receiver to obtain crude trisilylamine; simultaneously, the remaining material passes through a closed filtration unit to form a filter cake. And a T-shaped filter is arranged between the receiver and the rectifying tower group.
S160, passing the crude trisilylamine through a filter with the filtering precision of 1 mu m, and then entering a light component removal rectifying tower with the working pressure of-5 Kpa and the working temperature of 38 ℃ to obtain an intermediate product; and (3) conveying the intermediate product to a heavy component removal rectifying tower with the working pressure of-15 Kpa and the working temperature of 46 ℃ through a tower kettle of the light component removal rectifying tower, and obtaining high-purity trisilylamine through the tower top of the heavy component removal rectifying tower.
After the high-purity trisilylamine obtained in the above examples 1-6 was subjected to GC-MS detection, the composition reached 99.5%; wherein the compositions of the highly pure trisilylamine obtained in examples 3-6 all exceeded 99.62%.
The utility model discloses a preparation method and device of high-purity trisilyl alkylamine carries out the low temperature mixture back through earlier with chlorosilane and alkane solvent, adopts and controls the temperature with intelligence, stirring, heating and closed filtration and carry out the integrated four unification reactors and react and obtain thick trisilyl alkylamine, utilizes the rectifying column to carry out the rectification under reduced pressure at last and obtains high-purity trisilyl alkylamine. Compared with the prior liquid phase reaction method for preparing trisilylamine, the utility model firstly mixes monochlorosilane and alkane solvent at low temperature, and then carries out low-temperature stirring reaction in a four-in-one reactor, thereby effectively avoiding local heat accumulation and reducing more synthesis side reactions; the closed filter unit is one part of the four-in-one reactor, so that the transfer link of materials in the air is reduced, and the risk of introducing impurities is reduced; through adopting and carrying out the four unification reactors that integrate with intelligent accuse temperature, stirring, heating and closed filtration, effectively shorten the preparation flow, reduced safe risk and environmental protection risk.
However, it will be appreciated by those skilled in the art that various modifications may be made to the apparatus for preparing high purity trisilylamine provided by the present invention without departing from the scope of the invention. Therefore, the scope of the present invention should be determined by the content of the appended claims.
Claims (10)
1. The preparation device of the high-purity trisilylamine is characterized by comprising a low-temperature mixer, a four-in-one reactor and a rectifying tower group which are sequentially connected;
the low-temperature mixer is used for fully mixing monochlorosilane and alkane solvent to form a mixed material; the output end of the low-temperature mixer and the output end of the liquid nitrogen storage tank are communicated with the input end of the four-in-one reactor; wherein the input end of the low-temperature mixer is communicated with the alkane solvent storage tank and the monochlorosilane storage tank;
the four-in-one reactor comprises an intelligent temperature control unit for controlling the reaction temperature, a stirring unit for mechanically stirring the mixed material and the liquid ammonia to obtain a reaction liquid, a heating unit for heating the reaction liquid under reduced pressure to obtain volatile materials and residual materials, and a closed filtering unit for filtering the residual materials to form a filter cake;
and the volatile material output end of the four-in-one reactor is communicated with the rectifying tower group through a condenser and a receiver.
2. The apparatus for preparing highly pure trisilylamine according to claim 1, wherein the rectifying column set comprises a light component removing rectifying column and a heavy component removing rectifying column;
the output end of the receiver is connected with the input end of the light component removal rectifying tower; the tower kettle of the light component removal rectifying tower is connected with the input end of the heavy component removal rectifying tower;
the top of the de-heavy rectifying tower is a high-purity trisilylamine output end.
3. The apparatus for preparing high-purity trisilylamine according to claim 2, wherein the light component removal rectifying column and the heavy component removal rectifying column are both packed columns, and the packing of the packed columns is one of stainless steel theta ring packing, triangular spiral packing or glass spring packing.
4. The apparatus for preparing highly pure trisilylamine according to claim 1, wherein a dryer is provided between the input end of the low temperature mixer and the alkane solvent storage tank.
5. The apparatus for preparing highly pure trisilylamine according to claim 4, wherein the filler of the dryer is one of 4A molecular sieve, 5A molecular sieve, activated carbon or artificial zeolite.
6. The apparatus for preparing highly pure trisilylamine according to claim 1, wherein a nitrogen gas delivery device for purging and displacing the mixture with nitrogen gas is provided between the output end of the low temperature mixer and the four-in-one reactor, and the nitrogen gas delivery device is communicated with the nitrogen gas inlet of the four-in-one reactor.
7. The apparatus for preparing highly pure trisilylamine according to claim 1, wherein the intelligent temperature control unit of the four-in-one reactor is a jacket covering the outside of the reactor.
8. The apparatus for preparing highly pure trisilylamine according to claim 1, wherein the stirring unit of the four-in-one reactor is a stirring blade provided in the reactor.
9. The apparatus for preparing highly pure trisilylamine according to claim 1, wherein a filter is disposed between the receiver and the rectifying tower set, and the filter is a T-type filter or a Y-type filter.
10. The apparatus for preparing highly pure trisilylamine according to claim 1, wherein the heating medium in the bottom of the rectifying tower group is hot water or heat conducting oil.
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| CN115636846B (en) * | 2022-11-02 | 2024-07-23 | 洛阳中硅高科技有限公司 | Preparation method and device of high-purity trisilylamine |
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