High-quality boron isotope separation process and device

Abstract

The invention provides a high-quality boron isotope separation process and device, the device comprises an exchange rectification system, a complexing system, a complex cracking system and a boron-11 refining system, natural abundance boron trifluoride isotopes are separated through an exchange rectification tower, and cyclic regeneration of boron trifluoride and anisole is realized by adopting the complexing system and the cracking system. A boron-11 refining system is arranged to further improve the abundance of boron-11. According to the method, the industrial continuous production of the high-quality boron trifluoride-10 with the abundance of 99% and the high-quality boron trifluoride-11 with the abundance of 99.9% can be synchronously realized, the process is simple and clear, and the operability is high.

Description

Technical Field

[0001] The present invention belongs to the field of boron isotope separation and production, and specifically relates to a process and a device for separating and producing high-quality boron 10 and boron 11. Background Art

[0002] Boron has two stable isotopes in nature, boron-10 and boron-11, with natural abundances of 19.78% and 80.22% respectively. Both boron isotopes have extremely high application value. Boron-10 has strong neutron absorption ability with an absorption cross section of 3837 targets. It can be used as a neutron absorber in nuclear reactors, a gamma-ray shielding material, and a targeted drug for boron neutron capture therapy (BNCT). The "Guide Catalog for the First Batch Application Demonstration of Key New Materials (2024 Edition)" points out that the performance requirement of boron-10 acid is an abundance greater than or equal to 95%. The drug effect in BNCT is controlled by the abundance of boron-10, and the preferred boron-10 abundance is greater than 99%; the neutron absorption capacity of boron-11 is extremely weak, with an absorption cross section of only 0.005 targets. It can be doped in the reflector shell of a nuclear reactor to prevent the leakage of neutrons in the core, and can also be used in the manufacture of chips that resist high-energy particle bombardment in spacecraft. At the same time, high-abundance boron-11 can be used as a p-type doping source for silicon-based semiconductors. It can be applied to various links such as doping, oxidation diffusion, ion implantation, plasma etching, and silicon / germanium epitaxial growth. For example, the precision process in the semiconductor industry has high requirements for the abundance and purity of electronic special gas-grade boron trifluoride-11, among which the abundance requirement is greater than 99.8%. The broad application prospects also put forward high standards for the separation of boron isotopes.

[0003] Boron isotope separation methods include chemical exchange distillation, cryogenic distillation, extraction, adsorption separation, laser method, etc. Chemical exchange distillation uses the different binding abilities of isotope molecules and chelating agents to form complexes to achieve separation, and the separation coefficient of chemical exchange method is between 1.01 and 1.06; cryogenic distillation uses the difference in relative volatility of isotope molecules at low temperature (-100°C) to achieve separation, and the separation coefficient of cryogenic distillation for separating boron isotopes is between 1.003 and 1.008; extraction uses the difference in solubility of different isotope molecules by the extractant to achieve separation, and patent CN116726702A provides a method for extracting and separating boron isotopes. The hydrophobic deep eutectic solvent adopts a diol compound containing dihydroxyl groups as a hydrogen bond donor, a compound containing phenolic hydroxyl groups or a solid monohydric alcohol as a hydrogen bond acceptor, and the aqueous phase is a boric acid aqueous solution, which can achieve a separation coefficient ranging from 1.011 to 1.033; the adsorption separation method can be divided into ion exchange resin adsorption and organic-metal framework material (MOFs) adsorption. Patent CN116603391A invented a method for separating boron isotopes using DB564 or D403 resin. By repeatedly adjusting the pH value of the boric acid aqueous solution, the separation coefficient can be adjusted. 10 The abundance of B was enriched to between 86-92%.

[0004] Although different separation methods are being developed, extraction and resin adsorption methods have high development prospects as efficient, energy-saving and green processes, but such methods still have problems such as low separation coefficient, complex operation, difficulty in industrial scale-up and low yield. At present, only chemical exchange distillation has achieved industrial separation and production of boron isotopes in the world. The largest boron isotope producer in the world is the American company Cerridon, which uses anisole-boron trifluoride chemical exchange distillation system, and its output accounts for more than 85% of the world's total output at its maximum. In addition, Italy's SCL and Japan's Stellachemifa both use anisole-boron trifluoride system to achieve industrial production of boron isotope separation. The industrial separation of boron isotopes in China developed relatively late. Dalian Borntan Company achieved industrial production of 96.5% boron-10 acid in 2009; thereafter, Liaoning Honghao achieved an annual output of 7 tons of boron-10 acid in 2016; Shandong Heyi Gas Company developed an annual output of 1,000 kilograms of boron trifluoride-11 products in 2022. The key issue in the industrial production of chemical exchange distillation is how to increase the abundance while ensuring the output, and directly produce high-abundance and high-purity boron isotope products (boron-10 abundance greater than 99%, boron-11 abundance greater than 99.9%; corresponding product purity greater than 99%). The literature "Principles of Chemical Isotope Separation" and "Basic Chemistry and Application of Isotopes" summarize the flow chart of the chemical exchange distillation process, as shown in the attached figure. Figure 1 As shown, it is divided into three parts: exchange distillation, complexation, and cracking, which is also the basis of the existing chemical exchange process. The document Engineering-Scale Studies of Boron Isotope Separation conducted a bench test of chemical exchange distillation to enrich boron isotopes. In the results given in the document, the maximum abundance of boron-10 is only 22%, and the maximum abundance of boron-11 is only 83%, which is far from meeting the high abundance requirements. Patent CN102773016A discloses a multi-tower series boron isotope separation process, and the maximum abundance of boron-10 and boron-11 is only 95%, which also does not meet the high abundance requirements. Patents CN115920632A and CN115608156B innovate the complexation and cracking processes respectively, improve the efficiency of complexation and cracking reactions, but still do not completely solve the problem of achieving high abundance of boron-10 and boron-11 after exchange distillation. In summary, there is no report on the separation process of high-abundance boron-10 and high-abundance boron-11 co-production. In particular, high-abundance boron-11 products have never been seen. Summary of the invention

[0005] An analysis of the existing chemical exchange distillation process found that the cracking of the boron trifluoride-10-anisole complex is limited by chemical equilibrium. If the cracking is not thorough, the anisole circulating back to the complexation reactor will inevitably carry the boron-10 component, which seriously affects the abundance of the boron-11 product. Calculations show that the abundance of the boron-11 product will be greater than 99.9% only when the boron trifluoride-10-anisole complex fraction in the cracked stream is less than 10 ppm. This requires the complex to be nearly completely cracked.

[0006] Based on the above analysis, the present invention provides a process and device for high-quality boron isotope separation, in particular, a process method for continuously producing high-quality boron-11 (99.9% abundance), which is characterized by using natural abundance boron trifluoride raw material, and using a boron-11 refining system to further enrich boron-11 on the basis of exchange distillation, complexation, and cracking; its feed is the boron-11 obtained by the first-stage exchange distillation enrichment, and the second-stage chemical exchange distillation process is carried out, and a deep cracker is used to achieve complete decomposition of the boron-10 complex to further increase the boron-11 abundance, and then simultaneously obtain high-abundance boron-10 and boron-11 products. In order to achieve the purpose of complete cracking of the complex, the cracking reaction temperature of the deep cracker is higher than that of all other cracking reactors, and it is operated at a slight negative pressure.

[0007] The technical solution of the present invention is as follows:

[0008] A process for high-quality boron isotope separation, comprising an exchange distillation system, a complexation system, a complex cracking system and a boron-11 refining system, wherein:

[0009] Exchange distillation system: After the temperature of natural abundance boron trifluoride raw material is stabilized by the feed heat exchanger, it enters the tower from the middle and upper part of the boron-10 refining tower;

[0010] Complexation system: The top stream of the boron-10 refining tower enters the complexation reactor to complex with anisole to generate boron trifluoride-anisole complex. The gas phase product of the complexation reactor is taken out of the boron-11 refining system as a high-abundance boron-11 crude product. The liquid phase product of the complexation reactor is used as a cold end liquid reflux and returns to the boron-10 refining tower through the boron-10 refining tower reflux pump;

[0011] Complex cracking system: The stream from the bottom of the boron-10 refining tower enters the low-temperature cracking tower and the reboiler of the low-temperature cracking tower through a low-temperature cracking delivery pump to complete preliminary cracking. The liquid stream from the low-temperature cracking reboiler passes through the high-temperature cracking tower and the reboiler of the high-temperature cracking tower in turn through a high-temperature cracking delivery pump to complete further cracking of the complex. The liquid stream flowing out of the reboiler of the high-temperature cracking tower is the purified anisole, which enters the complexing reactor after being cooled by the anisole cooler to complex with the boron trifluoride gas at the top of the boron-10 refining tower; the top stream of the low-temperature cracking tower is cooled by the low-temperature cracking tower condenser to obtain a high-abundance boron trifluoride-10 gas phase, part of which is produced as a product, and part returns to the bottom of the boron-10 refining tower as a gas phase hot end reflux; the gas streams of the low-temperature cracking tower reboiler and the high-temperature cracking tower are combined and sent to the bottom of the low-temperature cracking tower; the gas stream of the high-temperature cracking tower reboiler returns to the high-temperature cracking tower;

[0012] In the boron-11 refining system, the gas phase product of the complex reactor is sent to the bottom of the boron-11 refining tower for refining, the top stream of the boron-11 refining tower enters the boron-11 complex reactor, the gas phase stream of the boron-11 complex reactor is extracted as the refined high-abundance boron-11 product, and the liquid phase stream returns to the top of the boron-11 refining tower as the liquid phase cold end reflux; the complex stream at the bottom of the boron-11 refining tower enters the boron-11 complex low-temperature cracking tower and the boron-11 complex low-temperature cracking tower reboiler through the boron-11 complex low-temperature cracking pump for preliminary cracking, and the liquid phase stream of the boron-11 complex low-temperature cracking tower reboiler is sent to the boron-11 complex low-temperature cracking tower reboiler through the boron-11 complex The high-temperature cracking pump of the complex is sent to the boron-11 complex high-temperature cracking tower and the reboiler of the boron-11 complex high-temperature cracking tower to complete further cracking of the complex. The liquid phase discharge stream of the reboiler of the boron-11 complex high-temperature cracking tower enters the deep cracking reactor for deep impurity removal to remove impurities in the stream and obtain high-purity circulating anisole. The liquid phase stream of the deep cracking reactor returns to the boron-11 complex reactor, and the gas phase stream is discharged; the top stream of the boron-11 complex low-temperature cracking tower is condensed and impurities are removed by the condenser of the boron-11 complex low-temperature cracking tower, and part of it is discharged, and part of it is used as the gas phase hot end reflux of the boron-11 refining tower kettle.

[0013] In the exchange distillation system, the boron-10 refining tower adopts a packed tower structure to realize gas-liquid countercurrent contact reaction, the top product is a gas phase enriched in boron-11, the bottom product is a liquid phase enriched in boron-10, the theoretical plate number of the boron-10 refining tower is 312 to 378, the temperature is 23 to 27°C; the reflux ratio is 108 to 192.

[0014] In the complexing system, the complexing reactor is a shell-and-tube reactor with a reaction temperature of 20-27° C. and a pressure of 0.8-1.2 bara. The flow rate of the boron trifluoride-11 enriched product of the gas phase material in the complexing reactor is controlled at 83-92% of the total flow rate of the boron trifluoride feed, and the concentration is controlled at 90-93%.

[0015] In the complex cracking system, the low-temperature cracking reaction temperature is 110-140°C, and the high-temperature cracking reaction temperature is 160-180°C.

[0016] In the boron-11 refining system, the boron-11 refining tower adopts a packed tower structure, with a theoretical plate number of 337-382 and a reflux ratio of 280-287; the deep cracking reactor adopts a fixed bed packed reactor, the reaction temperature of the deep cracking reactor is 169-183°C, and the pressure is 0.71-0.96 bara; the gas phase fraction of the deep cracking reactor is controlled between 8% and 13%. The abundance of high-quality boron trifluoride-11 produced in the gas phase of the boron-11 complexing reactor is controlled at 99.9%, and the appropriate production flow rate is 48-56% of the total boron trifluoride feed flow.

[0017] The recovery rate of boron trifluoride-10 enriched in the gas phase of the low-temperature cracking tower condenser is 7% to 15% based on the feed amount, and the concentration is controlled at 85 to 99%.

[0018] A process for separation of high-quality boron isotopes, wherein the process is provided with a regeneration cycle of raw materials boron trifluoride and anisole; the raw material anisole enters the system from a complexation reactor and a boron-11 complexation reactor, reacts with boron trifluoride to form a complex, and the complexation stream enters a cracking system after passing through a boron-10 refining tower and a boron-11 refining tower, and successively passes through a low-temperature cracking tower and a high-temperature cracking tower to obtain cracked anisole, which is then returned to the complexation reactor for circulation; an additional deep cracking reactor is provided in the boron-11 refining system to remove impurities and purify anisole, and the deep cracking reactor The liquid phase discharge returns to the complexation reactor through a heat exchanger to realize circulation; the boron trifluoride raw material enters the process from the boron-10 refining tower, and exists in the form of boron trifluoride gas and boron trifluoride-anisole complex in the process. The gas phase boron trifluoride in the exchange distillation tower is transported to the complexation reaction to generate the boron trifluoride-anisole complex. The boron trifluoride-anisole complex enters the cracking system after the isotope exchange reaction, and is cracked into boron trifluoride and anisole in the cracking system. The pure boron trifluoride returns to the exchange distillation tower as the tower bottom gas phase circulation, completing the material circulation of boron trifluoride.

[0019] The waste material flow rate discharged from the deep cracking reactor is controlled at 340-500 kmol / h, and circulating anisole is supplemented accordingly.

[0020] The invention discloses a device for high-quality boron isotope separation process, comprising an exchange distillation system, a complexation system, a complex cracking system and a boron-11 refining system; the device is characterized in that the main body of the exchange distillation system is a boron-10 refining tower (T-101); the main equipment of the complexation system is a complexation reactor (R-201); the complex cracking system comprises a low-temperature cracking tower (T-301) and a high-temperature cracking tower (T-302); the boron-11 refining system comprises a boron-11 refining tower (T-401), a boron-11 complexation reactor (R-401), a boron-11 complex low-temperature cracking tower (T-402), a boron-11 complex high-temperature cracking tower (T-403) and a deep cracking reactor (R-402); the connection sequence is: the top pipeline of the boron-10 refining tower (T-101) and the complexation reactor (R-201); the boron-11 refining tower (T-4 ...) are connected in a high-temperature cracking tower (T-202); the boron-11 refining tower (T-401) and the complexation reactor (R-201) are connected in a high-temperature cracking tower (T-202); the boron-11 refining tower (T-401) and the complexation reactor (R-201) are The boron-10 refining tower (T-101) is connected to the complex reactor (R-201), the tower kettle pipeline of the boron-10 refining tower (T-101) is connected to the low-temperature cracking tower (T-301), the tower kettle pipeline of the low-temperature cracking tower (T-301) is connected to the high-temperature cracking tower (T-302), the tower kettle pipeline of the high-temperature cracking tower (T-302) is connected to the complex reactor (R-201), the gas phase discharge of the complex reactor (R-201) is connected to the boron-11 refining tower (T-401), the tower top pipeline of the boron-11 refining tower (T-401) is connected to the boron-11 complex reactor (R-401), and the tower kettle pipeline of the boron-11 refining tower (T-401) is connected to the boron-11 complex low-temperature cracking tower (T-402), the boron-11 complex high-temperature cracking tower (T-403) and the deep cracking reactor (R-402) in sequence.

[0021] The specific instructions are as follows:

[0022] A process for high-quality boron isotope separation includes an exchange distillation system, a complexation system, a complex cracking system and a boron-11 refining system, wherein each system is briefly described as follows:

[0023] Exchange distillation system: Natural abundance boron trifluoride and enriched boron trifluoride-11 complex undergo an exchange reaction, and the reaction equation is as follows.

[0024] 11 BF 3 ·CH 3 OC 6 H 5 + 10 BF 3 → 10 BF 3 ·CH 3 OC 6 H 5 + 11 BF 3

[0025] Complexation system: exchange distillation system enriched 11 BF3 It undergoes complexation reaction with anisole, and the reaction equation is as follows.

[0026] 11 BF 3 +CH 3 OC 6 H 5 → 11 BF 3 ·CH 3 OC 6 H 5

[0027] Complex cleavage system: 11 BF 3 -Anisole complex is thermally cracked, and the reaction equation is as follows.

[0028] 11 BF 3 ·CH 3 OC 6 H 5 → 11 BF 3 +CH 3 OC 6 H 5

[0029] Boron-11 refining system: The initially enriched boron trifluoride-11 obtained by the exchange distillation system is further enriched to obtain high-abundance boron-11. The reaction equation is as follows.

[0030] 11 BF 3 ·CH 3 OC 6 H 5 + 10 BF 3 → 10 BF 3 ·CH 3 OC 6 H 5 + 11 BF 3

[0031] 11 BF 3 +CH 3 OC 6 H 5 → 11 BF 3 ·CH 3 OC 6 H 5

[0032] 11 BF 3 ·CH3 OC 6 H 5 → 11 BF 3 +CH 3 OC 6 H 5

[0033] use Figure 1 A high-quality boron isotope separation device is specifically described, comprising an exchange distillation system, a complexation system, a complex cracking system and a boron-11 refining system; the main body of the exchange distillation system is a boron-10 refining tower (T-101); the main equipment of the complexation system is a complexation reactor (R-201); the complex cracking system includes a low-temperature cracking tower (T-301) and a high-temperature cracking tower (T-302); the boron-11 refining system includes a boron-11 refining tower (T-401), a boron-11 complexation reactor (R-401), a boron-11 complex low-temperature cracking tower (T-402), a boron-11 complex high-temperature cracking tower (T-403) and a deep cracking reactor (R-402); the connection sequence is that the top pipeline of the boron-10 refining tower (T-101) and the complexation reaction system are connected to each other. The tower kettle pipeline of the boron-10 refining tower (T-101) is connected to the low-temperature cracking tower (T-301), the tower kettle pipeline of the low-temperature cracking tower (T-301) is connected to the high-temperature cracking tower (T-302), the tower kettle pipeline of the high-temperature cracking tower (T-302) is connected to the complexing reactor (R-201), the gas phase discharge of the complexing reactor (R-201) is connected to the boron-11 refining tower (T-401), the tower top pipeline of the boron-11 refining tower (T-401) is connected to the boron-11 complexing reactor (R-401), and the tower kettle pipeline of the boron-11 refining tower (T-401) is connected to the boron-11 complex low-temperature cracking tower (T-402), the boron-11 complex high-temperature cracking tower (T-403) and the deep cracking reactor (R-402) in sequence.

[0034] The material flow is as follows:

[0035] For the exchange distillation system, the natural abundance boron trifluoride raw material enters the tower from the middle and upper part of the boron-10 refining tower (T-101) after the temperature is stabilized through the feed heat exchanger (E-101). The exchange distillation tower is a packed tower structure and is not equipped with a separate condenser and reboiler.

[0036] For the complexation system, the top stream of the boron-10 refining tower (T-101) (mainly the initially enriched boron-11 stream) enters the complexation reactor (R-201) to complex with anisole to form a boron trifluoride-anisole complex. The gas phase product of the complexation reactor is taken out of the boron-11 refining system as a high-abundance boron-11 crude product, and the liquid phase product of the complexation reactor (mainly the initially enriched boron trifluoride-11-anisole complex) is used as a cold end liquid reflux and returns to the boron-10 refining tower (T-101) through the boron-10 refining tower reflux pump (P-201).

[0037] For the complex cracking system, the bottom stream of the boron-10 refining tower (T-101) (mainly enriched boron-10) enters the low-temperature cracking tower (T-301) and the low-temperature cracking tower reboiler (E-302) through the low-temperature cracking delivery pump (P-101) to complete the initial cracking. The liquid stream of the low-temperature cracking reboiler (E-302) (mainly the complex that has not been completely cracked) passes through the high-temperature cracking delivery pump (P-301) and passes through the high-temperature cracking tower (T-302) and the high-temperature cracking tower reboiler (E-303) in turn to complete the further cracking of the complex. The liquid stream flowing out of the high-temperature cracking tower reboiler (E-303) is the purified anisole, which is cooled by the anisole cooler (E-304) and then enters The complexing reactor (R-201) is complexed with the boron trifluoride gas at the top of the boron-10 refining tower; the top stream of the low-temperature cracking tower (T-301) is cooled by the low-temperature cracking tower condenser (E-301) to obtain a high-abundance boron trifluoride-10 gas phase, part of which is produced as a product, and part returns to the bottom of the boron-10 refining tower (T-101) as a gas phase hot end reflux; the gas phase streams of the low-temperature cracking tower reboiler (E-302) and the high-temperature cracking tower (T-302) (mainly enriched boron trifluoride-10) are combined and sent to the bottom of the low-temperature cracking tower (T-301); the gas phase stream of the high-temperature cracking tower reboiler (E-303) (mainly enriched boron trifluoride-10) returns to the high-temperature cracking tower (T-302).

[0038] For the boron-11 refining system, the gas phase product of the complexing reactor (R-201) is sent to the bottom of the boron-11 refining tower (T-401) for refining, and the top stream of the boron-11 refining tower (T-401) enters the boron-11 complexing reactor (R-401). The gas phase stream of the boron-11 complexing reactor (R-401) is extracted as the refined high-abundance boron-11 product, and the liquid phase stream returns to the top of the boron-11 refining tower (T-401) as the liquid phase cold end reflux. The complex stream at the bottom of the boron-11 refining tower (T-401) passes through the boron-11 complex low-temperature cracking pump (P-401) and enters the boron-11 complex low-temperature cracking tower (T-402) and the boron-11 complex low-temperature cracking tower reboiler (E-402) for preliminary cracking. The liquid stream of the boron-11 complex low-temperature cracking tower reboiler (E-402) is sent to the boron-11 complex high-temperature cracking tower ( The boron-11 complex high temperature cracking tower (T-402) and the boron-11 complex high temperature cracking tower reboiler (E-403) complete the further cracking of the complex. The liquid phase discharge stream of the boron-11 complex high temperature cracking tower reboiler (E-403) enters the deep cracking reactor (R-402) for deep impurity removal to remove impurities in the stream and obtain high-purity circulating anisole. The liquid phase stream of the deep cracking reactor (R-402) returns to the boron-11 complex reactor (R-401), and the gas phase stream is emptied. The top stream of the boron-11 complex low temperature cracking tower (T-402) is partially emptied after condensation and impurity removal in the boron-11 complex low temperature cracking tower condenser (E-401), and part of it is used as the gas phase hot end reflux of the tower bottom of the boron-11 refining tower (T-401).

[0039] The process of the present invention is provided with a regeneration cycle of raw materials boron trifluoride and anisole. The raw material anisole enters the system from a complexation reactor (R-201) and a boron-11 complexation reactor (R-401), reacts with boron trifluoride to generate a complex, and the complexation stream enters a cracking system after passing through a boron-10 refining tower (T-101) and a boron-11 refining tower (T-401), passes through a low-temperature cracking tower and a high-temperature cracking tower in sequence to obtain cracked anisole, and returns to the complexation reactor to realize circulation. The boron-11 refining system is additionally provided with a deep cracking reactor (R-402) to remove impurities and purify anisole. The liquid phase discharge of the deep cracking reactor (R-402) is returned to the complexing reactor through a heat exchanger (E-404) to realize circulation. The boron trifluoride raw material enters the process from the boron-10 refining tower (T-101), and exists in the form of boron trifluoride gas and boron trifluoride-anisole complex in the process. The gas phase boron trifluoride in the exchange distillation tower is transported to the complexing reaction to generate the boron trifluoride-anisole complex. The boron trifluoride-anisole complex enters the cracking system after the isotope exchange reaction, and is cracked into boron trifluoride and anisole in the cracking system. The pure boron trifluoride returns to the exchange distillation tower as the tower bottom gas phase circulation, and the material circulation of boron trifluoride is completed.

[0040] The exchange and distillation system of the present invention is composed of a boron-10 refining tower (T-101), and a packed tower structure is adopted to realize gas-liquid countercurrent contact reaction. The top product of the tower is a gas phase enriched in boron-11, and the bottom product of the tower is a liquid phase enriched in boron-10. The suitable theoretical plate number of the boron-10 refining tower (T-101) is 312 to 378. The isotope exchange temperature reaction degree in the tower is jointly controlled by the return liquid phase temperature of the complexing reactor (R-201) and the return gas phase temperature of the low-temperature cracking tower (T-301), and the suitable temperature is 23 to 27°C.

[0041] The complexation system of the present invention is composed of a complexation reactor (R-201), which is a tubular reactor, wherein the reactor feed gas phase part comes from the overhead stream of the boron-10 refining tower (T-101), and the liquid phase part includes supplemented fresh anisole and anisole decomposed from a high-temperature cracking tower (T-302) in the cracking system. The reaction temperature is preferably 20-27° C., and the pressure is 0.8-1.2 bara.

[0042] The complex cracking system of the present invention is composed of a low-temperature cracking tower (T-301), a low-temperature cracking tower reboiler (E-302), a high-temperature cracking tower reboiler (E-303) and a high-temperature cracking tower (T-302), and both towers adopt a packing structure. The boron trifluoride-anisole complex enriched in boron-10 produced by the bottom of the exchange distillation tower (T-101) is used as a feed stream and is preliminarily decomposed in the low-temperature cracking tower (T-301). The suitable temperature for the low-temperature cracking reaction is 110-140°C. The complex that is not completely cracked further enters the low-temperature cracking tower (T-302) for complete cracking. The suitable temperature for the high-temperature cracking reaction is 160-180°C. The cracking gas produced by the cracking system is condensed by the low-temperature cracking tower condenser (E-301) and then extracted.

[0043] The boron-11 refining system of the present invention is composed of a boron-11 refining tower (T-402), a boron-11 complexing reactor (R-401), a boron-11 complex low-temperature cracking tower (T-402), a boron-11 complex high-temperature cracking tower (T-403) and a deep cracking reactor (R-402). The boron-11 refining system uses the product of preliminary enrichment of boron-11 in the complexing reactor (R-201) in the complexing system as a raw material, and completes the enrichment of high-quality boron trifluoride-11 through the boron-11 refining tower (T-401). The boron-11 refining tower adopts a packed tower structure, and the material is fed from the bottom of the tower, and the suitable theoretical plate number is 337 to 382. A matching boron-11 complex reactor is arranged on the top of the refining tower to realize liquid phase circulation, and a boron-11 complex cracking device is arranged at the bottom of the tower, including a boron-11 complex low-temperature cracking tower (T-402), a boron-11 complex high-temperature cracking tower (T-402), and a deep cracking reactor (R-402), wherein the deep cracking reactor (R-402) adopts a fixed bed filling reactor to remove trace boron-10 impurities in anisole after cracking, and the suitable reaction temperature of the deep cracking reactor (R-402) is 169-183°C, and the suitable pressure is 0.71-0.96 bara.

[0044] Preferably, the reflux ratio of the Boron-10 refining tower (T-101) is 108 to 192;

[0045] Preferably, the recovery rate of enriched boron trifluoride-10 is between 7% and 15% (based on the feed amount);

[0046] Preferably, the recovery rate of boron trifluoride-11 in the refined boron-11 system is between 48% and 56% (based on the feed amount);

[0047] Preferably, in the boron-11 refining system, the gas phase fraction of the deep cracking reactor (R-402) is controlled between 8% and 13%.

[0048] The beneficial technical effects of the present invention are:

[0049] 1. The present invention adopts boron trifluoride-anisole chemical exchange distillation method to separate boron isotopes. Compared with extraction method and resin adsorption method, the technical process is short, the equipment is simple, the operating conditions are suitable, and the separation coefficient is high, which can meet the industrial mass production requirement.

[0050] 2. The present invention connects the industrial processes of boron-10 refining and boron-11 refining, and realizes the continuous production of two high-quality boron isotopes at the same time, greatly improving the production efficiency. The abundance of boron-10 can reach 99%, and the abundance of boron-11 can reach 99.9%.

[0051] 3. The present invention has discovered that the main factor limiting the abundance of boron isotopes is the trace impurities remaining in the process. A deep cracking reactor is innovatively used to control the trace impurities in the process. The fraction of boron-10 substances returned to the top stream of the exchange distillation tower of the boron-11 refining system is less than 0.01%, of which the fraction of boron trifluoride-10-anisole complex is less than 10 ppm, thereby maximizing the abundance of boron-11. BRIEF DESCRIPTION OF THE DRAWINGS

[0052] Figure 1 It is a schematic diagram of the process flow of separating high-quality boron isotopes of the present invention;

[0053] Among them: T-101——boron-10 refining tower, T-301——low temperature cracking tower, T-302——high temperature cracking tower, T-401——boron-11 refining tower, T-402——boron-11 complex low temperature cracking tower, T-403——boron-11 complex high temperature cracking tower, R-201——complexing reactor, R-401——boron-11 complexing reactor, R-402——deep cracking reactor;

[0054] E-101 - feed heat exchanger, E-301 - low temperature cracking tower condenser, E-302 - low temperature cracking tower reboiler, E-303 - high temperature cracking tower reboiler, E-304 - anisole cooler, E-401 - boron-11 complex low temperature cracking tower condenser, E-402 - boron-11 complex low temperature cracking tower reboiler, E-403 - boron-11 complex high temperature cracking tower reboiler, E-404 - circulating anisole cooler;

[0055] P-101——boron-10 refining tower kettle production pump, P-201——complexation reactor discharge pump, P-301——low-temperature cracking tower kettle production pump, P-302——high-temperature cracking tower kettle production pump, P-401——boron-11 refining tower kettle production pump, P-402——boron-11 complexation reactor discharge pump, P-403——boron-11 complex low-temperature cracking tower kettle production pump, P-404——boron-11 complex high-temperature cracking tower kettle production pump. DETAILED DESCRIPTION

[0056] The present invention provides a process and device for high-quality boron isotope separation, in particular, a process for continuously producing high-quality boron-11 (99.9% abundance). The following is a description of the method and device of the present invention in conjunction with the accompanying drawings.

[0057] The present invention is achieved by Figure 1 The method shown implements:

[0058] The present invention relates to a boron isotope separation device, comprising an exchange distillation system, a complex system, a complex cracking system and a boron-11 refining system. The exchange distillation system mainly comprises a boron-10 refining tower (T-101), and the boron-10 refining tower (T-101) is connected to its auxiliary equipment feed heat exchanger (E-101) and a boron-10 refining tower kettle extraction pump (P-101);

[0059] The complexing system mainly includes a complexing reactor (R-201), and the complexing reactor (R-201) is connected to a boron-10 refining tower (T-101) through its auxiliary equipment, a complexing reactor discharge pump (P-201).

[0060] The cracking system mainly comprises a low-temperature cracking tower (T-301) and a high-temperature cracking tower (T-302), wherein the low-temperature cracking tower (T-301) is connected to its auxiliary equipment, a low-temperature cracking tower condenser (E-301), a low-temperature cracking tower reboiler (3E-302) and a low-temperature cracking tower kettle extraction pump (P-301), and the high-temperature cracking tower (T-302) is connected to its auxiliary equipment, a high-temperature cracking tower reboiler (E-303), a high-temperature cracking tower kettle extraction pump (P-302) and an anisole cooler (E-303).

[0061] The boron-11 refining system mainly comprises a boron-11 refining tower (T-401), a boron-11 complex low-temperature cracking tower (T-402), a boron-11 complex high-temperature cracking tower (T-403), a deep cracking reactor (R-402) and a boron-11 complex reactor (R-401) which are connected in sequence, wherein the boron-11 refining tower (T-401) is connected to the boron-11 complex low-temperature cracking tower (T-402) through its auxiliary equipment boron-11 refining tower kettle extraction pump (P-401), and the boron-11 complex low-temperature cracking tower (T-402) is connected to the boron-11 complex low-temperature cracking tower (T-402) and its auxiliary equipment boron-11 complex low-temperature cracking tower condenser (E-401 ), the boron-11 complex low-temperature cracking tower reboiler (E-402) and the boron-11 complex low-temperature cracking tower kettle extraction pump (P-403), the boron-11 complex high-temperature cracking tower (T-403) and its auxiliary equipment boron-11 complex high-temperature cracking tower reboiler (E-403), the boron-11 complex high-temperature cracking tower kettle discharge pump (P-404), the deep cracking reactor (R-402) and the circulating anisole cooler (E-404) are connected, and the boron-11 complex reactor (R-401) is connected to the boron-11 refining tower (T-401) through its auxiliary equipment boron-11 complex reactor discharge pump (P-402).

[0062] The high-quality boron isotope separation process of the present invention is as follows:

[0063] The boron-10 refining tower (T-101) is used to complete the chemical exchange reaction of boron isotopes to enrich the boron-10 isotope. The natural abundance boron trifluoride raw material is fed from the middle of the tower, the boron-11-rich liquid phase from the complexing reactor (R-201) is fed from the top of the tower, and the boron-10-rich gas phase from the low-temperature cracking tower (T-301) is fed from the bottom of the tower. After the isotope exchange reaction, the boron-11 isotope is gradually enriched in the gas phase at the top of the tower. The gas phase at the top of the boron-10 refining tower is enriched with boron-11 as the feed stream of the complexing reactor (R-201). At the same time, the boron-10 isotope is gradually enriched in the liquid phase of the bottom of the tower. The bottom stream is sent to the low-temperature cracking tower (301) for feeding through the boron-10 refining tower bottom extraction pump (P-101).

[0064] The complexation reactor (R-201) is used for complex regeneration and production of high-quality boron trifluoride-10. The feed gas phase stream comes from the high-abundance boron trifluoride-10 at the top of the boron-10 refining tower (T-101), and the feed liquid phase stream comes from the high-purity anisole in the bottom of the high-temperature cracking tower (T-302). Since the complexation reaction is a highly exothermic reaction, the temperature of the complexation reactor (R-201) needs to be strictly controlled during the reaction. The generated complex is sent to the boron-10 refining tower for feeding through the complexation reactor discharge pump (P-201), and the gas phase product of the complexation reactor is sent to the boron-11 refining tower (T-401) as feed for the boron-11 refining system.

[0065] The low-temperature cracking tower (T-301), the high-temperature cracking tower (T-302) and its attached low-temperature cracking tower reboiler (E-302) and high-temperature cracking tower reboiler (E-303) are used to separate boron trifluoride from anisole to realize material circulation. The complex extracted from the boron-10 refining tower (T-101) first enters the low-temperature cracking tower (T-301), completes heat exchange with the mixed gas phase from the low-temperature cracking tower kettle reboiler (T-301) and the top of the high-temperature cracking tower (T-302), and part of the complex is cracked here. After the rising gas phase is initially cooled down, it exits the tower and condenses anisole and boron trifluoride-anisole complex through the low-temperature cracking tower condenser (E-301). The gas phase is partially extracted as a high-quality boron trifluoride-10 gas phase product, and most of it returns to the boron-10 refining tower (T-101) as the tower kettle gas phase reflux, and the liquid phase returns to the low-temperature cracking tower (T-301); the low-temperature cracking tower (T-301) kettle discharge enters the low-temperature cracking tower reboiler (E302) for further cracking. The reboiler is heated by steam, and the cracked gas phase boron trifluoride-10 returns to the low temperature cracking tower. The bottom of the warm cracking tower (T-301) serves as gas reflux and provides heat for cracking in the tower. The liquid phase after passing through the low-temperature cracking tower reboiler (E302) is transported by the low-temperature cracking tower bottom discharge pump (P-301) to the high-temperature cracking tower (T-302) for feeding and further cracking. The top discharge of the high-temperature cracking tower (T-302) is a gas mixture of boron trifluoride and anisole, which is sent to the bottom of the low-temperature cracking tower (T-301) for feeding. The discharge from the bottom of the high-temperature cracking tower (T-302) enters the high-temperature cracking tower reboiler (E-303) to ensure sufficient cracking. The gas phase stream of the high-temperature cracking tower reboiler (E-303) returns to the high-temperature cracking tower (T-302) as gas phase reflux, and the liquid phase stream is the circulating anisole, which is sent to the complexing reactor (R-201) for circulation by the high-temperature cracking tower bottom extraction pump (P-302).

[0066] The boron-11 refining tower (T-401) is used to purify boron trifluoride-11. The initially enriched boron trifluoride-11 is extracted from the complexing reactor (R-201) and fed from the bottom of the refining tower. The boron-11 refining tower (T-401) adopts a packed tower structure and is only provided with a distillation section. The enriched gas phase at the top of the boron-11 refining tower (T-401) is the boron-11 product, which is transported to the boron-11 complexing reactor (R-401). The bottom stream of the boron-11 refining tower (T-401) is transported by the boron-11 refining tower bottom extraction pump (P-401) to the boron-11 complex low-temperature cracking tower (T-402) for feeding.

[0067] The boron-11 complexation reactor (R-401) is used for complexation reaction to generate boron-11 complex, realize the liquid phase reflux of the top of the boron-11 refining tower (T-401), and produce high-quality boron trifluoride-11. The obtained liquid phase boron-11 complex is sent to the top of the boron-11 refining tower (T-401) for reflux by the boron-11 complexation reactor discharge pump (P-402).

[0068] The boron-11 complex low-temperature cracking tower (T-402), the boron-11 complex high-temperature cracking tower (T-403), the deep cracking reactor (R-402) and its ancillary equipment, the boron-11 complex low-temperature cracking tower condenser (E-401), the boron-11 complex low-temperature cracking tower reboiler (E-402), the boron-11 complex high-temperature cracking tower reboiler (E-403) and the circulating anisole cooler (E-404) are used to separate the boron trifluoride-anisole complex enriched with boron-11. The bottom stream of the boron-11 refining tower (T-401) is sent to the boron-11 complex low-temperature cracking tower (T-402) for cracking through the boron-11 refining tower bottom extraction pump (P-401). The boron trifluoride gas after cracking at the top of the boron-11 complex low-temperature cracking tower (T-402) is condensed by the boron-11 complex low-temperature cracking tower condenser (E-401), part of which is discharged as waste gas, and part of which is returned to the bottom of the boron-11 refining tower (T-401) as gas phase reflux. The bottom stream of the low temperature cracking tower (T-402) of the complex enters the reboiler (E-402) of the low temperature cracking tower of the boron-11 complex for further cracking. The gas phase of the reboiler (E-402) of the low temperature cracking tower of the boron-11 complex returns to the bottom of the low temperature cracking tower of the boron-11 complex as the gas phase reflux. The liquid phase is sent to the high temperature cracking tower of the boron-11 complex (T-403) through the extraction pump (P-403) of the bottom of the low temperature cracking tower of the boron-11 complex for further cracking. The operating temperature of the high temperature cracking tower (T-403) of the boron complex is higher than that of the low temperature cracking tower (T-402) of the boron-11 complex. The gas phase stream from the top of the high temperature cracking tower (T-403) of the boron-11 complex returns to the bottom of the low temperature cracking tower (T-402) of the boron-11 complex as gas phase reflux. The liquid phase in the bottom enters the reboiler (E-403) of the high temperature cracking tower of the boron-11 complex to be fully cracked. The gas phase of the reboiler (E-403) of the high temperature cracking tower of the boron-11 complex returns to the boron-11 complex. The bottom of the complex low-temperature cracking tower (T-402) is used as the gas phase for reflux. Since the liquid phase contains trace impurities, it is further sent to the deep cracking reactor (R-402) by the extraction pump (P-404) of the bottom of the boron-11 complex high-temperature cracking tower to remove trace boron-10. The gas phase of the deep cracking reactor (R-402) is discharged as waste gas, and the pure liquid anisole is cooled by the circulating anisole cooler (E-404) and used as the feed of the boron-11 complex reactor (R-401).

[0069] As the first embodiment of the present invention, the feed abundance of boron trifluoride-10:boron trifluoride-11=19.78:80.22, the feed flow rate is 21.6 kmol / h, the theoretical number of plates of the boron-10 refining tower (T-101) is 312, the raw material is fed from the 177th plate, the complex reactor (R-201) has a constant reaction temperature of 23°C, a pressure of 1.0 bara, and the reflux ratio R sent back to the boron-10 refining tower (T-101) is 192. The low temperature cracking tower (T-301) is provided with 10 theoretical plates, the condensing temperature of the low temperature cracking tower condenser (E-301) is 25° C., the reboiling temperature of the low temperature cracking tower reboiler (E-302) is 110° C., the high temperature cracking tower (T-302) is provided with 10 theoretical plates, the reboiling temperature of the high temperature cracking tower reboiler (E-303) is 174° C., and the temperature of the anisole cooler (E-304) is set at 25° C. The extraction flow rate of boron trifluoride-10 is 1.8 kmol / h, the abundance is 85%, and the heating unit consumption of the process is 164.98 Gcal / t. The boron-11 refining tower (T-401) has 371 theoretical plates, a feed abundance of 93%, a reflux ratio of 287, a deep cracking reactor (R-402) with a reaction temperature of 183°C and a pressure of 0.71 bara; the boron-11 complexing reactor (R-401) has an anisole supplement flow rate of 402 kmol / h, a boron trifluoride-11 production abundance of 99.9%, a yield of 48%, and a refining section heating unit consumption of 81.24 Gcal / t.

[0070] As a second embodiment of the present invention, the feed flow rate of the raw material boron trifluoride is 21.6 kmol / h, the feed abundance of boron trifluoride-10:boron trifluoride-11=19.78:80.22, the theoretical number of plates of the boron-10 refining tower (T-101) is 378, the raw material is fed from the 210th plate, the complex reactor (R-201) has a constant reaction temperature of 20°C and a pressure of 1.2 bara, and the reflux ratio R sent back to the boron-10 refining tower (T-101) is 142. The low temperature cracking tower (T-301) is provided with 10 theoretical plates, the condensing temperature of the low temperature cracking tower condenser (E-301) is 27° C., the reboiling temperature of the low temperature cracking tower reboiler (E-302) is 128° C., the high temperature cracking tower (T-302) is provided with 10 theoretical plates, the reboiling temperature of the high temperature cracking tower reboiler (E-303) is 180° C., and the temperature of the anisole cooler (E-304) is set at 25° C. The extraction flow rate of boron trifluoride-10 is 2.8 kmol / h, the abundance is 99%, and the heating unit consumption of the process is 177.20 Gcal / t. The boron-11 refining tower (T-401) has 337 theoretical plates, a feed abundance of 90%, a reflux ratio of 277, a deep cracking reactor (R-402) with a reaction temperature of 183°C and a pressure of 0.84 bara; the boron-11 complexing reactor (R-401) has an anisole supplement flow rate of 340 kmol / h, a boron trifluoride-11 extraction abundance of 99.9%, a yield of 56%, and a refining section heating unit consumption of 78.44 Gcal / t.

[0071] As the third embodiment of the present invention, the feed flow rate of the raw material boron trifluoride is 21.6 kmol / h, the feed abundance of boron trifluoride-10:boron trifluoride-11=19.78:80.22, the theoretical number of plates of the boron-10 refining tower (T-101) is 345, the raw material is fed from the 196th plate, the complex reactor (R-201) has a constant reaction temperature of 27°C and a pressure of 0.8 bara, and the reflux ratio R sent back to the boron-10 refining tower (T-101) is 108. The low temperature cracking tower (T-301) is provided with 10 theoretical plates, the condensing temperature of the low temperature cracking tower condenser (E-301) is 22° C., the reboiling temperature of the low temperature cracking tower reboiler (E-302) is 140° C., the high temperature cracking tower (T-302) is provided with 10 theoretical plates, the reboiling temperature of the high temperature cracking tower reboiler (E-303) is 160° C., and the temperature of the anisole cooler (E-304) is set at 25° C. The extraction flow rate of boron trifluoride-10 is 3.2 kmol / h, the abundance is 97%, and the heating unit consumption of the process is 340.38 Gcal / t. The boron-11 refining tower (T-401) has 382 theoretical plates, a feed abundance of 91%, a reflux ratio of 280, a deep cracking reactor (R-402) with a reaction temperature of 169°C and a pressure of 0.96 bara; the boron-11 complexing reactor (R-401) has an anisole supplement flow rate of 500 kmol / h, a boron trifluoride-11 production abundance of 99.9%, a yield of 53%, and a heating unit consumption of 80.42 Gcal / t in the refining section.

[0072] In one embodiment of the present invention, the device further comprises a pump for conveying materials. Those skilled in the art know that the material conveying between the distillation towers can utilize the potential difference and rely on the gravity of the material to realize the conveying of the raw materials in the distillation tower; however, when the material conveying cannot be realized by gravity, one or more material conveying pumps are arranged at appropriate pipeline positions to realize the conveying of the material.

[0073] The equipment not particularly mentioned in the present invention is conventional equipment and can be implemented by using methods and equipment known to those skilled in the art.

[0074] Although the present invention has been described in conjunction with specific embodiments and the accompanying drawings, it is not intended that the present invention be limited to the specific forms described herein. On the contrary, the scope of the present invention is limited only by the appended claims. In addition, although individual features may be included in different claims, these features may be advantageously combined, and inclusion in different claims does not mean that the combination of features is not feasible and / or advantageous. References to "first", "second", etc. do not exclude plural numbers.

Claims

1. A process for high-quality boron isotope separation, characterized in that: It includes exchange distillation system, complex system, complex cracking system and boron-11 refining system, among which: Exchange distillation system: After the temperature of natural abundance boron trifluoride raw material is stabilized by the feed heat exchanger, it enters the tower from the middle and upper part of the boron-10 refining tower; Complexation system: The top stream of the boron-10 refining tower enters the complexation reactor to complex with anisole to generate boron trifluoride-anisole complex. The gas phase product of the complexation reactor is taken out of the boron-11 refining system as a high-abundance boron-11 crude product. The liquid phase product of the complexation reactor is used as a cold end liquid reflux and returns to the boron-10 refining tower through the boron-10 refining tower reflux pump; Complex cracking system: The stream from the bottom of the boron-10 refining tower enters the low-temperature cracking tower and the reboiler of the low-temperature cracking tower through a low-temperature cracking delivery pump to complete preliminary cracking. The liquid stream from the low-temperature cracking reboiler passes through the high-temperature cracking tower and the reboiler of the high-temperature cracking tower in turn through a high-temperature cracking delivery pump to complete further cracking of the complex. The liquid stream flowing out of the reboiler of the high-temperature cracking tower is the purified anisole, which enters the complexing reactor after being cooled by the anisole cooler to complex with the boron trifluoride gas at the top of the boron-10 refining tower; the top stream of the low-temperature cracking tower is cooled by the low-temperature cracking tower condenser to obtain a high-abundance boron trifluoride-10 gas phase, part of which is produced as a product, and part returns to the bottom of the boron-10 refining tower as a gas phase hot end reflux; the gas streams of the low-temperature cracking tower reboiler and the high-temperature cracking tower are combined and sent to the bottom of the low-temperature cracking tower; the gas stream of the high-temperature cracking tower reboiler returns to the high-temperature cracking tower; In the boron-11 refining system, the gas phase product of the complex reactor is sent to the bottom of the boron-11 refining tower for refining, the top stream of the boron-11 refining tower enters the boron-11 complex reactor, the gas phase stream of the boron-11 complex reactor is extracted as the refined high-abundance boron-11 product, and the liquid phase stream returns to the top of the boron-11 refining tower as the liquid phase cold end reflux; the complex stream at the bottom of the boron-11 refining tower enters the boron-11 complex low-temperature cracking tower and the boron-11 complex low-temperature cracking tower reboiler through the boron-11 complex low-temperature cracking pump for preliminary cracking, and the liquid phase stream of the boron-11 complex low-temperature cracking tower reboiler is pumped through the boron-11 complex The high-temperature cracking pump of the complex is sent to the boron-11 complex high-temperature cracking tower and the reboiler of the boron-11 complex high-temperature cracking tower to complete further cracking of the complex. The liquid phase discharge stream of the reboiler of the boron-11 complex high-temperature cracking tower enters the deep cracking reactor for deep impurity removal to remove impurities in the stream and obtain high-purity circulating anisole. The liquid phase stream of the deep cracking reactor returns to the boron-11 complex reactor, and the gas phase stream is discharged; the top stream of the boron-11 complex low-temperature cracking tower is condensed and impurities are removed by the condenser of the boron-11 complex low-temperature cracking tower, and part of it is discharged, and part of it is used as the gas phase hot end reflux of the boron-11 refining tower kettle.

2. The process for separation of high-quality boron isotopes as claimed in claim 1, characterized in that the exchange In the distillation system, the boron-10 refining tower adopts a packed tower structure to realize gas-liquid countercurrent contact reaction. The top product is a gas phase enriched in boron-11, and the bottom product is a liquid phase enriched in boron-10. The theoretical plate number of the boron-10 refining tower is 312 to 378, the temperature is 23 to 27°C; the reflux ratio is 108 to 192.

3. The process for high-quality boron isotope separation according to claim 1, characterized in that: In the complexing system, the complexing reactor is a shell-and-tube reactor with a reaction temperature of 20-27°C and a pressure of 0.8-1.2 bara; the flow rate of the boron trifluoride-11 enriched effluent from the gas phase of the complexing reactor is controlled at 83-92% of the total flow rate of the boron trifluoride feed, and the concentration is controlled at 90-93%.

4. The process for high-quality boron isotope separation according to claim 1, characterized in that: In the complex cracking system, the low-temperature cracking reaction temperature is 110-140°C, and the high-temperature cracking reaction temperature is 160-180°C.

5. The process for separation of high-quality boron isotopes according to claim 1, characterized in that: In the boron-11 refining system, the boron-11 refining tower adopts a packed tower structure, with a theoretical plate number of 337-382 and a reflux ratio of 280-287; the deep cracking reactor adopts a fixed bed packed reactor, the reaction temperature of the deep cracking reactor is 169-183°C, and the pressure is 0.71-0.96 bara; the gas phase fraction of the deep cracking reactor is controlled between 8% and 13%; the abundance of high-quality boron trifluoride-11 produced in the gas phase in the boron-11 complexing reactor is controlled at 99.9%, and the production flow rate is 48-56% of the total boron trifluoride feed flow.

6. The process for separation of high-quality boron isotopes as claimed in claim 1, characterized in that: The recovery rate of boron trifluoride-10 enriched in the gas phase of the low-temperature cracking tower condenser is 7% to 15% based on the feed amount, and the concentration is controlled at 85 to 99%.

7. The process for separation of high-quality boron isotopes as claimed in claim 1, characterized in that: The process is provided with a regeneration cycle of raw materials boron trifluoride and anisole; the raw material anisole enters the system from a complexing reactor and a boron-11 complexing reactor, reacts with boron trifluoride to form a complex, and the complexing stream enters a cracking system after passing through a boron-10 refining tower and a boron-11 refining tower, and successively passes through a low-temperature cracking tower and a high-temperature cracking tower to obtain cracked anisole, which is then returned to the complexing reactor to realize circulation; a deep cracking reactor is additionally provided in the boron-11 refining system to realize impurity removal and purification of anisole, and the liquid phase discharge of the deep cracking reactor is subjected to heat exchange The boron trifluoride raw material enters the process from the boron-10 refining tower, and exists in the form of boron trifluoride gas and boron trifluoride-anisole complex in the process. The gas phase boron trifluoride in the exchange distillation tower is transported to the complex reaction to generate the boron trifluoride-anisole complex. The boron trifluoride-anisole complex enters the cracking system after the isotope exchange reaction, and is cracked into boron trifluoride and anisole in the cracking system. The pure boron trifluoride returns to the exchange distillation tower as the bottom gas phase circulation, completing the material circulation of boron trifluoride.

8. The process for separation of high-quality boron isotopes as claimed in claim 7, characterized in that: The waste material flow rate discharged from the deep cracking reactor is controlled at 340-500 kmol / h, and circulating anisole is supplemented accordingly.

9. A device for realizing a high-quality boron isotope separation process according to claim 1, comprising an exchange distillation system, a complex system, a complex cracking system and a boron-11 refining system; wherein: The main body of the exchange distillation system is the boron-10 refining tower (T-101); the main equipment of the complexing system is the complexing reactor (R-201); the complex cracking system includes a low-temperature cracking tower (T-301) and a high-temperature cracking tower (T-302); the boron-11 refining system includes a boron-11 refining tower (T-401), a boron-11 complexing reactor (R-401), a boron-11 complex low-temperature cracking tower (T-402), a boron-11 complex high-temperature cracking tower (T-403) and a deep cracking reactor (R-402); the connection sequence is that the top pipeline of the boron-10 refining tower (T-101) is connected to the complexing reactor (R-201), and the boron-10 refining tower (T-101) is connected to the tower The kettle pipeline is connected to the low-temperature cracking tower (T-301), the kettle pipeline of the low-temperature cracking tower (T-301) is connected to the high-temperature cracking tower (T-302), the kettle pipeline of the high-temperature cracking tower (T-302) is connected to the complexing reactor (R-201), the gas phase discharge of the complexing reactor (R-201) is connected to the boron-11 refining tower (T-401), the top pipeline of the boron-11 refining tower (T-401) is connected to the boron-11 complexing reactor (R-401), and the kettle pipeline of the boron-11 refining tower (T-401) is connected to the boron-11 complex low-temperature cracking tower (T-402), the boron-11 complex high-temperature cracking tower (T-403) and the deep cracking reactor (R-402) in sequence.

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