Hydrogen and oxygen combination device and method for producing deuterium-rich water by using hydrogen and oxygen combination device

Abstract

The invention discloses a hydrogen-oxygen combination device and a method for producing deuterium-rich water, the hydrogen-oxygen combination device comprises: a material supply device for providing oxygen and inert gas for a recycle gas supercharging device, and respectively providing deuterium / hydrogen with a set proportion and supplementing oxygen for a gas mixing device; the circulating gas pressurizing device receives oxygen and inert gas, mixes and pressurizes the oxygen and the inert gas to form pressurized circulating gas, and quantitatively supplies the pressurized circulating gas to the gas mixing device; the gas mixing device is used for receiving deuterium / hydrogen, supplementing oxygen and pressurizing circulating gas and carrying out homogeneous mixing to form mixed gas to be supplied to the reaction device; the reaction device receives the mixed gas, deuterium / hydrogen in the mixed gas is in contact with excessive oxygen and completely reacts with the excessive oxygen, and a gas-liquid mixture generated after the complete reaction is fed into the gas-liquid separation device; and the gas-liquid separation device is used for receiving the gas-liquid mixture and separating and collecting liquid-phase heavy water, and the gas phase returns to the circulating gas supercharging device through a circulating gas return pipe. The invention provides an industrial solution with safety, reaction efficiency and operation stability.

Description

Technical Field

[0001] This invention belongs to the field of deuterated chemical synthesis, and particularly relates to the field of hydrogen / deuterium oxidation technology, specifically a hydrogen oxidation apparatus and a method for producing deuterium-rich water. Background Technology

[0002] The most widely used process for deuterium / oxygen fusion is the heating catalytic method, which heats a mixture of hydrogen and oxygen to the temperature required by the catalyst. Under the combined action of heating and catalysis, hydrogen and oxygen rapidly combine to form water.

[0003] In existing technologies, hydrogen hydration processes are primarily used to achieve energy conversion or safe elimination. Examples include their application in catalytic burners to release energy, providing high-temperature flames in hydrogen-oxygen cutting systems, and serving as the power generation principle for hydrogen fuel cells. These applications mainly aim to achieve efficient utilization of reaction heat, stable power output, or processing efficiency within a specific concentration range. However, in the field of deuterated chemical synthesis, especially in production processes using deuterium gas as the deuterium source, unreacted deuterium gas is discharged as deuterium-rich hydrogen tail gas. Deuterium, as a scarce and expensive isotope resource, directly impacts the cost of the final product due to its atom economy. Therefore, a closed-loop recycling system capable of efficiently converting deuterium-rich hydrogen tail gas into deuterium-rich water and realizing a deuterium resource loop is crucial for the synthesis of deuterated chemicals using deuterium gas as the deuterium source.

[0004] Chinese patent application CN119746727A discloses a hydrogen-oxygen recombination device. The device is equipped with a buffer section and a synthesis section. Hydrogen and oxygen are first mixed in the buffer section to form a mixed gas. The mixed gas flowing out of the outlet of the buffer section undergoes a hydrogen-oxygen recombination reaction in the synthesis section. In this technical solution, the oxygen transported by the second pipeline is located in the middle of the buffer section, while the hydrogen transported by the first pipeline enters the buffer section from the top through the main pipeline. Before entering the combination section, there may be a risk of uneven mixing of hydrogen and oxygen in certain areas, leading to the accumulation of unreacted hydrogen within the system, which significantly exacerbates the inherent safety risks of the system. On the other hand, according to the data from the embodiment, when the hydrogen flow rate is 200 ml / min, the conversion rate is 93.3%, but when the hydrogen flow rate increases to 300 ml / min, the conversion rate drops to 90.2%, indicating that the reaction is not complete. This not only leads to the waste of hydrogen / deuterium sources and increases the burden of subsequent tail gas treatment, but also reflects the inadequacy of its mixing and reaction efficiency. Finally, the combination section uses external electric heating to heat the reaction, but for the large amount of reaction heat generated by large-scale, continuous production, there is a lack of efficient and timely removal of excess reaction heat, making it difficult to achieve precise and uniform control of the reaction temperature. This can easily lead to catalyst sintering and deactivation due to local overheating, affecting reaction stability and catalyst life, and making it difficult to support long-term stable operation.

[0005] Therefore, in order to overcome the problem of recovering deuterium-rich hydrogen tail gas in the field of deuterated chemical synthesis using deuterium gas as a deuterium source in existing technologies, a closed-loop circulating hydroxide synthesis device is needed for the production of deuterium-rich water. Summary of the Invention

[0006] The purpose of this invention is to address the problems existing in the prior art by providing a hydrogenation hydration apparatus and a method for producing deuterium-rich water. This hydrogenation hydration apparatus successfully overcomes key technical bottlenecks such as high safety risks, difficulty in temperature control, and easy deactivation of catalysts during the hydrogenation hydration process, providing an industrial solution that combines safety, reaction efficiency, and operational stability.

[0007] The objective of this invention is achieved through the following technical solution:

[0008] A hydrogen hydroxide annealing apparatus includes a feeding device, a circulating gas booster device, a gas mixing device, a reaction device, a gas-liquid separation device, and corresponding connecting pipelines, control valves, and monitoring instruments, wherein:

[0009] The feeding device is used to supply oxygen and inert gas to the circulating gas booster device, and to supply a set ratio of deuterium / hydrogen and supplementary oxygen to the mixing device, or to supply deuterium / hydrogen to the mixing device and to supply a set ratio of supplementary oxygen to the circulating gas returning to the circulating gas booster device.

[0010] The circulating gas booster is used to receive oxygen and inert gas, or to receive circulating gas, or to receive supplementary oxygen and circulating gas, and to boost the gas to form pressurized circulating gas or pressurized circulating gas containing supplementary oxygen, which is then quantitatively supplied to the gas mixing device.

[0011] A gas mixing device is used to receive separate deuterium / hydrogen, separate supplementary oxygen, separate pressurized circulating gas, or receive separate deuterium / hydrogen, pressurized circulating gas containing supplementary oxygen, or receive separate deuterium / hydrogen, separate supplementary oxygen and separate pressurized circulating gas to form a supplementary pressurized circulating gas, and homogenize and mix them to form a mixed gas for supply to the reaction device.

[0012] Reaction apparatus: used to receive the mixed gas, and the deuterium / hydrogen in the mixed gas comes into contact with excess oxygen and reacts completely. The gas-liquid mixture generated after the complete reaction is sent to the gas-liquid separation device.

[0013] Gas-liquid separation device: used to receive gas-liquid mixtures and separate and collect the liquid phase heavy water and the gas phase circulating gas, which is returned to the circulating gas booster device through the circulating gas return pipe.

[0014] The volume percentage of deuterium / hydrogen in the circulating gas booster and gas-liquid separation devices is ≤1‰, and the volume percentage of deuterium / hydrogen in the gas mixing device and reaction device is ≤2%.

[0015] The feeding device is equipped with a separate flame arrester on the pipeline supplying oxygen and supplementing oxygen to the circulating gas pressurizing device; a separate flame arrester is installed on the pipeline supplying inert gas to the circulating gas pressurizing device; a second flame arrester is installed on the pipeline supplying deuterium / hydrogen to the gas mixing device; a fifth flame arrester is installed on the circulating gas supply pipeline supplying pressurized circulating gas containing supplementing oxygen to the gas mixing device; a sixth flame arrester is installed on the pipeline supplying mixed gas to the reaction device from the gas mixing device; and a seventh flame arrester is installed on the pipeline supplying gas-liquid mixture from the reaction device to the gas-liquid separation device; a flame arrester is installed at the end of the circulating gas return pipe supplying circulating gas from the gas-liquid separation device to the circulating gas pressurizing device, or the end of the circulating gas return pipe is connected to the pipeline supplying oxygen and supplementing oxygen and located in front of the flame arrester on that pipeline, or the end of the circulating gas return pipe is connected to the pipeline supplying inert gas and located in front of the flame arrester on that pipeline; or the feeding device... A flame arrester is separately installed on the pipeline supplying oxygen to the circulating gas booster; a flame arrester is separately installed on the pipeline supplying inert gas to the circulating gas booster; a second flame arrester is installed on the pipeline supplying deuterium / hydrogen to the gas mixing device from the feeder; and a flame arrester is installed on the pipeline supplying supplementary oxygen to the gas mixing device from the feeder; a fifth flame arrester is installed on the circulating gas supply pipeline supplying pressurized circulating gas from the circulating gas booster to the gas mixing device; a sixth flame arrester is installed on the pipeline supplying mixed gas from the gas mixing device to the reaction device; and a seventh flame arrester is installed on the pipeline supplying gas-liquid mixture from the reaction device to the gas-liquid separation device; a flame arrester is installed at the end of the circulating gas return pipe from the gas-liquid separation device to the circulating gas booster; or the end of the circulating gas return pipe is connected to the oxygen supply pipeline and located in front of the flame arrester on that pipeline; or the end of the circulating gas return pipe is connected to the inert gas supply pipeline and located in front of the flame arrester on that pipeline.Alternatively, a flame arrester may be separately installed on the pipeline supplying oxygen from the feeding device to the circulating gas pressurizing device; a flame arrester may be separately installed on the pipeline supplying inert gas from the feeding device to the circulating gas pressurizing device; a second flame arrester may be installed on the pipeline supplying deuterium / hydrogen from the feeding device to the gas mixing device; a fifth flame arrester may be installed on the circulating gas supply pipeline supplying pressurized circulating gas from the circulating gas pressurizing device to the gas mixing device; and the end of the oxygen supplement branch pipeline supplying supplementary oxygen from the feeding device to the gas mixing device may be connected to the circulating gas supply pipeline before the fifth flame arrester; a sixth flame arrester may be installed on the pipeline supplying mixed gas from the gas mixing device to the reaction device; and the gas supply branch pipeline supplying supplementary oxygen from the feeding device to the gas mixing device may be connected to the circulating gas supply pipeline before the fifth flame arrester; and a sixth flame arrester may be installed on the pipeline supplying mixed gas from the gas mixing device to the reaction device. A seventh flame arrester is installed on the pipeline providing the gas-liquid mixture from the liquid separator. A flame arrester is also installed at the end of the circulating gas return pipe from the gas-liquid separator to the circulating gas booster; or the end of the circulating gas return pipe is connected to the oxygen supply pipeline and located in front of the flame arrester on that pipeline; or the end of the circulating gas return pipe is connected to the inert gas supply pipeline and located in front of the flame arrester on that pipeline. Alternatively, a third flame arrester is installed on the circulating gas replenishment pipe from the feeding device to the circulating gas booster, providing oxygen and inert gas, as well as supplementing oxygen; and a second flame arrester is installed on the pipeline from the feeding device to the gas mixing device, providing deuterium / hydrogen gas separately. A fifth flame arrester is installed on the circulating gas supply pipeline from the pressurizing device to the mixing device, which provides pressurized circulating gas containing supplemental oxygen. A sixth flame arrester is installed on the pipeline from the mixing device to the reaction device, and a seventh flame arrester is installed on the pipeline from the reaction device to the gas-liquid separator. A flame arrester is installed at the end of the circulating gas return pipe from the gas-liquid separator to the circulating gas pressurizing device, or the end of the circulating gas return pipe is connected to the circulating gas replenishment pipe in front of the third flame arrester; or a third flame arrester is installed on the circulating gas replenishment pipe from the feeding device to the circulating gas pressurizing device, which provides oxygen and inert gas. A second flame arrester is installed on the pipeline that separately supplies deuterium / hydrogen, and a flame arrester is installed on the oxygen supply branch pipe that separately supplies supplemental oxygen to the gas mixing device from the feeding device. A fifth flame arrester is installed on the circulating gas supply pipeline that supplies pressurized circulating gas to the gas mixing device from the circulating gas boosting device. A sixth flame arrester is installed on the pipeline that supplies mixed gas to the reaction device from the gas mixing device, and a seventh flame arrester is installed on the pipeline that supplies gas-liquid mixture to the gas-liquid separation device from the reaction device. A flame arrester is installed at the end of the circulating gas return pipe that supplies circulating gas to the circulating gas boosting device from the gas-liquid separation device, or the end of the circulating gas return pipe is connected to the circulating gas supply pipe in front of the third flame arrester.Alternatively, a third flame arrester may be installed on the circulating gas replenishment pipe of the feeding device supplying oxygen and inert gas to the circulating gas booster device; a second flame arrester may be installed on the pipe of the feeding device supplying deuterium / hydrogen gas separately to the mixing device; a fifth flame arrester may be installed on the circulating gas supply pipe of the circulating gas booster device supplying pressurized circulating gas to the mixing device, and the end of the oxygen replenishment branch pipe of the feeding device supplying supplementary oxygen to the mixing device may be connected to the circulating gas supply pipe in front of the fifth flame arrester; a sixth flame arrester may be installed on the pipe of the mixing device supplying mixed gas to the reaction device, and a seventh flame arrester may be installed on the pipe of the reaction device supplying gas-liquid mixture to the gas-liquid separator; and a flame arrester may be installed at the end of the circulating gas return pipe of the gas-liquid separator supplying circulating gas to the circulating gas booster device, or the end of the circulating gas return pipe may be connected to the circulating gas replenishment pipe in front of the third flame arrester.

[0016] The feeding device includes a deuterium / hydrogen valve group pipeline for supplying deuterium as a chemical raw material, an oxygen valve group pipeline for supplying oxygen as a chemical raw material, and an inert gas valve group pipeline for supplying inert gas as a protective medium. The deuterium / hydrogen valve group pipeline is sequentially equipped with a deuterium / hydrogen pressure reducing valve, a deuterium / hydrogen ball valve, a deuterium / hydrogen mass flow controller, and a first flame arrester. The oxygen valve group pipeline is sequentially equipped with an oxygen pressure reducing valve, an oxygen ball valve, and an oxygen mass flow controller. The inert gas valve group pipeline is sequentially equipped with an inert gas pressure reducing valve, an inert gas ball valve, and an inert gas mass flow controller. The deuterium / hydrogen valve group pipeline downstream of the first flame arrester, equipped with a control valve and a second flame arrester, is directly connected to the mixing tank of the mixing device to provide deuterium / hydrogen separately.The oxygen valve assembly pipeline with control valves and flame arresters downstream of the oxygen mass flow controller is directly connected to the low-pressure buffer tank of the circulating gas booster to provide oxygen and supplementary oxygen. Similarly, the inert gas valve assembly pipeline with control valves and flame arresters downstream of the inert gas mass flow controller is directly connected to the low-pressure buffer tank of the circulating gas booster to provide inert gas. Alternatively, the oxygen valve assembly pipeline with control valves and flame arresters downstream of the oxygen mass flow controller is directly connected to the low-pressure buffer tank of the circulating gas booster to provide oxygen, and the oxygen valve assembly pipeline downstream of the oxygen mass flow controller is connected to the mixing tank via a supplementary oxygen branch pipeline with control valves and flame arresters to directly provide supplementary oxygen. The inert gas valve assembly pipeline with control valves and flame arresters downstream of the oxygen and inert gas mass flow controllers is directly connected to the low-pressure buffer tank of the circulating gas pressurization device to provide inert gas; or the oxygen valve assembly pipeline with control valves and flame arresters downstream of the oxygen mass flow controllers is directly connected to the low-pressure buffer tank of the circulating gas pressurization device to provide oxygen and the inert gas valve assembly pipeline with control valves and flame arresters downstream of the oxygen mass flow controllers is directly connected to the low-pressure buffer tank of the circulating gas pressurization device to provide inert gas, and the oxygen valve assembly pipeline downstream of the oxygen mass flow controllers is connected to the mixing tank via an oxygen supplement branch pipeline with control valves and flame arresters to provide pressurization. The circulating gas supply pipeline indirectly supplies supplementary oxygen to the mixing tank, or the oxygen valve group pipeline downstream of the oxygen mass flow controller and the inert gas valve group pipeline downstream of the inert gas mass flow controller are connected to the low-pressure buffer tank of the circulating gas booster device through a circulating gas supplementary pipeline equipped with a control valve and a third flame arrester to supply oxygen and inert gas, and supplementary oxygen. Alternatively, the oxygen valve group pipeline downstream of the oxygen mass flow controller and the inert gas valve group pipeline downstream of the inert gas mass flow controller are connected to the low-pressure buffer tank of the circulating gas booster device through a circulating gas supplementary pipeline equipped with a control valve and a third flame arrester to supply oxygen and inert gas, while the oxygen valve group pipeline downstream of the oxygen mass flow controller... The system connects to the mixing tank via an oxygen supply branch pipe equipped with a control valve and a flame arrester to directly supply supplementary oxygen to the mixing tank. The inlet side of the oxygen supply branch pipe is located before the control valve on the circulating gas supply pipe. Alternatively, the oxygen valve group pipeline after the oxygen mass flow controller and the inert gas valve group pipeline after the inert gas mass flow controller are connected to the low-pressure buffer tank of the circulating gas pressurization device via a circulating gas supply pipe equipped with a control valve and a third flame arrester to supply oxygen and inert gas. Simultaneously, the oxygen valve group pipeline after the oxygen mass flow controller is connected to the circulating gas supply pipeline that provides pressurized circulating gas to the mixing tank via the oxygen supply branch pipe equipped with a control valve and a flame arrester to indirectly supply supplementary oxygen to the mixing tank.

[0017] The circulating gas booster device includes a low-pressure buffer tank, a booster pump, and a circulating gas mass flow controller. A third flame arrester is installed on the circulating gas replenishment pipe on the inlet side of the low-pressure buffer tank. Monitoring instruments and control valves are installed on the pipeline between the low-pressure buffer tank and the booster pump, and a fourth flame arrester is installed on the pipeline on the output side of the booster pump. The low-pressure buffer tank is used to receive oxygen and inert gas supplied by the feeding device, and the oxygen and inert gas mix in the low-pressure buffer tank to form circulating gas; or to receive circulating gas supplied by the circulating gas return pipe, and the circulating gas is buffered and stabilized in the low-pressure buffer tank; or to receive supplementary oxygen supplied by the feeding device and circulating gas supplied by the circulating gas return pipe, and the supplementary oxygen and... The circulating gas is mixed in the low-pressure buffer tank to form circulating gas containing supplemental oxygen. The booster pump is used to receive the circulating gas output from the low-pressure buffer tank or the circulating gas containing supplemental oxygen and pressurize it to form pressurized circulating gas or pressurized circulating gas containing supplemental oxygen. The pressurized circulating gas or pressurized circulating gas containing supplemental oxygen is quantitatively supplied to the mixing device through a circulating gas supply pipeline equipped with a fourth flame arrester, control valves, monitoring instruments and a circulating gas mass flow controller. Alternatively, the pressurized circulating gas or pressurized circulating gas containing supplemental oxygen is first delivered to the high-pressure buffer tank through the fourth flame arrester, and the high-pressure buffer tank then quantitatively supplies the gas to the mixing device through a circulating gas supply pipeline equipped with control valves, monitoring instruments and a circulating gas mass flow controller.

[0018] The low-pressure buffer tank is equipped with a low-pressure buffer tank hydrogen analyzer, and the high-pressure buffer tank is equipped with a high-pressure buffer tank hydrogen analyzer.

[0019] A gas bypass is configured between the low-pressure buffer tank and the high-pressure buffer tank. If the pressure of the pressurized circulating gas in the high-pressure buffer tank is too high and exceeds the backup pressure of the gas bypass, the pressurized circulating gas can flow back to the low-pressure buffer tank through the gas bypass.

[0020] The gas mixing device includes a gas mixing tank. Flame arresters are installed on both the inlet and outlet pipes of the gas mixing tank. A hydrogen analyzer and an oxygen analyzer are installed on the outlet pipe of the gas mixing tank, located before the flame arresters. The gas mixing tank is used to receive deuterium / hydrogen, supplementary oxygen, and pressurized circulating gas respectively, and homogenize them to form a mixed gas for supply to the reaction device. Alternatively, the gas mixing tank is used to receive deuterium / hydrogen, supplementary oxygen, and pressurized circulating gas respectively, and homogenize them to form an oxygen-supplemented pressurized circulating gas for supply to the reaction device. Or, the gas mixing tank is used to receive deuterium / hydrogen, supplementary oxygen, and circulating gas respectively, and homogenize them to form a pressurized circulating gas containing supplementary oxygen for supply to the reaction device.

[0021] The aforementioned reaction apparatus includes a tubular reactor, with flame arresters installed on both the inlet and outlet pipes of the tubular reactor, and an annular jacket installed outside the tubular reactor. This allows for precise control of the internal reaction temperature of the tubular reactor within the range of 100℃ to 200℃. The annular jacket, through which the high-temperature heat medium is input, circulates the high-temperature heat medium via a closed-loop high-temperature forced circulation system, providing heat preservation heating to the tubular reactor or continuously removing excess reaction heat from the tubular reactor in real time.

[0022] The annular jacket that receives the high-temperature heat medium circulates the high-temperature heat medium through a closed-loop high-temperature forced circulation system, which enables precise control of the internal reaction temperature within the range of 100℃ to 200℃. This effectively eliminates the risk of local overheating, prevents catalyst sintering and deactivation, and ensures the long-term activity and reaction stability of the catalyst.

[0023] The tubular reactor is equipped with a reactor hydrogen analyzer and a temperature monitoring instrument that is linked to the annular jacket.

[0024] The catalyst packed in the tubular reactor is a supported metal catalyst, wherein the active metal component of the supported metal catalyst is selected from at least one of palladium, platinum, nickel, rhodium, and iridium, and the support of the supported metal catalyst is selected from at least one of hydrophobic materials, metal oxides, or molecular sieves.

[0025] The supported metal catalyst is preferably at least one of platinum / hydrophobic ceramic, platinum / polytetrafluoroethylene, platinum / styrene-divinylbenzene copolymer, palladium / alumina, palladium / molecular sieve, nickel / alumina, rhodium / cerium oxide, and iridium / hydrophobic ceramic.

[0026] The gas-liquid separation device includes a primary cooler, a storage tank, and a gas-liquid separator. The input end of the primary cooler is connected to the output end of the tubular reactor in the reaction device through a pipeline equipped with a seventh flame arrester. The output end of the primary cooler is connected to the storage tank through a pipeline equipped with a control valve. The top of the storage tank is connected to the gas-liquid separator through a pipeline equipped with a control valve and monitoring instruments. The top of the gas-liquid separator is connected to the low-pressure buffer tank in the circulating gas pressurization device through a circulating gas return pipe equipped with a circulating gas mass flow controller. A third flame arrester is installed at the end of the circulating gas return pipe, or a third flame arrester is installed on the input pipe of the low-pressure buffer tank connected to the end of the circulating gas return pipe.

[0027] The liquid storage tanks are arranged in pairs in parallel between the primary cooler and the gas-liquid separator.

[0028] A sampling valve is installed on the pipeline at the front of the storage tank.

[0029] A circulating gas hydrogen analyzer and a circulating gas oxygen analyzer are arranged on the circulating gas return pipe in front of the circulating gas mass flow controller.

[0030] The circulating gas return pipe is equipped with a controller bypass, which is connected in parallel with the circulating gas return pipe section where the circulating gas mass flow controller is located. When it is not necessary to control the circulating gas flow, the circulating gas can pass directly through the circulating gas bypass instead of the circulating gas return pipe with the circulating gas mass flow controller.

[0031] A venting valve 29 is installed on the circulating gas return pipe, operating based on dual-mode control logic to simultaneously achieve the core functions of impurity management and pressure safety. In the first control mode, the venting valve performs a steady-state impurity discharge function, controlling its exhaust flow rate within 1 / 10 to 1 / 50 of the total flow rate of newly replenished deuterium / hydrogen feedstock to the hydroxide fusion unit, thereby achieving quantitative and continuous discharge of non-condensable impurities. When the pressure of the high-pressure buffer tank falls below the set pressure safety threshold due to venting, the hydroxide fusion unit immediately generates a compensation signal, driving the inert gas inlet valve group to open and replenish inert gas into the hydroxide fusion unit until the pressure of the hydroxide fusion unit recovers to the set pressure. In the second control mode, the venting valve operates as a pressure safety interlock device. The hydroxide fusion unit monitors the pressure of the circulating gas circuit in real time. When the monitored pressure exceeds the preset pressure safety threshold, the venting valve will immediately trigger an independent pressure interlock signal. This pressure interlock signal takes precedence over the first control mode, and the hydroxide fusion unit will immediately drive the venting valve to switch to emergency discharge mode for rapid pressure relief until the pressure of the hydroxide fusion unit recovers to the preset pressure.

[0032] The gas-liquid separation device also includes a secondary cooler, which is arranged between the liquid storage tank and the gas-liquid separator. The top of the liquid storage tank is connected to the secondary cooler through a pipeline with control valves and monitoring instruments. The output end of the secondary cooler is directly connected to the gas-liquid separator. The secondary cooler and the primary cooler are linked by cooling water, with cooling water entering from the bottom of the secondary cooler and exiting from the top, and the cooling water output by the secondary cooler entering from the bottom of the primary cooler and exiting from the top.

[0033] A method for producing deuterium-rich water using a hydroxide hydration device, comprising the following steps:

[0034] A. The feeding device supplies oxygen and inert gas to the circulating gas booster device in proportion. The oxygen and inert gas are first mixed and then pressurized in the circulating gas booster device to form pressurized circulating gas, which is then quantitatively supplied to the mixing device. After being homogenized and mixed in the mixing device, the pressurized circulating gas passes through the reaction device and the gas-liquid separation device in sequence and returns to the circulating gas booster device. This ensures that the closed loop of circulating gas booster device → mixing device → reaction device → gas-liquid separation device → circulating gas booster device is pre-filled with a set proportion of circulating gas before proceeding to step B.

[0035] B. Deuterium / hydrogen, supplementary oxygen, and pressurized circulating gas are supplied separately to the mixing device via a flame arrester, or deuterium / hydrogen and pressurized circulating gas containing supplementary oxygen are supplied separately to the mixing device via a flame arrester, or deuterium / hydrogen, supplementary oxygen, and pressurized circulating gas are supplied separately to the mixing device via a flame arrester to form a supplementary oxygen pressurized circulating gas. After homogenization and mixing in the mixing device, the mixed gas is supplied to the reaction device via the sixth flame arrester and proceeds to step C.

[0036] C. The deuterium / hydrogen in the mixed gas reacts completely with excess oxygen in a tubular reactor with an internal temperature of 100℃~200℃. The resulting gas-liquid mixture is sent to the gas-liquid separation device through the seventh flame arrester.

[0037] D. The liquid heavy water separated by the gas-liquid separator is collected in the storage tank, and the gas phase circulating gas returns to the circulating gas booster through the circulating gas return pipe to form pressurized circulating gas or pressurized circulating gas containing supplemental oxygen to participate in the circulation again.

[0038] The feed volume ratio of oxygen and inert gas supplied by the feeding device to the circulating gas booster device in step A is (10-30):(68-89); the inlet pressure of the booster pump in the circulating gas booster device in step A is 0.8atm to 1.0atm and the outlet pressure is 1.5atm to 2.0atm.

[0039] In step A, the oxygen is high-purity oxygen, and the inert gas is argon or nitrogen.

[0040] In step A, the feed flow rate of oxygen is 0.01 to 10 L / min, and the feed flow rate of inert gas is 0.01 to 10 L / min.

[0041] In step B, the feed flow rate of the deuterium / hydrogen is 0.1 to 1 L / min.

[0042] In step B, the volume percentage content of deuterium / hydrogen in the mixed gas is 1% to 2%, the volume percentage content of oxygen is 10% to 30%, and the sum of the volume percentage contents of oxygen and inert gas is 98% to 99%; the deuterium abundance in the deuterium / hydrogen in step B is 0.015% to 99.9%; and the feed volume ratio of deuterium / hydrogen to supplementary oxygen in step B is 2:1.

[0043] The volume hourly space velocity (VHSV) of the mixed gas in the tubular reactor in step C is 2000 h⁻¹. -1 ~5000h -1 The mass content of the active metal component in the supported metal catalyst in the tubular reactor in step C is 0.1% to 20%.

[0044] A further preferred embodiment is that the mass content of the active metal component in the supported metal catalyst in the tubular reactor in step C is 5% to 10%.

[0045] The gas-liquid separation device in step D includes a primary cooler, a storage tank, and a gas-liquid separator. The gas-liquid mixture output from the tubular reactor is condensed by the primary cooler and enters the storage tank. The gas phase enters the gas-liquid separator from the top of the storage tank for further gas-liquid separation. The separated liquid phase is transported back to the storage tank, and the gas phase returns to the circulating gas pressurization device via a circulating gas return pipe equipped with a circulating gas mass flow controller to form pressurized circulating gas for re-entry into the cycle. Alternatively, the gas-liquid separation device in step D includes a primary cooler, a storage tank, a secondary cooler, and a gas-liquid separator. The gas-liquid mixture output from the tubular reactor is condensed by the primary cooler and enters the storage tank. The gas phase enters the gas-liquid separator from the top of the storage tank and enters the gas-liquid separator for further gas-liquid separation. The separated liquid phase is transported back to the storage tank, and the separated gas phase returns to the circulating gas pressurization device via a circulating gas return pipe equipped with a circulating gas mass flow controller to form pressurized circulating gas or pressurized circulating gas containing supplemental oxygen for re-entry into the cycle.

[0046] Hydrogen analyzers are installed on the low-pressure buffer tank of the circulating gas booster, the outlet side of the mixing tank of the mixing device, the tubular reactor of the reaction device, and the gas phase outlet side of the gas-liquid separator of the gas-liquid separation device to control the deuterium / hydrogen concentration in the closed loop of circulating gas booster → mixing device → reaction device → gas-liquid separation device → circulating gas booster. The volume percentage of deuterium / hydrogen in the circulating gas booster and gas-liquid separation devices is ≤1‰, and the volume percentage of deuterium / hydrogen in the mixing device and reaction device is ≤2%.

[0047] The hydroxide annealing device provided by this invention is equipped with a multivariable collaborative control unit. Through real-time monitoring and a closed-loop feedback mechanism, it dynamically adjusts the feed of deuterium / hydrogen, oxygen, and inert gas, respectively. The specific control logic is as follows:

[0048] 1. Deuterium / hydrogen concentration safety interlock control

[0049] The hydrogen analyzer in the hydrogen hydroxide fusion unit monitors the volumetric concentration of deuterium / hydrogen in real time. When the monitored concentration exceeds the preset safety threshold, a safety interlock is immediately triggered: an alarm signal is generated and a cut-off command is sent to the control valve on the deuterium / hydrogen feed line to stop the injection of deuterium / hydrogen. At this time, the hydrogen hydroxide fusion unit continues to circulate, using the excess oxygen in the circulation loop to continue the reaction and consume deuterium / hydrogen. When the hydrogen analyzer detects that the concentration of deuterium / hydrogen in the circulating gas booster and gas-liquid separator has dropped to a safe range (≤1‰), the hydrogen hydroxide fusion unit automatically releases the interlock, restarts the deuterium / hydrogen feed, and adjusts it to stabilize it at the preset target concentration value based on the concentration feedback signal.

[0050] 2. Oxygen concentration feedback regulation and control

[0051] The oxygen analyzer in the hydroxide fusion unit monitors the volume concentration of oxygen in the circulating gas in real time, and dynamically adjusts the value within a set range.

[0052] When the monitored oxygen concentration is higher than 120% of the preset target value, an adjustment command is triggered to automatically reduce or cut off the oxygen feed rate. The oxygen hydration unit continues to consume oxygen in the circulation state. After the monitored oxygen concentration returns to the set target value, the oxygen hydration unit resumes the set oxygen feed rate.

[0053] When the monitored concentration is lower than 80% of the preset target value, the adjustment command is also triggered to automatically increase the oxygen feed rate to increase the oxygen partial pressure; after the monitored oxygen concentration rises back to the set value, the oxygen hydration unit resumes the set oxygen feed rate.

[0054] In the above control logic, the deuterium / hydrogen control loop mainly serves as a safety protection link, while the oxygen control loop serves as the main process regulation link. The two are integrated through the central control system of the hydroxide fusion unit for signal integration and command coordination. Under the premise of ensuring that the hydroxide fusion unit is always outside the explosion limit range, a high-precision dynamic balance of the reaction components is achieved, thereby ensuring the long-term safe, stable and continuous operation of the hydroxide fusion unit in closed-loop state.

[0055] The present invention has the following advantages over the prior art:

[0056] 1. Intrinsic safety and elimination of the root causes of risk

[0057] Active concentration control: By precisely controlling the deuterium / hydrogen feed rate, the volume percentage of deuterium / hydrogen in the mixing tank is always maintained at an extremely low level of no more than 2%; this value is far below the lower explosive limit of hydrogen (~4%), thereby eliminating the possibility of the mixed gas reaching the explosive limit from the source and achieving intrinsic safety.

[0058] Pre-setting of the reaction environment and isolation of the process: Before starting the hydrogen hydroxide unit, the system is pre-filled with oxygen and inert gas to ensure that deuterium / hydrogen immediately comes into contact with excess oxygen and reacts, leaving no unreacted deuterium / hydrogen residue; at the same time, through a unique process design, the circulating gas and deuterium / hydrogen are combined in the mixing tank, ensuring that there is no pre-mixing path between deuterium / hydrogen and oxygen before the three-component mixing tank, fundamentally physically isolating the conditions for the formation of explosive mixtures and further reducing potential risks;

[0059] Multiple inerting treatments and partial pressure control: The introduction of inert gas not only acts as a carrier gas, but also effectively reduces the partial pressure of deuterium / hydrogen and oxygen in the system, significantly improving the safety margin of the mixed gas and inhibiting the propagation of the combustion chain reaction. In addition, the circulating gas of the hydrogen hydroxide unit contains deuterium-rich water vapor generated by the reaction. The presence of deuterium-rich water vapor significantly increases the humidity of the circulating gas. Its high specific heat capacity and molecular properties can further inhibit flame propagation and produce an excellent inerting effect on the mixed gas. Together with the inert gas, it forms a second physical and chemical barrier to suppress combustion and explosion.

[0060] 2. Reaction efficiency and process intensification

[0061] Pressurized reaction enhances mass transfer: A mixture of deuterium / hydrogen, oxygen and inert gas is introduced into the reactor under pressure. Pressurized operation significantly enhances the adsorption capacity and concentration of reactant molecules on the catalyst surface, greatly enhancing the gas-solid phase mass transfer process, thereby significantly improving the catalytic reaction rate and single-pass conversion efficiency.

[0062] High-efficiency heat transfer and precise temperature control: The combination of a ring-shaped jacketed tubular reactor with injected high-temperature heat medium and a closed high-temperature forced circulation system can continuously and efficiently remove the excess heat generated in the reaction zone, completely solving the inherent "hot spots" and local overheating problems in fixed-bed catalytic reactions, and achieving precise and stable control of the reaction temperature within a narrow range of 100℃ to 200℃.

[0063] 3. Catalyst protection and long-term stability

[0064] By eliminating local overheating, deactivation caused by sintering of catalyst active components, grain growth, or deformation of support structure is effectively prevented. The stable and uniform temperature field ensures that the catalyst can maintain its initial activity and selectivity for a long time, greatly extending the service life of the catalyst. This ensures that the entire hydroxide unit can operate efficiently, stably, continuously, and continuously for a long time, reducing operation and maintenance costs and the frequency of shutdowns for replacement. Attached Figure Description

[0065] Appendix Figure 1 A schematic diagram of the hydroxide annealing apparatus provided by the present invention.

[0066] Wherein: 1—Deuterium / hydrogen valve assembly pipeline; 101—Deuterium / hydrogen pressure reducing valve; 102—Deuterium / hydrogen balloon valve; 103—Deuterium / hydrogen mass flow controller; 104—First flame arrester; 2—Oxygen valve assembly pipeline; 201—Oxygen pressure reducing valve; 202—Oxygen ball valve; 203—Oxygen mass flow controller; 3—Inert gas valve assembly pipeline; 301—Inert gas pressure reducing valve; 302—Inert gas balloon valve; 303—Inert gas mass flow controller; 4—Low-pressure buffer tank; 5—Low-pressure buffer tank hydrogen analyzer; 6—Booster pump; 7—High-pressure buffer tank; 8—High-pressure buffer tank hydrogen analyzer; 9—Circulating... 10—Five-stage flame arrester; 11—Mixing tank; 12—Mixing tank hydrogen analyzer; 13—Mixing tank oxygen analyzer; 14—Tubular reactor; 15—Reactor hydrogen analyzer; 16—Seventh-stage flame arrester; 17—First-stage cooler; 18—Sampling valve; 19—Liquid storage tank; 20—Second-stage cooler; 21—Gas-liquid separator; 22—Circulating gas hydrogen analyzer; 23—Circulating gas oxygen analyzer; 24—Circulating gas mass flow controller; 25—Third-stage flame arrester; 26—Fourth-stage flame arrester; 27—Second-stage flame arrester; 28—Sixth-stage flame arrester; 29—Relief valve. Detailed Implementation

[0067] The technical solution of the present invention will now be clearly and completely described with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments.

[0068] like Figure 1The diagram shows a hydrogen hydroxide condensation apparatus, comprising a feeding device, a circulating gas pressurization device, a gas mixing device, a reaction device, a gas-liquid separation device, and corresponding connecting pipes, control valves, and monitoring instruments. The feeding device supplies oxygen and inert gas to the circulating gas pressurization device, and supplies a predetermined ratio of deuterium / hydrogen and supplementary oxygen to the gas mixing device, or supplies deuterium / hydrogen to the gas mixing device and a predetermined ratio of supplementary oxygen to the circulating gas returning to the circulating gas pressurization device. The circulating gas pressurization device receives oxygen and inert gas, or receives circulating gas, or receives supplementary oxygen and circulating gas, and mixes and pressurizes them to form pressurized circulating gas or pressurized circulating gas containing supplementary oxygen, which is then quantitatively supplied to the gas mixing device. The gas mixing device receives separate deuterium / hydrogen and separate supplementary oxygen... The system consists of a gas exchange device, a gas exchange device, and a gas exchange unit. The exchange unit receives oxygen, a separate pressurized circulating gas, or a gas exchange unit containing deuterium / hydrogen, a separate pressurized circulating gas, and a separate pressurized circulating gas. These components are homogenized and mixed to form a mixed gas, which is then supplied to the reaction device. The reaction device receives the mixed gas, and the deuterium / hydrogen in the mixed gas comes into contact with excess oxygen and reacts completely. The resulting gas-liquid mixture is then sent to a gas-liquid separation device. The gas-liquid separation device receives the gas-liquid mixture and separates and collects the liquid phase heavy water and the gas phase circulating gas, which is then returned to the circulating gas pressurization device via a circulating gas return pipe. The volume percentage of deuterium / hydrogen in the aforementioned circulating gas pressurization device and gas-liquid separation device is ≤1‰, and the volume percentage of deuterium / hydrogen in the gas mixing device and reaction device is ≤2%.

[0069] like Figure 1As shown, the feeding device includes a deuterium / hydrogen valve assembly pipeline 1 supplying deuterium as a chemical raw material, an oxygen valve assembly pipeline 2 supplying oxygen as a chemical raw material, and an inert gas valve assembly pipeline 3 supplying inert gas as a protective medium. The deuterium / hydrogen valve assembly pipeline 1 is sequentially equipped with a deuterium / hydrogen pressure reducing valve 101, a deuterium / hydrogen ball valve 102, a deuterium / hydrogen mass flow controller 103, a first flame arrester 104, and other control valves. The oxygen valve assembly pipeline 2 is sequentially equipped with an oxygen pressure reducing valve 201, an oxygen ball valve 202, an oxygen mass flow controller 203, and other control valves. The inert gas valve assembly pipeline 3 is sequentially equipped with an inert gas pressure reducing valve 301, an inert gas ball valve 302, an inert gas mass flow controller 303, and other control valves. The circulating gas pressurization device includes a third flame arrester 25, a low-pressure buffer tank 4, a low-pressure buffer tank hydrogen analyzer 5, a booster pump 6, a high-pressure buffer tank 7, and a high-pressure buffer tank hydrogen separator. The system includes: a gas analyzer 8, a circulating gas mass flow controller 9, and corresponding connecting pipes and other control valves and monitoring instruments; a gas mixing device including a second flame arrester 27, a fifth flame arrester 10, a gas mixing tank 11, a gas mixing tank hydrogen analyzer 12, a gas mixing tank oxygen analyzer 13, a sixth flame arrester 28, and corresponding connecting pipes and other control valves and monitoring instruments; a reaction device including a tubular reactor 14, a reactor hydrogen analyzer 15, a seventh flame arrester 16, an annular jacket and a matching closed-loop high-temperature forced circulation system, and corresponding connecting pipes and other control valves and monitoring instruments; and a gas-liquid separation device including a primary cooler 17, a sampling valve 18, a liquid storage tank 19, a secondary cooler 20, a gas-liquid separator 21, a circulating gas hydrogen analyzer 22, a circulating gas oxygen analyzer 23, a circulating gas mass flow controller 24, and corresponding connecting pipes and other control valves and monitoring instruments.

[0070] The deuterium / hydrogen valve assembly pipeline 1, which has a control valve and a second flame arrester 27, located downstream of the first flame arrester 104, is directly connected to the mixing tank 11 of the mixing device. The oxygen valve assembly pipeline 2, located downstream of the oxygen mass flow controller 203, and the inert gas valve assembly pipeline 3, located downstream of the inert gas mass flow controller 303, are connected in parallel to the circulating gas replenishment pipeline. The circulating gas replenishment pipeline, which has a control valve and a third flame arrester 25, is connected to the low-pressure buffer tank 4 of the circulating gas pressurization device. At the same time, the oxygen valve assembly pipeline 2, located downstream of the oxygen mass flow controller 203, is connected to the fifth flame arrester 1 via an oxygen replenishment branch pipeline with a control valve and a flame arrester. On the circulating gas supply pipeline at the front of the 0, a fifth flame arrester 10 at the end of the circulating gas supply pipeline is connected to the mixing tank 11 to indirectly provide supplementary oxygen; monitoring instruments and control valves are arranged on the pipeline between the low-pressure buffer tank 4 and the booster pump 6, and a fourth flame arrester 26 is arranged on the pipeline on the output side of the booster pump 6. The low-pressure buffer tank 4 is used to receive oxygen and inert gas provided by the feeding device, and the oxygen and inert gas are mixed in the low-pressure buffer tank 4 to form circulating gas. The booster pump 6 is used to receive the circulating gas output from the low-pressure buffer tank 4 at a pressure of 0.8 atm to 1.0 atm and pressurize it to 1.5 atm to 2.0 atm forms pressurized circulating gas, which is first delivered to high-pressure buffer tank 7 via fourth flame arrester 26. High-pressure buffer tank 7 is then connected to mixing tank 11 through circulating gas supply pipeline equipped with control valves, monitoring instruments and circulating gas mass flow controller 9 to provide pressurized circulating gas or pressurized circulating gas containing supplementary oxygen. Mixing tank 11 is used to receive separate deuterium / hydrogen, separate supplementary oxygen, separate pressurized circulating gas, or receive separate deuterium / hydrogen, pressurized circulating gas containing supplementary oxygen, or receive separate deuterium / hydrogen, separate supplementary oxygen and separate pressurized circulating gas to form oxygen-supplemented pressurized gas. The circulating gas is homogenized and mixed to form a mixed gas. The mixed gas tank 11 supplies pressurized mixed gas to the tubular reactor 14 through a pipeline equipped with a sixth flame arrester 28. A hydrogen analyzer 12 and an oxygen analyzer 13 are arranged on the output pipeline of the mixed gas tank 11, located before the sixth flame arrester 28. An annular jacket is installed outside the tubular reactor 14, which allows for precise control of the internal reaction temperature of the tubular reactor 14 within the range of 100℃ to 200℃. The annular jacket, through which the high-temperature heat medium is input, circulates the high-temperature heat medium through a closed-loop high-temperature forced circulation system, providing insulation for the tubular reactor 14. Excess heat of reaction is continuously removed from the tubular reactor 14, which is equipped with a reactor hydrogen analyzer 15 and a temperature monitoring instrument linked to the annular jacket. The deuterium / hydrogen gas in the mixed gas input to the tubular reactor 14 reacts completely with excess oxygen at an internal temperature of 100℃~200℃. The resulting gas-liquid mixture is output to the primary cooler 17 via a pipeline equipped with a seventh flame arrester 16. The gas-liquid mixture cooled by the primary cooler 17 is divided into two streams and enters paired storage tanks 19. The liquid phase, rich in deuterium water, remains in the storage tank 19, while the gas phase enters through the top of the storage tank 19. The secondary cooler 20 condenses the liquid again, and the resulting gas-liquid mixture is sent to the gas-liquid separator 21 for further separation. The liquid phase, rich in deuterium water, is then transported to the storage tank 19. The circulating gas phase is sent directly back to the low-pressure buffer tank 4 via a circulating gas return pipe equipped with a circulating gas mass flow controller 24, or it can be mixed with continuously supplied supplementary oxygen before being sent back to the low-pressure buffer tank 4. After being pressurized again by the booster pump 6, it continues to participate in the circulation. Combined with a continuously supplied deuterium / hydrogen and supplementary oxygen, or a continuously supplied deuterium / hydrogen, continuous production of deuterium-rich water is achieved.

[0071] The catalyst packed in the tubular reactor 14 is a supported metal catalyst, wherein the active metal component of the supported metal catalyst is selected from at least one of palladium, platinum, nickel, rhodium, and iridium, and the support for the supported metal catalyst is selected from at least one of hydrophobic materials, metal oxides, or molecular sieves; the supported metal catalyst is preferably at least one of platinum / hydrophobic ceramics, platinum / polytetrafluoroethylene, platinum / styrene-divinylbenzene copolymer, palladium / alumina, palladium / molecular sieve, nickel / alumina, rhodium / cerium oxide, and iridium / hydrophobic ceramics.

[0072] The following specific embodiments illustrate the hydroxide annealing apparatus provided by the present invention.

[0073] Example 1

[0074] A method for producing deuterium-rich water using a hydroxide fusion device, characterized by the following steps: A) High-purity oxygen and argon are mixed in a volume ratio of 20:78, respectively, through oxygen valve group pipeline 2 and inert gas valve group pipeline 3, via a circulating gas replenishment pipe to a low-pressure buffer tank 4. The mixture is then pressurized to 2.0 atm by a booster pump 6 (the inlet pressure of the booster pump 6 is maintained at 1.0 atm) to obtain pressurized circulating gas. This pressurized circulating gas is then transported to a high-pressure buffer tank 7. The pressurized circulating gas output from the high-pressure buffer tank 7 is precisely controlled by a circulating gas mass flow controller 9 to a total flow rate of 9.8 L / min. After being fully homogenized in a mixing tank 11, it sequentially passes through a tubular reactor 14, a primary condenser 17, a storage tank 19, and a gas-liquid separator 21. Finally, it returns to the low-pressure buffer tank 4 via a circulating gas return pipe equipped with a circulating gas mass flow controller 24, thus pre-filling the closed-loop circulation of the hydroxide fusion device with a specific ratio of oxygen and argon circulating gas before proceeding to step B.

[0075] B. After the oxygen and argon circulating gas circulation is stabilized, deuterium / hydrogen gas (deuterium abundance 0.03%, abbreviated as 0.03%D) is introduced into the mixing tank 11 through the deuterium / hydrogen valve group pipeline 1 at a flow rate of 0.2L / min. The continuously replenished high-purity oxygen is introduced into the low-pressure buffer tank 4 through the oxygen valve group pipeline 2 at a flow rate of 0.1L / min after being mixed with the circulating gas returned by the circulating gas replenishment pipe and the circulating gas return pipe. Then, it is pressurized to 2.0atm by the booster pump 6 to obtain pressurized circulating gas containing replenished oxygen. The pressurized circulating gas containing replenished oxygen is delivered to the high-pressure buffer tank 7. The pressurized circulating gas containing replenished oxygen output from the high-pressure buffer tank 7 is sent into the mixing tank 11 through the circulating gas mass flow controller 9 with a total flow rate of 9.9L / min. It is then fully mixed with the continuously replenished deuterium / hydrogen gas. The resulting three-component reaction gas enters the tubular reactor 14 after being safely protected by the fifth flame arrester 10.

[0076] C. The deuterium / hydrogen in the mixed gas reacts with excess oxygen in a tubular reactor 14 filled with platinum / styrene-divinylbenzene copolymer to undergo a hydrogenation reaction. The volume hourly space velocity (VHSV) of the three-component reaction gas is 3000 h⁻¹. -1 The internal temperature of the tubular reactor 14 is controlled at 150°C, and the gas-liquid mixture generated after the reaction is sent to the first-stage cooler 17 via the seventh flame arrester 16.

[0077] D. The liquid-phase deuterium-rich water product obtained by the primary cooler 17 is collected in the storage tank 19. The uncondensed gas phase mainly consists of excess oxygen, argon and trace amounts of uncondensed deuterium-rich water vapor. It is used as circulating gas and enters the gas-liquid separator 21 for further separation of the liquid phase and sent to the storage tank 19. The circulating gas phase separated by the gas-liquid separator 21 is sent to the circulating gas replenishment pipe through the circulating gas return pipe with the circulating gas mass flow controller 24 and mixed with the continuously replenished high-purity oxygen. After being returned to the low-pressure buffer tank 4 through the third flame arrester 25, it is then pressurized by the booster pump 6 and sent to the high-pressure buffer tank 7. The total flow rate is accurately controlled to 9.8 L / min by the circulating gas mass flow controller 9 and enters the mixing tank 11 to complete the circulation of the circulating gas.

[0078] The hydroxide fusion device provided in this embodiment executes the following control logic throughout the entire process of feeding-reaction-circulation: When the oxygen analyzer 23 detects that the oxygen content in the circulating gas exceeds 24.49% (i.e., exceeds the set value of 120%), the oxygen feed rate is reduced to 0.02 L / min, and the hydroxide fusion device continues to operate and consume oxygen. After the oxygen concentration recovers to the set target value, the oxygen feed rate is restored to 0.1 L / min; when the oxygen analyzer detects that the oxygen content in the circulating gas is lower than 16.33% (i.e., lower than the set value of 80%), the oxygen feed rate is increased to 0.12 L / min. After the oxygen concentration recovers to the set target value, the oxygen feed rate is restored to 0.1 L / min. When hydrogen analyzer 22, hydrogen analyzer 5, or hydrogen analyzer 8 detects a deuterium / hydrogen volume concentration in the circulating gas exceeding 1‰, or when hydrogen analyzer 12 or hydrogen analyzer 15 detects a deuterium / hydrogen volume concentration in the mixed gas or reactor exceeding 2%, the deuterium / hydrogen feed is stopped. The reaction continues using excess oxygen in the circulating loop until the deuterium / hydrogen volume concentration in the circulating gas is ≤1‰, at which point the deuterium / hydrogen feed is restarted. Under this dynamic adjustment mechanism, after 10 hours of stable operation, the storage tank 19 collected 96.00 g (0.03%D) of deuterium-rich water, with a yield of 99.55%. After 720 hours of continued stable operation, the storage tank 19 collected 6910.46 g (0.03%D) of deuterium-rich water, with a yield of 99.53%.

[0079] Example 2

[0080] This embodiment is basically the same as Embodiment 1, except that: in step B of this embodiment, deuterium / hydrogen (0.03%D) is introduced into the mixing tank 11 through the deuterium / hydrogen valve group pipeline 1 at a flow rate of 0.1L / min via the second flame arrester 27, and newly added high-purity oxygen is introduced into the mixing tank 11 through the oxygen valve group pipeline 2 at a flow rate of 0.05L / min via the fifth flame arrester 10.

[0081] Example 3

[0082] This embodiment is basically the same as Embodiment 1, except that: in step B of this embodiment, deuterium / hydrogen (0.03%D) is introduced into the mixing tank 11 through the deuterium / hydrogen valve group pipeline 1 at a flow rate of 0.16L / min via the second flame arrester 27, and newly added high-purity oxygen is introduced into the low-pressure buffer tank 4 through the oxygen valve group pipeline 2 at a flow rate of 0.08L / min via the third flame arrester 25.

[0083] Example 4

[0084] This embodiment is basically the same as embodiment three, except that: in step A of this embodiment, high-purity oxygen and argon are delivered to the hydrogen hydroxide device at a volume ratio of 10:89, and the total flow rate of the circulating gas is 9.9L / min.

[0085] Example 5

[0086] This embodiment is basically the same as Embodiment 1, except that the deuterium abundance of deuterium / hydrogen in the reaction system of this embodiment is 5% (5%D).

[0087] Example 6

[0088] This embodiment is basically the same as Embodiment 1, except that the deuterium abundance of deuterium / hydrogen in the reaction system of this embodiment is 99.9% (99.9%D).

[0089] Example 7

[0090] This embodiment is basically the same as Embodiment 1, except that the internal temperature of the tubular reactor 14 in the reaction system of this embodiment is controlled at 120°C.

[0091] Example 8

[0092] This embodiment is basically the same as Embodiment 1, except that: in this embodiment, the gas-liquid mixture output from the tubular reactor 14 in the reaction system is cooled by the primary cooler 17 and then input into the secondary cooler 20 for secondary condensation.

[0093] Example 9

[0094] This embodiment is basically the same as Embodiment 1, except that the volume hourly space velocity (VHSV) of the three-component reactant gas in this embodiment is 5000 h⁻¹. -1 .

[0095] Example 10

[0096] This embodiment is basically the same as Embodiment 1, except that: in this embodiment, the exhaust flow rate of the vent valve 29 on the circulating gas return pipe in the reaction system is maintained at 1 / 10 of the deuterium / hydrogen feed gas flow rate of the hydrogen hydroxide preparation device, that is, the exhaust flow rate of the vent valve 29 is 0.02L / min, and the flow rate of the supplementary argon gas is 0.02L / min.

[0097] Comparative Example 1

[0098] This comparative example is basically the same as Example 1, except that the temperature of the high-temperature heat medium in the annular jacket of the tubular reactor 14 in this comparative example is controlled at 300°C.

[0099] Comparative Example 2

[0100] This comparative example is basically the same as Example 1, except that the tubular reactor 14 in the reaction system of this comparative example uses resistance heating to control the temperature at 150°C.

[0101] Comparative Example 3

[0102] This comparative example is basically the same as Example 1, except that the hydroxide fusion apparatus in this comparative example is a single-pass reactor. That is, after the deuterium / hydrogen and oxygen are mixed, the tail gas (including unreacted gas and product vapor) produced after the single-pass reaction in the tubular reactor directly enters the condensation and recovery unit. There is no circulating gas return pipeline or corresponding gas circulation system, and the unreacted gas is not recycled. Specific operating conditions are as follows: deuterium / hydrogen (0.03%D) is used as the raw material, with a feed rate of 0.2 L / min; oxygen is introduced at a feed rate of 0.1 L / min; and argon, used as the carrier gas, is introduced at a feed rate of 9.8 L / min.

[0103] Table 1 summarizes the process parameters and reaction data for the trihydric hydroxide reaction of Examples 1 to 1 Comparative.

[0104]

[0105] Table 1

[0106] Table 1 shows that: in Comparative Example 1, the temperature of the high-temperature heat medium in the annular jacket of the tubular reactor 14 was controlled at 300℃, which reduced the catalyst conversion rate and may have caused partial catalyst deactivation. After 10 hours of system operation, the deuterium / hydrogen content in the circulating gas was 0.097% as detected by the circulating gas hydrogen analyzer 22. In Comparative Example 2, the tubular reactor used resistance heating, which reduced the catalyst conversion rate. This may be because the electric heating method could not effectively remove the excess heat released by the reaction, leading to an increase in the internal temperature of the reaction and partial catalyst deactivation. After 10 hours of system operation, the deuterium / hydrogen content in the circulating gas was 0.104% as detected by the circulating gas hydrogen analyzer 22. In Comparative Example 3, a non-closed-loop single-pass reaction process was used. On the one hand, the unreacted deuterium / hydrogen was directly emitted, resulting in raw material loss. On the other hand, the tail gas carried incompletely condensed deuterium-rich water vapor, causing product loss. In addition, the single-pass reaction process introduces a large amount of argon dilution gas, which causes a sharp increase in the processing load of the hydroxide unit and a low energy efficiency ratio. As a result, the process has poor atom economy, high operating costs, and difficulty in achieving complete resource recovery.

[0107] The above embodiments are merely illustrative of the technical solutions of the present invention and are not intended to limit it. Although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some or all of the technical features therein; and these modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the technical solutions of the embodiments of the present invention. All technologies not covered in this invention can be implemented using existing technologies.

Claims

1. A hydroxide annealing apparatus, characterized in that: It includes a feeding device, a circulating gas booster device, a gas mixing device, a reaction device, and a gas-liquid separation device, wherein: The feeding device is used to supply oxygen and inert gas to the circulating gas booster device, and to supply a set ratio of deuterium / hydrogen and supplementary oxygen to the mixing device, or to supply deuterium / hydrogen to the mixing device and to supply a set ratio of supplementary oxygen to the circulating gas returning to the circulating gas booster device. The circulating gas booster is used to receive oxygen and inert gas, or to receive circulating gas, or to receive supplementary oxygen and circulating gas, and to mix and boost them to form pressurized circulating gas or pressurized circulating gas containing supplementary oxygen, which is then quantitatively supplied to the gas mixing device. A gas mixing device is used to receive separate deuterium / hydrogen, separate supplementary oxygen, separate pressurized circulating gas, or receive separate deuterium / hydrogen, pressurized circulating gas containing supplementary oxygen, or receive separate deuterium / hydrogen, separate supplementary oxygen and separate pressurized circulating gas to form a supplementary pressurized circulating gas, and homogenize and mix them to form a mixed gas for supply to the reaction device. Reaction apparatus: used to receive the mixed gas, and the deuterium / hydrogen in the mixed gas comes into contact with excess oxygen and reacts completely. The gas-liquid mixture generated after the complete reaction is sent to the gas-liquid separation device. Gas-liquid separation device: used to receive gas-liquid mixtures and separate and collect the liquid phase heavy water and the gas phase, which is returned to the circulating gas booster device through the circulating gas return pipe.

2. The hydroxide annealing apparatus according to claim 1, characterized in that: The volume percentage of deuterium / hydrogen in the circulating gas booster and gas-liquid separation devices is ≤1‰, and the volume percentage of deuterium / hydrogen in the gas mixing device and reaction device is ≤2%.

3. The hydroxide annealing apparatus according to claim 1, characterized in that: A flame arrester is separately installed on the pipeline that supplies oxygen and supplemental oxygen to the circulating gas pressurizing device; a flame arrester is separately installed on the pipeline that supplies inert gas to the circulating gas pressurizing device; a second flame arrester (27) is installed on the pipeline that supplies deuterium / hydrogen to the gas mixing device; a fifth flame arrester (10) is installed on the circulating gas supply pipeline that supplies pressurized circulating gas containing supplemental oxygen to the gas mixing device; a sixth flame arrester (28) is installed on the pipeline that supplies mixed gas to the reaction device; and a seventh flame arrester (16) is installed on the pipeline that supplies gas-liquid mixture to the gas-liquid separation device; a flame arrester is installed at the end of the circulating gas return pipe that supplies circulating gas to the circulating gas pressurizing device, or the end of the circulating gas return pipe is connected to the pipeline that supplies oxygen and supplemental oxygen and is located in front of the flame arrester on that pipeline, or the end of the circulating gas return pipe is connected to the pipeline that supplies inert gas and is located in front of the flame arrester on that pipeline. Alternatively, a flame arrester may be separately installed on the pipeline from the feeding device to the circulating gas pressurizing device for supplying oxygen, a flame arrester may be separately installed on the pipeline from the feeding device to the circulating gas pressurizing device for supplying inert gas, a second flame arrester (27) may be installed on the pipeline from the feeding device to the gas mixing device for supplying deuterium / hydrogen, and a flame arrester may be installed on the pipeline from the feeding device to the gas mixing device for supplying supplementary oxygen, and a fifth flame arrester (10) may be installed on the circulating gas supply pipeline from the circulating gas pressurizing device to the gas mixing device for supplying pressurized circulating gas. A sixth flame arrester (28) is provided on the pipeline that supplies the mixed gas to the reaction device, and a seventh flame arrester (16) is provided on the pipeline that supplies the gas-liquid mixture to the gas-liquid separation device. A flame arrester is provided at the end of the circulating gas return pipe that supplies the circulating gas to the circulating gas boosting device, or the end of the circulating gas return pipe is connected to the pipeline that supplies oxygen and is located in front of the flame arrester on that pipeline, or the end of the circulating gas return pipe is connected to the pipeline that supplies inert gas and is located in front of the flame arrester on that pipeline. Alternatively, a flame arrester may be separately installed on the pipeline from the feeding device to the circulating gas pressurizing device for supplying oxygen, a flame arrester may be separately installed on the pipeline from the feeding device to the circulating gas pressurizing device for supplying inert gas, a second flame arrester (27) may be installed on the pipeline from the feeding device to the gas mixing device for supplying deuterium / hydrogen, a fifth flame arrester (10) may be installed on the circulating gas supply pipeline from the circulating gas pressurizing device to the gas mixing device for supplying pressurized circulating gas, and the end of the oxygen supplement branch pipe from the feeding device to the gas mixing device for supplying supplementary oxygen may be connected to the circulating gas supply branch pipe in front of the fifth flame arrester (10). On the gas supply pipeline, a sixth flame arrester (28) is provided on the pipeline from the gas mixing device to the reaction device and a seventh flame arrester (16) is provided on the pipeline from the reaction device to the gas-liquid separation device. A flame arrester is provided at the end of the circulating gas return pipe from the gas-liquid separation device to the circulating gas boosting device, or the end of the circulating gas return pipe is connected to the pipeline supplying oxygen and is located in front of the flame arrester on that pipeline, or the end of the circulating gas return pipe is connected to the pipeline supplying inert gas and is located in front of the flame arrester on that pipeline. Alternatively, the feeding device provides oxygen and inert gas to the circulating gas booster and the circulating gas replenishment pipe for supplementing oxygen, and the feeding device provides a third flame arrester (25) to the circulating gas booster and the circulating gas replenishment pipe for supplementing oxygen, and the feeding device provides a second flame arrester (27) to the gas mixing device for separately providing deuterium / hydrogen, the circulating gas booster provides a fifth flame arrester (10) to the circulating gas supply pipe for providing pressurized circulating gas containing supplemented oxygen to the gas mixing device, the gas mixing device provides a sixth flame arrester (28) to the gas mixing device for providing mixed gas to the reaction device, and the reaction device provides a seventh flame arrester (16) to the gas-liquid separation device for providing gas-liquid mixture, and the gas-liquid separation device provides a flame arrester at the end of the circulating gas return pipe for providing circulating gas to the circulating gas booster, or the end of the circulating gas return pipe is connected to the circulating gas replenishment pipe in front of the third flame arrester (25). Alternatively, a third flame arrester (25) may be provided on the circulating gas replenishment pipe of the feeding device that provides oxygen and inert gas to the circulating gas boosting device; a second flame arrester (27) may be provided on the pipeline of the feeding device that provides deuterium / hydrogen gas separately to the mixing device; a flame arrester may be provided on the oxygen replenishment branch pipe of the feeding device that provides supplemental oxygen separately to the mixing device; a fifth flame arrester (10) may be provided on the circulating gas supply pipeline of the circulating gas boosting device that provides pressurized circulating gas to the mixing device; a sixth flame arrester (28) may be provided on the pipeline of the mixing device that provides mixed gas to the reaction device; a seventh flame arrester (16) may be provided on the pipeline of the reaction device that provides gas-liquid mixture to the gas-liquid separation device; a flame arrester may be provided at the end of the circulating gas return pipe of the gas-liquid separation device that provides circulating gas to the circulating gas boosting device; or the end of the circulating gas return pipe may be connected to the circulating gas replenishment pipe in front of the third flame arrester (25). Alternatively, a third flame arrester (25) may be provided on the circulating gas replenishment pipe that supplies oxygen and inert gas to the circulating gas booster device, a second flame arrester (27) may be provided on the pipeline that supplies deuterium / hydrogen gas separately to the gas mixing device, a fifth flame arrester (10) may be provided on the circulating gas supply pipeline that supplies pressurized circulating gas to the gas mixing device, and the end of the oxygen replenishment branch pipe that supplies supplementary oxygen to the gas mixing device may be connected to the circulating gas supply pipeline in front of the fifth flame arrester (10), a sixth flame arrester (28) may be provided on the pipeline that supplies mixed gas to the reaction device, and a seventh flame arrester (16) may be provided on the pipeline that supplies gas-liquid mixture to the gas-liquid separation device, and a flame arrester may be provided at the end of the circulating gas return pipe that supplies circulating gas to the circulating gas booster device, or the end of the circulating gas return pipe may be connected to the circulating gas replenishment pipe in front of the third flame arrester (25).

4. The hydroxide annealing apparatus according to any one of claims 1-3, characterized in that: The feeding device includes a deuterium / hydrogen valve assembly pipeline (1) for supplying deuterium as a chemical raw material, an oxygen valve assembly pipeline (2) for supplying oxygen as a chemical raw material, and an inert gas valve assembly pipeline (3) for supplying an inert gas as a protective medium. The deuterium / hydrogen valve assembly pipeline (1) is sequentially equipped with a deuterium / hydrogen pressure reducing valve (101), a deuterium / hydrogen ball valve (102), a deuterium / hydrogen mass flow controller (103), and a first flame arrester (104). The oxygen valve assembly pipeline (2) is sequentially equipped with an oxygen pressure reducing valve (201), an oxygen ball valve (202), and an oxygen mass flow controller (203). The inert gas valve assembly pipeline (3) is sequentially equipped with an inert gas pressure reducing valve (301), an inert gas ball valve (302), and an inert gas ball valve (303). 02), Inert gas mass flow controller (303); wherein the deuterium / hydrogen valve group pipeline (1) with control valve and second flame arrester (27) on the rear side of the first flame arrester (104) is directly connected to the mixing tank (11) of the mixing device to provide deuterium / hydrogen separately; the oxygen valve group pipeline (2) with control valve and flame arrester on the rear side of the oxygen mass flow controller (203) is directly connected to the low-pressure buffer tank (4) of the circulating gas booster device to provide oxygen and supplement oxygen; the inert gas valve group pipeline (3) with control valve and flame arrester on the rear side of the inert gas mass flow controller (303) is directly connected to the low-pressure buffer tank (4) of the circulating gas booster device to provide inert gas. Alternatively, the oxygen valve assembly pipeline (2) with control valves and flame arresters on the rear side of the oxygen mass flow controller (203) can be directly connected to the low-pressure buffer tank (4) of the circulating gas booster device to provide oxygen, and the oxygen valve assembly pipeline (2) on the rear side of the oxygen mass flow controller (203) can be directly connected to the mixing tank (11) through the oxygen supplement branch pipeline with control valves and flame arresters to provide supplementary oxygen; the inert gas valve assembly pipeline (3) with control valves and flame arresters on the rear side of the inert gas mass flow controller (303) can be directly connected to the low-pressure buffer tank (4) of the circulating gas booster device to provide inert gas. Alternatively, the oxygen valve assembly pipeline (2) with control valves and flame arresters on the rear side of the oxygen mass flow controller (203) can be directly connected to the low-pressure buffer tank (4) of the circulating gas pressurization device to provide oxygen; the inert gas valve assembly pipeline (3) with control valves and flame arresters on the rear side of the inert gas mass flow controller (303) can be directly connected to the low-pressure buffer tank (4) of the circulating gas pressurization device to provide inert gas; and the oxygen valve assembly pipeline (2) on the rear side of the oxygen mass flow controller (203) can be connected to the circulating gas supply pipeline that provides pressurized circulating gas to the mixing tank (11) through an oxygen supplement branch pipeline with control valves and flame arresters to indirectly provide supplementary oxygen to the mixing tank (11). Alternatively, the oxygen valve assembly pipeline (2) behind the oxygen mass flow controller (203) and the inert gas valve assembly pipeline (3) behind the inert gas mass flow controller (303) are connected to the low-pressure buffer tank (4) of the circulating gas booster device through a circulating gas replenishment pipeline with a control valve and a third flame arrester (25) to provide oxygen and inert gas and replenish oxygen. Alternatively, the oxygen valve assembly pipeline (2) behind the oxygen mass flow controller (203) and the inert gas valve assembly pipeline (3) behind the inert gas mass flow controller (303) are connected to the low-pressure buffer tank (4) of the circulating gas booster device through a circulating gas replenishment pipeline with a control valve and a third flame arrester (25) to provide oxygen and inert gas. At the same time, the oxygen valve assembly pipeline (2) behind the oxygen mass flow controller (203) is connected to the mixing tank (11) through an oxygen replenishment branch pipeline with a control valve and a flame arrester to directly provide supplementary oxygen to the mixing tank (11), and the inlet side of the oxygen replenishment branch pipeline is located in front of the control valve on the circulating gas replenishment pipeline. Alternatively, the oxygen valve assembly pipeline (2) behind the oxygen mass flow controller (203) and the inert gas valve assembly pipeline (3) behind the inert gas mass flow controller (303) are connected to the low-pressure buffer tank (4) of the circulating gas pressurization device through a circulating gas replenishment pipeline with a control valve and a third flame arrester (25) to provide oxygen and inert gas. At the same time, the oxygen valve assembly pipeline (2) behind the oxygen mass flow controller (203) is connected to the circulating gas supply pipeline that provides pressurized circulating gas to the mixing tank (11) through an oxygen replenishment branch pipeline with a control valve and a flame arrester to indirectly provide supplementary oxygen to the mixing tank (11).

5. The hydroxide annealing apparatus according to any one of claims 1-3, characterized in that: The circulating gas booster device includes a low-pressure buffer tank (4), a booster pump (6), and a circulating gas mass flow controller (9). A third flame arrester (25) is arranged on the circulating gas replenishment pipe on the inlet side of the low-pressure buffer tank (4). Monitoring instruments and control valves are arranged on the pipeline between the low-pressure buffer tank (4) and the booster pump (6), and a fourth flame arrester (26) is arranged on the pipeline on the output side of the booster pump (6). The low-pressure buffer tank (4) is used to receive oxygen and inert gas provided by the feeding device, and the oxygen and inert gas are mixed in the low-pressure buffer tank (4) to form circulating gas, or to receive circulating gas supplied by the circulating gas return pipe, and the circulating gas is buffered and stabilized in the low-pressure buffer tank (4), or to receive supplementary oxygen provided by the feeding device and circulating gas supplied by the circulating gas return pipe. The supplementary oxygen and the circulating gas are mixed in the low-pressure buffer tank (4) to form a circulating gas containing supplementary oxygen. The booster pump (6) is used to receive the circulating gas or the circulating gas containing supplementary oxygen output from the low-pressure buffer tank (4) and pressurize it to form a pressurized circulating gas or a pressurized circulating gas containing supplementary oxygen. The pressurized circulating gas or the pressurized circulating gas containing supplementary oxygen is quantitatively supplied to the mixing device through a circulating gas supply pipeline equipped with a fourth flame arrester (26), control valves, monitoring instruments and a circulating gas mass flow controller (9). Alternatively, the pressurized circulating gas or the pressurized circulating gas containing supplementary oxygen is first transported to the high-pressure buffer tank (7) through the fourth flame arrester (26) and then quantitatively supplied to the mixing device through a circulating gas supply pipeline equipped with control valves, monitoring instruments and a circulating gas mass flow controller (9).

6. The hydroxide annealing apparatus according to any one of claims 1-3, characterized in that: The gas mixing device includes a gas mixing tank (11), with flame arresters arranged on both the input and output pipelines of the gas mixing tank (11), and a gas mixing tank hydrogen analyzer (12) and a gas mixing tank oxygen analyzer (13) arranged on the output pipeline of the gas mixing tank (11) before the flame arresters; the gas mixing tank (11) is used to receive deuterium / hydrogen, supplementary oxygen, and pressurized circulating gas respectively and homogenize them to form a mixed gas for supply to the reaction device, or the gas mixing tank (11) is used to receive deuterium / hydrogen, supplementary oxygen and pressurized circulating gas to form an oxygen-supplemented pressurized circulating gas respectively and homogenize them to form a mixed gas for supply to the reaction device, or the gas mixing tank (11) is used to receive deuterium / hydrogen, supplementary oxygen and circulating gas to form a pressurized circulating gas containing supplementary oxygen respectively and homogenize them to form a mixed gas for supply to the reaction device.

7. The hydroxide annealing apparatus according to any one of claims 1-3, characterized in that: The reaction apparatus includes a tubular reactor (14), with flame arresters arranged on both the inlet and outlet pipes of the tubular reactor (14) and an annular jacket installed outside the tubular reactor (14).

8. The hydroxide annealing apparatus according to claim 7, characterized in that: The catalyst packed in the tubular reactor (14) is a supported metal catalyst, wherein the active metal component of the supported metal catalyst is selected from at least one of palladium, platinum, nickel, rhodium and iridium, and the support of the supported metal catalyst is selected from at least one of hydrophobic materials, metal oxides or molecular sieves.

9. The hydroxide annealing apparatus according to any one of claims 1-3, characterized in that: The gas-liquid separation device includes a primary cooler (17), a storage tank (19), and a gas-liquid separator (21). The input end of the primary cooler (17) is connected to the output end of the tubular reactor (14) in the reaction device through a pipeline with a seventh flame arrester (16). The output end of the primary cooler (17) is connected to the storage tank (19) through a pipeline with a control valve. The top of the storage tank (19) is connected to the gas-liquid separator (21) through a pipeline with a control valve and a monitoring instrument. The top of the gas-liquid separator (21) is connected to the low-pressure buffer tank (4) in the circulating gas booster device through a circulating gas return pipe with a circulating gas mass flow controller (24). A third flame arrester (25) is provided at the end of the circulating gas return pipe or a third flame arrester (25) is provided on the input pipe of the low-pressure buffer tank (4) connected to the end of the circulating gas return pipe.

10. The hydroxide annealing apparatus according to claim 9, characterized in that: The gas-liquid separation device also includes a secondary cooler (20), which is arranged between the liquid storage tank (19) and the gas-liquid separator (21). The top of the liquid storage tank (19) is connected to the secondary cooler (20) through a pipeline with control valves and monitoring instruments. The output end of the secondary cooler (20) is directly connected to the gas-liquid separator (21).

11. A method for producing deuterium-rich water using a hydroxide annealing apparatus according to any one of claims 1-10, characterized in that: The steps of this method are as follows: A. The feeding device supplies oxygen and inert gas to the circulating gas booster device in proportion. The oxygen and inert gas are first mixed and then pressurized in the circulating gas booster device to form pressurized circulating gas, which is then quantitatively supplied to the mixing device. After being homogenized and mixed in the mixing device, the pressurized circulating gas passes through the reaction device and the gas-liquid separation device in sequence and returns to the circulating gas booster device. This ensures that the closed loop of the circulating gas booster device, the mixing device, the reaction device, the gas-liquid separation device, and the circulating gas booster device is pre-filled with a set proportion of circulating gas before proceeding to step B. B. Deuterium / hydrogen and supplementary oxygen and pressurized circulating gas are supplied separately to the mixing device via the flame arrester, or deuterium / hydrogen and pressurized circulating gas containing supplementary oxygen are supplied separately to the mixing device via the flame arrester, or deuterium / hydrogen, supplementary oxygen and pressurized circulating gas are supplied separately to the mixing device via the flame arrester to form supplementary oxygen and pressurized circulating gas, and after homogenization and mixing in the mixing device, the mixed gas is supplied to the reaction device via the sixth flame arrester (28) and enters step C; C. The deuterium / hydrogen in the mixed gas reacts completely with the excess oxygen in a tubular reactor (14) with an internal temperature of 100℃~200℃. The gas-liquid mixture after the reaction is sent to the gas-liquid separation device through the seventh flame arrester (16). D. The liquid phase heavy water separated by the gas-liquid separation device is collected in the storage tank (19). The gas phase circulating gas returns to the circulating gas booster device through the circulating gas return pipe to form pressurized circulating gas or pressurized circulating gas containing supplemented oxygen to participate in the circulation again.

12. The method for producing deuterium-rich water using the hydroxide annealing apparatus according to claim 11, characterized in that: The feed volume ratio of oxygen and inert gas supplied by the feeding device to the circulating gas booster device in step A is (10-30):(68-89); the inlet pressure of the booster pump (6) in the circulating gas booster device in step A is 0.8atm~1.0atm and the outlet pressure is 1.5atm~2.0atm.

13. The method for producing deuterium-rich water using the hydroxide annealing apparatus according to claim 11, characterized in that: In step B, the volume percentage content of deuterium / hydrogen in the mixed gas is 1%–2%, the volume percentage content of oxygen is 10%–30%, and the sum of the volume percentage contents of oxygen and inert gas is 98%–99%; the deuterium abundance in the deuterium / hydrogen in step B is 0.015%–99.9%; and the feed volume ratio of deuterium / hydrogen to supplementary oxygen in step B is 2:

1.

14. The method for producing deuterium-rich water using the hydroxide hydration apparatus according to claim 11, characterized in that: The volume hourly space velocity (VHSV) of the mixed gas in the tubular reactor (14) in step C is 2000 h⁻¹. -1 ~5000h -1 The mass content of the active metal component in the supported metal catalyst in the tubular reactor (14) in step C is 0.1% to 20%.

15. The method for producing deuterium-rich water using the hydroxide hydration apparatus according to claim 11, characterized in that: The gas-liquid separation device in step D includes a primary cooler (17), a storage tank (19), and a gas-liquid separator (21). The gas-liquid mixture output from the tubular reactor (14) is condensed by the primary cooler (17) and enters the storage tank (19). The gas phase enters the gas-liquid separator (21) through the top of the storage tank (19) for gas-liquid separation. The separated liquid phase is transported back to the storage tank (19), and the gas phase returns to the circulating gas booster device through the circulating gas return pipe equipped with a circulating gas mass flow controller (24) to form pressurized circulating gas to participate in the circulation again; or the gas-liquid separation device in step D includes a primary cooler. (17), storage tank (19), secondary cooler (20) and gas-liquid separator (21), the gas-liquid mixture output from the tubular reactor (14) is condensed by the primary cooler (17) and enters the storage tank (19). The gas phase is sent to the secondary cooler (20) through the top of the storage tank (19) and condensed before entering the gas-liquid separator (21) for gas-liquid separation. The separated liquid phase is transported back to the storage tank (19). The separated gas phase is returned to the circulating gas booster device through the circulating gas return pipe equipped with a circulating gas mass flow controller (24) to form pressurized circulating gas or pressurized circulating gas containing supplementary oxygen to participate in the circulation again.

Images