A vertical oxidation combustion collection system for sediment or biogenic radioactive organic carbon deuterium samples and methods of use thereof

Abstract

This invention relates to a vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples and its method of use, comprising: a vertical oxidation-combustion device for oxidizing and combusting the sample and catalyzing it into products to be separated; and a sample collection device comprising: a water vapor trapping module for collecting tritium samples; and a carbon trapping module for collecting... 14 Sample C; A rear-mounted protection module is used to discharge exhaust gas, collect waste liquid, and prevent external air interference with sample collection. This invention, by placing the collection port below the collection container, allows for the collection of tritium samples from combustion products under gravity. 14 Sample C is collected more thoroughly and can also prevent tritium from entering. 14 C-sample collection module, to avoid 14 Sample C enters the post-protection module; more importantly, nitrogen blowing or inert gas blowing can completely remove and collect any residual tritium sample in the collection module. 14 Like C, avoid the occurrence of the memory effect.

Description

TECHNICAL FIELD

[0001] The present application relates to sample combustion collection technology, in particular to a vertical oxidation combustion collection system for sediment or biological radioactive organic carbon-tritium samples and a method of use thereof. BACKGROUND

[0002] Nuclear facilities discharge a certain amount of tritium (T or 3 H) and 14 C into the environment during operation, which participate in ecological circulation and corresponding metabolic processes in the environment in the form of mainly HTO and carbon dioxide (CO2), respectively. 14 Therefore, the degree of pollution of an area by tritium and 14 C can be evaluated by monitoring the content of tritium and 14 C in soil, water, and plant samples in the area.

[0003] In the commonly used method for analyzing tritium and 14 C, the sample needs to be converted into a liquid state, enriched, and then measured using a liquid scintillation counter to improve the accuracy of the measurement of tritium and 14 C and avoid the influence of the measurement accuracy caused by the low content of tritium and 14 C in the environment. At this time, it is necessary to consider how to collect the sample in a liquid state to avoid memory effect and incomplete collection.

[0004] A device for preparing an organic tritium carbon sample and an oxidation combustion method thereof were disclosed in CN106969953A, published on July 21, 2017, and entitled "A device for preparing an organic tritium carbon sample and an oxidation combustion method thereof". The device comprises a reaction working tube, an oxidation combustion furnace, and an absorption device. The reaction working tube comprises a tube body, a first gas inlet hole, a second gas inlet hole, and a gas outlet hole. The oxidation combustion furnace is internally provided with a heating zone, which is divided into a catalytic reaction zone, a sample stacking zone, and a sample recovery zone in sequence, and each of the lower parts is provided with a temperature controller. The reaction working tube is horizontally arranged in the oxidation combustion furnace, the tube body passes through the heating zone, and the gas outlet hole is connected with the absorption device. The absorption device comprises a collection bottle and a low-temperature cold trap, the collection bottle is arranged in the low-temperature cold trap, and the gas outlet hole is connected with the collection bottle. Carbon dioxide and water vapor are introduced into the collection bottle from the gas outlet hole together with nitrogen, at the same time, the cooling liquid in the cooling liquid guide pipe flows into the cooling liquid guide pipe from the cooling liquid inlet pipe driven by the circulating water tank, and then circulates back to the circulating water tank from the cooling liquid outlet pipe. The cooling liquid in the cooling liquid guide pipe around the outside of the collection bottle circulates, so that the temperature on the outside of the collection bottle is maintained at a stable low temperature. Carbon dioxide and water vapor are pre-cooled and condensed in the collection bottle, so as to be collected and detected. The tritium sample generated by the sample is collected by the cold trap, and the carbon sample is absorbed by bubbling sodium hydroxide solution, and then measured by a liquid scintillation counter. However, the tritium sample and the carbon sample may have memory effect or incomplete collection. SUMMARY

[0005] In order to solve the problems existing in the prior art, the present invention aims to provide a vertical oxidation combustion collection system for sediment or biological radioactive organic carbon tritium samples.

[0006] The present invention discloses a vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples, comprising: a vertical oxidation-combustion device for oxidizing and combusting the sample and catalyzing it into products to be separated; and a sample collection device for collecting tritium samples from the products to be separated. 14 Sample C, the tritium sample comprising tritium water, the 14 C-sample includes 14 The product formed by carbon dioxide and alkaline solution, the sample collection device includes: a water vapor capture module, including a first blowing section, a first collection port, a first collection container, and a first connecting section. The first collection container is connected to the vertical oxidation combustion device through the first connecting section, and the first collection port is connected to the bottom of the first collection container for discharging the contents of the first collection container from the first collection container under the action of gravity. The first blowing section is connected to the top of the first collection container for blowing the residue after discharging the contents of the first collection container out from the first collection port; a carbon capture module, including a second blowing section, a second collection port, a second collection container, and a second connecting section. The second collection container is connected to the first collection container through the second connecting section, and... The second collection port is connected to the bottom of the second collection container and is used to discharge the contents of the second collection container from the second collection container under the action of gravity. The second blowing part is connected to the top of the second collection container and is used to blow out the residue after the contents of the second collection container are discharged from the second collection container from the second collection port. The rear protection module includes an exhaust part, a third collection port, a third collection container and a third connecting part. The third collection container is connected to the second collection container through the third connecting part, and the third collection port is connected to the lower part of the third collection container and is used to discharge the contents of the third collection container from the third collection container under the action of gravity. The exhaust part is connected to the third collection container and is used to discharge the gas in the third collection container and prevent air backflow.

[0007] Preferably, the vertical oxidation combustion device includes: a combustion oxidation module, which includes a vertically separable combustion tube, at least two air inlet pipes, an air intake section, and a heater; the combustion tube includes a base and a fixing section, the base being separable from or combined with the fixing section by lifting; the combustion tube has a combustion chamber that is opened and closed by lifting the base and the fixing section; the air inlet pipes extend into the combustion chamber from above and below, respectively, to introduce combustion-supporting gas into the combustion chamber in the vertical direction, so that the combustion-supporting gas forms a vortex to promote the complete combustion of the sample and form a first product; the air intake section is disposed on the top of the fixing section, for drawing out the first product; the heater is sleeved on the outside of the combustion tube, for heating the sample to reach the ignition point and burn; an oxidation catalysis module, which is connected to the air intake section, for further oxidizing and catalyzing the first product to form a second product; and a three-way catalysis module, which is connected to the oxidation catalysis module, for further detoxifying the second product through an oxidation-reduction reaction and making it the product to be separated.

[0008] Preferably, the heater includes at least one heating part and one air-cooling part. The heating part is sleeved on the outer side of the combustion tube and is used to heat the sample to reach the ignition point and burn. The air-cooling part includes a shell and an air cooler. The shell is sleeved on the outer side of the combustion tube and is a double-layer shell with a cavity between the two layers. The air outlet and air inlet of the air cooler are connected to the cavity between the double-layer shell.

[0009] Preferably, there are two intake pipes, one of which extends into the combustion chamber from the top of the fixing part or from the side of the fixing part, and the other intake pipe extends into the combustion chamber from the base.

[0010] Preferably, the oxidation catalytic module includes a copper foam mesh with a surface composition of copper oxide and a first quartz filter. The copper foam mesh is located in the channel through which the first product flows from the air intake to the three-way catalytic module, and is used to catalytically oxidize the first product with copper oxide when it passes through the heated copper foam mesh to form the second product. The first quartz filter is located between the copper foam mesh and the combustion chamber to prevent the copper foam mesh and copper oxide from falling into the combustion chamber.

[0011] Preferably, the heater further includes another heating element, which is sleeved on the outer side of the air intake element, for heating to form copper oxide on the surface of the foamed copper mesh; the temperature of each heating element is independently controlled.

[0012] Preferably, the three-way catalytic module includes a platinum-rhodium-palladium three-way catalytic converter, a second quartz filter, and a quartz catalytic tube. One end of the quartz catalytic tube is connected to the air intake section. The platinum-rhodium-palladium three-way catalytic converter is located inside the quartz catalytic tube. The second quartz filter is located at the end of the platinum-rhodium-palladium three-way catalytic converter near the air intake section, and is used to prevent the platinum-rhodium-palladium three-way catalytic converter from moving along the quartz catalytic tube toward the air intake section.

[0013] Preferably, the first collection container includes an inner tube and an outer condenser tube, the inner tube being connected to the vertical oxidation combustion device through the first connecting part, and the outer condenser tube being sleeved outside the inner tube.

[0014] Preferably, the inner tube is connected to the second collection container via the second connecting part, and the contents of the second collection container include alkaline solution.

[0015] Preferably, the first blowing section uses nitrogen blowing or inert gas blowing; the second blowing section uses nitrogen blowing or inert gas blowing.

[0016] This invention also provides a method for using the vertical oxidation combustion collection system for sediment or biological radioactive organic carbon-tritium samples as described in any of the above technical solutions, comprising the following steps: Step 1, placing the sample into the vertical oxidation combustion device, where combustion, oxidation, and catalysis form the product to be separated; Step 2, allowing the product to be separated to enter the inner tube through the first connecting part, condensing it through the outer condenser tube, and then entering the second collection container through the second connecting part, opening the first collection port to discharge the contents of the first collection container, and then using nitrogen or inert gas from the first blowing part to blow the contents of the first collection container out of the inner tube through the first collection port. The residue after the contents; Step 3, the part of the product to be separated that enters the second collection container is absorbed by alkaline solution. After complete absorption, it enters the third collection container through the third connection part. Then, the contents of the second collection container are discharged by opening the second collection port. Then, nitrogen or inert gas in the second blowing part is used to blow the residue after the contents of the second collection container are discharged from the second collection port; Step 4, the remaining part of the product to be separated that enters the third collection container is discharged as the contents of the third collection container through the third collection port, and part is discharged through the exhaust part. Beneficial effects

[0017] The vertical oxidation combustion collection system for sediment or biological radioactive organic carbon-tritium samples described in this invention has the advantage that, by placing the collection port at the bottom of the collection container, tritium samples in the combustion products can be collected by gravity. 14 Sample C is collected more thoroughly and can also prevent tritium from entering. 14C-sample collection module, to avoid 14 Sample C enters the post-protection module; more importantly, nitrogen blowing or inert gas blowing can completely remove and collect any residual tritium sample in the collection module. 14 Sample C is used to avoid the memory effect. Simultaneously, residual material is blown out of the collection port using nitrogen or inert gas blowing methods, which helps ensure complete sample collection. Attached Figure Description

[0018] Figure 1 This is a schematic diagram of the structure of a vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples as described in this invention. Figure One ;

[0019] Figure 2 This is a schematic diagram of the structure of a vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples as described in this invention. Figure Two ;

[0020] Figure 3 This is a schematic diagram of a vertical oxidation combustion device for tritium carbon in sediments and organisms as described in this invention. Figure One ;

[0021] Figure 4 This is a schematic diagram of a vertical oxidation combustion device for tritium carbon in sediments and organisms as described in this invention. Figure Two .

[0022] Explanation of reference numerals in the attached figures: Detailed Implementation

[0023] This invention provides a vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples, comprising: a vertical oxidation-combustion device 100 for oxidizing and combusting the sample and catalyzing it into products to be separated; and a sample collection device 200 for collecting tritium samples from the products to be separated. 14 Sample C, the tritium sample comprising tritium water, the 14 C-sample includes 14The product formed by CO2 and alkaline solution, the sample collection device 200 includes: a water vapor capture module 210, including a first blowing section 211, a first collection port 212, a first collection container 213, and a first connecting part 214. The first collection container 213 is connected to the vertical oxidation combustion device 100 through the first connecting part 214, and the first collection port 212 is connected to the bottom of the first collection container 213 for discharging the contents of the first collection container from the first collection container 213 under the action of gravity. The first blowing section 211 is connected to the top of the first collection container 213 for blowing out the residue after discharging the contents of the first collection container from the first collection container 213 through the first collection port 212; and a carbon capture module 220, including a second blowing section 221, a second collection port 222, a second collection container 223, and a second connecting part 224. The second collection container 223 is connected to the first collection container 213 through the second connecting part 224. The second collection port 222 is connected to the bottom of the second collection container 223, and is used to discharge the contents of the second collection container 223 from the second collection container 223 under the action of gravity. The second blowing part 221 is connected to the top of the second collection container 223, and is used to blow out the residue after the contents of the second collection container 223 are discharged from the second collection container 223 through the second collection port 222. The rear protection module 230 includes an exhaust part 231, a third collection port 232, a third collection container 233 and a third connecting part 234. The third collection container 233 is connected to the second collection container 223 through the third connecting part 234, and the third collection port 232 is connected to the lower part of the third collection container 233, and is used to discharge the contents of the third collection container 233 from the third collection container 233 under the action of gravity. The exhaust part 231 is connected to the third collection container 233, and is used to discharge the gas in the third collection container 233 and prevent air backflow.

[0024] The vertical oxidation combustion collection system for sediment or biological radioactive organic carbon-tritium samples described in this invention has the advantage that, by placing the collection port at the bottom of the collection container, tritium samples in the combustion products can be collected by gravity. 14 Sample C is collected more thoroughly and can also prevent tritium from entering. 14 C-sample collection module, to avoid 14 Sample C enters the post-protection module; more importantly, nitrogen blowing or inert gas blowing can completely remove and collect any residual tritium sample in the collection module. 14 Sample C is used to avoid the memory effect. Simultaneously, residual material is blown out of the collection port using nitrogen or inert gas blowing methods, which helps ensure complete sample collection.

[0025] Valves for opening and closing can be provided on the first connecting part 214, the second connecting part 224, the third connecting part 234, the first collecting port 212, the second collecting port 222, the third collecting port 232, the first blowing part 211, and the second blowing part 221. When the valve is open, the first connecting part 214, the second connecting part 224, and the third connecting part 234 are in a connected state, the first collecting port 212, the second collecting port 222, and the third collecting port 232 are in an open and collectable state, and the first blowing part 211 and the second blowing part 221 are in a blowable state. When the valve is closed, the first connecting part 214, the second connecting part 224, and the third connecting part 234 are in a disconnected state, the first collecting port 212, the second collecting port 222, and the third collecting port 232 are in a closed and non-collectable state, and the first blowing part 211 and the second blowing part 221 are in a non-blowable state.

[0026] Preferably, the vertical oxidation combustion device 100 includes: a combustion oxidation module, the combustion oxidation module including a vertical detachable combustion pipe 111, at least two air inlet pipes 112, an air intake section 113, and a heater 114; the combustion pipe 111 includes a base 1111 and a fixing section 1112, the base 1111 can be separated or combined with the fixing section 1112 by lifting, and the combustion pipe 111 is provided with a combustion chamber 1113 that is opened and closed by lifting the base 1111 and the fixing section 1112; the air inlet pipes 112 extend into the combustion chamber 1113 from above and below, respectively, for feeding air into the combustion chamber 1113 in the vertical direction. Combustion-supporting gas is introduced to create a vortex, promoting complete combustion of the sample and forming a first product. A gas-drawing section 113 is positioned on top of the fixing section 1112 to draw out the first product. A heater 114 is fitted around the combustion tube 111 to heat the sample to its ignition point and induce combustion. An oxidation catalytic module, connected to the gas-drawing section 113, further oxidizes and catalyzes the first product to form a second product. A three-way catalytic module, connected to the oxidation catalytic module, further neutralizes the second product through an oxidation-reduction reaction, making it the product to be separated.

[0027] In specific implementation, the air inlet pipe 112 can be configured with 2-4 pipes. For example, 1-2 pipes can be configured on the upper part of the fixing part 1112, all of which introduce the combustion-supporting gas from the outside of the fixing part 1112 through the housing of the fixing part 1112 to the area above the combustion chamber 1113 and allow the combustion-supporting gas to flow downwards (i.e., the fixing part 112 points towards the base 1111). 1-2 pipes can be configured on the base 1111, all of which introduce the combustion-supporting gas from the outside of the base 1111 through the base 1111 to the area below the combustion chamber 1113 and allow the combustion-supporting gas to flow upwards (i.e., the base 1111 points towards the fixing part 1112). Specifically, the sample is burned with the aid of oxygen in the air inlet pipe 112 on the base 1111, and after mixing with the oxygen in the air inlet pipe 112 above the fixing part 1112, it is further fully burned to form the first product. The heater 114 can heat the sample by heat conduction. To achieve the heating function of the heater 114, the heater 114 and its installation position on the combustion tube 111 can utilize existing heating components and installation positions. Those skilled in the art can select existing heating components and installation positions according to actual needs. The first product is catalytically oxidized by the oxidation catalytic module to form the second product, which is then further rendered harmless by the three-way catalytic module through an oxidation-reduction reaction to form the product to be separated.

[0028] The combustion-supporting gas is preferably oxygen. Due to the high efficiency and thoroughness of combustion and post-treatment (oxidation, catalysis, reduction), the sample processing volume is no less than 100 g of biological radioactive sample or 200 g of sediment / soil sample each time.

[0029] The vertical oxidation combustion device for sediment or biological radioactive organic carbon-tritium samples described in this invention has the advantage that, taking oxygen as the combustion-supporting gas, the sample on the base is heated by passing oxygen through it, and after reaching the ignition temperature, it burns rapidly, producing gases (mainly carbon monoxide (CO, containing...). 14 CO), hydrocarbons (mainly incompletely combusted hydrocarbons CH4), n , including 14 C hydrogen compounds 14 CH n CT of carbon-tritium compounds n , 14 C-tritium compounds 14 CT n (where the subscript n represents the number of atoms, the same below), carbon dioxide (CO2, containing...) 14 CO2, water (H2O, including H2O and T2O), and particulate matter (mainly incompletely burned hydrocarbons C). n Hm O k , including 14 C n H m O k C n T m O k and 14 C n T n O k The combustion tube contains particulate matter (where the subscripts n, m, and k represent the number of atoms, the same below). In the middle of the combustion tube, the gas and particulate matter rise with the airflow and continue to burn under the action of oxygen, releasing a large amount of heat to accelerate combustion. At the upper part of the combustion tube, a downward-flowing pure oxygen stream is added through the air inlet pipe, which merges with the rising airflow, effectively supplementing oxygen and accelerating combustion. At the same time, the downward-flowing pure oxygen stream merges with the rising airflow, inevitably forming a vortex microenvironment in the upper region of the combustion tube. Some incompletely burned particulate matter will also boil and burn like the undulating airflow, which is more conducive to the complete combustion of the sample. In addition to oxygen, in systems where other combustion-supporting gases are present, such as hydrogen, alkanes, or one of the combustion-supporting gases, the above-mentioned vortex environment can also be formed through the present invention to promote the combustion of the corresponding system samples. Furthermore, the present invention is based on a three-stage cascade modular oxidation catalysis design, which effectively overcomes the shortcomings of incomplete combustion in dual-zone systems. The conversion efficiency of tritium water and carbon dioxide is higher. The vertical dual-path oxygen-supporting combustion design based on the boiling combustion principle has high heat utilization efficiency and more complete combustion.

[0030] Preferably, the heater 114 includes at least one heating part 1141 and an air-cooling part. The heating part 1141 is sleeved on the outer side of the combustion tube 111 and is used to heat the sample to reach the ignition point and burn. The air-cooling part includes a shell and an air cooler. The shell is sleeved on the outer side of the combustion tube 111 and is a double-layer shell with a cavity between the two layers. The air outlet and air inlet of the air cooler are connected to the cavity between the double-layer shell.

[0031] In specific implementation, the heating element 1141 is sleeved on the outer side of the combustion tube 111. Its placement must enable this function, allowing the sample to reach its ignition point and burn through heating. Those skilled in the art can select the heater used for the heating element and the placement position of the heating element 1141 based on existing technology and actual needs. After the air-cooling unit (not shown in the figure) is activated, air (e.g., cold air) flows from the air inlet (not shown in the figure) of the air-cooling unit through the cavity between the double-layered shells and returns to the air-cooling unit from the air outlet (not shown in the figure), is processed (e.g., cooled), and then sent back to the air inlet of the air-cooling unit. The air-cooling unit can employ an existing air-cooling system, and those skilled in the art can select an existing air-cooling system based on actual needs.

[0032] Preferably, there are two intake pipes 112, one of which extends into the combustion chamber 1113 from the top of the fixing part 1112 or from the side of the fixing part 1112, and the other intake pipe 112 extends into the combustion chamber 1113 from the base 1111.

[0033] In specific implementation, when one of the intake pipes 112 extends into the combustion chamber 1113 from the top of the fixing part 1112, and the other intake pipe 112 extends into the combustion chamber 1113 from the base 1111, the sample is burned under the action of the combustion-supporting gas (oxygen) in the intake pipe 112 and the heater (heating the sample to the ignition point to make the sample burn) to form gas and particulate matter. The gas and particulate matter rise to the middle of the combustion chamber for further combustion. After further combustion, the gas and a small amount of particulate matter form a vortex in the upper part of the combustion chamber with the combustion-supporting gas (oxygen) flowing from the top of the fixing part 1112 toward the base 111 in the intake pipe 112 and are fully burned. When the intake pipe 112 extends into the combustion chamber 1113 from the side of the fixing part 1112, the principle is the same as above. When the intake pipe 112 extends into the combustion chamber 1113 from the top of the fixing part 1112, it can extend from the upper part or upper opening of the fixing part 1112 and be fixed by a sealing component such as a plug, cap, or end cap. The sealing component is provided with a through hole (not shown in the figure) that can accommodate the intake pipe 112 and the air intake part 113. The fitting and positional relationship between the sealing component, the intake pipe 112, and the air intake part 113 on the upper part or upper opening of the fixing part 1112 adopts the positional relationship and fitting relationship in the prior art. Those skilled in the art can select the positional relationship and fitting relationship in the prior art according to actual needs, and open through holes in the double-layer shell as appropriate. When the intake pipe 112 extends into the combustion chamber 1113 from the side of the fixing part 1112, it is necessary to open through holes in the double-layer shell.

[0034] Preferably, the oxidation catalytic module includes a copper foam mesh 121 with a surface composition of copper oxide and a first quartz filter 122. The copper foam mesh 121 is located in the channel through which the first product flows from the air intake section 113 to the three-way catalytic module, and is used to catalytically oxidize the first product with copper oxide when it passes through the heated copper foam mesh 121 to form the second product. The first quartz filter 122 is located between the copper foam mesh 121 and the combustion chamber 1113, and is used to prevent the copper foam mesh 121 and copper oxide from falling into the combustion chamber 1113.

[0035] In practice, the copper foam mesh 121 described before the reaction is oxidized at high temperature, producing CuO on its surface. During the sample reaction, copper oxide plays a dual role as both an oxidant and a catalyst, facilitating the combustion of the sample to form further combustible gases (carbon monoxide (CO, etc.)). 14 CO, hydrocarbons (CH) n Unburned hydrocarbon components, containing 14 CH n CT n , 14 CT n ) accelerates combustion, producing carbon dioxide (CO2, containing 14 The combustion rate of CO2 and water (H2O, including H2O and T2O) reaches 90%. Simultaneously, at high temperatures, copper oxide can also catalyze the combustion of carbon monoxide (CO, containing...). 14 CO is oxidized to carbon dioxide or carbon-14 carbon dioxide (CO2, containing CO) 14 CO2), catalytic hydrocarbons (CH2) n , including 14 CH n CT scan n , 14 CT n ) and O2 react to produce carbon dioxide (CO2, containing 14 CO2), (H2O, including HTO, T2O), or carbon monoxide (CO, including HTO, T2O), or carbon monoxide (CO, including HTO, T2O), 14 CO is oxidized by CuO to produce carbon dioxide (CO2, containing CO). 14 (CO2), at which point CuO is reduced to Cu. After further catalytic oxidation of CuO, the combustion rate of the sample can reach 90%, reducing the working pressure of the three-way catalytic module.

[0036] Preferably, the heater 114 further includes another heating part 1141, which is sleeved on the outer side of the air intake part 113 and is used to form copper oxide on the surface of the foam copper mesh 121 by heating; the temperature of each heating part 1141 is independently controlled.

[0037] In specific implementation, the heating element 1141 is sleeved on the outer side of the gas-inducing element 113. Its placement must allow for this function, even if the copper foam mesh generates copper oxide at high temperatures. Those skilled in the art can select the heater used for the heating element and the placement position of the heating element 1141 based on existing technology and actual needs. The temperature of each heating element 1141 is independently controlled by a separate control unit, facilitating the selection of reaction conditions for different samples.

[0038] Preferably, the three-way catalytic module includes a platinum-rhodium-palladium three-way catalytic converter 131, a second quartz filter 132, and a quartz catalytic tube 133. One end of the quartz catalytic tube 133 is connected to the air intake section 113. The platinum-rhodium-palladium three-way catalytic converter 131 is located inside the quartz catalytic tube 133. The second quartz filter 132 is located at the end of the platinum-rhodium-palladium three-way catalytic converter 131 near the air intake section 113, and is used to prevent the platinum-rhodium-palladium three-way catalytic converter 131 from moving along the quartz catalytic tube 133 toward the air intake section 113.

[0039] In specific implementation, the platinum-rhodium-palladium three-way catalyst 131 provides a surface with the platinum-rhodium-palladium three-way catalyst. The support for the platinum-rhodium-palladium three-way catalyst is a porous ceramic. The platinum-rhodium-palladium three-way catalyst enables the redox reaction of the gas oxidized and catalyzed by the oxidation catalysis module to proceed efficiently at a relatively low temperature. During the redox reaction, carbon monoxide (CO, containing...)... 14 CO, hydrocarbons (CH) n Unburned fuel components, containing 14 CH n ), carbon-tritium compounds (CT) n , including 14 CT n ) and nitrogen oxides (NO) n These harmful gases are converted into relatively harmless carbon dioxide (CO2) under the catalysis of a platinum-rhodium-palladium ternary catalyst. 14 The gases emitted include CO2, water (H2O, including tritium water HTO and T2O), and nitrogen (N2). Carbon monoxide (CO, containing...) is also present. 14 CO, hydrocarbons (CH) n , including 14 CH n CT scan n , 14 CT n In the presence of a platinum-rhodium-palladium ternary catalyst, it reacts with other substances to produce carbon dioxide (CO, containing...) 14 CO, water (H2O, including H2O and T2O), nitrogen oxides (NO) nUnder the action of a catalyst, nitrogen oxides (NOx) are reduced to nitrogen (N2), which is a reduction process. Through this redox process, the catalytically oxidized gas is rendered harmless, easy to collect, and avoids environmental pollution caused by gas leaks. Furthermore, nitrogen oxides (NOx) are also reduced. n The tritium is converted into nitrogen (N2), which effectively reduces the acidity of water (tritium water) and the quenching and color effects of subsequent liquid flashover, thereby improving the measurement efficiency of tritium carbon.

[0040] Preferably, the first collection container 213 includes an inner tube 2131 and an outer condenser tube 2132. The inner tube 2131 is connected to the vertical oxidation combustion device 100 through the first connecting part 214, and the outer condenser tube 2132 is sleeved outside the inner tube 2131.

[0041] In specific implementation, when the product to be separated enters the inner tube 2131 from the vertical oxidation combustion device 100 through the first connection part 214, the outer condenser tube 2132 condenses the water vapor and / or gaseous tritium water in the product to be separated into the inner tube 2131 through condensation. At this time, some nitrogen oxides (NOx) are released. n (If any) it also dissolves in the condensed water (containing tritium), forming the contents of the first collection container.

[0042] Preferably, the inner tube 2131 is connected to the second collection container 223 through the second connecting part 224, and the contents of the second collection container include alkaline solution.

[0043] In practice, a portion of the products to be separated enters the second collection container 223 from the inner tube 2131 via the second connection 224. Carbon dioxide and carbon-14 carbon dioxide are absorbed by the alkaline solution and form the contents of the second collection container. The remaining products to be separated enter the third collection container 233.

[0044] Preferably, the first blowing section 211 adopts a nitrogen blowing method or an inert gas blowing method; the second blowing section 221 adopts a nitrogen blowing method or an inert gas blowing method.

[0045] In practice, the airflow rates of the first air blowing section 211 and the second air blowing section 221 are independent of each other.

[0046] This invention also provides a method for using the vertical oxidation combustion collection system for sediment or biological radioactive organic carbon-tritium samples as described in any of the above technical solutions, comprising: Step 1, placing the sample into the vertical oxidation combustion device, where combustion, oxidation, and catalysis form the product to be separated; Step 2, allowing the product to be separated to enter the inner tube 2131 through the first connecting part 214, condensing it through the outer condenser tube 2132, and then entering the second collection container 223 through the second connecting part 224, opening the first collection port 212 to discharge the contents of the first collection container, and then using nitrogen or inert gas from the first blowing part 211 to blow the contents of the first collection container out of the inner tube 2131 through the first collection port 212 to discharge the contents of the first collection container. The residue; Step 3, a portion of the product to be separated that has entered the second collection container 223 is absorbed by alkaline solution. After complete absorption, it enters the third collection container 233 through the third connection part 234. The contents of the second collection container are then discharged through the second collection port 222. Nitrogen or inert gas in the second blowing part 221 is then used to blow the residue of the contents of the second collection container 223 out through the second collection port 222. Step 4, the remaining product to be separated that has entered the third collection container 233 is discharged as the contents of the third collection container through the third collection port 232, and part of it is discharged in gas form through the exhaust part 231.

[0047] The above method is simple to operate, has high collection efficiency, no memory effect, and is environmentally friendly and pollution-free. The post-protection module also prevents external environmental pollution and influence on the sample.

[0048] The following are embodiments of the present invention.

[0049] like Figure 1 and Figure 2 As shown in Embodiment 1 of the present invention, a vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples includes: a vertical oxidation-combustion device 100 for oxidizing and combusting the sample and catalyzing it into products to be separated; and a sample collection device 200 for collecting tritium samples from the products to be separated. 14 C. Carbon dioxide, the sample collection device 200 includes: a water vapor capture module 210, a carbon capture module 220, and a post-protection module 230.

[0050] The water vapor capture module 210 includes a first air blowing section 211, a first collection port 212, a first collection container 213, and a first connecting section 214. The first collection container 213 is connected to the vertical oxidation combustion device 100 through the first connecting section 214, and the first collection port 212 is connected to the bottom of the first collection container 213 for discharging the contents of the first collection container 213 under the action of gravity. The first air blowing section 211 is connected to the top of the first collection container 213 for discharging the contents of the first collection container 213. 213. The residue after discharging the contents of the first collection container is blown out from the first collection port 212. The first collection container 213 includes an inner tube 2131 and an outer condenser tube 2132. The inner tube 2131 is connected to the vertical oxidation combustion device through the first connecting part 214. The outer condenser tube 2132 is sleeved outside the inner tube 2131. A valve (not shown in the figure) is provided on the first connecting part 214, a valve (not shown in the figure) is provided on the first collection port 212, and a valve (not shown in the figure) is provided on the first blowing part 211.

[0051] The carbon capture module 220 includes a second blowing section 221, a second collection port 222, a second collection container 223, and a second connecting section 224. The second collection container 223 is connected to the first collection container 213 via the second connecting section 224. More specifically, the inner tube 2131 is connected to the second collection container via the second connecting section 224, and the second collection port 222 is connected to the bottom of the second collection container 223 for discharging the contents of the second collection container 223 under the action of gravity. The contents of the second collection container include alkaline solution. The second blowing section 221 is connected to the top of the second collection container 223 for blowing out the residue after the contents of the second collection container 223 are discharged from the second collection port 222. A valve (not shown in the figure) is provided on the second connecting section 224, the second collection port 222, and the second blowing section 221.

[0052] The rear protection module 230 includes an exhaust section 231, a third collection port 232, a third collection container 233, and a third connecting section 234. The third collection container 233 is connected to the second collection container 223 through the third connecting section 234, and the third collection port 232 is connected to the lower part of the third collection container 233 for discharging the contents of the third collection container from the third collection container 233 under the action of gravity. The exhaust section 231 is connected to the third collection container 233 for discharging gas from the third collection container 233 and preventing air backflow. A valve (not shown in the figure) is provided on the third collection port 232, and a valve is provided on the third connecting section 234.

[0053] In specific implementation, the product to be separated is generated by the vertical oxidation combustion device. The product to be separated enters the inner tube 2131 through the first connection 214, is condensed by the outer condenser 2132, and then enters the second collection container 223 through the second connection 224. The valves on the first and second connections 214 are then closed, and the valve on the first collection port 212 is opened to discharge the contents of the first collection container. Then, the valve on the first blowing section 211 is opened to allow nitrogen gas to be blown out of the first collection port 212 from the inner tube 2131, leaving the residue after the contents of the first collection container have been discharged. The portion of the product to be separated that enters the second collection container 223 is then... The product is absorbed by alkaline solution. After complete absorption, it enters the third collection container 233 through the third connecting part 234. The valve on the third connecting part 234 is closed, and the valve on the second collection port 222 is opened to discharge the contents of the second collection container. Then, the valve on the second blowing part 221 is opened to allow nitrogen gas to be blown out of the second collection container 223 from the second collection port 222, leaving the residue after discharging the contents of the second collection container. Of the remaining product to be separated in the third collection container 233, a portion is discharged as the contents of the third collection container by opening the valve on the third collection port 232, and a portion is discharged as gas through the exhaust part 231. The collected contents and residues are then tested.

[0054] According to the present invention, the nitrogen flow rate in the first blowing section 211 is 0.15L / min-0.5L / min, and the nitrogen flow rate in the second blowing section 221 is 0.15L / min-0.5L / min. The nitrogen flow rates in the first blowing section 211 and the second blowing section 221 are controlled independently by two flow meters.

[0055] like Figure 1 and Figure 3As shown, Embodiment 2 of the present invention differs from Embodiment 1 in that the vertical oxidation combustion device 100 includes a combustion oxidation module, which comprises a vertical detachable combustion pipe 111, two air inlet pipes 112, an air intake section 113, and a heater 114. The combustion pipe 111 includes a base 1111 and a fixing section 1112. The base 1111 can be separated from or combined with the fixing section 1112 by lifting. The combustion pipe 111 has a combustion chamber 1113 that is opened and closed by lifting the base 1111 and the fixing section 1112. The air inlet pipes 112 extend into the combustion chamber 1113 from above and below, respectively, for feeding air into the combustion chamber 1113 in the vertical direction. Combustion chamber 1113 is circulated with combustion-supporting gas, which forms a vortex to promote complete combustion of the sample and form a first product. Gas intake 113 is located on top of fixing part 1112 and is used to draw out the first product. Heater 114 is sleeved outside combustion tube 111 and is used to heat the sample to its ignition point and cause combustion. An oxidation catalytic module, connected to gas intake 113, is used to further oxidize and catalyze the first product to form a second product. A three-way catalytic module, connected to the oxidation catalytic module, is used to further neutralize the second product through an oxidation-reduction reaction and make it the product to be separated.

[0056] Of the two intake pipes 112, one intake pipe 112 extends into the combustion chamber 1113 from the side of the fixing part 1112, and the other intake pipe 112 extends into the combustion chamber 1113 from the base 1111;

[0057] The heater 114 includes two heating parts 1141 and one air-cooling part 1142. The heating parts 1141 are sleeved on the outer side of the combustion tube 111 and are used to heat the sample to reach the ignition point and burn it. The air-cooling part 1142 includes a shell and an air cooler. The shell is sleeved on the outer side of the combustion tube 111 and is a double-layered shell with a cavity between the two layers. The air outlet and air inlet of the air cooler are connected to the cavity between the double-layered shell.

[0058] The oxidation catalytic module includes a copper foam mesh 121 with copper oxide as its surface component and a first quartz filter 122. The copper foam mesh 121 is located in the channel through which the first product flows from the air intake section 113 to the three-way catalytic module, and is used to catalytically oxidize the first product with copper oxide when it passes through the heated copper foam mesh 121 to form the second product. The first quartz filter 122 is located between the copper foam mesh 121 and the combustion chamber 1113, and is used to prevent the copper foam mesh 121 and copper oxide from falling into the combustion chamber 1113.

[0059] The heater 114 also includes another heating part 1141, which is sleeved on the outer side of the air intake part 113 and is used to form copper oxide on the surface of the foam copper mesh 121 by heating; the temperature of each heating part 1141 is independently controlled.

[0060] The three-way catalytic converter module includes a platinum-rhodium-palladium three-way catalytic converter 131, a second quartz filter 132, and a quartz catalytic tube 133. One end of the quartz catalytic tube 133 is connected to the air intake section 113. The platinum-rhodium-palladium three-way catalytic converter 131 is located inside the quartz catalytic tube 133. The second quartz filter 132 is located at the end of the platinum-rhodium-palladium three-way catalytic converter 131 near the air intake section 113, and is used to prevent the platinum-rhodium-palladium three-way catalytic converter 131 from moving along the quartz catalytic tube 133 toward the air intake section 113.

[0061] The rest is the same as in Example 1.

[0062] In specific implementation, the process of generating the product to be separated is as follows: lower the base 1111, place the sample in it, and then raise the base 1111 so that it is integrated with the fixing part 1112; control the heating temperature of the other heating part 1141 from room temperature to 800°C at a heating rate of 10°C / min, and continuously heat the foam copper mesh 121 at a constant temperature; use a heating device (not shown in the figure) to heat the platinum-rhodium-palladium three-way catalyst 131 at a heating temperature from room temperature to 600°C at a heating rate of 10°C / min. After the foamed copper mesh 121 and the platinum-rhodium-palladium three-way catalytic converter 131 reach 800°C and 600°C respectively, the combustion-supporting gas is introduced from above and below the combustion tube 111 through the air inlet pipe 112, and the heating temperature of the heating unit 1141 is controlled to rise from room temperature to 800°C at a heating rate of 10°C / min. Then, the sample is heated at a constant temperature to its ignition point, and the process of heating or constant temperature oxidation, catalysis, and reduction is continued until the gas formed by the combustion of the sample is rendered harmless, forming the product to be separated. Then, the product to be separated is collected according to the steps of Example 1.

[0063] More specifically, of the two intake pipes 112, the oxygen flow rate of the intake pipe 112 extending from the base 1111 into the combustion chamber 1113 is 0.12L / min-0.5L / min, and the oxygen flow rate of the intake pipe 112 extending from the side of the fixing part 1112 into the combustion chamber 1113 is 0.12L / min-0.5L / min. The oxygen flow rates in the two intake pipes 112 are independently controlled by two flow meters (the flow rates of nitrogen and oxygen required for the specific experiment are adjusted according to the organic matter and oil content in the sample).

[0064] like Figure 2 and Figure 4As shown, in Embodiment 3 of the present invention, one of the two intake pipes 112 extends from the top of the fixing part 1112 into the combustion chamber 1113, and the other intake pipe 112 extends from the base 1111 into the combustion chamber 1113; the rest is the same as in Embodiment 2.

[0065] The vertical oxidation combustion collection system for sediment or biological radioactive organic carbon-tritium samples described in this invention has the advantage of placing the collection port below the flow path of the combustion products or for absorbing the combustion products. 14 Below sample C, the tritium sample in the combustion products can be separated by gravity. 14 Sample C is collected more thoroughly and can also prevent tritium from entering. 14 C-sample collection module, to avoid 14 Sample C enters the post-protection module; more importantly, nitrogen blowing or inert gas blowing can thoroughly remove and collect the tritium sample in the collection module. 14 C-type samples are used to avoid the memory effect and to ensure the tritium sample and... 14 Sample C was collected completely.

[0066] In the description of this invention, it should be understood that the orientation or positional relationship indicated by directional terms such as "front, back, up, down, left, right", "horizontal, vertical, horizontal" and "top, bottom" is generally based on the orientation or positional relationship shown in the accompanying drawings, and is only for the convenience of describing this invention and simplifying the description. Unless otherwise stated, these directional terms do not indicate or imply that the device or element referred to must have a specific orientation or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation on the scope of protection of this invention.

[0067] For those skilled in the art, various other corresponding changes and modifications can be made based on the technical solutions and concepts described above, and all such changes and modifications should fall within the protection scope of the claims of this invention.

Claims

1. A vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples, characterized in that, include: A vertical oxidation combustion device (100) is used to oxidize and combust the sample and catalyze it into the product to be separated; Sample collection device (200) for collecting tritium samples from the products to be separated and 14 Sample C, the tritium sample comprising tritium water, the 14 C-sample includes 14 The product formed by carbon dioxide and alkaline solution, the sample collection device (200) includes: The water vapor capture module (210) includes a first air blowing section (211), a first collection port (212), a first collection container (213), and a first connecting section (214). The first collection container (213) is connected to the vertical oxidation combustion device (100) through the first connecting section (214), and the first collection port (212) is connected to the bottom of the first collection container (213) for discharging the contents of the first collection container from the first collection container (213) under the action of gravity. The first air blowing section (211) is connected to the top of the first collection container (213) for blowing the residue after the contents of the first collection container are discharged from the first collection container (213) out from the first collection port (212). The carbon capture module (220) includes a second blowing section (221), a second collection port (222), a second collection container (223), and a second connecting section (224). The second collection container (223) is connected to the first collection container (213) through the second connecting section (224), and the second collection port (222) is connected to the bottom of the second collection container (223) for discharging the contents of the second collection container from the second collection container (223) under the action of gravity. The second blowing section (221) is connected to the top of the second collection container (223) for blowing the residue after the contents of the second collection container are discharged from the second collection container (223) out from the second collection port (222). The rear protection module (230) includes an exhaust section (231), a third collection port (232), a third collection container (233), and a third connecting section (234). The third collection container (233) is connected to the second collection container (223) through the third connecting section (234), and the third collection port (232) is connected to the lower part of the third collection container (233) for discharging the contents of the third collection container from the third collection container (233) under the action of gravity. The exhaust section (231) is connected to the third collection container (233) for discharging the gas in the third collection container (233) and preventing air backflow.

2. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 1, characterized in that, The vertical oxidation combustion device (100) includes: A combustion oxidation module, comprising a vertically detachable combustion tube (111), at least two air inlet pipes (112), an air intake section (113), and a heater (114); the combustion tube (111) comprises a base (1111) and a fixing part (1112), the base (1111) being detachable or detachable from the fixing part (1112) by means of lifting, and the combustion tube (111) having a combustion chamber (1) that is opened and closed by lifting the base (1111) and the fixing part (1112). 113); the air inlet pipe (112) extends into the combustion chamber (1113) from the top and bottom respectively, and is used to introduce combustion-supporting gas into the combustion chamber (1113) in the vertical direction respectively, so that the combustion-supporting gas forms a vortex to promote the complete combustion of the sample and form the first product; the air intake part (113) is disposed on the top of the fixing part (1112) and is used to draw out the first product; the heater (114) is sleeved on the outside of the combustion pipe (111) and is used to heat the sample to reach the ignition point and burn; An oxidation catalysis module, which is connected to the gas intake section (113), is used to further oxidize and catalyze the first product to form a second product; A three-way catalytic module, which is connected to the oxidation catalytic module, is used to further render the second product harmless through an oxidation-reduction reaction and make it the product to be separated.

3. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 2, characterized in that, The heater (114) includes at least one heating part (1141) and an air-cooling part. The heating part (1141) is sleeved on the outer side of the combustion tube (111) and is used to heat the sample to reach the ignition point and burn. The air-cooling part includes a shell and an air cooler. The shell is sleeved on the outer side of the combustion tube (111) and is a double-layer shell with a cavity between the two layers. The air outlet and air inlet of the air cooler are connected to the cavity between the double-layer shell.

4. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 2, characterized in that, There are two intake pipes (112), one of which extends into the combustion chamber (1113) from the top of the fixing part (1112) or from the side of the fixing part (1112), and the other intake pipe (112) extends into the combustion chamber (1113) from the base (1111).

5. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 3, characterized in that, The oxidation catalytic module includes a copper foam mesh (121) with copper oxide as its surface component and a first quartz filter (122). The copper foam mesh (121) is located in the channel through which the first product flows from the air intake (113) to the three-way catalytic module. It is used to catalytically oxidize the first product with copper oxide when it passes through the heated copper foam mesh (121) to form the second product. The first quartz filter (122) is located between the copper foam mesh (121) and the combustion chamber (1113) to prevent the copper foam mesh (121) and copper oxide from falling into the combustion chamber (1113).

6. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 5, characterized in that, The heater (114) also includes another heating part (1141), which is sleeved on the outer side of the air intake part (113) and is used to form copper oxide on the surface of the foam copper mesh (121) by heating; the temperature of each heating part (1141) is independently controlled.

7. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 1, characterized in that, The first collection container (213) includes an inner tube (2131) and an outer condenser tube (2132). The inner tube (2131) is connected to the vertical oxidation combustion device (100) through the first connecting part (214), and the outer condenser tube (2132) is sleeved outside the inner tube (2131).

8. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 7, characterized in that, The inner tube (2131) is connected to the second collection container (223) through the second connecting part (224), and the contents of the second collection container include alkaline solution.

9. The vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to claim 1, characterized in that, The first blowing section (211) uses nitrogen blowing or inert gas blowing; the second blowing section (221) uses nitrogen blowing or inert gas blowing.

10. A method of using a vertical oxidation-combustion collection system for sediment or biological radioactive organic carbon-tritium samples according to any one of claims 7, characterized in that, Step 1: Place the sample into a vertical oxidation combustion device, where combustion, oxidation, and catalysis will form the product to be separated. Step 2: The product to be separated is allowed to enter the inner tube (2131) through the first connecting part (214), condensed by the outer condenser (2132), and then enter the second collection container (223) through the second connecting part (224). The contents of the first collection container are discharged by opening the first collection port (212). Then, nitrogen or inert gas in the first blowing part (211) is used to blow out the residue of the contents of the first collection container from the inner tube (2131) through the first collection port (212). Step 3: A portion of the product to be separated that has entered the second collection container (223) is absorbed by an alkaline solution. After complete absorption, the product enters the third collection container (233) through the third connecting part (234). The contents of the second collection container are then discharged by opening the second collection port (222). Nitrogen or inert gas in the second blowing part (221) is then used to blow the contents of the second collection container (223) out of the second collection port (222) to remove the residue. Step four, the remaining product to be separated in the third collection container (233) is discharged as the contents of the third collection container through the third collection port (232), and part of it is discharged through the exhaust section (231).

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