CN216646382U - Visual fixed bed reactor for evaluating hydrazine nitrate in catalytic decomposition nitric acid - Google Patents

Visual fixed bed reactor for evaluating hydrazine nitrate in catalytic decomposition nitric acid Download PDF

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CN216646382U
CN216646382U CN202123038316.4U CN202123038316U CN216646382U CN 216646382 U CN216646382 U CN 216646382U CN 202123038316 U CN202123038316 U CN 202123038316U CN 216646382 U CN216646382 U CN 216646382U
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reactor
feed liquid
jacket shell
output core
liquid output
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史海
赵许群
梁兵连
张旭
左臣
郑卫芳
李保乐
曹智
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Dalian Institute of Chemical Physics of CAS
China Institute of Atomic of Energy
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Dalian Institute of Chemical Physics of CAS
China Institute of Atomic of Energy
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Abstract

The utility model discloses a visual fixed bed reactor for evaluating and catalyzing and decomposing hydrazine nitrate in nitric acid, which consists of a reactor cylinder, a feeding coil, a jacket shell, a feed liquid output core pipe, an orifice plate and a screw cap. The feed liquid output core pipe is movable and used for fixing the catalyst bed layer and preventing the catalyst bed layer from loosening in the reaction process. The reactor cylinder and the feeding coil are arranged in the jacket shell, so that feed liquid preheating and catalyst bed layer heating are simultaneously carried out. The utility model has the advantages of simple assembly, convenient heating and small occupied space, and can effectively save energy consumption.

Description

Visual fixed bed reactor for evaluating hydrazine nitrate in catalytic decomposition nitric acid
Technical Field
The utility model belongs to the field of nuclear power waste treatment and environmental protection, and particularly relates to a visual fixed bed reactor for a laboratory for evaluating catalytic decomposition of hydrazine nitrate in nitric acid.
Background
Nuclear power is a green low-carbon clean energy with high technical maturity, and is an important preferred technical route for solving energy problems for human beings in the future. However, the safety problem of the strongly radioactive waste, namely the spent fuel, is one of the main factors restricting the large-scale popularization and application of nuclear power. The nuclear reactor nuclear fuel has low overall utilization rate, spent fuel containing unconverted uranium is an important nuclear element resource, and at present, a nuclear fuel closed circulation route is adopted to separate, purify and further utilize nuclear elements such as uranium, plutonium and neptunium in the spent fuel. For example, PUREX procedure: dissolving spent fuel rods by nitric acid, extracting tributyl phosphate and n-dodecane organic diluent, and reducing and back-extracting by reducing agents such as hydrazine nitrate and/or hydroxylamine nitrate to realize separation, purification and enrichment of each nuclear element. In the process, a large amount of nitric acid waste liquid containing hydrazine nitrate is generated, according to the minimization principle of post-treatment of radioactive waste of spent fuel, the waste liquid is required to recycle nitric acid in the subsequent process, and the distilled residue is subjected to vitrification solidification and deep burying treatment. Hydrazine nitrate has strong reducibility, is an easily-oxidized and explosive substance with high energy content, and needs to be removed in order to eliminate the explosion risk in the concentration treatment process of waste liquid. The method for removing the hydrazine nitrate mainly comprises the steps of adding an oxidant such as sodium nitrite or introducing dinitrogen tetroxide gas and the like to oxidize the hydrazine nitrate into products such as nitrogen, water, nitrogen oxides and the like, and has the following defects: the consumption of the oxidant is high, the cost is high, the reaction is extremely violent, and certain safety risk exists; when sodium nitrite is used as an oxidant, new solid waste sodium nitrate is easily generated; the nitrogen dioxide utilization is low and there is a risk of leakage. The mode of adopting continuous catalytic decomposition to nitric acid hydrazine in spent fuel waste liquid has advantages of safety, high efficiency and economy, however spent fuel waste liquid usually has radioactivity, and from the practical application consideration, traditional reaction device is difficult to prevent feed liquid from leaking when the catalyst is changed, and moreover, the reaction process is a reaction of a large amount of in-situ gas production, and easily causes abrasion to the catalyst, so that the bed layer becomes flexible, and on the basis, the reaction device for preventing the catalytic bed from becoming flexible, and simply and quickly changing the catalyst is needed to be provided. The continuous catalytic technique generally employs a fixed bed apparatus, a trickle bed apparatus, a fluidized bed apparatus, etc., of which the fixed bed apparatus is used in many applications. The preheating of the reaction liquid and the heating of the reactor of the traditional fixed bed device are generally carried out separately and are both carried out in an electric heating mode; the traditional fixed bed device has the problems of inconvenient disassembly of the reactor and complex operation. The device that the laboratory was used is mainly so that build, and easy and simple to handle is main, and traditional fixed bed device leads to the device occupation space too big because the structure is complicated. Secondly, traditional fixed bed device is made by non-transparent material, is not convenient for observe the stationary bed catalyst and participate in the reaction flow state's of reaction state, and experimental phase is difficult to observe experimental phenomenon, when appearing the uncontrollable phenomenon such as temperature runaway, can not in time discover and control the reaction, causes the difficulty to the improvement of experimental scheme, also makes the fixed bed reaction of experimental phase have certain danger.
SUMMERY OF THE UTILITY MODEL
In order to solve the problems of complex structure, large occupied space and inconvenient operation of the traditional fixed bed device, the utility model provides a visual fixed bed reactor for a laboratory for evaluating catalytic decomposition of hydrazine nitrate in nitric acid, and the reactor can be effectively used for evaluating the performance of a catalyst.
The technical scheme adopted by the utility model for solving the technical problems is as follows:
a visual fixed bed reactor for evaluating catalytic decomposition of hydrazine nitrate in nitric acid is characterized by comprising a reactor cylinder, a feeding coil, a jacket shell, a feed liquid output core pipe and an orifice plate, wherein the reactor cylinder, the feeding coil, the jacket shell, the feed liquid output core pipe and the orifice plate are all made of transparent materials;
the jacket shell is a hollow closed chamber surrounded by the shell;
the reactor barrel is a hollow barrel with openings at the upper end and the lower end, and the lower opening end of the barrel is connected with one end of the feeding coil pipe;
the reactor cylinder and the feeding coil are arranged in the jacket shell, the upper opening end of the reactor cylinder penetrates through the jacket shell and extends out of the jacket shell, and the upper opening end of the reactor cylinder is connected with a feed liquid output core pipe; the other end of the feeding coil pipe penetrates through the jacket shell and extends out of the jacket shell; a heat conducting liquid inlet and a heat conducting liquid outlet are arranged on the jacket shell;
a pore plate is transversely arranged at the lower part in the reactor cylinder body, the pore plate is a flat plate with through holes, the reactor cylinder body positioned above the pore plate is used as a cavity for filling catalyst, and the reactor cylinder body positioned below the pore plate is used as a cavity for filling ceramic rings
The feed liquid output core pipe is a hollow pipe, and the outer diameter of the hollow pipe is consistent with the inner diameter of the reactor barrel.
The screw cap is provided with a through hole, one end of the feed liquid output core pipe penetrates through the through hole of the screw cap and the upper opening end of the reactor cylinder body and is inserted into the reactor cylinder body, an external thread is arranged on the outer wall surface of the circular upper opening end of the reactor cylinder body extending out of the jacket shell, the screw cap is screwed in the upper opening end of the reactor cylinder body, a sealing O ring is arranged between the screw cap and the upper opening end, and the reactor cylinder body, the feed liquid output core pipe and the screw cap are sealed by the fluororubber sealing O ring.
The material liquid output core pipe is positioned above the catalyst bed layer.
The reactor cylinder is a cylinder made of quartz or glass, the feeding coil pipe is a spirally wound quartz or glass pipe, the jacket shell is a cavity made of quartz or glass, the feed liquid output core pipe is a pipe body made of polytetrafluoroethylene, quartz or glass, and the pore plate is a flat plate made of quartz or glass.
The feed liquid output core pipe of the utility model can be moved and used for fixing the catalyst bed layer and preventing the catalyst bed layer from loosening in the reaction process. The reactor barrel and the feeding coil are arranged in the jacket shell, so that feed liquid preheating and catalyst bed layer heating are carried out simultaneously. The utility model has the advantages of simple assembly, convenient heating and small occupied space, and can effectively save energy consumption.
The utility model has the beneficial effects that:
(1) the reactor has simple structure and convenient catalyst filling.
(2) The preheating of the reaction liquid and the heating of the reactor are simultaneously carried out, the energy consumption is saved, and the heating mode is convenient.
(3) The quartz or glass material is adopted, so that the reaction process and the reactant state can be conveniently observed, and meanwhile, the acid corrosion resistance is high, and the safety of the experiment is effectively improved.
Drawings
FIG. 1 is a schematic structural view of the present invention;
description of reference numerals: 1-reactor cylinder, 2-feeding coil, 3-jacket shell, 4-material liquid output core pipe, 5-orifice plate, 6-screw cap, 7-heat conducting liquid inlet, 8-heat conducting liquid outlet, 9-cavity filled with catalyst, 10-cavity filled with ceramic ring.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The structure of the visual fixed bed reactor for evaluating the catalytic decomposition of the hydrazine nitrate in the nitric acid is that the reactor comprises a reactor cylinder body 1, a feeding coil pipe 2, a jacket shell 3, a feed liquid output core pipe 4 and an orifice plate 5 which are all made of transparent materials;
the jacket shell 3 is a hollow closed chamber surrounded by the shell;
the reactor barrel 1 is a hollow barrel with openings at the upper end and the lower end, and the lower opening end of the barrel is connected with one end of the feeding coil pipe 2;
the reactor cylinder 1 and the feeding coil 2 are arranged in a jacket shell 3, the upper opening end of the reactor cylinder 1 penetrates through the jacket shell 3 and extends out of the jacket shell 3, and a feed liquid output core pipe 4 is connected with the upper opening end of the reactor cylinder 1; the other end of the feeding coil 2 penetrates through the jacket shell 3 and extends out of the jacket shell 3; a heat conducting liquid inlet 7 and a heat conducting liquid outlet 8 are arranged on the jacket shell 3;
a pore plate 5 is transversely arranged at the lower part in the reactor cylinder body 1, the pore plate 5 is a flat plate with through holes, a cavity 9 for filling catalyst is arranged in the reactor cylinder body 1 above the pore plate 5, and a cavity 10 for filling ceramic rings is arranged in the reactor cylinder body 1 below the pore plate 5;
the feed liquid output core pipe 4 is a hollow pipe, and the outer diameter of the hollow pipe is consistent with the inner diameter of the reactor barrel 1.
The screw cap 6 is provided with a through hole, one end of the feed liquid output core tube 4 passes through the through hole of the screw cap 6 and the upper opening end of the reactor cylinder and is inserted into the reactor cylinder, an external thread is arranged on the outer wall surface of the circular upper opening end of the reactor cylinder 1 extending out of the jacket shell 3, the screw cap 6 is screwed on the upper opening end of the reactor cylinder, a sealing O ring is arranged between the screw cap and the upper opening end, and the reactor cylinder 1, the feed liquid output core tube 4 and the screw cap 6 are sealed by the fluororubber sealing O ring.
The feed liquid output core pipe 4 is positioned above the catalyst bed layer.
The reactor cylinder 1 is a quartz cylinder, the feeding coil 2 is a spirally coiled glass tube, the jacket shell 3 is glass, the feed liquid output core tube 4 is a transparent polytetrafluoroethylene tube, and the orifice plate 5 is a quartz flat plate.
The ruthenium-based catalyst is a carbon-supported ruthenium catalyst with the ruthenium mass content of 5%;
example 1
Placing the pore plate 5 in a reactor cylinder 1, loading 10g ruthenium-based catalyst, compacting a catalyst bed layer by using a feed liquid output core pipe 4, fixing the feed liquid output core pipe 4 by using a screw cap 6, and introducing circulating water from a heat-conducting liquid inlet 7, wherein the temperature of the circulating water is set to be 60 ℃. Feed liquid of 0.1mol/L hydrazine nitrate, 1.0mol/L nitric acid and 0.06g/L hexavalent uranium passes through the feeding coil pipe 2 at the flow rate of 0.5mL/min, and enters a catalytic bed layer for reaction after being preheated. The reacted feed liquid is sampled and analyzed, and the content of the hydrazine nitrate in the solution is 0.0002 mol/L.
Example 2
Placing the pore plate 5 in a reactor cylinder 1, loading 15g ruthenium-based catalyst, compacting a catalyst bed layer by using a feed liquid output core pipe 4, fixing the feed liquid output core pipe 4 by using a screw cap 6, and introducing circulating water from a heat-conducting liquid inlet 7, wherein the temperature of the circulating water is set to be 60 ℃. Feed liquid of 0.1mol/L hydrazine nitrate, 1.0mol/L nitric acid and 0.06g/L hexavalent uranium passes through the feeding coil pipe 2 at the flow rate of 1.5mL/min, and enters a catalytic bed layer for reaction after being preheated. The reacted feed liquid is sampled and analyzed, and the content of the hydrazine nitrate in the solution is 0.00001 mol/L.
Example 3
Placing the pore plate 5 in a reactor cylinder 1, loading 10g ruthenium-based catalyst, compacting a catalyst bed layer by using a feed liquid output core pipe 4, fixing the feed liquid output core pipe 4 by using a screw cap 6, and introducing circulating water from a heat-conducting liquid inlet 7, wherein the temperature of the circulating water is set to be 80 ℃. Feed liquid of 0.1mol/L hydrazine nitrate, 1.0mol/L nitric acid and 0.06g/L hexavalent uranium passes through the feeding coil pipe 2 at the flow rate of 1mL/min, and enters the catalytic bed layer for reaction after being preheated. The reacted feed liquid was sampled and analyzed, and no hydrazine nitrate was detected in the solution.
Example 4
Placing the pore plate 5 in a reactor cylinder 1, loading 6g ruthenium-based catalyst, compacting a catalyst bed layer by using a material liquid output core pipe 4, fixing the material liquid output core pipe 4 by using a screw cap 6, introducing circulating water from a heat-conducting liquid inlet 7, and setting the temperature of the circulating water to be 50 ℃. Feed liquid of 0.1mol/L hydrazine nitrate, 1.0mol/L nitric acid and 0.06g/L hexavalent uranium passes through the feeding coil pipe 2 at the flow rate of 0.3mL/min, and enters a catalytic bed layer for reaction after being preheated. The reacted feed liquid is sampled and analyzed, and the content of the hydrazine nitrate in the solution is 0.00005 mol/L.
Example 5
Placing the pore plate 5 in a reactor cylinder 1, loading 10g ruthenium-based catalyst, compacting a catalyst bed layer by using a feed liquid output core pipe 4, fixing the feed liquid output core pipe 4 by using a screw cap 6, and introducing circulating water from a heat-conducting liquid inlet 7, wherein the temperature of the circulating water is set to be 90 ℃. Feed liquid of 0.1mol/L hydrazine nitrate, 1.0mol/L nitric acid and 0.06g/L hexavalent uranium passes through the feeding coil pipe 2 at the flow rate of 0.5mL/min, and enters a catalytic bed layer for reaction after being preheated. The reacted feed liquid was sampled and analyzed, and no hydrazine nitrate was detected in the solution.

Claims (5)

1. A visual fixed bed reactor for evaluating catalytic decomposition of hydrazine nitrate in nitric acid is characterized by comprising a reactor cylinder (1), a feeding coil (2), a jacket shell (3), a feed liquid output core pipe (4) and an orifice plate (5), wherein the reactor cylinder, the feeding coil (2), the jacket shell, the feed liquid output core pipe and the orifice plate are all made of transparent materials;
the jacket shell (3) is a hollow closed chamber surrounded by the shell;
the reactor barrel (1) is a hollow barrel with openings at the upper end and the lower end, and the lower opening end of the barrel is connected with one end of the feeding coil pipe (2);
the reactor barrel (1) and the feeding coil pipe (2) are arranged in the jacket shell (3), the upper opening end of the reactor barrel (1) penetrates through the jacket shell (3) and extends out of the jacket shell (3), and the upper opening end of the reactor barrel (1) is connected with a material liquid output core pipe (4); the other end of the feeding coil pipe (2) penetrates through the jacket shell (3) and extends out of the jacket shell (3); a heat-conducting liquid inlet (7) and a heat-conducting liquid outlet (8) are arranged on the jacket shell (3);
the lower part in the reactor cylinder body (1) is transversely provided with a pore plate (5), the pore plate (5) is a flat plate with through holes, the reactor cylinder body (1) positioned above the pore plate (5) is used as a chamber (9) for filling catalyst, and the reactor cylinder body (1) positioned below the pore plate (5) is used as a chamber (10) for filling ceramic rings.
2. The visual fixed bed reactor according to claim 1, characterized in that the feed liquid output core tube (4) is a hollow tube with an outer diameter consistent with the inner diameter of the reactor cylinder (1).
3. The visual fixed bed reactor of claim 1 or 2, characterized in that the nut (6) is provided with a through hole, one end of the feed liquid output core tube (4) passes through the through hole of the nut (6) and the upper opening end of the reactor cylinder and is inserted into the reactor cylinder, an external thread is arranged on the outer wall surface of the circular upper opening end of the reactor cylinder (1) extending out of the jacket shell (3), the nut (6) is screwed on the upper opening end of the reactor cylinder, a sealing O ring is arranged between the nut and the upper opening end, and the reactor cylinder (1), the feed liquid output core tube (4) and the nut (6) are sealed by a fluororubber sealing O ring.
4. The visual fixed bed reactor according to claim 1, characterized in that the feed liquid output core tube (4) is located above the catalyst bed.
5. The visual fixed bed reactor according to claim 1, characterized in that the reactor cylinder (1) is a cylinder made of quartz or glass, the feeding coil pipe (2) is a spirally wound quartz or glass pipe, the jacket shell (3) is a cavity made of quartz or glass, the feed liquid output core pipe (4) is a pipe body made of polytetrafluoroethylene, quartz or glass, and the orifice plate (5) is a flat plate made of quartz or glass.
CN202123038316.4U 2021-12-06 2021-12-06 Visual fixed bed reactor for evaluating hydrazine nitrate in catalytic decomposition nitric acid Active CN216646382U (en)

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CN202123038316.4U CN216646382U (en) 2021-12-06 2021-12-06 Visual fixed bed reactor for evaluating hydrazine nitrate in catalytic decomposition nitric acid

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Application Number Priority Date Filing Date Title
CN202123038316.4U CN216646382U (en) 2021-12-06 2021-12-06 Visual fixed bed reactor for evaluating hydrazine nitrate in catalytic decomposition nitric acid

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