CN-118145760-B - Electrochemical carbon film reaction device for removing cesium ions in water body and operation process

CN118145760BCN 118145760 BCN118145760 BCN 118145760BCN-118145760-B

Abstract

The invention discloses an electrochemical carbon membrane reaction device for removing cesium ions in a water body and an operation process, and relates to the field of cesium ion separation. The device mainly comprises a functional carbon film anode, a functional carbon film cathode, a stabilized voltage power supply, a water pump, a sensor and a device shell. In the operation process, cesium ion-containing liquid to be treated is conveyed from a raw water tank to an opening A by a water pump to enter an anode chamber, sequentially penetrates through a carbon membrane anode and a carbon membrane cathode, reaches a cathode chamber and finally flows into a water production tank from an opening B to obtain a treated water body. The invention simultaneously uses the electrostatic repulsion of the carbon film anode and the electrochemical adsorption of the carbon film cathode as core processes to remove cesium ions in water, and can realize the recovery and regeneration of the device performance by periodically removing concentrated solution and inverting electrode. The process has the advantages of simple equipment, simple operation steps, low production cost and high cesium ion removal rate, and can be applied to effectively separating and removing cesium ions in water bodies such as industrial wastewater, salt lake water, nuclear wastewater, seawater and the like.

Inventors

PAN ZONGLIN
LI YUTONG
WANG CHUNYU
Fan xinfei
SONG CHENGWEN
WANG TONGHUA

Assignees

大连海事大学

Dates

Publication Date: 20260505
Application Date: 20240321

Claims (9)

1. An electrochemical carbon membrane reaction device for removing cesium ions in a water body is characterized by comprising a membrane module, a power supply (3), a raw water tank (8) and a water production tank (9), wherein the membrane module comprises a membrane module shell (6), a carbon membrane anode (1) and a carbon membrane cathode (2) are arranged in the membrane module shell (6), the carbon membrane anode (1) and the carbon membrane cathode (2) are arranged in parallel and are respectively connected with the positive electrode and the negative electrode of the power supply (3), a cavity formed by the carbon membrane anode (1) and the membrane module shell (6) is an anode chamber (6-1), a cavity formed by the carbon membrane cathode (2) and the membrane module shell (6) is a cathode chamber (6-2), a buffer chamber (6-3) is formed by the carbon membrane anode (1), the carbon membrane cathode (2) and the membrane module shell (6), the buffer chamber (6-3) is positioned between the anode chamber (6-1) and the cathode chamber (6-2), the anode chamber (6-1) is connected with the raw water tank (8), the cesium ions are produced in the buffer chamber (6-2) and the water tank (6-3), the cesium ion sensor II (5-2) is arranged in the cathode chamber (6-2), the anode chamber (6-1) is provided with an A water inlet and a C water outlet, the cathode chamber (6-2) is provided with a B water outlet and an E water outlet, and the buffer chamber (6-3) is provided with a D water inlet; the carbon film cathode (2) is obtained by loading Prussian blue or Prussian blue analogues on a carbon film substrate.
2. The electrochemical carbon membrane reaction device for removing cesium ions in water body according to claim 1, wherein the carbon membrane anode (1) and the carbon membrane cathode (2) are of porous flat plate structures, the size of the membrane pores is 0.05-10 μm, and the porosity is 10-90%; The carbon film anode (1) is a homogeneous film or a composite film prepared by taking one or more of graphite, petroleum coke, coal, carbon fiber, active carbon, graphene, carbon nano tube and MOF pyrolytic carbon as precursors; the precursor material of the carbon film matrix of the carbon film cathode (2) is consistent with that of the carbon film anode, and the loading method is one of dipping-ion exchange, chemical deposition, electrochemical deposition, in-situ growth and physical doping.
3. The electrochemical carbon membrane reaction device for removing cesium ions in water body according to claim 1, wherein a water pump (4) is arranged between the anode chamber (6-1) and the raw water tank (8), and between the cathode chamber (6-2) and the water producing tank (9).
4. The electrochemical carbon membrane reaction device for removing cesium ions in a water body according to claim 1, wherein valves are arranged at the water inlet A, the water outlet C, the water outlet B, the water outlet E and the water inlet D.
5. The electrochemical carbon membrane reaction device for removing cesium ions in a water body according to claim 1, wherein one or more membrane modules are connected in parallel.
6. The operation process of the electrochemical carbon film reaction device for removing cesium ions in a water body according to any one of claims 1-5, wherein the operation process is characterized in that a C-port valve (7-3), a D-port valve (7-4) and an E-port valve (7-5) are kept closed, a liquid to be treated containing cesium ions is conveyed from a raw water tank (8) to an A water inlet by a water pump (4) to enter an anode chamber (6-1), sequentially penetrates through a carbon film anode (1) and a carbon film cathode (2), reaches the cathode chamber (6-2) and finally flows into a water production tank (9) from a B water outlet, and cesium ions in the water body are trapped in the anode chamber (6-1) by the carbon film anode (1) during operation, and are further removed when a permeate passes through the carbon film cathode (2) due to overhigh concentration of a concentrated liquid in the anode chamber (6-1).
7. The process for operating an electrochemical carbon membrane reaction device for removing cesium ions in a water body according to claim 6, wherein the operating voltage of the device is 1.0-20V.
8. The operation process of the electrochemical carbon membrane reaction device for removing cesium ions in water according to claim 6, wherein: The cesium ion sensor I (5-1) can monitor the concentration of cesium ions in the buffer chamber (6-3) in real time, and in the operation process, when the existence of cesium ions in the buffer chamber (6-3) or the concentration of cesium ions reaches a certain threshold value is detected, the concentration of cesium ions in the anode chamber (6-1) is indicated to be higher, the carbon membrane anode (1) cannot completely intercept cesium ions in water, at the moment, a power supply (3) is disconnected, an A port valve (7-1) and a B port valve (7-2) are closed, a C port valve (7-3) and a D port valve (7-4) are opened, concentrated solution in the anode chamber (6-1) is discharged from the C port by pumping clear water or cleaning liquid from a D water inlet, then the A port valve (7-1) and the B port valve (7-2) are opened, the C port valve (7-3) and the D port valve (7-4) are closed, and the power supply (3) is opened, and the device is restored to normal operation; The cesium ion sensor II (5-2) can monitor the concentration of cesium ions in the cathode chamber (6-2) in real time, and in the operation process, when the existence of cesium ions in the cathode chamber (6-2) or the concentration of cesium ions reaches a certain threshold value is detected, the adsorption of the carbon film cathode (2) reaches saturation, the power supply (3) is reversed to realize the desorption regeneration of the carbon film cathode (2), meanwhile, the A port valve (7-1) and the B port valve (7-2) are closed, the D port valve (7-4) and the E port valve (7-5) are opened, the cesium ion-containing solution desorbed by the carbon film cathode (2) is discharged from the E water outlet by pumping clear water or cleaning liquid from the D water inlet, then the A port valve (7-1) and the B port valve (7-2) are opened, the D port valve (7-4) and the E port valve (7-5) are closed, the power supply (3) is opened, and the device is restored to normal operation.
9. The process for operating an electrochemical carbon membrane reactor for removing cesium ions from a water body according to claim 6, wherein said cesium ion-containing liquid to be treated is at least one of industrial wastewater containing cesium ions, salt lake water, nuclear wastewater, and seawater.

Description

Electrochemical carbon film reaction device for removing cesium ions in water body and operation process Technical Field The invention relates to an electrochemical carbon membrane reaction device for removing cesium ions in a water body and an operation process, and belongs to the technical field of water treatment. Background The nuclear energy is used as a renewable energy source, and is widely applied in various fields due to the characteristics of low carbon emission, high efficiency, low cost and the like. However, environmental problems caused by various radioactive contaminants, such as radionuclide-containing nuclear waste, nuclear wastewater, and nuclear sewage generated by sudden accidents, are inevitably generated due to the worldwide development and rapid development of nuclear energy. There are often a number of radionuclides present in aqueous radioactive waste streams, 137-cesium being a high level of waste nuclides, constituting a considerable risk to the environment and health. 137-cesium presents a great threat to the environment and to human health due to its long half-life (about 30 years), high solubility in water and radioactivity as a source of gamma radiation. And because 137-cesium has poor degradability and is easy to accumulate, somatic and genetic problems may be caused to organisms. The current method for removing cesium ions in water mainly comprises a chemical precipitation method, a solvent extraction method, a membrane separation method, a biological treatment method, an adsorption method and the like. The method has the advantages that the method still has some defects in the process of removing the radioactive cesium in water, for example, a great amount of salts are introduced by a chemical precipitation method, anions or pH values of precipitants in water may exceed standards, certain extracting agents in a solvent extraction method have strong toxicity, the biological treatment method has strict treatment condition requirements and low treatment efficiency, and the membrane separation technology mainly has the mechanism of physical interception, has low comprehensive efficiency and faces the problem of membrane pollution. Disclosure of Invention Aiming at the problems in the prior art, the invention provides an electrochemical carbon film reaction device for removing cesium ions in water and an operation process, wherein a porous conductive carbon film is used as a core component, and the electric field rejection function of a carbon film anode and the electrochemical adsorption function of a carbon film cathode are cooperatively utilized by introducing electrochemical action. The electrochemical carbon film reaction device can realize the efficient removal of cesium ions in water and is easy to regenerate. The device and the operation process thereof have the advantages of simple equipment, simple operation steps, low operation cost, high cesium ion removal rate and the like. The electrochemical carbon membrane reaction device for removing cesium ions in water comprises a membrane module, a power supply, a raw water tank and a water production tank, wherein the membrane module comprises a membrane module shell, a carbon membrane anode and a carbon membrane cathode are arranged in the membrane module shell, the carbon membrane anode and the carbon membrane cathode are arranged in parallel and are respectively connected with the positive electrode and the negative electrode of the power supply, a cavity formed by the carbon membrane anode and the membrane module shell is an anode chamber, a cavity formed by the carbon membrane cathode and the membrane module shell is a cathode chamber, a cavity formed by the carbon membrane anode, the carbon membrane cathode and the membrane module shell is a buffer chamber, the buffer chamber is positioned between the anode chamber and the cathode chamber, the anode chamber is connected with the raw water tank, the cathode chamber is connected with the water production tank, a cesium ion sensor I is arranged in the buffer chamber, a cesium ion sensor II is arranged in the cathode chamber and can monitor the concentration of cesium ions in a solution, the anode chamber is provided with an A water inlet and a C water outlet, and the cathode chamber is provided with a B water outlet and a D water inlet. Furthermore, the carbon film anode and the carbon film cathode are both porous flat plate structures, and have good conductivity, the film pore size is 0.05-10 mu m, and the porosity is 10-90%. Further, the carbon film anode is a homogeneous film or a composite film prepared by taking one or more of graphite, petroleum coke, coal, carbon fiber, active carbon, graphene, carbon nano tube, MOF pyrolytic carbon and the like as precursors. Further, the carbon film cathode is a functional carbon film cathode, and is obtained by loading Prussian blue or Prussian blue analogues on a carbon film substrate, wherein the Prussian blue analogues compri