CN113019117A - DBD plasma reaction device and CO conversion2Plasma system - Google Patents

DBD plasma reaction device and CO conversion2Plasma system Download PDF

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Publication number
CN113019117A
CN113019117A CN202110246652.3A CN202110246652A CN113019117A CN 113019117 A CN113019117 A CN 113019117A CN 202110246652 A CN202110246652 A CN 202110246652A CN 113019117 A CN113019117 A CN 113019117A
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China
Prior art keywords
inner electrode
plasma reaction
glass tube
quartz glass
electrode
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CN202110246652.3A
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Inventor
丁红蕾
邱凯娜
潘卫国
周柒
杜威
穆啸天
马骏驰
张凯
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Shanghai University of Electric Power
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Shanghai University of Electric Power
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Priority to CN202110246652.3A priority Critical patent/CN113019117A/en
Publication of CN113019117A publication Critical patent/CN113019117A/en
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/74General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86Catalytic processes
    • B01D53/8671Removing components of defined structure not provided for in B01D53/8603 - B01D53/8668
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2257/00Components to be removed
    • B01D2257/50Carbon oxides
    • B01D2257/504Carbon dioxide
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2259/00Type of treatment
    • B01D2259/80Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
    • B01D2259/818Employing electrical discharges or the generation of a plasma
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02ATECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters

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  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Plasma Technology (AREA)

Abstract

The present invention provides a DBD plasma reaction device having such features, including a support; the quartz glass tube is used for containing reactants of the plasma reaction and serving as a barrier medium of the plasma reaction; the two sealing devices are respectively connected with two ends of the quartz glass tube, are used for sealing the quartz glass tube and are placed on the bracket; the inner electrode assembly comprises an inner electrode and two connecting rods respectively connected with the two ends of the inner electrode, the inner electrode is arranged in the quartz glass tube, the connecting rods penetrate through the quartz glass tube and the sealing device, and the inner electrode is connected with the positive electrode of the power supply through the connecting rods; the outer electrode is arranged on the outer wall of the quartz glass tube, has the same length as the inner electrode and corresponds to the inner electrode in position, is connected with the cathode of the power supply and is used for generating an electric field with the inner electrode so as to carry out plasma reaction; the air inlet is arranged on a sealing device and is used for introducing reactants; and the air outlet is arranged on the other sealing device and is used for outputting the product.

Description

DBD plasma reaction device and CO conversion2Plasma system
Technical Field
The invention relates to the field of gas pollution treatment, in particular to a DBD plasma reaction device and CO conversion2The plasma system of (1).
Background
China uses CO from 20072The annual emission amount is nearly 60 hundred million tonnage in the world from the first to the present, and with the rapid development of China, the energy consumption amount is increasing day by day, and in 2018, the CO in China2The annual emission reaches 198.7 hundred million tons, and a large amount of CO2Is discharged into the atmosphere, and brings great influence to the environment of China. Thus, for CO2The emission reduction work is imperative. However, CO2As a nonpolar covalent compound, C ═ O bond energy is 783kJ/mol and Δ G ═ 394kJ/mol, and is very stable at room temperature, and the activation energy required for decomposition is very large, and is severely limited by thermodynamic equilibrium. In the conventional CO2In the process, CO2Has been treated as exhaust gas, but in fact CO2Is a potential substance which can be reduced to high-energy chemical substances such as CH4、CH3OH and the like, thereby participating in carbon cycle and becoming the largest and most abundant carbon resource. CO commonly used at present2The conversion and utilization technologies comprise thermal catalysis, photocatalysis, electrocatalysis, biocatalysis, low-temperature plasma catalysis and the like. Among them, the thermocatalytic technique is limited by CO2Self-strong thermal stability, conversion of CO2The energy consumption is extremely high, resulting in the pure thermal conversion of CO2The technology is poor in economical efficiency, and if fossil energy is adopted as energy, secondary greenhouse gas emission is easily caused, so that the technology is not environment-friendly; although photocatalysis uses light energy as an energy source, CO2The conversion rate and energy are the lowest, and the popularization is difficult; electrocatalysis has better CO2Conversion, but product selectivity is too poorTo be further studied; expensive and volatile enzymes in biocatalysis make this technology difficult to popularize; the low-temperature plasma catalysis has the advantages of more superior product selectivity than electrocatalysis, higher energy efficiency than photocatalysis, lower reaction temperature than thermocatalysis, simple and easy disassembly of the device, quick start and stop and the like, and gradually becomes CO2An important member of the transformation technology.
At present, researchers at home and abroad catalyze CO by low-temperature plasma2The technology has been extensively studied and classified into glow discharge, corona discharge, sliding arc discharge, microwave discharge, radio frequency discharge, Dielectric Barrier Discharge (DBD), and the like according to the form of plasma discharge. Among them, the DBD plasma is concerned by its advantages of wide pressure range, wide discharge frequency range, uniform and stable discharge, and the ability to add filling materials in the reactor. The DBD plasma is classified into a flat plate type and a cylindrical type according to the reactor structure. Compared with a flat-plate DBD reactor, the cylindrical DBD reactor has the advantages of better air tightness, capability of generating a large amount of high-energy activity, uniform and stable discharge, simple structure, good tightness, no dead angle, contribution to uniform gas distribution, easiness in cleaning, gas collection and the like.
Disclosure of Invention
The present invention has been made to solve the above problems, and an object of the present invention is to further improve the performance of a cylindrical DBD plasma separator, and to provide a DBD plasma reaction apparatus and a CO conversion apparatus2The plasma system of (1).
The present invention provides a DBD plasma reaction apparatus having such features, including: a bracket placed on a horizontal plane; the quartz glass tube is used for containing reactants of the plasma reaction and serving as a barrier medium of the plasma reaction; the two sealing devices are respectively connected with two ends of the quartz glass tube, are used for sealing the quartz glass tube and are horizontally placed on the bracket together with the quartz glass tube; the inner electrode assembly comprises an inner electrode and two connecting rods respectively connected with the two ends of the inner electrode, the inner electrode is arranged in the quartz glass tube, the diameter of the inner electrode is smaller than that of the quartz glass tube, the connecting rods penetrate through the quartz glass tube and the sealing device and are used for fixing the inner electrode, and the inner electrode is connected with the positive electrode of the power supply through the connecting rods; the outer electrode is arranged on the outer wall of the quartz glass tube, has the same length as the inner electrode, corresponds to the position of the inner electrode, is connected with the negative electrode of the power supply, and is used for being matched with the inner electrode to generate an electric field so as to enable the reactant to perform plasma reaction to generate a product; the gas inlet is arranged on a sealing device, is communicated with the quartz glass tube and is used for introducing reactants; the gas outlet is arranged on the other sealing device, is communicated with the quartz glass tube and is used for outputting a product; the inner electrode is in a thread structure, and the outer electrode is in a diamond aluminum mesh structure and is used for reinforcing an electric field between the inner electrode and the outer electrode, so that the conversion rate of reaction gas is improved.
The DBD plasma reaction apparatus according to an embodiment of the present invention may further include: wherein the reactant is CO2And H2The product is CH4
The DBD plasma reaction apparatus according to an embodiment of the present invention may further include: wherein the discharge frequency of the plasma reaction is 0-60 kHz, the discharge voltage is 0-12 kV, and the gas flow rate is 50 mL/min.
The DBD plasma reaction apparatus according to an embodiment of the present invention may further include: wherein the quartz glass tube has an outer diameter of 16mm, an inner diameter of 14mm and a length of 200 mm.
The DBD plasma reaction apparatus according to an embodiment of the present invention may further include: wherein, the total length of the inner electrode component is 290mm, and the length of the inner electrode is 100 mm.
The invention provides for converting CO2Has the characteristics that it comprises: DBD plasma reaction device for introducing CO2And H2Plasma reaction to generate CH4(ii) a And a power supply for supplying electric power to the DBD plasma reaction apparatus; wherein the DBD plasma reaction apparatus is the DBD plasma reaction apparatus according to any one of claims 1 to 5.
Conversion of CO provided in the invention2Plasma of (2)The system may further include: water electrolysis apparatus for generating H by water electrolysis process2The power supply is also used for supplying electric energy to the water electrolysis equipment.
Conversion of CO provided in the invention2The plasma system of (2) may further have the following features: the power supply is a solar cell, the solar cell comprises a solar energy converter and a storage battery, the solar energy converter is used for absorbing solar energy outdoors and generating electric energy, and the storage battery is used for storing the electric energy generated by the solar energy converter.
Action and Effect of the invention
The invention relates to a DBD plasma reaction device and CO conversion2Compared with the traditional DBD plasma reactor, the DBD plasma reaction device has the advantages that the outer electrode is separated from the quartz glass tube, so that the edge effect is enhanced, and the inner electrode is in a thread structure, so that a stronger electric field is formed, and the CO of the plasma reaction is improved2And (4) conversion rate.
Drawings
FIG. 1 is a diagram of CO conversion in an example of the present invention2Schematic diagram of a plasma system of (1);
FIG. 2 is a perspective view of a DBD plasma reaction device (including an external electrode) according to an embodiment of the present invention;
FIG. 3 is a perspective view of a DBD plasma reaction device (without an external electrode) in an embodiment of the present invention;
FIG. 4 is a sectional view of a DBD plasma reaction device (without an external electrode) in an embodiment of the present invention;
fig. 5 is a perspective view of a bracket of a DBD plasma reaction device according to an embodiment of the present invention.
Detailed Description
In order to make the technical means, creation features, achievement objects and effects of the present invention easy to understand, the following embodiments are provided to explain the DBD plasma reaction apparatus and CO conversion apparatus according to the present invention with reference to the accompanying drawings2The plasma system of (1) is specifically described.
< example >
FIG. 1 shows the conversion of CO in this example2Schematic diagram of a plasma system of (1).
As shown in FIG. 1, CO in the present embodiment2The plasma system 100 includes a DBD plasma reaction device 10, a solar cell 20, and an electrolytic water device 30.
The DBD plasma reaction device 10 is used for introducing CO2And H2Plasma reaction to generate CH4
Fig. 2 is a perspective view of a DBD plasma reaction device (including an external electrode) in this embodiment, fig. 3 is a perspective view of the DBD plasma reaction device (without the external electrode) in this embodiment, fig. 4 is a cross-sectional view of the DBD plasma reaction device (without the external electrode) in this embodiment, and fig. 5 is a perspective view of a bracket of the DBD plasma reaction device in this embodiment.
As shown in fig. 2 to 5, the DBD plasma reaction device 10 in the present embodiment includes a support 17, a quartz glass tube 11, two sealing devices 12, an inner electrode assembly 13, an outer electrode 14, a gas inlet 15, and a gas outlet 16.
The support 17 is placed on a horizontal plane and comprises a base and two vertical plates vertically arranged on the base. The upper ends of the two vertical plates are provided with grooves.
The quartz glass tube 11 is used for accommodating a reactant CO of a plasma reaction2And acts as a barrier medium for plasma reactions. The quartz glass tube is a transparent glass tube, and has an outer diameter of 16mm, an inner diameter of 14mm and a length of 200 mm.
Two sealing devices 12 are respectively connected to both ends of the silica glass tube 11, seal the silica glass tube 11, and are respectively placed at two grooves of the holder 17, thereby keeping the silica glass tube 11 horizontal. The sealing device 12 comprises a small cap 121 of tetrafluoro, a cap 122 of tetrafluoro glass tube, a large cap 123 of tetrafluoro, a fire gasket 124 of tetrafluoro, a large O-ring 125 and a sealing rubber ring 126.
The big tetrafluoro cap 123 is arranged on the outer wall of the quartz glass tube 11, the big O-shaped ring 125 is arranged in the big tetrafluoro cap 123 and sleeved on the outer wall of the quartz glass tube 11, the tetrafluoro fire gasket 124 is arranged in a gap between the big O-shaped ring 125 and the big tetrafluoro cap 123, the big tetrafluoro glass tube cap 122 is connected with the big tetrafluoro cap 123, the sealing rubber ring 126 is arranged in the small tetrafluoro cap 121, and the small tetrafluoro cap 121 is connected with the big tetrafluoro glass tube cap 122. The small tetrafluoro cap 121, the tetrafluoro glass tube cap 122, the big tetrafluoro cap 123, the tetrafluoro fire gasket 124, the big O-ring 125 and the sealing rubber ring 126 seal each part of the quartz glass tube 11, and prevent gas leakage.
The inner electrode assembly 13 includes an inner electrode 131 and two connection bars 132.
The internal electrode 131 has a screw-like structure and is disposed inside the quartz glass tube 11 with a diameter of 12 mm.
Two connecting rods 132 are connected to both ends of the inner electrode 131 and are inserted through the quartz glass tube 11, the tetrafluoro glass tube cap 122, and the tetrafluoro small cap 121, thereby fixing the inner electrode 131.
The total length of the inner electrode assembly 13 is 290mm, and the inner electrode 131 is 110 mm. The inner electrode 131 is connected to the positive electrode of the power supply through a connection rod 132.
Compared with the cylindrical structure, the inner electrode 131 with the thread-shaped structure can generate more high-energy electrons with higher energy level under the same condition, the catalyst distribution is more uniform, and CO is promoted2And (4) conversion rate.
The outer electrode 14 is of a diamond aluminum mesh structure, is arranged on the outer wall of the quartz glass tube 11, has the same length as the inner electrode 131, corresponds to the inner electrode 131, is connected with the negative electrode of a power supply, and is matched with the inner electrode 131 to generate an electric field to enable the reactant CO to be in a CO state2And H2Plasma reaction is carried out to generate a product CH4. The discharge frequency of the plasma reaction was 13kHz, the discharge voltage was 6kV, and the gas flow rate was 15 mL/min.
Compared with the conventional DBD plasma reactor, the DBD plasma reaction apparatus 10 in this embodiment enhances the edge effect due to the outer electrode 14 being separated outside the quartz glass tube 11, thereby forming a stronger local electric field, generating more electrons with higher energy in the discharge process, enhancing the electron impact dissociation process, and enhancing CO2And (4) conversion rate.
The air inlet 15 being arranged in a sealing arrangement12 and is communicated with the quartz glass tube 11 for introducing the reactant CO2And H2
An outlet port 16 is provided on the other sealing device 12 and communicates with the silica glass tube 11 for outputting the product CH4
The solar cell 20, i.e., a power source of the DBD plasma reaction device 10, supplies electric power to the DBD plasma reaction device 10 through a transformer. The solar cell 20 includes a solar energy converter 21 for absorbing solar energy outdoors and generating electric energy, and a storage battery 22 for storing the electric energy generated by the solar energy converter 21.
The water electrolysis apparatus 30 is for generating H through a water electrolysis process2The solar cell 20 also supplies electric power to the electrolyzed water apparatus 30 through a transformer.
Effects and effects of the embodiments
According to the DBD plasma reaction device and the CO conversion device of the embodiment2Compared with the traditional DBD plasma reactor, the DBD plasma reaction device has the advantages that the outer electrode is separated from the quartz glass tube, so that the edge effect is enhanced, and the inner electrode is in a thread structure, so that a stronger electric field is formed, and the CO of the plasma reaction is improved2And (4) conversion rate.
According to the DBD plasma reaction device and the CO conversion device of the embodiment2Compared with the conventional DBD plasma reactor, the plasma system of the embodiment relates to the conversion of CO2The plasma system combines the electric energy generated by the solar renewable energy source, one part of the electric energy is used for the DBD plasma reaction device to generate plasma, and the other part of the electric energy is used for electrolyzing water to produce hydrogen, so that the utilization rate of the renewable energy source is improved, and the electric energy-saving and environment-friendly effects are achieved.
The above embodiments are preferred examples of the present invention, and are not intended to limit the scope of the present invention.
The DBD plasma reaction device in this embodiment adopts a diamond-shaped aluminum mesh outer electrode, and the DBD plasma reaction device in the present invention may also adopt a coil outer electrode.

Claims (8)

1. A DBD plasma reaction apparatus connected to an external power supply, comprising:
a bracket placed on a horizontal plane;
the quartz glass tube is used for containing reactants of a plasma reaction and serving as a barrier medium of the plasma reaction;
the two sealing devices are respectively connected with two ends of the quartz glass tube, are used for sealing the quartz glass tube and are horizontally placed on the bracket together with the quartz glass tube;
the inner electrode assembly comprises an inner electrode and two connecting rods which are respectively connected to two ends of the inner electrode, the inner electrode is arranged in the quartz glass tube, the diameter of the inner electrode is smaller than that of the quartz glass tube, the connecting rods penetrate through the quartz glass tube and the sealing device and are used for fixing the inner electrode, and the inner electrode is connected with the positive electrode of the power supply through the connecting rods;
the outer electrode is arranged on the outer wall of the quartz glass tube, has the same length as the inner electrode, corresponds to the position of the inner electrode, is connected with the negative electrode of the power supply, and is used for being matched with the inner electrode to generate an electric field so as to enable the reactant to perform the plasma reaction to generate a product;
the gas inlet is arranged on one sealing device, is communicated with the quartz glass tube and is used for introducing the reactant; and
the gas outlet is arranged on the other sealing device, is communicated with the quartz glass tube and is used for outputting the product;
the inner electrode is in a thread structure, and the outer electrode is in a diamond aluminum mesh structure and is used for reinforcing an electric field between the inner electrode and the outer electrode, so that the conversion rate of the reaction gas is improved.
2. The DBD plasma reaction apparatus according to claim 1, wherein:
wherein the reactant is CO2And H2The product is CH4
3. The DBD plasma reaction apparatus according to claim 2, wherein:
wherein the discharge frequency of the plasma reaction is 0-60 kHz, the discharge voltage is 0-12 kV, and the gas flow rate is 50 mL/min.
4. The DBD plasma reaction apparatus according to claim 1, wherein:
wherein, the quartz glass tube has an outer diameter of 16mm, an inner diameter of 14mm and a length of 200 mm.
5. The DBD plasma reaction apparatus according to claim 1, wherein:
wherein, the total length of the inner electrode assembly is 290mm, and the length of the inner electrode is 100 mm.
6. Conversion of CO2The plasma system of (a), comprising:
DBD plasma reaction device for introducing CO2And H2Plasma reaction to generate CH4(ii) a And
a power supply for supplying electric power to the DBD plasma reaction device;
wherein the DBD plasma reaction apparatus is the DBD plasma reaction apparatus according to any one of claims 1 to 5.
7. A process for converting CO according to claim 62The plasma system of (2), further comprising:
an apparatus for electrolysis of water for generation of H by an electrolytic water process2And the power supply is also used for supplying electric energy to the water electrolysis equipment.
8. A process for converting CO according to claim 62The plasma system of (2), characterized in that:
the solar energy conversion system comprises a power supply, a solar energy converter and a storage battery, wherein the power supply is a solar cell, the solar cell comprises the solar energy converter and the storage battery, the solar energy converter is used for absorbing solar energy outdoors and generating electric energy, and the storage battery is used for storing the electric energy generated by the solar energy converter.
CN202110246652.3A 2021-03-05 2021-03-05 DBD plasma reaction device and CO conversion2Plasma system Pending CN113019117A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113740140A (en) * 2021-07-30 2021-12-03 淮浙电力有限责任公司凤台发电分公司 Method for acquiring failure risk level of ferrite steel welded joint for thermal power plant

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE202008012371U1 (en) * 2008-09-11 2008-12-04 Helmholtz-Zentrum Für Umweltforschung Gmbh - Ufz Apparatus for treating gases, in particular for drying natural gas or biogas
CN101344026A (en) * 2008-08-21 2009-01-14 上海交通大学 System for low temperature plasma pre-oxidizing NOx of auxiliary NH3-SCR fine purification diesel engine
CN105188246A (en) * 2015-11-02 2015-12-23 安徽理工大学 Online atmospheric air plasma array device powered by multiple power supplies
CN106495165A (en) * 2016-11-23 2017-03-15 亚洲硅业(青海)有限公司 A kind of device and method for preparing trichlorosilane with silicon tetrachloride
CN111186816A (en) * 2020-01-17 2020-05-22 西安交通大学 Plasma carbon sequestration system and method

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101344026A (en) * 2008-08-21 2009-01-14 上海交通大学 System for low temperature plasma pre-oxidizing NOx of auxiliary NH3-SCR fine purification diesel engine
DE202008012371U1 (en) * 2008-09-11 2008-12-04 Helmholtz-Zentrum Für Umweltforschung Gmbh - Ufz Apparatus for treating gases, in particular for drying natural gas or biogas
CN105188246A (en) * 2015-11-02 2015-12-23 安徽理工大学 Online atmospheric air plasma array device powered by multiple power supplies
CN106495165A (en) * 2016-11-23 2017-03-15 亚洲硅业(青海)有限公司 A kind of device and method for preparing trichlorosilane with silicon tetrachloride
CN111186816A (en) * 2020-01-17 2020-05-22 西安交通大学 Plasma carbon sequestration system and method

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113740140A (en) * 2021-07-30 2021-12-03 淮浙电力有限责任公司凤台发电分公司 Method for acquiring failure risk level of ferrite steel welded joint for thermal power plant
CN113740140B (en) * 2021-07-30 2024-03-22 淮浙电力有限责任公司凤台发电分公司 Failure risk grade acquisition method for ferritic steel welded joint for thermal power plant

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