CN110510576A - A kind of high temperature gas cooled reactor coupling iodine selenium thermochemical cycles electrolytic hydrogen production method - Google Patents
A kind of high temperature gas cooled reactor coupling iodine selenium thermochemical cycles electrolytic hydrogen production method Download PDFInfo
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- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
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Abstract
The present invention relates to a kind of iodine selenium thermochemical cycles electrolytic hydrogen production methods, belong to Hydrogen Technology field.First using water as raw material, selenium and iodine is added, it reacts under normal pressure, obtains selenous acid solution and hydroiodic acid, rectifying concentration is carried out to hydroiodic acid, hydroiodic acid after rectifying concentration is decomposed, obtained hydrogen is decomposed as output of products, iodine is recycled, and obtained selenous acid solution is decomposed by electrolysis method, selenium is generated, selenium is used as feedstock circulation.Maximum temperature needed for the reaction process of the method for the present invention is 400-500 DEG C, avoids the problem of big regular hydrogen manufacturing production can not be carried out because reaction temperature is excessively high.Reactant iodine and selenium in the method for the present invention, can recycle, therefore greatly reduce the production cost of hydrogen manufacturing.This method can be very good to couple with newest clean energy resource high temperature gas cooled reactor, and thermal energy, electric energy and the mechanical energy of high temperature gas cooled reactor can be utilized by iodine selenium thermochemical cycle for hydrogen production process.
Description
Technical field
The present invention relates to a kind of high temperature gas cooled reactor to couple iodine selenium thermochemical cycles electrolytic hydrogen production method, belongs to Hydrogen Technology neck
Domain.
Background technique
Hydrogen Energy is a kind of ideal cleaning secondary energy sources, and widely distributed, burning does not generate pollution, and relative to electricity
Power, hydrogen is more convenient for storing transport, and can be paid more and more attention directly as fuel by the energy system of core of Hydrogen Energy.Heat
Chemical cycle hydrogen production by water decomposition is one of most promising method.The method of thermochemical cycle for hydrogen production common at present is that sulphur iodine follows
Ring hydrogen manufacturing, if Chinese patent application (application publication number CN104817057) discloses a kind of method of thermochemical cycle for hydrogen production,
This method includes 3 chemical reactions, as follows:
Bunsen reaction:
SO2+I2+2H2O→2HI+H2SO4(T=290-390K)
Sulfuric acid decomposition reaction:
H2SO4→H2O+SO2+0.5O2(T=970-1270K)
Hydroiodic acid decomposition reaction:
2HI→H2+I2(T=570-770K)
Theoretically, water can be with hydrogen manufacturing by thermal dissociation, but reaction needs 4000 DEG C or more of high temperature, and sulphur iodine recycles hydrogen manufacturing
Method is that the decomposition reaction of water is divided into several steps, can not only reduce reaction temperature in this way, but can to avoid hydrogen-oxygen separation problem,
And sulfur dioxide used in recycling and iodine can be recycled.The shortcomings that sulphur iodine circulation silicol process is the decomposition of sulfuric acid
Reaction still needs higher temperature, and also in laboratory scale, the heat dissipation that consumes energy is very high.If extensive hydrogen manufacturing, needs
The stabilization heat source of high temperature can be provided, and such eligible high-temperature stable heavy construction for being capable of providing 970K temperature or more is hot
Source there is not yet.
Summary of the invention
The purpose of the present invention is to propose to a kind of high temperature gas cooled reactor to couple iodine selenium thermochemical cycles electrolytic hydrogen production method, to existing
Heat chemistry sulphur iodine circulation process for making hydrogen improve, with using being capable of providing the stabilization heat source of high temperature-high temperature gas cooled reactor progress
Coupling, realizes extensive hydrogen manufacturing.
High temperature gas cooled reactor proposed by the present invention couples iodine selenium thermochemical cycles electrolytic hydrogen production method, comprising the following steps:
(1) using water as raw material, selenium and iodine is added, reacts under normal pressure, the molar ratio of water, selenium and iodine are as follows: water: selenium: iodine=
1:(0.3-2): (0.5-4), reaction temperature are 20 DEG C -30 DEG C, reaction time 30-120min, and reaction obtains selenous acid solution
And hydroiodic acid, reaction equation are as follows:
3H2O+Se+2I2→H2SeO3+4HI
Using Liquid liquid Separation method, selenous acid solution and hydroiodic acid are subjected to Liquid liquid Separation, obtain selenous acid solution and hydrogen
Acid iodide；
(2) rectifying is carried out to the hydroiodic acid that step (1) obtains, rectifying column feeding temperature is bubble point temperature, and tower pressure interior force is
1.1-1.5MPa, reaction time 10-50min；
(3) hydroiodic acid obtained to step (2) decomposes, and decomposition tower pressure interior force is 1.1-1.5MPa, and reaction temperature is
400 DEG C -500 DEG C, reaction time 30-120min, product H2And I2, as output of products, iodine returns in step (1) hydrogen
It is recycled, chemical equation is as follows:
2HI→H2+I2；
(4) the selenous acid solution in step (1) is electrolysed, using selenous acid solution as electrolyte, the cathode of electrolysis and
Anode is nickel sheet, and under normal pressure, reaction temperature is 10 DEG C -210 DEG C, decomposition voltage 0.10V-10V, reaction time 10-
120min, the selenium being electrolysed are precipitated in cathode, and selenium is used as feedstock circulation to use back to step (1) is middle.
High temperature gas cooled reactor proposed by the present invention couples iodine selenium thermochemical cycles electrolytic hydrogen production method, and features and advantages are such as
Under:
1, high temperature gas cooled reactor of the invention couples iodine selenium thermochemical cycles electrolytic hydrogen production method, the highest temperature needed for reaction process
Degree is 400 DEG C -500 DEG C, avoids the problem of big regular hydrogen manufacturing production can not be carried out because reaction temperature is excessively high.
2, electrolytic hydrogen production method of the invention, reactant iodine and selenium therein, can recycle, therefore greatly reduce
The production cost of hydrogen manufacturing.
3, high temperature gas cooled reactor of the invention couples iodine selenium thermochemical cycles electrolytic hydrogen production method, utilizes high temperature gas cooled reactor and iodine
Each chemical industry equipment of selenium thermochemical cycles system couples, since reactant selenium, intermediate product selenous acid and hydroiodic acid belong to strong corruption
Corrosion or severe toxicity, therefore, equipment, pipeline and pump etc. need corrosion-resistant and zero leakage, use torque Magnetic drive realization zero in process
Leakage.
4, high temperature gas cooled reactor of the invention couples iodine selenium thermochemical cycles electrolytic hydrogen production method, is used for and high temperature gas cooled reactor coupling
It closes, and high temperature gas cooled reactor can provide the energy of three kinds of forms, i.e. thermal energy, electric energy and mechanical energy, can be followed by iodine selenium heat chemistry
Ring hydrogen production process is utilized.The thermal energy that high temperature gas cooled reactor generates can be with cascade utilization, and heat is transmitted by Intermediate Heat Exchanger, and is set
Setting temperature gradient is 700 DEG C, 500 DEG C, 300 DEG C and 100 DEG C, makes full use of thermal energy, the utilization rate of thermal energy in this way
It can reach 99%.In addition, high temperature gas cooled reactor itself generates electricity, the electric energy of generation be can also be used in subsequent iodine selenium thermochemical cycles, be
The electrical equipments such as motor are utilized, and utilization rate can also reach 30-50%.In addition, a large amount of steam that high temperature gas cooled reactor generates
It can provide mechanical energy, directly coupled with the steam turbine in iodine selenium thermochemical cycles system, utilization efficiency is up to 90%.
5, high temperature gas cooled reactor of the invention couples iodine selenium thermochemical cycles electrolytic hydrogen production method, is not limited to high temperature gas-cooled
Heap is coupled, other high temperature heat sources also can be used to be coupled with iodine selenium thermochemical cycles electrolytic hydrogen production method.
Specific embodiment
High temperature gas cooled reactor proposed by the present invention couples iodine selenium thermochemical cycles electrolytic hydrogen production method, comprising the following steps:
(1) using water as raw material, selenium and iodine is added, reacts under normal pressure, the molar ratio of water, selenium and iodine are as follows: water: selenium: iodine=
1:(0.3-2): (0.5-4), reaction temperature are 20 DEG C -30 DEG C, reaction time 30-120min, and reaction obtains selenous acid solution
And hydroiodic acid, reaction equation are as follows:
3H2O+Se+2I2→H2SeO3+4HI
Using Liquid liquid Separation method, selenous acid solution and hydroiodic acid are subjected to Liquid liquid Separation, obtain selenous acid solution and hydrogen
Acid iodide；
(2) rectifying is carried out to the hydroiodic acid that step (1) obtains, rectifying column feeding temperature is bubble point temperature, and tower pressure interior force is
1.1-1.5MPa, reaction time 10-50min；
(3) hydroiodic acid obtained to step (2) decomposes, and decomposition tower pressure interior force is 1.1-1.5MPa, and reaction temperature is
400 DEG C -500 DEG C, reaction time 30-120min, product H2And I2, as output of products, iodine returns in step (1) hydrogen
It is recycled, chemical equation is as follows:
2HI→H2+I2；
(4) the selenous acid solution in step (1) is electrolysed, using selenous acid solution as electrolyte, the cathode of electrolysis and
Anode is nickel sheet, and under normal pressure, reaction temperature is 10 DEG C -210 DEG C, decomposition voltage 0.10V-10V, reaction time 10-
120min, the selenium being electrolysed are precipitated in cathode, and selenium is used as feedstock circulation to use back to step (1) is middle.
The embodiment of the method for the present invention introduced below:
Embodiment one
(1) using water as raw material, selenium and iodine is added, reacts under normal pressure, the molar ratio of water, selenium and iodine are as follows: water: selenium: iodine=
1:0.4:1, reaction temperature are 25 DEG C, reaction time 60min, and the mark of fully reacting is no longer to generate gas, and reaction obtains
Selenous acid solution and hydroiodic acid, reaction equation are as follows:
3H2O+Se+2I2→H2SeO3+4HI
The hydroiodic acid of above-mentioned generation and selenous acid are obviously layered because of density difference, and hydroiodic acid is in upper layer, selenous acid solution
In lower layer.Using Liquid liquid Separation method, selenous acid solution and hydroiodic acid are subjected to Liquid liquid Separation, obtain selenous acid solution and hydrogen iodine
Acid；
It (2) include following components in the hydroiodic acid obtained to step (1): I2, HI and H2O, mixed ternary solution are denoted as
HIx solution.HIx solution, which enters in HI rectifying decomposition unit, carries out rectifying, and rectifying column feeding temperature is bubble point temperature, tower pressure interior force
For 1.17MPa, reaction time 30min.
(3) hydroiodic acid after step (2) rectifying is decomposed, decomposition tower pressure interior force is 1.17MPa, and reaction temperature is
480 DEG C, reaction time 60min, product H2And I2, as output of products, iodine is returned in step (1) and is recycled hydrogen；This
The chemical principle of process such as chemical equation is as follows:
2HI→H2+I2
Hot environment in this step, is provided by high temperature gas cooled reactor, and the high-temperature steam of high temperature gas cooled reactor is passed by heat exchanger
To hydroiodic acid decomposition tower.
(4) the selenous acid solution in step (1) is electrolysed, using selenous acid solution as electrolyte, the cathode of electrolysis and
Anode is nickel sheet, and under normal pressure, reaction temperature is 25 DEG C, decomposition voltage 0.9V, reaction time 100min and is electrolysed
Selenium is precipitated in cathode.Selenium will be returned in step (1) and use as feedstock circulation.
Since step (1), step (2), step (3), step (4) have extremely toxic substance selenium, selenous acid and strong corrosive material
The participation of the substances such as hydroiodic acid, therefore, equipment, pipeline and pump etc. need corrosion-resistant and zero leakage, will use torque magnetic in process
Transmission is to realize zero leakage.
Embodiment two
(1) using water as raw material, selenium and iodine is added, reacts under normal pressure, the molar ratio of water, selenium and iodine are as follows: water: selenium: iodine=
1:0.5:1.2, reaction temperature are 28 DEG C, reaction time 50min, and the mark of fully reacting is no longer to generate gas, are reacted
To selenous acid solution and hydroiodic acid, reaction equation is as follows:
3H2O+Se+2I2→H2SeO3+4HI
The hydroiodic acid of above-mentioned generation and selenous acid are obviously layered because of density difference, and hydroiodic acid is in upper layer, selenous acid solution
In lower layer.Using Liquid liquid Separation method, selenous acid solution and hydroiodic acid are subjected to Liquid liquid Separation, obtain selenous acid solution and hydrogen iodine
Acid；
It (2) include following components in the hydroiodic acid obtained to step (1): I2, HI and H2O, mixed ternary solution are denoted as
HIx solution.HIx solution, which enters in HI rectifying decomposition unit, carries out rectifying, and rectifying column feeding temperature is bubble point temperature, tower pressure interior force
For 1.2MPa, reaction time 23min.
(3) hydroiodic acid after step (2) rectifying is decomposed, decomposition tower pressure interior force is 1.2MPa, reaction temperature 450
DEG C, reaction time 55min, product H2And I2, as output of products, iodine is returned in step (1) and is recycled hydrogen；This mistake
The chemical principle of journey such as chemical equation is as follows:
2HI→H2+I2
Hot environment in this step, is provided by high temperature gas cooled reactor, and the high-temperature steam of high temperature gas cooled reactor is passed by heat exchanger
To hydroiodic acid decomposition tower.
(4) the selenous acid solution in step (1) is electrolysed, using selenous acid solution as electrolyte, the cathode of electrolysis and
Anode is nickel sheet, and under normal pressure, reaction temperature is 200 DEG C, decomposition voltage 5V, reaction time 30min, the selenium being electrolysed
It is precipitated in cathode.Selenium will be returned in step (1) and use as feedstock circulation.
Since step (1), step (2), step (3), step (4) have extremely toxic substance selenium, selenous acid and strong corrosive material
The participation of the substances such as hydroiodic acid, therefore, equipment, pipeline and pump etc. need corrosion-resistant and zero leakage, will use torque magnetic in process
Transmission is to realize zero leakage.
Embodiment three
(1) using water as raw material, selenium and iodine is added, reacts under normal pressure, the molar ratio of water, selenium and iodine are as follows: water: selenium: iodine=
1:1:2, reaction temperature are 28 DEG C, reaction time 48min, and the mark of fully reacting is no longer to generate gas, and reaction obtains Asia
Selenic acid solution and hydroiodic acid, reaction equation are as follows:
3H2O+Se+2I2→H2SeO3+4HI
The hydroiodic acid of above-mentioned generation and selenous acid are obviously layered because of density difference, and hydroiodic acid is in upper layer, selenous acid solution
In lower layer.Using Liquid liquid Separation method, selenous acid solution and hydroiodic acid are subjected to Liquid liquid Separation, obtain selenous acid solution and hydrogen iodine
Acid；
It (2) include following components in the hydroiodic acid obtained to step (1): I2, HI and H2O, mixed ternary solution are denoted as
HIx solution.HIx solution, which enters in HI rectifying decomposition unit, carries out rectifying, and rectifying column feeding temperature is bubble point temperature, tower pressure interior force
For 1.3MPa, reaction time 20min.
(3) hydroiodic acid after step (2) rectifying is decomposed, decomposition tower pressure interior force is 1.3MPa, reaction temperature 450
DEG C, reaction time 57min, product H2And I2, as output of products, iodine is returned in step (1) and is recycled hydrogen；This mistake
The chemical principle of journey such as chemical equation is as follows:
2HI→H2+I2
Hot environment in this step, is provided by high temperature gas cooled reactor, and the high-temperature steam of high temperature gas cooled reactor is passed by heat exchanger
To hydroiodic acid decomposition tower.
(4) the selenous acid solution in step (1) is electrolysed, using selenous acid solution as electrolyte, the cathode of electrolysis and
Anode is nickel sheet, and under normal pressure, reaction temperature is 100 DEG C, decomposition voltage 8V, reaction time 40min, the selenium being electrolysed
It is precipitated in cathode.Selenium will be returned in step (1) and use as feedstock circulation.
Since step (1), step (2), step (3), step (4) have extremely toxic substance selenium, selenous acid and strong corrosive material
The participation of the substances such as hydroiodic acid, therefore, equipment, pipeline and pump etc. need corrosion-resistant and zero leakage, will use torque magnetic in process
Transmission is to realize zero leakage.
Claims (1)
1. a kind of high temperature gas cooled reactor couples iodine selenium thermochemical cycles electrolytic hydrogen production method, it is characterised in that this method includes following step
It is rapid:
(1) using water as raw material, selenium and iodine is added, reacts under normal pressure, the molar ratio of water, selenium and iodine are as follows: water: selenium: iodine=1:
(0.3-2): (0.5-4), reaction temperature be 20 DEG C -30 DEG C, reaction time 30-120min, reaction obtain selenous acid solution and
Hydroiodic acid, reaction equation are as follows:
3H2O+Se+2I2→H2SeO3+4HI
Using Liquid liquid Separation method, selenous acid solution and hydroiodic acid are subjected to Liquid liquid Separation, obtain selenous acid solution and hydroiodic acid；
(2) rectifying is carried out to the hydroiodic acid that step (1) obtains, rectifying column feeding temperature is bubble point temperature, tower pressure interior force 1.1-
1.5MPa, reaction time 10-50min；
(3) hydroiodic acid obtained to step (2) decomposes, and decomposition tower pressure interior force is 1.1-1.5MPa, reaction temperature 400
DEG C -500 DEG C, reaction time 30-120min, product H2And I2, for hydrogen as output of products, iodine returns to circulation in step (1)
It uses, chemical equation is as follows:
2HI→H2+I2；
(4) the selenous acid solution in step (1) is electrolysed, using selenous acid solution as electrolyte, the cathode and anode of electrolysis
For nickel sheet, under normal pressure, reaction temperature is 10 DEG C -210 DEG C, decomposition voltage 0.10V-10V, reaction time 10-120min,
It is electrolysed obtained selenium to be precipitated in cathode, selenium is used as feedstock circulation to use back to step (1) is middle.
Priority Applications (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201910768032.9A CN110510576B (en) | 2019-08-20 | 2019-08-20 | High-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method |
| GB2202726.2A GB2601271B (en) | 2019-08-20 | 2020-08-13 | Method for producing hydrogen by means of iodine selenium thermochemical cycle electrolysis |
| PCT/CN2020/108768 WO2021031964A1 (en) | 2019-08-20 | 2020-08-13 | Method for producing hydrogen by means of iodine selenium thermochemical cycle electrolysis |
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| CN201910768032.9A CN110510576B (en) | 2019-08-20 | 2019-08-20 | High-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2021031964A1 (en) * | 2019-08-20 | 2021-02-25 | 中核能源科技有限公司 | Method for producing hydrogen by means of iodine selenium thermochemical cycle electrolysis |
| CN113401867A (en) * | 2021-07-20 | 2021-09-17 | 西安热工研究院有限公司 | Sulfur-iodine circulating hydrogen production system and method utilizing high-temperature gas cooled reactor |
| CN113526461A (en) * | 2020-04-17 | 2021-10-22 | 孟想 | Single selenium thermochemical cycle hydrogen production method |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116812865B (en) * | 2023-08-29 | 2023-12-05 | 浙江百能科技有限公司 | System and process for thermochemical selenium-iodine cyclic hydrogen production and simultaneous removal of CO in flue gas |
| CN117568848B (en) * | 2024-01-17 | 2024-04-02 | 浙江百能科技有限公司 | Device and method for producing hydrogen by electrolyzing hydroiodic acid |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2021031964A1 (en) * | 2019-08-20 | 2021-02-25 | 中核能源科技有限公司 | Method for producing hydrogen by means of iodine selenium thermochemical cycle electrolysis |
| GB2601271A (en) * | 2019-08-20 | 2022-05-25 | Chinergy Co Ltd | Method for producing hydrogen by means of iodine selenium thermochemical cycle electrolysis |
| GB2601271B (en) * | 2019-08-20 | 2024-04-17 | Chinergy Co Ltd | Method for producing hydrogen by means of iodine selenium thermochemical cycle electrolysis |
| CN113526461A (en) * | 2020-04-17 | 2021-10-22 | 孟想 | Single selenium thermochemical cycle hydrogen production method |
| CN113401867A (en) * | 2021-07-20 | 2021-09-17 | 西安热工研究院有限公司 | Sulfur-iodine circulating hydrogen production system and method utilizing high-temperature gas cooled reactor |
| CN113401867B (en) * | 2021-07-20 | 2023-10-31 | 西安热工研究院有限公司 | Sulfur-iodine circulating hydrogen production system and method by utilizing high-temperature gas cooled reactor |
Also Published As
| Publication number | Publication date |
|---|---|
| GB2601271A (en) | 2022-05-25 |
| GB202202726D0 (en) | 2022-04-13 |
| CN110510576B (en) | 2020-12-11 |
| GB2601271B (en) | 2024-04-17 |
| WO2021031964A1 (en) | 2021-02-25 |
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