CN110510576B - High-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method - Google Patents
High-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method Download PDFInfo
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Abstract
The invention relates to a thermochemical circulating electrolysis hydrogen production method of iodine and selenium, belonging to the technical field of hydrogen energy. Firstly, water is taken as a raw material, selenium and iodine are added, reaction is carried out under normal pressure to obtain selenious acid solution and hydroiodic acid, the hydroiodic acid is rectified and concentrated, the hydroiodic acid after rectification and concentration is decomposed, the hydrogen obtained by decomposition is output as a product, the iodine is recycled, the obtained selenious acid solution is decomposed by an electrolytic method to generate selenium, and the selenium is recycled as a raw material. The highest temperature required in the reaction process of the method is 400-. The reactants iodine and selenium in the method can be recycled, so that the production cost of hydrogen production is greatly reduced. The method can be well coupled with the latest clean energy high-temperature gas cooled reactor, and the heat energy, the electric energy and the mechanical energy of the high-temperature gas cooled reactor can be utilized by the iodine selenium thermochemical cycle hydrogen production process.
Description
Technical Field
The invention relates to a high-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method, and belongs to the technical field of hydrogen energy.
Background
Hydrogen energy is an ideal clean secondary energy, is widely distributed, does not produce pollution when being combusted, is more convenient to store and transport compared with electric power, can be directly used as fuel, and is increasingly paid attention to energy systems taking hydrogen energy as a core. The thermochemical cycle of splitting water to produce hydrogen is one of the most promising methods. The currently common thermochemical cycle hydrogen production method is sulfur-iodine cycle hydrogen production, and for example, chinese patent application (application publication No. CN104817057) discloses a thermochemical cycle hydrogen production method, which 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)
and (3) hydroiodic acid decomposition reaction:
2HI→H2+I2(T＝570-770K)
theoretically, water can be produced into hydrogen through thermal dissociation, but the reaction needs high temperature of more than 4000 ℃, the sulfur-iodine circulating hydrogen production method divides the decomposition reaction of the water into a plurality of steps, so that the reaction temperature can be reduced, the problem of hydrogen-oxygen separation can be avoided, and sulfur dioxide and iodine used in circulation can be recycled. The disadvantage of the sulfur-iodine cycle hydrogen production method is that the decomposition reaction of sulfuric acid still needs higher temperature, and is still in laboratory scale, and the energy consumption and heat consumption are very high. If large-scale hydrogen production is carried out, a stable heat source capable of providing high temperature is needed, and the heat source meeting the condition and capable of providing high-temperature stable large-scale engineering above 970K does not exist.
Disclosure of Invention
The invention aims to provide a high-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolytic hydrogen production method, which improves the existing thermochemical sulfur iodine cycle hydrogen production process to couple a high-temperature stable heat source and a high-temperature gas cooled reactor to realize large-scale hydrogen production.
The invention provides a high-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method, which comprises the following steps:
(1) taking water as a raw material, adding selenium and iodine, and reacting at normal pressure, wherein the molar ratio of the water to the selenium to the iodine is as follows: water, selenium and iodine, wherein the iodine is 1, (0.3-2) and (0.5-4), the reaction temperature is 20-30 ℃, the reaction time is 30-120min, selenious acid solution and hydroiodic acid are obtained by reaction, and the reaction equation is as follows:
3H2O+Se+2I2→H2SeO3+4HI
carrying out liquid-liquid separation on selenious acid solution and hydroiodic acid by using a liquid-liquid separation method to obtain selenious acid solution and hydroiodic acid;
(2) rectifying the hydroiodic acid obtained in the step (1), wherein the feeding temperature of a rectifying tower is the bubble point temperature, the pressure in the tower is 1.1-1.5MPa, and the reaction time is 10-50 min;
(3) decomposing the hydroiodic acid obtained in the step (2), wherein the pressure in a decomposition tower is 1.1-1.5MPa, the reaction temperature is 400-500 ℃, and the reaction temperature is during reactionThe time is 30-120min, and the product is H2And I2Hydrogen is output as a product, iodine is returned to the step (1) for recycling, and the chemical reaction equation is as follows:
2HI→H2+I2；
(4) and (2) electrolyzing the selenious acid solution in the step (1), taking the selenious acid solution as an electrolyte, taking the cathode and the anode of electrolysis as nickel sheets, and under the normal pressure, the reaction temperature is 10-210 ℃, the electrolysis voltage is 0.10-10V, the reaction time is 10-120min, separating out the selenium obtained by electrolysis at the cathode, and returning the selenium to the step (1) to be used as a raw material for recycling.
The method for producing hydrogen by high-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis has the characteristics and advantages that:
1. the method for producing hydrogen by high-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis needs the highest temperature of 400-500 ℃ in the reaction process, and avoids the problem that large-scale hydrogen production cannot be carried out due to overhigh reaction temperature.
2. The electrolytic hydrogen production method of the invention can recycle the reactants iodine and selenium, thereby greatly reducing the production cost of hydrogen production.
3. The invention relates to a method for preparing hydrogen by coupling a high-temperature gas cooled reactor with iodine selenium thermochemical cycle electrolysis, which couples the high-temperature gas cooled reactor with various chemical equipment of an iodine selenium thermochemical cycle system.
4. The invention relates to a high-temperature gas-cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method, which is used for coupling with a high-temperature gas-cooled reactor, wherein the high-temperature gas-cooled reactor can provide three forms of energy, namely heat energy, electric energy and mechanical energy, which can be utilized by the iodine selenium thermochemical cycle hydrogen production process. The heat energy generated by the high-temperature gas cooled reactor can be utilized in a gradient manner, the heat is transferred through the intermediate heat exchanger, the temperature gradients are set to be 700 ℃, 500 ℃, 300 ℃ and 100 ℃, the heat energy is fully utilized in such a manner, and the utilization rate of the heat energy can reach 99%. In addition, the electric energy generated by the high-temperature gas cooled reactor can be utilized in the subsequent iodine-selenium thermochemical cycle and used by electric equipment such as a motor, and the utilization rate of the electric energy can reach 30-50%. In addition, a large amount of steam generated by the high-temperature gas cooled reactor can also provide mechanical energy, and is directly coupled with a steam turbine in the iodine-selenium thermochemical circulating system, and the utilization efficiency can reach 90%.
5. The method for producing hydrogen by iodine selenium thermochemical cycle electrolysis by coupling the high-temperature gas cooled reactor is not limited to coupling the high-temperature gas cooled reactor, and other high-temperature heat sources can be coupled with the method for producing hydrogen by iodine selenium thermochemical cycle electrolysis.
Detailed Description
The invention provides a high-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method, which comprises the following steps:
(1) taking water as a raw material, adding selenium and iodine, and reacting at normal pressure, wherein the molar ratio of the water to the selenium to the iodine is as follows: water, selenium and iodine, wherein the iodine is 1, (0.3-2) and (0.5-4), the reaction temperature is 20-30 ℃, the reaction time is 30-120min, selenious acid solution and hydroiodic acid are obtained by reaction, and the reaction equation is as follows:
3H2O+Se+2I2→H2SeO3+4HI
carrying out liquid-liquid separation on selenious acid solution and hydroiodic acid by using a liquid-liquid separation method to obtain selenious acid solution and hydroiodic acid;
(2) rectifying the hydroiodic acid obtained in the step (1), wherein the feeding temperature of a rectifying tower is the bubble point temperature, the pressure in the tower is 1.1-1.5MPa, and the reaction time is 10-50 min;
(3) decomposing the hydroiodic acid obtained in the step (2), wherein the pressure in a decomposition tower is 1.1-1.5MPa, the reaction temperature is 400-500 ℃, the reaction time is 30-120min, and the product is H2And I2Hydrogen is output as a product, iodine is returned to the step (1) for recycling, and the chemical reaction equation is as follows:
2HI→H2+I2；
(4) and (2) electrolyzing the selenious acid solution in the step (1), taking the selenious acid solution as an electrolyte, taking the cathode and the anode of electrolysis as nickel sheets, and under the normal pressure, the reaction temperature is 10-210 ℃, the electrolysis voltage is 0.10-10V, the reaction time is 10-120min, separating out the selenium obtained by electrolysis at the cathode, and returning the selenium to the step (1) to be used as a raw material for recycling.
The following describes embodiments of the method of the invention:
example one
(1) Taking water as a raw material, adding selenium and iodine, and reacting at normal pressure, wherein the molar ratio of the water to the selenium to the iodine is as follows: selenium and iodine in water are 1:0.4:1, the reaction temperature is 25 ℃, the reaction time is 60min, the complete reaction mark is that no gas is generated, selenious acid solution and hydroiodic acid are obtained by reaction, and the reaction equation is as follows:
3H2O+Se+2I2→H2SeO3+4HI
the hydriodic acid and the selenious acid generated in the process are obviously layered due to different densities, wherein the hydriodic acid is on the upper layer, and the selenious acid solution is on the lower layer. Carrying out liquid-liquid separation on selenious acid solution and hydroiodic acid by using a liquid-liquid separation method to obtain selenious acid solution and hydroiodic acid;
(2) the hydroiodic acid obtained in the step (1) comprises the following components: i is2HI and H2O, mixed ternary solution is denoted as HIx solution. And (3) feeding the HIx solution into an HI rectification decomposition unit for rectification, wherein the feeding temperature of a rectification tower is the bubble point temperature, the pressure in the tower is 1.17MPa, and the reaction time is 30 min.
(3) Decomposing the hydroiodic acid rectified in the step (2), wherein the pressure in a decomposition tower is 1.17MPa, the reaction temperature is 480 ℃, the reaction time is 60min, and the product is H2And I2Outputting hydrogen as a product, and returning iodine to the step (1) for recycling; the chemical reaction principle of the process is shown as the following chemical reaction equation:
2HI→H2+I2
the high temperature environment in the step is provided by a high temperature gas cooled reactor, and high temperature steam of the high temperature gas cooled reactor is transmitted into a hydroiodic acid decomposition tower through a heat exchanger.
(4) And (2) electrolyzing the selenious acid solution in the step (1), taking the selenious acid solution as an electrolyte, taking the cathode and the anode of electrolysis as nickel sheets, and separating out the selenium obtained by electrolysis at the cathode under the conditions of normal pressure, reaction temperature of 25 ℃, electrolysis voltage of 0.9V and reaction time of 100 min. The selenium is returned to the step (1) to be used as a raw material for recycling.
Because the toxic substances selenium, selenious acid, the strong corrosive substances hydroiodic acid and the like participate in the steps (1), (2), (3) and (4), the equipment, the pipeline, the pump and the like need to be resistant to corrosion and have zero leakage, and the zero leakage is realized by using torque magnetic transmission in the process.
Example two
(1) Taking water as a raw material, adding selenium and iodine, and reacting at normal pressure, wherein the molar ratio of the water to the selenium to the iodine is as follows: selenium and iodine are mixed together at the ratio of 1:0.5:1.2, the reaction temperature is 28 ℃, the reaction time is 50min, the sign of complete reaction is that no gas is generated, selenious acid solution and hydroiodic acid are obtained by reaction, and the reaction equation is as follows:
3H2O+Se+2I2→H2SeO3+4HI
the hydriodic acid and the selenious acid generated in the process are obviously layered due to different densities, wherein the hydriodic acid is on the upper layer, and the selenious acid solution is on the lower layer. Carrying out liquid-liquid separation on selenious acid solution and hydroiodic acid by using a liquid-liquid separation method to obtain selenious acid solution and hydroiodic acid;
(2) the hydroiodic acid obtained in the step (1) comprises the following components: i is2HI and H2O, mixed ternary solution is denoted as HIx solution. And (3) feeding the HIx solution into an HI rectification decomposition unit for rectification, wherein the feeding temperature of a rectification tower is the bubble point temperature, the pressure in the tower is 1.2MPa, and the reaction time is 23 min.
(3) Decomposing the hydroiodic acid rectified in the step (2), wherein the pressure in a decomposition tower is 1.2MPa, the reaction temperature is 450 ℃, the reaction time is 55min, and the product is H2And I2Outputting hydrogen as a product, and returning iodine to the step (1) for recycling; the chemical reaction principle of the process is shown as the following chemical reaction equation:
2HI→H2+I2
the high temperature environment in the step is provided by a high temperature gas cooled reactor, and high temperature steam of the high temperature gas cooled reactor is transmitted into a hydroiodic acid decomposition tower through a heat exchanger.
(4) And (2) electrolyzing the selenious acid solution in the step (1), taking the selenious acid solution as an electrolyte, taking the cathode and the anode of electrolysis as nickel sheets, and separating out the selenium obtained by electrolysis at the cathode under normal pressure at the reaction temperature of 200 ℃, the electrolysis voltage of 5V and the reaction time of 30 min. The selenium is returned to the step (1) to be used as a raw material for recycling.
Because the toxic substances selenium, selenious acid, the strong corrosive substances hydroiodic acid and the like participate in the steps (1), (2), (3) and (4), the equipment, the pipeline, the pump and the like need to be resistant to corrosion and have zero leakage, and the zero leakage is realized by using torque magnetic transmission in the process.
EXAMPLE III
(1) Taking water as a raw material, adding selenium and iodine, and reacting at normal pressure, wherein the molar ratio of the water to the selenium to the iodine is as follows: selenium and iodine in water are 1:1:2, the reaction temperature is 28 ℃, the reaction time is 48min, the complete reaction mark is that no gas is generated, selenious acid solution and hydroiodic acid are obtained by reaction, and the reaction equation is as follows:
3H2O+Se+2I2→H2SeO3+4HI
the hydriodic acid and the selenious acid generated in the process are obviously layered due to different densities, wherein the hydriodic acid is on the upper layer, and the selenious acid solution is on the lower layer. Carrying out liquid-liquid separation on selenious acid solution and hydroiodic acid by using a liquid-liquid separation method to obtain selenious acid solution and hydroiodic acid;
(2) the hydroiodic acid obtained in the step (1) comprises the following components: i is2HI and H2O, mixed ternary solution is denoted as HIx solution. And (3) feeding the HIx solution into an HI rectification decomposition unit for rectification, wherein the feeding temperature of a rectification tower is the bubble point temperature, the pressure in the tower is 1.3MPa, and the reaction time is 20 min.
(3) Decomposing the hydroiodic acid rectified in the step (2), wherein the pressure in a decomposition tower is 1.3MPa, the reaction temperature is 450 ℃, the reaction time is 57min, and the product is H2And I2Outputting hydrogen as a product, and returning iodine to the step (1) for recycling; the chemical reaction principle of the process is shown as the following chemical reaction equation:
2HI→H2+I2
the high temperature environment in the step is provided by a high temperature gas cooled reactor, and high temperature steam of the high temperature gas cooled reactor is transmitted into a hydroiodic acid decomposition tower through a heat exchanger.
(4) And (2) electrolyzing the selenious acid solution in the step (1), taking the selenious acid solution as an electrolyte, taking the cathode and the anode of electrolysis as nickel sheets, and separating out the selenium obtained by electrolysis at the cathode under normal pressure at the reaction temperature of 100 ℃, the electrolysis voltage of 8V and the reaction time of 40 min. The selenium is returned to the step (1) to be used as a raw material for recycling.
Because the toxic substances selenium, selenious acid, the strong corrosive substances hydroiodic acid and the like participate in the steps (1), (2), (3) and (4), the equipment, the pipeline, the pump and the like need to be resistant to corrosion and have zero leakage, and the zero leakage is realized by using torque magnetic transmission in the process.
Claims (1)
1. A high-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method is characterized by comprising the following steps:
(1) taking water as a raw material, adding selenium and iodine, and reacting at normal pressure, wherein the molar ratio of the water to the selenium to the iodine is as follows: water, selenium and iodine, wherein the iodine is 1, (0.3-2) and (0.5-4), the reaction temperature is 20-30 ℃, the reaction time is 30-120min, selenious acid solution and hydroiodic acid are obtained by reaction, and the reaction equation is as follows:
3H2O+Se+2I2→H2SeO3+4HI
carrying out liquid-liquid separation on selenious acid solution and hydroiodic acid by using a liquid-liquid separation method to obtain selenious acid solution and hydroiodic acid;
(2) rectifying the hydroiodic acid obtained in the step (1), wherein the feeding temperature of a rectifying tower is the bubble point temperature, the pressure in the tower is 1.1-1.5MPa, and the reaction time is 10-50 min;
(3) decomposing the hydroiodic acid obtained in the step (2), wherein the pressure in a decomposition tower is 1.1-1.5MPa, the reaction temperature is 400-500 ℃, the reaction time is 30-120min, and the product is H2And I2Hydrogen is output as a product, iodine is returned to the step (1) for recycling, and the chemical reaction equation is as follows:
2HI→H2+I2；
(4) and (2) electrolyzing the selenious acid solution in the step (1), taking the selenious acid solution as an electrolyte, taking the cathode and the anode of electrolysis as nickel sheets, and under the normal pressure, the reaction temperature is 10-210 ℃, the electrolysis voltage is 0.10-10V, the reaction time is 10-120min, separating out the selenium obtained by electrolysis at the cathode, and returning the selenium to the step (1) to be used as a raw material for recycling.
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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 |
| 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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| CN110510576B (en) * | 2019-08-20 | 2020-12-11 | 中核能源科技有限公司 | High-temperature gas cooled reactor coupled iodine selenium thermochemical cycle electrolysis hydrogen production method |
| CN113526461A (en) * | 2020-04-17 | 2021-10-22 | 孟想 | Single selenium thermochemical cycle hydrogen production method |
| 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 |
| 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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| GB2601271A (en) | 2022-05-25 |
| GB202202726D0 (en) | 2022-04-13 |
| CN110510576A (en) | 2019-11-29 |
| GB2601271B (en) | 2024-04-17 |
| WO2021031964A1 (en) | 2021-02-25 |
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