CN110776941B - Biomass hydrogen production device and method with methane tri-reforming function - Google Patents
Biomass hydrogen production device and method with methane tri-reforming function Download PDFInfo
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 114
- 239000002028 Biomass Substances 0.000 title claims abstract description 84
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 82
- 239000001257 hydrogen Substances 0.000 title claims abstract description 81
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 73
- 238000002407 reforming Methods 0.000 title claims abstract description 36
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 33
- 238000000034 method Methods 0.000 title abstract description 18
- 239000007789 gas Substances 0.000 claims abstract description 107
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims abstract description 97
- 238000006243 chemical reaction Methods 0.000 claims abstract description 36
- 230000015572 biosynthetic process Effects 0.000 claims abstract description 32
- 238000003786 synthesis reaction Methods 0.000 claims abstract description 32
- 238000002309 gasification Methods 0.000 claims abstract description 31
- 238000005406 washing Methods 0.000 claims abstract description 25
- 238000001179 sorption measurement Methods 0.000 claims abstract description 23
- 238000000926 separation method Methods 0.000 claims abstract description 18
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 18
- 238000000746 purification Methods 0.000 claims abstract description 7
- 238000006057 reforming reaction Methods 0.000 claims abstract description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 28
- 239000002253 acid Substances 0.000 claims description 19
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 18
- 238000010521 absorption reaction Methods 0.000 claims description 18
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 15
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 12
- 229910052760 oxygen Inorganic materials 0.000 claims description 12
- 239000001301 oxygen Substances 0.000 claims description 12
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 11
- 239000001569 carbon dioxide Substances 0.000 claims description 11
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 10
- 238000003795 desorption Methods 0.000 claims description 10
- 229910052717 sulfur Inorganic materials 0.000 claims description 10
- 239000011593 sulfur Substances 0.000 claims description 10
- 229910052799 carbon Inorganic materials 0.000 claims description 9
- 150000002431 hydrogen Chemical class 0.000 claims description 9
- 229910052757 nitrogen Inorganic materials 0.000 claims description 9
- 239000012535 impurity Substances 0.000 claims description 8
- 230000008929 regeneration Effects 0.000 claims description 7
- 238000011069 regeneration method Methods 0.000 claims description 7
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 6
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 claims description 6
- 229910000037 hydrogen sulfide Inorganic materials 0.000 claims description 6
- 238000000629 steam reforming Methods 0.000 claims description 5
- 238000011084 recovery Methods 0.000 claims description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 3
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims description 3
- 229910021529 ammonia Inorganic materials 0.000 claims description 3
- 239000000446 fuel Substances 0.000 claims description 3
- DOTMOQHOJINYBL-UHFFFAOYSA-N molecular nitrogen;molecular oxygen Chemical compound N#N.O=O DOTMOQHOJINYBL-UHFFFAOYSA-N 0.000 claims description 3
- 230000002000 scavenging effect Effects 0.000 claims description 2
- 239000005864 Sulphur Substances 0.000 claims 1
- 230000008569 process Effects 0.000 abstract description 7
- 238000005265 energy consumption Methods 0.000 abstract description 4
- 230000009467 reduction Effects 0.000 abstract description 2
- 238000012824 chemical production Methods 0.000 abstract 1
- 238000004064 recycling Methods 0.000 abstract 1
- 239000002994 raw material Substances 0.000 description 10
- 239000000047 product Substances 0.000 description 8
- 239000006200 vaporizer Substances 0.000 description 6
- 239000003054 catalyst Substances 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 238000004088 simulation Methods 0.000 description 3
- 241000209140 Triticum Species 0.000 description 2
- 235000021307 Triticum Nutrition 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000001833 catalytic reforming Methods 0.000 description 2
- 239000003245 coal Substances 0.000 description 2
- 230000018109 developmental process Effects 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 239000010902 straw Substances 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 230000000295 complement effect Effects 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 239000003502 gasoline Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 238000009834 vaporization Methods 0.000 description 1
- 230000008016 vaporization Effects 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
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Abstract
Description
（一）技术领域(1) Technical field
本发明涉及生物质能源的开发和应用领域，特别涉及一种带有甲烷三重整的生物质制氢装置及方法。The invention relates to the development and application fields of biomass energy, in particular to a biomass hydrogen production device and method with triple reforming of methane.
（二）背景技术(2) Background technology
每单位质量的氢气释放出的热量是每单位质量汽油的三倍，且氢气燃烧的最终产物只有水，可被认为是一种绝对清洁的燃料，因此，长期以来被认为是一种有潜力取代化石燃料的清洁能源。其中，制氢技术是氢能利用最重要的技术环节。The heat released per unit mass of hydrogen is three times that of gasoline per unit mass, and the final product of hydrogen combustion is only water, which can be considered as an absolutely clean fuel. Therefore, it has long been regarded as a potential replacement for Clean energy from fossil fuels. Among them, hydrogen production technology is the most important technical link of hydrogen energy utilization.
生物质资源分布广、储量大，地球上每年生长的生物质总量约1400亿-1800亿t(吨)，相当于目前世界总能耗的10倍。生物质自身是氢的载体，其中包含的氢元素的重量组分约为6%，相当于每千克生物质可产生约0.672m 3的气态氢，占生物质总能量的40%以上。与其他能源相比，生物质具有挥发分高、炭活性强、硫、氮含量低、灰分小、燃烧时对环境污染小等特点，被喻为绿色煤炭。因此，无论从能源角度还是环境角度，发展生物质制氢技术都具有积极和重要的意义。Biomass resources are widely distributed and have large reserves. The total amount of biomass grown on the earth each year is about 140 billion to 180 billion t (tons), which is equivalent to 10 times the current world's total energy consumption. Biomass itself is the carrier of hydrogen, which contains about 6% hydrogen by weight, which is equivalent to about 0.672m3 of gaseous hydrogen per kilogram of biomass, accounting for more than 40% of the total biomass energy. Compared with other energy sources, biomass has the characteristics of high volatile content, strong carbon activity, low sulfur and nitrogen content, low ash content, and low environmental pollution when burned, and is known as green coal. Therefore, the development of biomass hydrogen production technology is of positive and important significance from both an energy perspective and an environmental perspective.
生物质制氢新方法不仅可以通过控制组分进料比来调节合成气产物比，并且可以实现系统的自供热，将CO2回收利用，提高氢气产率，降低能耗，因此受到人们的高度重视和广泛关注。The new method of biomass hydrogen production can not only adjust the ratio of synthesis gas products by controlling the ratio of components to feed, but also can realize the self-heating of the system, recycle CO2 , improve the hydrogen production rate, and reduce energy consumption, so it is popular among people. Highly regarded and widely concerned.
专利（CN1214972C）公开了一种生物质下吸式气化炉催化制氢方法，对生物质气化制燃气催化从而制的富氢气体。这些方法实现了制备高纯度氢，但也存在着很多问题，比如生物质催化重整制氢方法需要寻求高效的催化剂及催化剂反应器，同时催化重整制氢中催化剂本身也有催化剂失活的难题需要解决。The patent (CN1214972C) discloses a method for catalyzing hydrogen production in a biomass downdraft gasifier, which is a hydrogen-rich gas produced by catalyzing biomass gasification to produce gas. These methods achieve the production of high-purity hydrogen, but there are also many problems. For example, the method of producing hydrogen by catalytic reforming of biomass requires the search for efficient catalysts and catalyst reactors. At the same time, the catalyst itself in the production of hydrogen by catalytic reforming also has the problem of catalyst deactivation. needs to be resolved.
专利（CN1292979C）公开了一种煤与生物质共超临界水催化气化制氢装置及方法，使得气体产物中氢气含量升高，而且使气体产物中二氧化碳的浓度提高，二氧化碳容易被分离出来并进行处理，从而实现二氧化碳零排放制氢。但这种方法对于反应器和反应条件较为苛刻，系统控制较为复杂。Patent (CN1292979C) discloses a hydrogen production device and method by co-supercritical water catalytic gasification of coal and biomass, which increases the hydrogen content in the gas product, and increases the concentration of carbon dioxide in the gas product, so that the carbon dioxide can be easily separated and eliminated. Processed to achieve zero carbon dioxide emission hydrogen production. However, this method is relatively harsh for the reactor and reaction conditions, and the system control is relatively complicated.
（三）发明内容(3) Contents of the invention
本发明的目的是提供一种带有甲烷三重整的生物质制氢新方法。The purpose of the present invention is to provide a new method for producing hydrogen from biomass with triple reforming of methane.
本发明的另一个目的是提供一种环境友好、成本低、工艺简单的生物质制氢的装置。此装置集生物质热解、气化、重整过程于一体，气化产物中氢气含量高，焦油含量少，并可将CO2回收利用，对建立可持续的能源系统具有重要的意义。Another object of the present invention is to provide an environment-friendly, low-cost and simple process for producing hydrogen from biomass. This device integrates biomass pyrolysis, gasification, and reforming processes. The gasification product has high hydrogen content, low tar content, and can recycle CO2 , which is of great significance to the establishment of a sustainable energy system.
本发明是通过如下技术方案实现的：The present invention is achieved through the following technical solutions:
一种带有甲烷三重整的生物质制氢装置，包括连接生物质送料管的生物质预处理单元，其特征在于：所述生物质预处理单元通过管道依次连接EFB汽化炉、甲烷三重整单元、水煤气转换单元、低温甲醇洗单元和变压吸附单元，空分单元通过氮气管连通生物质预处理单元并通过氧气管连通EFB汽化炉。A biomass hydrogen production device with methane triple reforming, comprising a biomass pretreatment unit connected to a biomass feeding pipe, characterized in that: the biomass pretreatment unit is sequentially connected to an EFB vaporizer and a methane triple reforming unit through a pipeline. , water gas conversion unit, low temperature methanol washing unit and pressure swing adsorption unit, the air separation unit is connected to the biomass pretreatment unit through a nitrogen pipe and is connected to the EFB vaporizer through an oxygen pipe.
本发明的更优技术方案为：The more optimal technical scheme of the present invention is:
所述EFB汽化炉、甲烷三重整单元、水煤气转换单元上均连通有水蒸气管，实现装置内部混合气的水蒸气洗涤。The EFB gasification furnace, the methane triple reforming unit, and the water-gas conversion unit are all connected with a steam pipe, so as to realize the steam washing of the mixed gas in the device.
所述空分单元包括依次连通的膨胀机和氮氧分离塔；甲烷三重整单元包括串联的甲烷水蒸气重整反应器和平推流反应器；水煤气转换单元为固定床反应器；变压吸附单元为吸收塔。The air separation unit includes an expander and a nitrogen-oxygen separation tower connected in sequence; the methane triple-reforming unit includes a series-connected methane steam reforming reactor and a plug flow reactor; the water-gas conversion unit is a fixed-bed reactor; a pressure swing adsorption unit for the absorption tower.
所述低温甲醇洗单元包括串联的酸性气体吸收塔、CO2解析塔、H2S富集塔和甲醇再生塔，对酸性气体、二氧化碳、硫化氢和甲醇进行回收处理，实现合成气的提纯。The low-temperature methanol washing unit includes an acid gas absorption tower, a CO 2 desorption tower, an H 2 S enrichment tower and a methanol regeneration tower connected in series, and recovers the acid gas, carbon dioxide, hydrogen sulfide and methanol to realize the purification of synthesis gas.
所述CO2解析塔通过二氧化碳输送管、变压吸附单元通过甲烷输送管分别连接甲烷三重整单元；H2S富集塔通过硫化氢输送管连接克劳斯单元，实现回收废气的利用。The CO 2 desorption tower is respectively connected to the methane triple reforming unit through the carbon dioxide conveying pipe and the pressure swing adsorption unit through the methane conveying pipe; the H 2 S enrichment tower is connected to the Claus unit through the hydrogen sulfide conveying pipe, so as to realize the utilization of recovered waste gas.
所述克劳斯单元为硫磺回收装置，将硫化氢转化为硫磺进行回收。The Claus unit is a sulfur recovery device, which converts hydrogen sulfide into sulfur for recovery.
采用上述装置进行生物质制氢的方法，包括如下步骤：The method for producing hydrogen from biomass by using the above-mentioned device comprises the following steps:
（1）空分单元为EFB汽化炉提供高纯度氧气，并为生物质预处理单元提供高纯度氮气用于装置内部的扫气，生物质为燃料进入EFB汽化炉反应得到生物质粗合成气，并经水蒸气洗涤得到生物质气化气；(1) The air separation unit provides high-purity oxygen for the EFB vaporizer, and provides high-purity nitrogen for the biomass pretreatment unit for scavenging inside the device. And through steam washing to obtain biomass gasification gas;
（2）生物质气化气送入甲烷三重整单元，将其中的甲烷、二氧化碳进一步转化为一氧化碳和氢气，之后送入水煤气转换单元，使得到的气体的氢碳比具有可调性；(2) The biomass gasification gas is sent to the methane triple reforming unit, and the methane and carbon dioxide therein are further converted into carbon monoxide and hydrogen, and then sent to the water-gas conversion unit, so that the hydrogen-carbon ratio of the obtained gas is adjustable;
（3）合成气体在送入低温甲醇洗单元进行提纯，净化后的合成气送入变压吸附单元进行氢气分离，得到甲烷和氢气。(3) The synthesis gas is sent to the low temperature methanol washing unit for purification, and the purified synthesis gas is sent to the pressure swing adsorption unit for hydrogen separation to obtain methane and hydrogen.
根据本发明的另一优选实施方式，EFB汽化炉中的气化温度为1200-1300℃；氧气当量比为0.35-0.45；所述水蒸气与所述生物质的质量比为0.5-0.7，水蒸气洗涤后去除生物质粗合成气中的焦油、苯酚、氨杂质，上述杂质经底部释放管排出；所述水煤气转换单元温度为250-300℃；压力为3.5-4MPa，所述低温甲醇洗单元温度为-50--60℃，理论塔板数为35块。According to another preferred embodiment of the present invention, the gasification temperature in the EFB gasification furnace is 1200-1300°C; the oxygen equivalence ratio is 0.35-0.45; the mass ratio of the water vapor to the biomass is 0.5-0.7, the water After steam washing, the tar, phenol and ammonia impurities in the crude synthesis gas of biomass are removed, and the above impurities are discharged through the bottom release pipe; the temperature of the water-gas conversion unit is 250-300 ° C; the pressure is 3.5-4MPa, and the low-temperature methanol washing unit The temperature is -50--60℃, and the number of theoretical plates is 35.
根据本发明的另一优选实施方式，三重整反应是在800℃左右反应温度下的常压反应，氢碳比可在1.5-2.5范围内调节。According to another preferred embodiment of the present invention, the triple reforming reaction is a normal pressure reaction at a reaction temperature of about 800°C, and the hydrogen-carbon ratio can be adjusted within the range of 1.5-2.5.
根据本发明的另一优选实施方式，甲烷三重整单元中进行氢碳元素互补，能量匹配，匹配后的混合气中氢气摩尔分数为31.34%，送入水煤气转换单元，转化后的合成气中氢气摩尔分数为58.52%，低温甲醇洗单元净化后的合成气中氢气摩尔分数为97.32%，变压吸附单元分离出产品氢中氢气摩尔分数为99.96%。According to another preferred embodiment of the present invention, the hydrogen and carbon elements are complemented in the methane triple reforming unit, and the energy is matched, and the hydrogen mole fraction in the matched mixed gas is 31.34%, which is sent to the water-gas conversion unit, and the hydrogen in the reformed synthesis gas is hydrogen. The mole fraction is 58.52%, the mole fraction of hydrogen in the synthesis gas purified by the low temperature methanol washing unit is 97.32%, and the mole fraction of hydrogen in the product hydrogen separated by the pressure swing adsorption unit is 99.96%.
低温甲醇洗单元中，酸性气体吸收塔吸收酸性气体，CO2解析塔对酸性气体进行分析、脱除CO2，并将CO2送回甲烷三重整单元；H2S富集塔将H2S气体分离富集后送入克劳斯单元生产硫磺，甲醇再生塔将回收的吸甲醇送回酸性气体吸收塔；变压吸附单元分离出的甲烷送回甲烷三重整单元。In the low temperature methanol washing unit, the acid gas absorption tower absorbs the acid gas, the CO 2 desorption tower analyzes the acid gas, removes CO 2 , and sends the CO 2 back to the methane triple reforming unit; the H 2 S enrichment tower removes the H 2 S After the gas is separated and enriched, it is sent to the Claus unit to produce sulfur. The methanol regeneration tower sends the recovered absorbed methanol back to the acid gas absorption tower; the methane separated by the pressure swing adsorption unit is sent back to the methane triple reforming unit.
本发明与现有技术相比，主要有以下有益效果：Compared with the prior art, the present invention mainly has the following beneficial effects:
在生物质制氢过程中集成甲烷三重整反应，可实现近零CO2排放，大量节约能耗，甲烷三重整反应可将CO2回收利用，对建立可持续的能源系统，促进国民经济发展和保护生态环境具有重要的意义；The methane triple-reforming reaction is integrated in the process of biomass hydrogen production, which can achieve nearly zero CO 2 emissions and save a lot of energy. It is of great significance to protect the ecological environment;
氢气产率提高，可副产蒸汽、硫磺等产品，提高了生物质制氢技术的经济性。The hydrogen yield is increased, and products such as steam and sulfur can be by-produced, which improves the economy of biomass hydrogen production technology.
（四）附图说明(4) Description of drawings
下面结合附图对本发明作进一步的说明。The present invention will be further described below in conjunction with the accompanying drawings.
图1为本发明的设备工艺连接示意图。FIG. 1 is a schematic diagram of equipment process connection of the present invention.
图中，U1生物质预处理单元，U2空分单元，U3 EFB汽化炉，U4甲烷三重整单元，U5水煤气转换单元，U6低温甲醇洗单元，U7克劳斯单元，U8变压吸附单元，1生物质送料管，2空气管，3氮气管，4氧气管，5水蒸气管，6杂质输送管，7合成气管路，8净化气管路，9硫化氢输送管，10硫磺输送管，11氢气管，12二氧化碳输送管，13甲烷输送管。In the figure, U1 biomass pretreatment unit, U2 air separation unit, U3 EFB gasification furnace, U4 methane triple reforming unit, U5 water gas conversion unit, U6 low temperature methanol washing unit, U7 Claus unit, U8 pressure swing adsorption unit, 1 Biomass Feeding Pipe, 2 Air Pipe, 3 Nitrogen Pipe, 4 Oxygen Pipe, 5 Water Vapor Pipe, 6 Impurity Delivery Pipe, 7 Syngas Pipeline, 8 Purified Gas Pipeline, 9 Hydrogen Sulfide Delivery Pipe, 10 Sulfur Delivery Pipe, 11 Hydrogen Gas Pipe pipe, 12 carbon dioxide delivery pipes, 13 methane delivery pipes.
（五）具体实施方式(5) Specific implementation methods
附图为本发明的一种具体实施例。该实施例The accompanying drawing is a specific embodiment of the present invention. this example
以下结合附图进一步说明，并非限制本发明所涉及的范围。The following further description in conjunction with the accompanying drawings does not limit the scope of the present invention.
实施例1：一种带有甲烷三重整的生物质制氢装置Example 1: A biomass hydrogen production device with triple reforming of methane
该生物质制氢装置包括连接生物质送料管1的生物质预处理单元U1，生物质预处理单元U1通过管道依次连接EFB汽化炉U3、甲烷三重整单元U4、水煤气转换单元U5、低温甲醇洗单元U6和变压吸附单元U8，空分单元U2通过氮气管3连通生物质预处理单元U1并通过氧气管4连通EFB汽化炉U3。The biomass hydrogen production device includes a biomass pretreatment unit U1 connected to the
上述EFB汽化炉U3、甲烷三重整单元U4、水煤气转换单元U5上均连通有水蒸气管5；上述空分单元U2包括依次连通的膨胀机和氮氧分离塔；甲烷三重整单元U4包括串联的甲烷水蒸气重整反应器和平推流反应器；水煤气转换单元U5为固定床反应器；变压吸附单元U8为吸收塔；上述低温甲醇洗单元U6包括串联的酸性气体吸收塔、CO2解析塔、H2S富集塔和甲醇再生塔；上述CO2解析塔通过二氧化碳输送管12、变压吸附单元U8通过甲烷输送管13分别连接甲烷三重整单元U4；H2S富集塔通过硫化氢输送管9连接克劳斯单元U7；上述克劳斯单元U7为硫磺回收装置。Above-mentioned EFB vaporizer U3, methane triple reforming unit U4, water-gas conversion unit U5 are all communicated with
空分单元U2提供高纯度的氧气（99.5mol%）经氧气管4用作EFB汽化炉U3的氧化剂，提供高纯度氮气经氮气管3用作低温精馏装置中的汽提气或者生物质处理装置中的扫气；生物质为燃料进入EFB汽化炉U3反应得到生物质粗合成气；主要含有CO、CO2、H2、H2O和CH4，生物质粗合成气经水蒸气管5中水蒸气洗涤，经杂质输送管6去除焦油、苯酚、氨等杂质。甲烷三重整单元U4将生物质气化气中的CH4、CO2进一步转化为CO和H2，氢碳元素互补，能量匹配，达到制氢生产过程节能减排的目的，之后进入水煤气转换单元U5，使得反应出口得到的气体的氢碳比具有可调节性，合成气体中含有大量的杂质气体。因此，合成气体经合成气管路7进入低温甲醇洗单元U6进行下一步提纯，酸性气体吸收塔吸收酸性气体，CO2解析塔对酸性气体进行分析，将稀甲醇返回酸性气体吸收塔回收甲醇。净化后的合成气经净化气管路8送入变压吸附单元U8进行氢气分离得到甲烷和氢气，氢气经氢气管11导出；酸性气体净化单元脱除的CO2和变压吸附单元U8分离出的甲烷经二氧化碳输送管12、甲烷输送管13进入甲烷三重整单元U4生成三重整合成气，低温甲醇器单元U6分离出的富H2S气体经硫化氢输送管9送入克劳斯单元U7生产硫磺，经硫磺输送管10送出。The air separation unit U2 provides high-purity oxygen (99.5mol%) through the
实施例2：一种带有甲烷三重整的生物质制氢方法Embodiment 2: A kind of biomass hydrogen production method with methane triple reforming
本工艺以小麦秸秆为原料，原料消耗率为10.99t/h。第一步是对原料进行粉碎预处理，然后将粉碎后的原料与O2一起送入EFB汽化炉U3进行气化反应得到生物质粗合成气；主要含有CO、CO2、H2、H2O和CH4，气化温度为1300℃，氧气当量比为0.39，EFB汽化炉U3中的生物质粗合成气冷却后离开气化炉，产生一定量的高压蒸汽；为了增加氢气的含量，生物质粗合成气升温后进入水煤气转换单元U5进行下一步反应，CO通过水煤气转换单元U5转化为CO2，水蒸气与生物质的质量比为0.65，水煤气转换单元U5温度为280℃，压力为3.8MPa，压降为0.05MPa；然后转化合成气温度降低到-58℃后送到低温甲醇洗单元U6，吸收塔塔板数为35块，塔板压降0.015MPa, 选用PC-SAFT方程对低温甲醇洗单元进行建模，酸性气体吸收塔、CO2解吸塔、甲醇再生塔都选用RadFrac模块，选用RK-Soave方程对变压吸附单元(U8)进行建模，吸附塔选用Sep模块。This process uses wheat straw as raw material, and the raw material consumption rate is 10.99t/h. The first step is to pulverize the raw materials, and then send the pulverized raw materials together with O 2 to the EFB gasification furnace U3 for gasification reaction to obtain crude biomass synthesis gas; mainly contains CO, CO 2 , H 2 , H 2 O and CH 4 , the gasification temperature is 1300°C, and the oxygen equivalence ratio is 0.39. The biomass crude synthesis gas in EFB gasifier U3 is cooled and leaves the gasifier to generate a certain amount of high-pressure steam; in order to increase the hydrogen content, the After heating up, the crude synthesis gas enters the water-gas conversion unit U5 for the next reaction, CO is converted into CO 2 through the water-gas conversion unit U5, the mass ratio of water vapor to biomass is 0.65, the temperature of the water-gas conversion unit U5 is 280 ℃, and the pressure is 3.8 MPa, the pressure drop is 0.05MPa; then the temperature of the converted synthesis gas is lowered to -58°C and sent to the low-temperature methanol washing unit U6, the number of absorption tower plates is 35, and the pressure drop of the plate is 0.015MPa. The methanol washing unit is modeled, and the acid gas absorption tower, CO 2 desorption tower, and methanol regeneration tower all use the RadFrac module, and the RK-Soave equation is used to model the pressure swing adsorption unit (U8), and the adsorption tower uses the Sep module.
在甲烷三重整单元(U4)中的主要反应如下：The main reactions in the methane triple reforming unit (U4) are as follows:
甲烷干重整（DMR）：
甲烷水蒸气重整（SMR）：
甲烷部分氧化（MPO）：
模拟结果如表1所示：The simulation results are shown in Table 1:
经过模拟，生物质制氢工艺原料消耗量为10.99t/h，年制氢90000000Nm3，粗合成气氢气摩尔分数为22.90%，转化合成气氢气摩尔分数为53.48%，净化气中氢气摩尔分数为98.17%，产品氢中氢气摩尔分数为99.97%。After simulation, the raw material consumption of the biomass hydrogen production process is 10.99t/h, the annual hydrogen production is 90,000,000Nm 3 , the hydrogen mole fraction of the crude synthesis gas is 22.90%, the hydrogen mole fraction of the converted synthesis gas is 53.48%, and the hydrogen mole fraction in the purified gas is 98.17%, and the hydrogen mole fraction in the product hydrogen is 99.97%.
实施例3：一种带有甲烷三重整的生物质制氢方法Embodiment 3: a kind of biomass hydrogen production method with methane triple reforming
本工艺以小麦秸秆为原料，原料消耗率为10.99t/h。第一步是对原料进行粉碎预处理，然后将粉碎后的原料与O2一起送入EFB汽化炉U3进行气化反应得到生物质粗合成气；主要含有CO、CO2、H2、H2O和CH4，具体含量如表2所示，气化温度为1000℃，氧气当量比为0.39，EFB汽化炉U3中的生物质粗合成气冷却后离开气化炉，产生一定量的高压蒸汽；为了增加氢气的含量，生物质粗合成气升温后进入水煤气转换单元U5进行下一步反应，CO通过水煤气转换单元U5转化为CO2，水蒸气与生物质的质量比为0.65， 水煤气转换单元U5温度为280℃，压力为3.8MPa，压降为0.05MPa；然后转化合成气温度降低到-58℃后送到低温甲醇洗单元U6，吸收塔塔板数为35块，塔板压降0.015MPa, 选用PC-SAFT方程对低温甲醇洗单元进行建模，酸性气体吸收塔、CO2解吸塔、甲醇再生塔都选用RadFrac模块，选用RK-Soave方程对变压吸附单元(U8)进行建模，吸附塔选用Sep模块。This process uses wheat straw as raw material, and the raw material consumption rate is 10.99t/h. The first step is to pulverize the raw materials, and then send the pulverized raw materials together with O 2 to the EFB gasification furnace U3 for gasification reaction to obtain crude biomass synthesis gas; mainly contains CO, CO 2 , H 2 , H 2 The specific contents of O and CH 4 are shown in Table 2. The gasification temperature is 1000°C, and the oxygen equivalence ratio is 0.39. The biomass crude synthesis gas in the EFB gasifier U3 is cooled and leaves the gasifier to generate a certain amount of high-pressure steam. ; In order to increase the hydrogen content, the biomass crude synthesis gas is heated and then enters the water-gas conversion unit U5 for the next reaction, CO is converted into CO 2 through the water-gas conversion unit U5, the mass ratio of water vapor to biomass is 0.65, and the water-gas conversion unit U5 The temperature is 280°C, the pressure is 3.8MPa, and the pressure drop is 0.05MPa; then the temperature of the converted synthesis gas is lowered to -58°C and sent to the low-temperature methanol washing unit U6, the number of absorption tower plates is 35, and the pressure drop of the plate is 0.015MPa , The PC-SAFT equation is used to model the low-temperature methanol washing unit, the acid gas absorption tower, CO 2 desorption tower, and methanol regeneration tower are all selected from the RadFrac module, and the RK-Soave equation is used to model the pressure swing adsorption unit (U8), The adsorption tower selects the Sep module.
经过模拟，生物质制氢工艺原料消耗量为10.99t/h，年制氢89991000Nm3，粗合成气氢气摩尔分数为20.45%，转化合成气氢气摩尔分数为52.51%，净化气中氢气摩尔分数为97.24%，产品氢中氢气摩尔分数为99.96%。After simulation, the raw material consumption of the biomass hydrogen production process is 10.99t/h, the annual hydrogen production is 89991000Nm 3 , the hydrogen mole fraction of the crude synthesis gas is 20.45%, the hydrogen mole fraction of the converted synthesis gas is 52.51%, and the hydrogen mole fraction in the purified gas is 97.24%, and the hydrogen mole fraction in the product hydrogen is 99.96%.
以上所述的具体实施例，对本发明的目的、技术方案和有益效果进行了进一步详细说明，所应理解的是，以上所述仅为本发明的具体实施例而已，并不用于限制本发名，凡在本发明的精神和原则之内，所做的任何修改、等同替换、改进，均应包含在本发明的保护范围之内。The specific embodiments described above further describe the purpose, technical solutions and beneficial effects of the present invention in further detail. It should be understood that the above-mentioned specific embodiments are only specific embodiments of the present invention, and are not intended to limit the name of the present invention. , any modifications, equivalent replacements and improvements made within the spirit and principle of the present invention shall be included within the protection scope of the present invention.
Claims (5)
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| CN113753856B (en) * | 2021-09-27 | 2023-05-02 | 太原理工大学 | Organic solid waste gas integrated high-efficiency hydrogen production and methane production process |
| US11807530B2 (en) | 2022-04-11 | 2023-11-07 | Iogen Corporation | Method for making low carbon intensity hydrogen |
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