KR102631202B1 - Processing method of hydrogen gas using steel by-product gas - Google Patents
Processing method of hydrogen gas using steel by-product gas Download PDFInfo
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- 239000007789 gas Substances 0.000 title claims abstract description 116
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 37
- 229910000831 Steel Inorganic materials 0.000 title claims abstract description 15
- 239000006227 byproduct Substances 0.000 title claims abstract description 15
- 239000010959 steel Substances 0.000 title claims abstract description 15
- 238000003672 processing method Methods 0.000 title 1
- 230000015572 biosynthetic process Effects 0.000 claims abstract description 14
- 238000003786 synthesis reaction Methods 0.000 claims abstract description 14
- 238000004519 manufacturing process Methods 0.000 claims abstract description 12
- 238000006243 chemical reaction Methods 0.000 claims abstract description 11
- 239000000571 coke Substances 0.000 claims abstract description 9
- 238000000629 steam reforming Methods 0.000 claims abstract description 8
- 238000009628 steelmaking Methods 0.000 claims abstract description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052739 hydrogen Inorganic materials 0.000 claims description 23
- 238000000034 method Methods 0.000 claims description 23
- 239000001257 hydrogen Substances 0.000 claims description 22
- 150000001336 alkenes Chemical class 0.000 claims description 9
- 239000012535 impurity Substances 0.000 claims description 7
- 238000001179 sorption measurement Methods 0.000 claims description 6
- 238000005984 hydrogenation reaction Methods 0.000 claims description 3
- 238000001991 steam methane reforming Methods 0.000 description 14
- 238000000926 separation method Methods 0.000 description 13
- 238000000605 extraction Methods 0.000 description 11
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 9
- 229910002091 carbon monoxide Inorganic materials 0.000 description 7
- 239000003054 catalyst Substances 0.000 description 5
- 239000000446 fuel Substances 0.000 description 5
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 5
- HZAXFHJVJLSVMW-UHFFFAOYSA-N 2-Aminoethan-1-ol Chemical compound NCCO HZAXFHJVJLSVMW-UHFFFAOYSA-N 0.000 description 4
- 229910002092 carbon dioxide Inorganic materials 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 238000010521 absorption reaction Methods 0.000 description 3
- 239000003463 adsorbent Substances 0.000 description 3
- 235000011089 carbon dioxide Nutrition 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 238000010248 power generation Methods 0.000 description 3
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 2
- 239000005977 Ethylene Substances 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 239000000428 dust Substances 0.000 description 2
- 150000002431 hydrogen Chemical class 0.000 description 2
- 239000003949 liquefied natural gas Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 150000003464 sulfur compounds Chemical class 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 229910017709 Ni Co Inorganic materials 0.000 description 1
- 229910003267 Ni-Co Inorganic materials 0.000 description 1
- 229910003262 Ni‐Co Inorganic materials 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 238000006477 desulfuration reaction Methods 0.000 description 1
- 230000023556 desulfurization Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000012717 electrostatic precipitator Substances 0.000 description 1
- 230000014509 gene expression Effects 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000004615 ingredient Substances 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 238000002407 reforming Methods 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
- C01B3/382—Multi-step processes
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
- C01B3/12—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of water vapour with carbon monoxide
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/48—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents followed by reaction of water vapour with carbon monoxide
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
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- C—CHEMISTRY; METALLURGY
- C21—METALLURGY OF IRON
- C21B—MANUFACTURE OF IRON OR STEEL
- C21B7/00—Blast furnaces
- C21B7/002—Evacuating and treating of exhaust gases
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
- C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
- C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/042—Purification by adsorption on solids
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0465—Composition of the impurity
- C01B2203/0475—Composition of the impurity the impurity being carbon dioxide
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- C01—INORGANIC CHEMISTRY
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0465—Composition of the impurity
- C01B2203/048—Composition of the impurity the impurity being an organic compound
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1258—Pre-treatment of the feed
- C01B2203/1264—Catalytic pre-treatment of the feed
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- Y—GENERAL 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
- Y02P20/133—Renewable energy sources, e.g. sunlight
Abstract
본 발명은, (a) 제철 공정에서 발생되는 코크스 오븐 가스(COG)로부터 고순도 H2를 추출하고, 남은 COG 테일가스를 수득하는 단계; (b) 수증기 개질 반응(SMR)을 통해 상기 COG 테일가스를 합성가스로 전환하는 단계; (c) 수성가스 전환 반응(WGS)을 통해 상기 합성가스를 CO2 및 H2를 포함하는 가스로 전환하는 단계; (d) 상기 수성가스 전환 반응(WGS)을 통해 형성된 혼합가스로부터 상기 CO2를 포집 및 분리하는 단계; 및 (e) 상기 CO2를 분리하고 남은 혼합가스로부터 고순도 H2를 추출하는 단계; 를 포함하는 제철 부생가스를 이용한 고순도 수소가스 제조 방법을 제공한다. The present invention includes the steps of (a) extracting high purity H 2 from coke oven gas (COG) generated in a steelmaking process and obtaining the remaining COG tail gas; (b) converting the COG tail gas into synthesis gas through steam reforming reaction (SMR); (c) converting the synthesis gas into a gas containing CO 2 and H 2 through water gas shift reaction (WGS); (d) collecting and separating the CO 2 from the mixed gas formed through the water gas shift reaction (WGS); and (e) extracting high purity H 2 from the mixed gas remaining after separating the CO 2 ; Provides a method for producing high purity hydrogen gas using steel by-product gas containing.
Description
본 발명은 제철 부생가스를 이용한 고순도 수소가스 제조 방법에 관한 것으로, 보다 상세하게는 코크스오븐가스(COG)로부터 수소가스를 효율적으로 제조하는 방법에 관한 것이다. The present invention relates to a method for producing high-purity hydrogen gas using steel by-product gas, and more specifically, to a method for efficiently producing hydrogen gas from coke oven gas (COG).
재생에너지 중 하나인 수소에너지는 온실가스를 배출하지 않는 청정에너지로써 현재까지 활발한 연구가 진행되고 있다 종래에는 나프타 또는 액화 천연가스를 개질하여 수소를 제조하여 왔다. 그러나, 나프타 또는 액화 천연가스의 가격 상승으로 인하여 기존 석유화학회사나 수소를 사용하는 산업분야에서는 수소의 가격이 부담되기 때문에, 최근에는 저렴한 원료를 활용하여 수소를 제조함으로써 수소의 안정적 가격 확보 및 산업 경쟁력 확보가 가능한 방안이 고안되어 왔다.Hydrogen energy, one of the renewable energies, is a clean energy that does not emit greenhouse gases, and active research is being conducted to date. Conventionally, hydrogen has been produced by reforming naphtha or liquefied natural gas. However, due to the rise in the price of naphtha or liquefied natural gas, the price of hydrogen is burdensome for existing petrochemical companies and industrial fields that use hydrogen. Recently, hydrogen has been manufactured using inexpensive raw materials to secure a stable price of hydrogen and to secure a stable price for the industry. Measures to secure competitiveness have been devised.
국내 철강산업에서 발생하는 부생가스 중 코크스 오븐가스(COG)는 석탄을 건류하여 코크스를 제조하는 과정 중에 발생되는 철강 부생가스로서, 현재 철강사에서는 이러한 COG 자체를 압력변동흡착(Pressure Swing Absorption, PSA)하여 수소를 얻어 상업용으로 활용하거나, 제철 공정에서 자체적으로 사용하고 있다.Among the by-product gases generated in the domestic steel industry, coke oven gas (COG) is a steel by-product gas generated during the process of producing coke by drying coal. Currently, steel companies use this COG itself as pressure swing absorption (PSA). Hydrogen is obtained and used commercially or used internally in the steelmaking process.
다만, COG 내에는 수소 외에도 메탄, 일산화탄소가 주성분으로 함유되어 있어 COG 자체로부터 직접 수소가스를 추출할 경우에는, 추출 효율이 저조할 뿐만 아니라 대량의 수소 생산을 위해서는 대용량의 공정을 위한 장치 투자가 수반되어야 한다는 문제점이 존재한다. However, COG contains methane and carbon monoxide as main components in addition to hydrogen, so when hydrogen gas is extracted directly from COG itself, not only is the extraction efficiency low, but mass production of hydrogen requires investment in equipment for large-capacity processes. There is a problem that must be done.
본 발명은 상술한 문제를 포함하여 다양한 문제점을 해결하기 위한 것으로서, 코크스오븐가스(COG)로부터 수소가스가 고효율로 추출되어 제조되는 방법을 제공하는 것을 목적으로 한다. The present invention is intended to solve various problems, including the problems described above, and aims to provide a method for extracting and producing hydrogen gas from coke oven gas (COG) with high efficiency.
그러나 이러한 과제는 예시적인 것으로, 이에 의해 본 발명의 범위가 한정되는 것은 아니다.However, these tasks are illustrative and do not limit the scope of the present invention.
본 발명의 일 실시예에 따르면, 제철 부생가스를 이용한 고순도 수소가스 제조 방법이 제공된다.According to one embodiment of the present invention, a method for producing high purity hydrogen gas using steel by-product gas is provided.
상기 제철 부생가스를 이용한 고순도 수소가스 제조 방법은, (a) 제철 공정에서 발생되는 코크스 오븐 가스(COG)로부터 고순도 H2를 추출하고, 남은 COG 테일가스를 수득하는 단계; (b) 수증기 개질 반응(SMR)을 통해 상기 COG 테일가스를 합성가스로 전환하는 단계; (c) 수성가스 전환 반응(WGS)을 통해 상기 합성가스를 CO2 및 H2를 포함하는 가스로 전환하는 단계; (d) 상기 수성가스 전환 반응(WGS)을 통해 형성된 혼합가스로부터 상기 CO2를 포집 및 분리하는 단계; 및 (e) 상기 CO2를 분리하고 남은 혼합가스로부터 고순도 H2를 추출하는 단계; 를 포함한다.The method for producing high-purity hydrogen gas using the steelmaking by-product gas includes the steps of (a) extracting high-purity H 2 from coke oven gas (COG) generated in the steelmaking process and obtaining the remaining COG tail gas; (b) converting the COG tail gas into synthesis gas through steam reforming reaction (SMR); (c) converting the synthesis gas into a gas containing CO 2 and H 2 through water gas shift reaction (WGS); (d) collecting and separating the CO 2 from the mixed gas formed through the water gas shift reaction (WGS); and (e) extracting high purity H 2 from the mixed gas remaining after separating the CO 2 ; Includes.
상기 (a) 및 (e) 단계는 수소 압력변동흡착 공정(PSA)을 통해 상기 고순도 H2를 추출할 수 있다.In steps (a) and (e), the high purity H 2 can be extracted through a hydrogen pressure swing adsorption (PSA) process.
상기 (e) 단계 이후, 상기 고순도 H2가 추출되고 남은 잔여가스를 상기 수증기 개질 반응(SMR)에 투입하는 단계; 를 더 포함할 수 있다.After step (e), the high-purity H 2 is extracted and the remaining gas is input to the steam reforming reaction (SMR); It may further include.
상기 (a) 단계 이전에, 상기 COG 내 불순물을 처리하는 가스 전처리 단계; 를 더 포함할 수 있다.Before step (a), a gas pretreatment step of treating impurities in the COG; It may further include.
상기 (b) 단계 이전에, 상기 COG 테일가스로부터 올레핀을 제거하는 단계; 를 더 포함할 수 있다.Before step (b), removing olefins from the COG tail gas; It may further include.
본 발명의 일 실시예에 따르면, 수소 추출 공정의 효율을 증대시켜 수소 가스의 회수율을 높일 수 있다. According to an embodiment of the present invention, the recovery rate of hydrogen gas can be increased by increasing the efficiency of the hydrogen extraction process.
물론 이러한 효과에 의해 본 발명의 범위가 한정되는 것은 아니다.Of course, the scope of the present invention is not limited by this effect.
도 1은 본 발명의 실시예에 따른 제철 부생가스를 이용한 고순도 수소가스 제조 방법의 개략적인 구성도이다.Figure 1 is a schematic diagram of a method for producing high-purity hydrogen gas using steel by-product gas according to an embodiment of the present invention.
이하, 첨부된 도면을 참조하여 본 발명의 바람직한 실시 형태들을 설명한다. 본 발명의 실시 형태는 여러 가지 다른 형태로 변형될 수 있으며, 본 발명의 범위가 이하 설명하는 실시 형태로 한정되는 것은 아니다. 또한, 본 발명의 실시 형태는 당업계에서 평균적인 지식을 가진 자에게 본 발명을 더욱 완전하게 설명하기 위해서 제공되는 것이다. 따라서, 도면에서의 요소들의 형상 및 크기 등은 보다 명확한 설명을 위해 과장될 수 있으며, 도면상의 동일한 부호로 표시되는 요소는 동일한 요소이다. Hereinafter, preferred embodiments of the present invention will be described with reference to the attached drawings. Embodiments of the present invention may be modified into various other forms, and the scope of the present invention is not limited to the embodiments described below. Additionally, the embodiments of the present invention are provided to more completely explain the present invention to those with average knowledge in the art. Accordingly, the shapes and sizes of elements in the drawings may be exaggerated for clearer explanation, and elements indicated by the same symbol in the drawings are the same elements.
이하, 첨부된 도면을 참조하여 본 발명의 바람직한 실시예를 상세히 설명하기로 한다.Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the attached drawings.
도 1은 본 발명의 실시예에 따른 제철 부생가스를 이용한 고순도 수소가스 제조 방법의 개략적인 구성도이다.Figure 1 is a schematic diagram of a method for producing high-purity hydrogen gas using steel by-product gas according to an embodiment of the present invention.
도 1을 참조하면, 본 발명의 실시예에 따른 제철 부생가스를 이용한 고순도 수소가스 제조 방법은 (a) 제철 공정에서 발생되는 코크스 오븐 가스(이하, COG)로부터 고순도 수소가스(이하, 고순도 H2)를 추출하고, 남은 COG 테일가스를 수득하는 단계; (b) 수증기 개질 반응(Steam Methane Reforming, 이하 SMR)을 통해 상기 COG 테일가스를 합성가스로 전환하는 단계; (c) 수성가스 전환 반응(Water Gas Shift, 이하 WGS)을 통해 상기 합성가스를 이산화탄소(이하, CO2) 및 수소(이하, H2)를 포함하는 가스로 전환하는 단계; (d) 상기 WGS를 통해 형성된 가스로부터 상기 CO2를 포집 및 분리하는 단계; 및 (e) 상기 CO2를 분리하고 남은 혼합가스로부터 고순도 H2를 추출하는 단계; 를 포함한다.Referring to Figure 1, the method for producing high-purity hydrogen gas using steel by-product gas according to an embodiment of the present invention is (a) high-purity hydrogen gas (hereinafter, high-purity H 2 ) from coke oven gas (hereinafter, COG) generated in the steelmaking process. ) extracting and obtaining the remaining COG tail gas; (b) converting the COG tail gas into synthesis gas through steam methane reforming (SMR); (c) converting the synthesis gas into a gas containing carbon dioxide (hereinafter CO 2 ) and hydrogen (hereinafter H 2 ) through a water gas shift (WGS) reaction; (d) capturing and separating the CO 2 from the gas formed through the WGS; and (e) extracting high purity H 2 from the mixed gas remaining after separating the CO 2 ; Includes.
(a) 단계에 있어서, 고순도 H2는 COG로부터 수소 추출 공정, 예를 들어, 압력변동흡착 공정(Pressure Swing Adsorption, 이하 PSA)을 통해 선택적으로 추출될 수 있다. 이 때, COG는 H2의 함량이 45 내지 60%로서 H2가 주성분인 제철공정의 부생가스이다. 이렇게 추출된 고순도 H2는 연료전지차 또는 발전에 필요한 연료로서 투입됨으로써 경제적 효과의 구현이 가능할 수 있다.In step (a), high purity H 2 may be selectively extracted from COG through a hydrogen extraction process, for example, Pressure Swing Adsorption (PSA). At this time, COG has an H 2 content of 45 to 60% and is a by-product gas from the steelmaking process in which H 2 is the main component. The high purity H 2 extracted in this way can be used as fuel for fuel cell vehicles or power generation, thereby realizing economic effects.
COG 테일가스는 COG로부터 H2를 회수하고 남은 가스를 의미하는 것으로, 상기 COG 테일가스는 비연속적 또는 연속적으로 배출되게 된다. 따라서, 이를 이용할 수 있도록 포집하는 단계를 포함하는 것이 바람직하다. 예를 들어, 상기 COG 테일가스를 포집하기 위해서 저압의 저장용기를 이용할 수 있다. COG 테일가스는 H2 및 CH4를 포함하고, CO, CO2, N2 및 H2S로 이루어진 군에서 선택되는 하나 이상을 더 포함하는 것으로서, 특히, CH4의 함량은 COG 테일가스 총 부피에 대하여 30 내지 50부피%로서 COG 테일가스의 주성분이 될 수 있다.COG tail gas refers to the gas remaining after recovering H 2 from COG, and the COG tail gas is discharged discontinuously or continuously. Therefore, it is desirable to include a step of collecting it so that it can be used. For example, a low-pressure storage vessel can be used to collect the COG tail gas. COG tail gas contains H 2 and CH 4 and further contains one or more selected from the group consisting of CO, CO 2 , N 2 and H 2 S. In particular, the content of CH 4 is determined by the total volume of COG tail gas. It can be the main component of COG tail gas at 30 to 50% by volume.
한편, (a) 단계 이전에 COG 내 불순물을 처리하는 가스 전처리 단계; 를 더 포함할 수 있다. 가스 전처리 단계는 수소 추출 공정, 예를 들어, PSA 내 흡착제의 성능이 최대한 발현될 수 있도록 기체 내 불순물을 최소로 처리한다. Meanwhile, a gas pretreatment step of treating impurities in COG before step (a); It may further include. The gas pretreatment step treats impurities in the gas to a minimum so that the performance of the adsorbent in the hydrogen extraction process, for example, PSA, can be maximized.
가스 전처리 단계는 수소 추출을 위한 흡착제의 성능 저하를 발생시키는 먼지, 황 화합물 기타 불순물을 제거하여 정제된 가스를 형성하기 위한 모든 공정, 예를 들어, 전기집진기, 탈황 설비 및 온도순환흡착 공정(Temperature Swing Adsorption, 이하 TSA) 설비를 통한 공정을 포함할 수 있다. 이러한 가스 전처리 단계를 거친 정제 가스는 수소 추출 공정시 고순도 H2가 추출되도록 불순물을 최소로 포함할 수 있다.The gas pretreatment step is all processes to form purified gas by removing dust, sulfur compounds, and other impurities that deteriorate the performance of the adsorbent for hydrogen extraction, such as electrostatic precipitator, desulfurization equipment, and temperature cycling adsorption process (Temperature). It may include a process using a Swing Adsorption (TSA) facility. Refined gas that has gone through this gas pretreatment step may contain a minimum amount of impurities so that high purity H 2 can be extracted during the hydrogen extraction process.
(b) 단계에 있어서, 상기 포집된 COG 테일가스는 SMR 공정에 투입되어 합성가스를 형성시킬 수 있다. 보다 구체적으로, SMR을 통해 COG 테일가스에 포함된 CH4로부터 합성가스를 형성시킬 수 있고, 이 때, 합성가스는 CO, CO2 및 H2를 포함할 수 있다.In step (b), the collected COG tail gas can be input into the SMR process to form synthesis gas. More specifically, synthesis gas can be formed from CH 4 contained in COG tail gas through SMR, and at this time, the synthesis gas may include CO, CO 2 and H 2 .
SMR에 사용되는 촉매는, 예를 들어 Ni을 포함하는 촉매일 수 있고, 바람직하게는 Ni-Co를 포함하는 촉매일 수 있지만, 이에 한정되는 것은 아니다. SMR은, 850℃ 이상의 고온 조건에서 반응시킬 수 있지만, 이에 한정되는 것은 아니며, 800℃이하의 저온 조건에서도 반응을 수행할 수 있으며, 바람직하게는 650℃ 내지 850℃의 반응온도에서 반응을 수행할 수 있다. 또한, SMR은 1 내지 15bar의 압력조건에서 수행될 수 있으며, H2O/CH4의 부피비가 2.8 내지 3.2인 것이 바람직하지만, 이에 한정되는 것은 아니다.The catalyst used in SMR may be, for example, a catalyst containing Ni, preferably a catalyst containing Ni-Co, but is not limited thereto. SMR can be reacted at a high temperature of 850℃ or higher, but is not limited to this, and can also be reacted at a low temperature of 800℃ or lower. Preferably, the reaction is performed at a reaction temperature of 650℃ to 850℃. You can. Additionally, SMR can be performed under pressure conditions of 1 to 15 bar, and the volume ratio of H 2 O/CH 4 is preferably 2.8 to 3.2, but is not limited thereto.
한편, (b) 단계 이전에 COG 테일가스로부터 올레핀을 제거하는 단계; 를 더 포함할 수 있다. COG 테일가스에 올레핀 또는 에틸렌 성분이 존재하게 되면, SMR에 사용되는 촉매에 탄소가 부착되거나 코킹되어 수소화되는 현상이 발생하고, 이는 촉매 및 개질기 반응기 관 상에 고온 지점을 형성하는 문제점이 발생한다.Meanwhile, removing olefins from COG tail gas before step (b); It may further include. When olefin or ethylene components are present in the COG tail gas, carbon attaches to the catalyst used in SMR or is coked and hydrogenated, which causes the problem of forming high temperature spots on the catalyst and reformer reactor tubes.
따라서, SMR을 수행하기 전, COG 테일가스로부터 올레핀을 제거하고 이로부터 COG 테일가스 내 CH4의 함량을 증가시킬 필요성이 있다. 올레핀 제거 공정은, 예를 들어, COG 테일가스에 대한 수소화반응이나 pre-reformer 등에 의해 진행될 수 있으며, 이러한 수소화반응은 COG 테일가스 내 올레핀 또는 에틸렌을 제거하되 CH4 함량을 증대시킬 수 있다.Therefore, before performing SMR, there is a need to remove olefins from COG tail gas and thereby increase the content of CH 4 in the COG tail gas. The olefin removal process can be carried out, for example, by hydrogenation or pre-reformer for COG tail gas, and this hydrogenation reaction can remove olefin or ethylene in COG tail gas and increase CH 4 content.
또한, 올레핀 제거 효율 및 수소 고순도 수소 추출을 위해 올레핀 제거 공정을 수 행하기 전, 선행적으로 먼지, 황 화합물 및 기타 불순물을 제거하여 정제된 가스를 형성하는 공정이 수행될수 있다.In addition, for olefin removal efficiency and high-purity hydrogen extraction, a process of removing dust, sulfur compounds, and other impurities to form a purified gas may be performed before performing the olefin removal process.
(c) 단계에 있어서, WGS 공정을 통해 합성가스로부터 CO2 및 H2를 포함하는 가스를 형성시킬 수 있다. WGS란 합성가스 내의 CO 및 H2O가 반응하여 CO2 및 H2를 생성하는 반응으로 진행될 수 있다.In step (c), gas containing CO 2 and H 2 can be formed from synthesis gas through the WGS process. WGS can be a reaction in which CO and H 2 O in synthesis gas react to produce CO 2 and H 2 .
본 발명의 일 실시예에 있어서 WGS는 SMR과 연속된 절차로 진행되어 H2를 생성함으로써, 최종적으로 반응기 내 H2의 함량을 증폭시키는 효과가 구현될 수 있다. 이 때, WGS의 반응조건으로는 일반적으로 합성가스로부터 CO2 및 H2를 형성할 수 있는 조건이라면 특별히 제한되지 않는다.In one embodiment of the present invention, WGS is performed in succession with SMR to generate H 2 , ultimately achieving the effect of amplifying the content of H 2 in the reactor. At this time, the reaction conditions for WGS are generally not particularly limited as long as they are conditions capable of forming CO 2 and H 2 from synthesis gas.
이후, (d) 단계에 있어서, 상기 WGS를 통해 형성된 가스로부터 CO2를 포집 및 분리할 수 있다. (c) 단계에 따라 WGS를 거친 가스는 H2, CO2, N2, CH4 및 CO를 포함하는 혼합가스로서, 특히 H2가 65 내지 75 중량% 및 CO2가 15 내지 25 중량%의 분율로 포함된 혼합가스일 수 있다.Thereafter, in step (d), CO 2 can be captured and separated from the gas formed through the WGS. The gas that has undergone WGS according to step (c) is a mixed gas containing H 2 , CO 2 , N 2 , CH 4 and CO, and in particular, H 2 is 65 to 75% by weight and CO 2 is 15 to 25% by weight. It may be a mixed gas contained in fractions.
CO2를 포집하는 기술은, 예를 들어, 습식흡수법, 건식흡착법, 막분리법 및 심냉법 등이 있으며, 가장 널리 쓰이고 있는 기술은 MEA(monoethanolamine)를 이용한 습식 아민흡수법으로서 혼합가스에 포함된 CO2를 30% 이하로 희석된 MEA와 반응시켜 흡착한 후 용매를 가열하여 고순도 CO2를 분리해내는 동시에 MEA를 재생시키는 방법이다. 아울러, CO2를 포집하는 기술은, 예를 들어, CO2 PSA 공정일 수 있다.Technologies for capturing CO 2 include, for example, wet absorption, dry adsorption, membrane separation, and deep cooling. The most widely used technology is the wet amine absorption method using MEA (monoethanolamine), which removes the amine content contained in the mixed gas. This is a method of adsorbing CO 2 by reacting it with MEA diluted to 30% or less, then heating the solvent to separate high-purity CO 2 and regenerating MEA at the same time. In addition, the technology for capturing CO 2 may be, for example, a CO 2 PSA process.
본 발명의 일 실시예에 있어서, 상술한 공정에 의해 포집 및 분리된 고순도 CO2는 액화탄산 혹은 드라이아이스 등의 유가자원으로 활용됨으로써 경제성이 확보될 수 있다. 아울러, 상술한 포집 및 분리 공정에 의해 고순도 CO2가 분리되고 난 후 잔여가스는 일부 H2를 포함하는 혼합가스일 수 있다. 이러한 혼합가스는 발전 또는 제철소 연소 공정 및 환원가스로 활용될수 있다.In one embodiment of the present invention, high-purity CO 2 captured and separated through the above-described process can be used as a valuable resource such as liquefied carbon dioxide or dry ice, thereby ensuring economic efficiency. In addition, after high-purity CO 2 is separated through the above-described collection and separation process, the remaining gas may be a mixed gas containing some H 2 . This mixed gas can be used in power generation or steel mill combustion processes and as a reducing gas.
또한, 본 발명의 일 실시예에 있어서, 상기 WGS를 통해 형성된 가스로부터 CO2를 CO2 PSA를 통해 포집 및 분리할수 있다.Additionally, in one embodiment of the present invention, CO 2 can be captured and separated from the gas formed through the WGS through CO 2 PSA.
(e) 단계에 있어서, (d) 단계에 따라 CO2를 포집 및 분리하고 나면 그 이전보다 H2 분율이 상승된 상태의 혼합가스가 수소 추출공정에 투입될 수 있다. 이 때 고순도 H2는, 수소 추출공정, 예를 들어, PSA 공정을 통해 선택적으로 추출될 수 있다. 한편, 이렇게 추출된 고순도 H2는 연료전지차 또는 발전에 필요한 연료로서 투입되어 재활용될 수 있다.In step (e), after collecting and separating CO 2 according to step (d), the mixed gas with a higher H 2 fraction than before can be input into the hydrogen extraction process. At this time, high purity H 2 can be selectively extracted through a hydrogen extraction process, for example, a PSA process. Meanwhile, the high purity H 2 extracted in this way can be recycled and used as fuel for fuel cell vehicles or power generation.
이하, 본 발명을 실시예에 의거하여 구체적으로 설명하는 바, 본 발명이 다음 실시예에 의하여 한정되는 것은 아니다.Hereinafter, the present invention will be described in detail based on examples, but the present invention is not limited to the following examples.
실시예Example
(d) 단계에 따른 C02 포집 및 분리 단계 전, 후 혼합가스 내 H2 및 CO2의 분율을 비교하기 위해 표 1과 같이 혼합가스를 조성하는 각 성분의 분율을 도출하였다. In order to compare the fractions of H 2 and CO 2 in the mixed gas before and after the C0 2 collection and separation step according to step (d), the fractions of each component forming the mixed gas were derived as shown in Table 1.
표 1을 참조하면, (d) 단계에 따라 CO2 포집 및 분리한 이후, 혼합가스 내 제거된 CO2의 분율만큼 H2의 분율이 상대적으로 상승된 것을 확인할 수 있다. Referring to Table 1, it can be seen that after CO 2 capture and separation in step (d), the fraction of H 2 was relatively increased by the fraction of CO 2 removed in the mixed gas.
표 1의 실시예에 따르면, CO2 포집 및 분리 전 대비 이후 H2 의 비율은 1:1~1.46이며, CO2 포집 및 분리 전 대비 이후 CO2의 비율은 1:0.33~0.66이다. 또한, CO2 대비 H2 의 비율에 있어서, CO2 포집 및 분리 전의 상기 비율은 2.6~5이고 CO2 포집 및 분리 후 상기 비율은 15~99임에 비추어 볼 때, CO2 포집 및 분리 공정을 거치면서 CO2 대비 H2 의 비율이 상대적으로 상승된 것을 확인할수 있다. 따라서 후술할 바와 같이, 상기 CO2 포집 및 분리 공정을 통해 고순도 H2 가 효율적으로 추출될 수 있게 된다.According to the examples in Table 1, the ratio of H 2 before and after CO 2 capture and separation is 1:1 to 1.46, and the ratio of CO 2 before and after CO 2 capture and separation is 1:0.33 to 0.66. In addition, in terms of the ratio of H 2 to CO 2 , considering that the ratio before CO 2 capture and separation is 2.6 to 5 and after CO 2 capture and separation is 15 to 99, the CO 2 capture and separation process It can be seen that the ratio of H 2 to CO 2 has relatively increased over time. Therefore, as will be described later, high purity H 2 can be efficiently extracted through the CO 2 capture and separation process.
연속하여 (e) 단계에 따른 수소 추출 공정을 수행하였을 때, 혼합가스 내 H2가 차지하는 분율이 상승된 것에 따라 PSA 공정 내에서 흡착제를 통해 회수되는 H2의 순도 역시 향상될 수 있다. 즉, 수소 추출 공정에 선행하여 공정에 투입되는 혼합가스 내 H2의 분율을 상승시킴으로써 공정에서 흡착 및 분리되는 H2의 분율이 상승되고, 최종적으로 고순도 H2가 효율적으로 추출될 수 있게 된다.Hydrogen according to step (e) in succession When the extraction process is performed, H 2 in the mixed gas occupies As the fraction is increased, the purity of H 2 recovered through the adsorbent in the PSA process can also be improved. In other words, by increasing the fraction of H 2 in the mixed gas input to the process prior to the hydrogen extraction process, the fraction of H 2 adsorbed and separated in the process increases, and ultimately high-purity H 2 can be efficiently extracted.
한편, 표 1을 참조해보면, (d) 단계에 따라 C02 포집 및 분리를 거친 혼합가스는 H2 함량이 75 내지 95 중량%로서 H2가 주성분인 가스에 해당하는 것을 확인할 수 있다. 이에, (d) 단계를 거쳐 생성된 이러한 가스 자체로도 제철공정의 환원반응을 수행하기 위한 환원가스로서 활용될 수 있다.Meanwhile, referring to Table 1, it can be seen that the mixed gas that has undergone C0 2 collection and separation in step (d) has an H 2 content of 75 to 95% by weight and corresponds to a gas in which H 2 is the main component. Accordingly, this gas generated through step (d) itself can be used as a reducing gas to perform a reduction reaction in the steelmaking process.
이후, (e) 단계에 따라 고순도 H2가 추출되고 나면, 잔여가스가 SMR에 투입되는 단계; 를 더 포함할 수 있다. 즉, 잔여가스를 SMR의 연료로 재활용함으로써 전체적인 공정의 생산성뿐만 아니라 경제성까지 확보할 수 있는 효과를 구현할 수 있다.Afterwards, after high-purity H 2 is extracted in step (e), the remaining gas is introduced into the SMR; It may further include. In other words, by recycling the remaining gas as fuel for SMR, it is possible to achieve the effect of securing not only the productivity of the overall process but also economic efficiency.
본 발명에서 사용한 용어는 특정한 실시예를 설명하기 위한 것으로, 본 발명을 한정하고자 하는 것이 아니다. 단수의 표현은 문맥상 명백하지 않는 한, 복수의 의미를 포함한다고 보아야 할 것이다. "포함하다" 또는 "가지다" 등의 용어는 명세서 상에 기재된 특징, 숫자, 단계, 동작, 구성 요소 또는 이들을 조합한 것이 존재한다는 것을 의미하는 것이지, 이를 배제하기 위한 것이 아니다. 본 발명은 상술한 실시 형태 및 첨부된 도면에 의해 한정되는 것이 아니며, 첨부된 청구범위에 의해 한정하고자 한다. 따라서, 청구범위에 기재된 본 발명의 기술적 사상을 벗어나지 않는 범위 내에서 당 기술 분야의 통상의 지식을 가진 자에 의해 다양한 형태의 치환, 변형 및 변경이 가능할 것이며, 이 또한 본 발명의 범위에 속한다고 할 것이다.The terms used in the present invention are for describing specific embodiments and are not intended to limit the present invention. Singular expressions should be considered to have a plural meaning, unless it is clear from the context. Terms such as “include” or “have” mean that the features, numbers, steps, operations, components, or combinations thereof described in the specification exist, but are not intended to exclude them. The present invention is not limited by the above-described embodiments and attached drawings, but is intended to be limited by the attached claims. Accordingly, various forms of substitution, modification, and change may be made by those skilled in the art without departing from the technical spirit of the present invention as set forth in the claims, and this also falls within the scope of the present invention. something to do.
Claims (5)
(b) 수증기 개질 반응(SMR)을 통해 상기 COG 테일가스를 합성가스로 전환하는 단계;
(c) 수성가스 전환 반응(WGS)을 통해 상기 합성가스를 CO2 및 H2를 포함하는 가스로 전환하는 단계;
(d) 상기 수성가스 전환 반응(WGS)을 통해 형성된 혼합가스로부터 상기 CO2를 포집 및 분리하는 단계; 및
(e) 상기 CO2를 분리하고 남은 혼합가스로부터 고순도 H2를 추출하는 단계; 를 포함하고,
상기 (b) 단계 이전에, 상기 COG 테일가스에 대한 수소화 반응 또는 사전 개질기(pre-reformer)에 의해 올레핀을 제거하는 단계;
를 더 포함하는,
제철 부생가스를 이용한 고순도 수소가스 제조 방법.(a) extracting high purity H 2 from coke oven gas (COG) generated in the steelmaking process and obtaining the remaining COG tail gas;
(b) converting the COG tail gas into synthesis gas through steam reforming reaction (SMR);
(c) converting the synthesis gas into a gas containing CO 2 and H 2 through water gas shift reaction (WGS);
(d) collecting and separating the CO 2 from the mixed gas formed through the water gas shift reaction (WGS); and
(e) separating the CO 2 and extracting high purity H 2 from the remaining mixed gas; Including,
Before step (b), removing olefins from the COG tail gas by hydrogenation or a pre-reformer;
Containing more,
Method for producing high purity hydrogen gas using steel by-product gas.
상기 (a) 및 (e) 단계는
수소 압력변동흡착 공정(PSA)을 통해 상기 고순도 H2를 추출하는 것인,
제철 부생가스를 이용한 고순도 수소가스 제조 방법.According to claim 1,
The steps (a) and (e) are
Extracting the high purity H 2 through a hydrogen pressure swing adsorption process (PSA),
Method for producing high purity hydrogen gas using steel by-product gas.
상기 (e) 단계 이후, 상기 고순도 H2가 추출되고 남은 잔여가스를 상기 수증기 개질 반응(SMR)에 투입하는 단계; 를 더 포함하는,
제철 부생가스를 이용한 고순도 수소가스 제조 방법.According to claim 1,
After step (e), the high-purity H 2 is extracted and the remaining gas is input to the steam reforming reaction (SMR); Containing more,
Method for producing high purity hydrogen gas using steel by-product gas.
상기 (a) 단계 이전에, 상기 코크스 오븐 가스(COG) 내 불순물을 처리하는 가스 전처리 단계; 를 더 포함하는,
제철 부생가스를 이용한 고순도 수소가스 제조 방법.According to claim 1,
Before step (a), a gas pretreatment step of treating impurities in the coke oven gas (COG); Containing more,
Method for producing high purity hydrogen gas using steel by-product gas.
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