JP5804747B2 - 合成ガス製造装置への金属混入抑制方法 - Google Patents
合成ガス製造装置への金属混入抑制方法 Download PDFInfo
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- JP5804747B2 JP5804747B2 JP2011078808A JP2011078808A JP5804747B2 JP 5804747 B2 JP5804747 B2 JP 5804747B2 JP 2011078808 A JP2011078808 A JP 2011078808A JP 2011078808 A JP2011078808 A JP 2011078808A JP 5804747 B2 JP5804747 B2 JP 5804747B2
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- synthesis gas
- carbon dioxide
- gas
- production process
- fischer
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- 238000004519 manufacturing process Methods 0.000 title claims description 58
- 238000000034 method Methods 0.000 title claims description 46
- 229910052751 metal Inorganic materials 0.000 title claims description 18
- 239000002184 metal Substances 0.000 title claims description 18
- 238000011109 contamination Methods 0.000 title claims description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 175
- 239000007789 gas Substances 0.000 claims description 127
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 87
- 239000001569 carbon dioxide Substances 0.000 claims description 87
- 230000015572 biosynthetic process Effects 0.000 claims description 85
- 238000003786 synthesis reaction Methods 0.000 claims description 85
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 70
- 229910052759 nickel Inorganic materials 0.000 claims description 46
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 42
- 238000002407 reforming Methods 0.000 claims description 23
- 239000003345 natural gas Substances 0.000 claims description 19
- 239000003921 oil Substances 0.000 claims description 18
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 16
- 239000007788 liquid Substances 0.000 claims description 16
- 238000006243 chemical reaction Methods 0.000 claims description 12
- 239000000463 material Substances 0.000 claims description 11
- 229910052799 carbon Inorganic materials 0.000 claims description 8
- 239000007864 aqueous solution Substances 0.000 claims description 7
- 229930195733 hydrocarbon Natural products 0.000 claims description 7
- 150000002430 hydrocarbons Chemical class 0.000 claims description 7
- 238000001179 sorption measurement Methods 0.000 claims description 7
- 239000004215 Carbon black (E152) Substances 0.000 claims description 6
- 238000012856 packing Methods 0.000 claims description 5
- 239000002994 raw material Substances 0.000 claims description 5
- 239000003463 adsorbent Substances 0.000 claims description 4
- 238000006114 decarboxylation reaction Methods 0.000 claims description 4
- 150000003512 tertiary amines Chemical class 0.000 claims description 4
- 239000007795 chemical reaction product Substances 0.000 claims description 3
- 239000000047 product Substances 0.000 claims description 3
- 238000010521 absorption reaction Methods 0.000 description 29
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 24
- 229910002091 carbon monoxide Inorganic materials 0.000 description 24
- 239000003054 catalyst Substances 0.000 description 15
- 230000008929 regeneration Effects 0.000 description 11
- 238000011069 regeneration method Methods 0.000 description 11
- 238000006057 reforming reaction Methods 0.000 description 8
- 238000000926 separation method Methods 0.000 description 7
- 238000006477 desulfuration reaction Methods 0.000 description 6
- 230000023556 desulfurization Effects 0.000 description 6
- 238000011084 recovery Methods 0.000 description 6
- 239000000243 solution Substances 0.000 description 6
- 230000003197 catalytic effect Effects 0.000 description 4
- 229910052739 hydrogen Inorganic materials 0.000 description 4
- CRVGTESFCCXCTH-UHFFFAOYSA-N methyl diethanolamine Chemical compound OCCN(C)CCO CRVGTESFCCXCTH-UHFFFAOYSA-N 0.000 description 4
- -1 naphtha Substances 0.000 description 4
- 150000003141 primary amines Chemical class 0.000 description 4
- 238000004064 recycling Methods 0.000 description 4
- 229910001220 stainless steel Inorganic materials 0.000 description 4
- 239000010935 stainless steel Substances 0.000 description 4
- 150000001412 amines Chemical class 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 238000000629 steam reforming Methods 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- HZAXFHJVJLSVMW-UHFFFAOYSA-N 2-Aminoethan-1-ol Chemical compound NCCO HZAXFHJVJLSVMW-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- 239000002250 absorbent Substances 0.000 description 2
- 230000002745 absorbent Effects 0.000 description 2
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 239000003350 kerosene Substances 0.000 description 2
- 238000005038 synthesis gas manufacturing Methods 0.000 description 2
- 239000002918 waste heat Substances 0.000 description 2
- GIAFURWZWWWBQT-UHFFFAOYSA-N 2-(2-aminoethoxy)ethanol Chemical compound NCCOCCO GIAFURWZWWWBQT-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 1
- 239000002028 Biomass Substances 0.000 description 1
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- XSTXAVWGXDQKEL-UHFFFAOYSA-N Trichloroethylene Chemical group ClC=C(Cl)Cl XSTXAVWGXDQKEL-UHFFFAOYSA-N 0.000 description 1
- 229910001628 calcium chloride Inorganic materials 0.000 description 1
- 239000001110 calcium chloride Substances 0.000 description 1
- 235000011089 carbon dioxide Nutrition 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000004821 distillation Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- DHEIAYDROZXXGS-UHFFFAOYSA-N ethanol;iodine Chemical compound [I].CCO DHEIAYDROZXXGS-UHFFFAOYSA-N 0.000 description 1
- 238000005755 formation reaction Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 238000009616 inductively coupled plasma Methods 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 239000003209 petroleum derivative Substances 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 150000003335 secondary amines Chemical class 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 150000003464 sulfur compounds Chemical class 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Combustion & Propulsion (AREA)
- General Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Hydrogen, Water And Hydrids (AREA)
- Gas Separation By Absorption (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Description
式(1): CH4 + H2O → CO + 3H2
式(2): CH4 + CO2 → 2CO + 2H2
式(3): R-NH2 + CO2 + H2O → R-NH3 + + HCO3 -
天然ガスにH2O/Cモル比が1.1およびCO2/Cモル比が0.4となるようスチームおよび二酸化炭素を添加して、アルカリ土類金属酸化物担体上にVIII族金属を担持した改質触媒を充填したリフォーマーに、入口温度500℃、出口温度880℃、圧力2.0MPaG、GHSV3,000h-1の条件で導入し、合成ガスを製造した。得られた合成ガス(H2:58%、CO:28%、CO2:7%、CH4:7%)からCO2を分離回収するため、炭酸ガス吸収塔6に温度40℃、圧力2MPaGの条件で導入した。炭酸ガス吸収塔6はニッケルを含有しないステンレス材料SUS410のカスケードミニリングが充填された充填塔形式のものであり、導入された合成ガスは第三級アミンのMDEAを含む水溶液と向流で気液接触され、炭酸ガスが吸収除去された。炭酸ガスを吸収した吸収液は、再生塔7から炭酸ガス吸収塔へリサイクルされる高温の吸収液と熱交換された後、SUS410の充填物が充填されている再生塔7に温度100℃、圧力0.1MPaGで導入され、吸収液中の炭酸ガスがストリッピングされた。ストリッピングされた炭酸ガスは0.08MPaG、40℃に冷却された。この回収された炭酸ガス中のニッケルカルボニル濃度はニッケル金属換算で0.04ppmvであった。
実施例1と同じ合成ガス製造工程で得られた合成ガス(H2:58%、CO:28%、CO2:7%、CH4:7%)からCO2を分離回収するため、炭酸ガス吸収塔6に温度40℃、圧力2MPaGの条件で導入した。炭酸ガス吸収塔6はニッケルを含有するステンレス材料SUS304のカスケードミニリングが充填されており、導入された合成ガスは第一級アミンのモノエタノールアミンを含む水溶液と向流で気液接触され、炭酸ガスが吸収除去された。炭酸ガスを吸収した吸収液は、再生塔7から炭酸ガス吸収塔へリサイクルされる高温の吸収液と熱交換された後、SUS304の充填物が充填されている再生塔7に温度100℃、圧力0.1MPaGで導入され、吸収液中の炭酸ガスがストリッピングされた。ストリッピングされた炭酸ガスは0.08MPaG、40℃に冷却された。この回収された炭酸ガス中のニッケルカルボニル濃度はニッケル金属換算で2.0ppmvであった。
比較例1で回収された炭酸ガス(ニッケルカルボニル濃度がニッケル金属換算で2.0ppmv)を2.2MPaGまで昇圧後、250℃に昇温し、ニッケルカルボニル吸着材(商品名:Actisorb400、ズードケミー触媒社製)を充填した吸着装置にGHSV1,500h-1の空間速度で通過させたところ、炭酸ガス中のニッケルカルボニル濃度はニッケル金属換算で0.02ppmvに低減した。
2.合成ガス製造装置
3.廃熱ボイラー
4.合成ガス冷却器
5.脱炭酸装置
6.炭酸ガス吸収塔
7.再生塔
8.吸着装置
Claims (5)
- 天然ガスとスチームおよび/または二酸化炭素を含むガスとを合成ガス製造装置内で改質反応して合成ガスを製造する合成ガス製造工程と、該合成ガス製造工程で製造された合成ガスをフィッシャー・トロプシュ反応させた後、フィッシャー・トロプシュ反応生成物からガス状生成物を分離してフィッシャー・トロプシュ油を製造するフィッシャー・トロプシュ油製造工程と、該フィッシャー・トロプシュ油製造工程で製造されたフィッシャー・トロプシュ油を水素化処理および蒸留して各種炭化水素油を製造するアップグレーディング工程とからなるGTL(Gas−to−liquid)プロセスの合成ガス製造装置への金属混入抑制方法であって、
該合成ガス製造工程で製造された該合成ガス中の炭酸ガスを分離回収し、分離回収された該炭酸ガスを該合成ガス製造工程にリサイクルする際に、該リサイクルされる炭酸ガス中に含まれるニッケルの濃度が0.05ppmv以下であることを特徴とする合成ガス製造装置への金属混入抑制方法。 - 前記合成ガス中の炭酸ガスは、第三級アミンを含む水溶液で分離回収することを特徴とする請求項1記載の方法。
- 前記合成ガス中の炭酸ガスは、ニッケルを含まない材料からなる充填物を充填した脱炭酸装置で分離回収することを特徴とする請求項1または2記載の方法。
- 前記分離回収された炭酸ガスが、温度250℃〜400℃、圧力0.02〜3.0MPaG、GHSV500〜3,000h-1で活性炭を主成分とする吸着剤を有する吸着装置に導入された後、前記合成ガス製造装置に導入することを特徴とする請求項1〜3のいずれか記載の方法。
- 前記合成ガス製造装置に供給するガスは、原料である炭化水素由来の炭素モル数をCで表したとき、該ガスのH2O/Cモル比が0.1〜3.0および/またはCO2/Cモル比が0.1〜3.0であることを特徴とする請求項1〜4のいずれか記載の方法。
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