JP6077540B2 - 水素化熱分解生成物蒸気からの硫酸アンモニウムとしての硫化水素の除去 - Google Patents
水素化熱分解生成物蒸気からの硫酸アンモニウムとしての硫化水素の除去 Download PDFInfo
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- JP6077540B2 JP6077540B2 JP2014523979A JP2014523979A JP6077540B2 JP 6077540 B2 JP6077540 B2 JP 6077540B2 JP 2014523979 A JP2014523979 A JP 2014523979A JP 2014523979 A JP2014523979 A JP 2014523979A JP 6077540 B2 JP6077540 B2 JP 6077540B2
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- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 title claims description 18
- 229910052921 ammonium sulfate Inorganic materials 0.000 title claims description 18
- 235000011130 ammonium sulphate Nutrition 0.000 title claims description 18
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 title claims description 16
- 229910000037 hydrogen sulfide Inorganic materials 0.000 title claims description 11
- 238000000197 pyrolysis Methods 0.000 title claims 2
- 238000000034 method Methods 0.000 claims description 92
- 239000000047 product Substances 0.000 claims description 81
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 70
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 42
- 229930195733 hydrocarbon Natural products 0.000 claims description 25
- 150000002430 hydrocarbons Chemical class 0.000 claims description 25
- 230000003647 oxidation Effects 0.000 claims description 25
- 238000007254 oxidation reaction Methods 0.000 claims description 25
- 238000006243 chemical reaction Methods 0.000 claims description 22
- 239000002028 Biomass Substances 0.000 claims description 21
- 229910021529 ammonia Inorganic materials 0.000 claims description 21
- 239000007788 liquid Substances 0.000 claims description 18
- 229910052717 sulfur Inorganic materials 0.000 claims description 18
- UYJXRRSPUVSSMN-UHFFFAOYSA-P ammonium sulfide Chemical compound [NH4+].[NH4+].[S-2] UYJXRRSPUVSSMN-UHFFFAOYSA-P 0.000 claims description 17
- 239000004215 Carbon black (E152) Substances 0.000 claims description 14
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 14
- 229910052739 hydrogen Inorganic materials 0.000 claims description 13
- 239000011593 sulfur Substances 0.000 claims description 13
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 12
- 239000001257 hydrogen Substances 0.000 claims description 10
- 239000003054 catalyst Substances 0.000 claims description 9
- 239000003337 fertilizer Substances 0.000 claims description 8
- 230000003197 catalytic effect Effects 0.000 claims description 7
- 239000002689 soil Substances 0.000 claims description 6
- -1 CO 2 Inorganic materials 0.000 claims description 4
- 235000015097 nutrients Nutrition 0.000 claims description 4
- 238000011144 upstream manufacturing Methods 0.000 claims description 4
- 239000000446 fuel Substances 0.000 claims description 2
- 238000001816 cooling Methods 0.000 claims 4
- 238000001704 evaporation Methods 0.000 claims 3
- 230000008020 evaporation Effects 0.000 claims 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims 2
- 238000009833 condensation Methods 0.000 claims 2
- 230000005494 condensation Effects 0.000 claims 2
- 239000012084 conversion product Substances 0.000 claims 2
- 238000001914 filtration Methods 0.000 claims 2
- 238000000926 separation method Methods 0.000 claims 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims 1
- 229910002092 carbon dioxide Inorganic materials 0.000 claims 1
- 239000001569 carbon dioxide Substances 0.000 claims 1
- MPMSMUBQXQALQI-UHFFFAOYSA-N cobalt phthalocyanine Chemical group [Co+2].C12=CC=CC=C2C(N=C2[N-]C(C3=CC=CC=C32)=N2)=NC1=NC([C]1C=CC=CC1=1)=NC=1N=C1[C]3C=CC=CC3=C2[N-]1 MPMSMUBQXQALQI-UHFFFAOYSA-N 0.000 claims 1
- 230000006835 compression Effects 0.000 claims 1
- 238000007906 compression Methods 0.000 claims 1
- 125000004435 hydrogen atom Chemical class [H]* 0.000 claims 1
- 238000005984 hydrogenation reaction Methods 0.000 claims 1
- 230000001590 oxidative effect Effects 0.000 claims 1
- 125000004430 oxygen atom Chemical group O* 0.000 claims 1
- 230000001681 protective effect Effects 0.000 claims 1
- 238000000746 purification Methods 0.000 claims 1
- 125000004434 sulfur atom Chemical group 0.000 claims 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 18
- 239000002023 wood Substances 0.000 description 16
- 240000008042 Zea mays Species 0.000 description 13
- 235000005824 Zea mays ssp. parviglumis Nutrition 0.000 description 13
- 235000002017 Zea mays subsp mays Nutrition 0.000 description 13
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 13
- 235000005822 corn Nutrition 0.000 description 13
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- 239000008213 purified water Substances 0.000 description 10
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 9
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- 239000007864 aqueous solution Substances 0.000 description 8
- 238000010586 diagram Methods 0.000 description 8
- 239000000243 solution Substances 0.000 description 8
- 239000007789 gas Substances 0.000 description 7
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
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- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 4
- 150000001875 compounds Chemical class 0.000 description 4
- 239000012071 phase Substances 0.000 description 4
- 150000004763 sulfides Chemical class 0.000 description 4
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 3
- 239000001273 butane Substances 0.000 description 3
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 3
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 3
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
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- 241000894007 species Species 0.000 description 2
- 150000003464 sulfur compounds Chemical class 0.000 description 2
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- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- PQUCIEFHOVEZAU-UHFFFAOYSA-N Diammonium sulfite Chemical compound [NH4+].[NH4+].[O-]S([O-])=O PQUCIEFHOVEZAU-UHFFFAOYSA-N 0.000 description 1
- 239000008346 aqueous phase Substances 0.000 description 1
- 239000003637 basic solution Substances 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
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- 238000005457 optimization Methods 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
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- IEQIEDJGQAUEQZ-UHFFFAOYSA-N phthalocyanine Chemical compound N1C(N=C2C3=CC=CC=C3C(N=C3C4=CC=CC=C4C(=N4)N3)=N2)=C(C=CC=C2)C2=C1N=C1C2=CC=CC=C2C4=N1 IEQIEDJGQAUEQZ-UHFFFAOYSA-N 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002510 pyrogen Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
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- 239000007787 solid Substances 0.000 description 1
- 238000000629 steam reforming Methods 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- DHCDFWKWKRSZHF-UHFFFAOYSA-L thiosulfate(2-) Chemical compound [O-]S([S-])(=O)=O DHCDFWKWKRSZHF-UHFFFAOYSA-L 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 239000012808 vapor phase Substances 0.000 description 1
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- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
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- C10G1/06—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal by destructive hydrogenation
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- C01B17/00—Sulfur; Compounds thereof
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- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
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- 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
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- C01C1/24—Sulfates of ammonium
- C01C1/245—Preparation from compounds containing nitrogen and sulfur
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- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/74—Treatment of water, waste water, or sewage by oxidation with air
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- C05—FERTILISERS; MANUFACTURE THEREOF
- C05C—NITROGENOUS FERTILISERS
- C05C3/00—Fertilisers containing other salts of ammonia or ammonia itself, e.g. gas liquor
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- C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
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- C10G3/00—Production of liquid hydrocarbon mixtures from oxygen-containing organic materials, e.g. fatty oils, fatty acids
- C10G3/50—Production of liquid hydrocarbon mixtures from oxygen-containing organic materials, e.g. fatty oils, fatty acids in the presence of hydrogen, hydrogen donors or hydrogen generating compounds
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- C10K1/00—Purifying combustible gases containing carbon monoxide
- C10K1/002—Removal of contaminants
- C10K1/003—Removal of contaminants of acid contaminants, e.g. acid gas removal
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- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/04—Liquid carbonaceous fuels essentially based on blends of hydrocarbons
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- 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
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- 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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Description
2H2S + O2→S2 + 2H2O
このプロセスは公知であり、石油製品の精製および改質に広く適用されてきた。しかし、このプロセスは複雑であり、多くの場合、複数の反応工程が関与する。さらに、このプロセスは、分子ベースで25%以上のH2Sを含有する流れに対して、最も効率的に適用することができる。H2Sだけでなくアンモニアも含有する流れがクラウスプラントで処理される場合、H2Sと共にアンモニアも酸化される。アンモニアは、水素化熱分解プロセスからの潜在的価値を有する反応生成物であることから、これは望ましいものではない。
1. 脱酸素化凝縮性炭化水素(ガソリン、ディーゼル、および灯油に対応する特性を有する)、
2. 非凝縮性炭化水素蒸気(メタン、エタン、プロパン、およびブタンなど)、
3. その他の非凝縮性蒸気(CO2、CO、および水素)
4. 水、ならびにアンモニア(NH3)および硫化水素(H2S)などの液体水に可溶性である種。
1. 脱酸素化凝縮性炭化水素(ガソリン、ディーゼル、および灯油に対応する特性を有する)、
2. 非凝縮性炭化水素蒸気(メタン、エタン、プロパン、およびブタンなど)、
3. その他の非凝縮性蒸気(CO2、CO、およびH2)
4. 水、ならびにアンモニア(NH3)および硫化水素(H2S)などの液体水に可溶性である種、
を含んでなる。
Claims (18)
- バイオマスを処理して炭化水素燃料とするための方法であって、
水素化熱分解反応器中にてバイオマスを処理して、チャー(char)、並びに炭化水素および水蒸気を含むプロセス蒸気流を得ること、
前記プロセス蒸気流を凝縮温度まで冷却して、硫化アンモニウムを含む水性流を得ること、
前記水性流を、触媒反応器へ送ること、
前記触媒反応器へ空気を注入して、アンモニア、および硫酸アンモニウムを含有する水性生成物流を得ること、および
H2、CH4、CO、CO2、アンモニア、および硫化水素を含んでなる冷却された生成物蒸気流を得ること、
を含んでなることを特徴とする、方法。 - 内部に空気が注入された前記触媒反応器へ送られる、硫化アンモニウムを含む前記水性流を、約pH9〜12に維持し、および前記水性流中にて、硫黄1原子あたりの酸素原子の比を5超に維持すること、をさらに含んでなる、請求項1に記載の方法。
- 前記冷却された蒸気生成物流から硫化水素を除去すること、
をさらに含んでなる、請求項1に記載の方法。 - 前記冷却された蒸気生成物流から除去された前記硫化水素を、硫化アンモニウムを含む前記水性流と共に前記触媒反応器へ送り、前記水性流中に存在するアンモニアと反応させて、硫酸アンモニウムへ変換するための追加の硫化アンモニウムを形成し、これにより、硫化水素から硫酸アンモニウムへの全体としての高い変換率を得ること、
をさらに含んでなる、請求項3に記載の方法。 - 前記触媒反応器から排出される前記水性生成物流をサワー水ストリッパーで処理して、主としてアンモニアを含んでなる気体流、ならびに主として水および硫酸アンモニウムを含んでなる水性流を得ること、
をさらに含んでなる、請求項1に記載の方法。 - 前記冷却された蒸気生成物流から前記硫化水素を除去して、硫化水素をほとんどまたはまったく含有しない冷却された二次蒸気生成物流を得ること、
をさらに含んでなる、請求項1に記載の方法。 - 前記水素化熱分解反応器から前記チャーを、前記水性生成物流から回収された硫酸アンモニウムと組み合わせること、
をさらに含んでなる、請求項1に記載の方法。 - 前記硫酸アンモニウムと組み合わされた前記チャーをペレット化して、土壌改良剤でもある圧縮栄養剤を作り出すこと、
をさらに含んでなる、請求項7に記載の方法。 - 前記圧縮栄養剤が、農業用肥料をさらに含んでなる、請求項8に記載の方法。
- バイオマス変換生成物から硫黄を除去するための方法であって:
水素化熱分解反応器中にてバイオマスを処理して、チャー、ならびに水素、水蒸気、凝縮性炭化水素蒸気、非凝縮性炭化水素蒸気、一酸化炭素、および二酸化炭素を含有する加熱されたプロセス蒸気流を得ること、
前記加熱されたプロセス蒸気流を凝縮温度まで冷却して、液体炭化水素流、水、アンモニア、および硫化アンモニウムを含有する水性流、H 2 、CH 4 、CO、CO 2 、アンモニア、および硫化水素を含んでなる非凝縮性プロセス蒸気を含有する冷却された生成物蒸気流を分離すること、
前記水性流を、サワー水ストリッパーで処理して、精製液体水流、および硫化アンモニウムを含む溶液を得ること、
前記硫化アンモニウムを含む溶液を触媒反応器へ送り、これにより、触媒上にて硫化アンモニウムを硫酸アンモニウムへ酸化すること、
硫酸アンモニウムを含有する水性生成物流を得ること、
を含んでなることを特徴とする、バイオマス変換生成物から硫黄を除去するための方法。 - 硫酸アンモニウムを含有する前記水性生成物流からアンモニアを除去して、別個の精製気体アンモニア流を作り出す工程、
をさらに含んでなる、請求項10に記載の方法。 - 硫酸アンモニウムを含有する前記水性生成物流をボイラーに導入して、硫酸アンモニウムを、結晶化した硫酸アンモニウムおよび水蒸気に変換する工程、
をさらに含んでなる、請求項11に記載の方法。 - 過剰の水の蒸発およびろ過による結晶化した硫化アンモニウムの分離により、前記水性生成物流から結晶化した硫化アンモニウムを得ること、
をさらに含んでなる、請求項10に記載の方法。 - 前記過剰の水の蒸発により水蒸気が提供され、前記水蒸気を、水蒸気改質器へ送る工程、
をさらに含んでなる、請求項13に記載の方法。 - 前記水蒸気を、保護床を通して、前記水蒸気改質器の上流へ送り、僅かに残留するH2Sを前記水蒸気から除去する工程、
をさらに含んでなる、請求項14に記載の方法。 - 前記過剰の水の蒸発後であって、前記ろ過による結晶化した硫化アンモニウムの分離前に、前記水性生成物流を冷却しする工程、
をさらに含んでなる、請求項13に記載の方法。 - 前記触媒が、モノスルホン化コバルトフタロシアニンである、請求項10に記載の方法。
- 前記触媒反応器中での酸化前に、前記精製液体水流の一部を、硫化アンモニウムを含む溶液と再度組み合わせること、
をさらに含んでなる、請求項10に記載の方法。
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