JP6173333B2 - バイオメタンの製造方法 - Google Patents
バイオメタンの製造方法 Download PDFInfo
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- JP6173333B2 JP6173333B2 JP2014542793A JP2014542793A JP6173333B2 JP 6173333 B2 JP6173333 B2 JP 6173333B2 JP 2014542793 A JP2014542793 A JP 2014542793A JP 2014542793 A JP2014542793 A JP 2014542793A JP 6173333 B2 JP6173333 B2 JP 6173333B2
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- methanation
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- 238000004519 manufacturing process Methods 0.000 title claims description 17
- 238000000034 method Methods 0.000 claims description 79
- 238000002309 gasification Methods 0.000 claims description 48
- 239000007789 gas Substances 0.000 claims description 43
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 40
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 40
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 32
- 230000015572 biosynthetic process Effects 0.000 claims description 29
- 239000002028 Biomass Substances 0.000 claims description 28
- 238000003786 synthesis reaction Methods 0.000 claims description 28
- 238000000746 purification Methods 0.000 claims description 21
- 239000001257 hydrogen Substances 0.000 claims description 19
- 229910052739 hydrogen Inorganic materials 0.000 claims description 19
- 239000002994 raw material Substances 0.000 claims description 19
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 13
- 238000001816 cooling Methods 0.000 claims description 11
- 230000018044 dehydration Effects 0.000 claims description 11
- 238000006297 dehydration reaction Methods 0.000 claims description 11
- 239000004215 Carbon black (E152) Substances 0.000 claims description 10
- 229930195733 hydrocarbon Natural products 0.000 claims description 10
- 150000002430 hydrocarbons Chemical class 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims description 10
- 238000010992 reflux Methods 0.000 claims description 9
- 230000008569 process Effects 0.000 claims description 5
- 238000006243 chemical reaction Methods 0.000 description 31
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 22
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 15
- 229910001868 water Inorganic materials 0.000 description 11
- 239000003054 catalyst Substances 0.000 description 9
- 229910002092 carbon dioxide Inorganic materials 0.000 description 7
- 239000001569 carbon dioxide Substances 0.000 description 7
- 150000001875 compounds Chemical class 0.000 description 7
- 238000000926 separation method Methods 0.000 description 7
- 239000011269 tar Substances 0.000 description 7
- JJWKPURADFRFRB-UHFFFAOYSA-N carbonyl sulfide Chemical compound O=C=S JJWKPURADFRFRB-UHFFFAOYSA-N 0.000 description 6
- 150000002431 hydrogen Chemical class 0.000 description 6
- 238000004088 simulation Methods 0.000 description 6
- 238000001179 sorption measurement Methods 0.000 description 5
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 235000008733 Citrus aurantifolia Nutrition 0.000 description 4
- 235000011941 Tilia x europaea Nutrition 0.000 description 4
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 4
- 239000000571 coke Substances 0.000 description 4
- 238000002485 combustion reaction Methods 0.000 description 4
- 239000000356 contaminant Substances 0.000 description 4
- 238000010586 diagram Methods 0.000 description 4
- 239000004571 lime Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 230000000153 supplemental effect Effects 0.000 description 4
- 238000010521 absorption reaction Methods 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 230000008021 deposition Effects 0.000 description 3
- 239000012530 fluid Substances 0.000 description 3
- 238000002347 injection Methods 0.000 description 3
- 239000007924 injection Substances 0.000 description 3
- 239000003345 natural gas Substances 0.000 description 3
- 238000000197 pyrolysis Methods 0.000 description 3
- 239000003507 refrigerant Substances 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 239000002699 waste material Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- ODINCKMPIJJUCX-UHFFFAOYSA-N Calcium oxide Chemical compound [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 2
- 238000007792 addition Methods 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 229910000019 calcium carbonate Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 230000006835 compression Effects 0.000 description 2
- 238000007906 compression Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
- 239000010450 olivine Substances 0.000 description 2
- 229910052609 olivine Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 230000002829 reductive effect Effects 0.000 description 2
- 238000002407 reforming Methods 0.000 description 2
- 238000011144 upstream manufacturing Methods 0.000 description 2
- 239000011787 zinc oxide Substances 0.000 description 2
- 241001474374 Blennius Species 0.000 description 1
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- 241001465754 Metazoa Species 0.000 description 1
- 241000209140 Triticum Species 0.000 description 1
- 235000021307 Triticum Nutrition 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- 229910002090 carbon oxide Inorganic materials 0.000 description 1
- 235000013339 cereals Nutrition 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003610 charcoal Substances 0.000 description 1
- 238000004939 coking Methods 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 210000003608 fece Anatomy 0.000 description 1
- 239000010794 food waste Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 150000002484 inorganic compounds Chemical class 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 230000000670 limiting effect Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 238000010327 methods by industry Methods 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 235000014593 oils and fats Nutrition 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 230000036961 partial effect Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 239000004576 sand Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 238000011282 treatment Methods 0.000 description 1
- ZIBGPFATKBEMQZ-UHFFFAOYSA-N triethylene glycol Chemical compound OCCOCCOCCO ZIBGPFATKBEMQZ-UHFFFAOYSA-N 0.000 description 1
- 210000002700 urine Anatomy 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
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- C—CHEMISTRY; METALLURGY
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- C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
- C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
- C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
- C10K3/04—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment reducing the carbon monoxide content, e.g. water-gas shift [WGS]
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- 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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- 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
- C01B3/58—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction
- C01B3/586—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction the reaction being a methanation reaction
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
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- C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
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- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
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- C10J2300/00—Details of gasification processes
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
- C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
- C10J2300/1656—Conversion of synthesis gas to chemicals
- C10J2300/1662—Conversion of synthesis gas to chemicals to methane
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- C10J2300/00—Details of gasification processes
- C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
- C10J2300/1807—Recycle loops, e.g. gas, solids, heating medium, water
- C10J2300/1823—Recycle loops, e.g. gas, solids, heating medium, water for synthesis gas
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- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/04—Gasification
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- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/06—Heat exchange, direct or indirect
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- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/08—Drying or removing water
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- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/14—Injection, e.g. in a reactor or a fuel stream during fuel production
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- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
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- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Industrial Gases (AREA)
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- Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
Description
‐本質的に水素(H2)、一酸化炭素(CO)、二酸化炭素(CO2)及びメタン(CH4)からなる合成ガスを生成するためのバイオマスのガス化;
‐水素及び一酸化炭素をメタンに変換することからなる触媒メタン化;
‐特に発熱量(PCS)及びウォッベ指数に関して、天然ガスネットワークへの注入の仕様に適合したバイオメタンを製造するために、残留水素、残留一酸化炭素、水及び二酸化炭素を除去することを目的とした仕様への適合
からなる方法によって実施される。
CO+H2O⇔H2+CO2
に従って、ガス化リアクタの内部で発生する。
CO+3H2⇔CH4+H2O
で表されるという点にある。
CaO(s)+CO2(g)→CaCO3(s)
‐ガス化リアクタ内で合成ガスを生成するための原料のガス化ステップ;
‐精製ユニット内における炭化水素系原料のガス化ステップ時に生成された合成ガスの精製ステップ;
‐メタン化リアクタ内における精製された合成ガスのメタン化ステップ;及び
‐バイオメタンを得るためのメタン化ステップ時に得られた気体混合物の仕様適合ステップ
を含み、仕様適合ステップ時に、少なくとも過剰な一酸化炭素からなる流れを、ガス化リアクタに還流させる。
‐ガス化リアクタ内で合成ガスを生成するために、原料のガス化を実施するガス化リアクタ;
‐原料のガス化リアクタで生成された合成ガスの精製を実施する精製ユニット;
‐精製された合成ガスのメタン化を実施するメタン化リアクタ;及び
‐バイオメタンを得るための、メタン化ステップ時に得られた気体混合物の仕様適合手段
を備え、仕様適合手段は、少なくとも過剰な一酸化炭素からなる流れを、ガス化リアクタに還流させるのに適している。
‐ガス化(201):炭化水素系原料、例えばバイオマスの合成ガス(シンガス)への変換;
‐触媒の寿命に不利に作用する汚染物質を除去するためのガス化ステップ時に生成された合成ガスの精製(204);
‐シンガスのバイオメタンへの変換によるメタン化(206);並びに
‐バイオメタンを、他の成分、特に水素、残留一酸化炭素、水及び二酸化炭素から分離することで、バイオメタンの組成を仕様に適合するよう調節するための、合成ガスのメタン化ステップ時に得られた気体混合物の仕様への適合(207)
の各ステップを必要とする。
‐本来バイオメタンと呼ばれるもので、活用されるメタンからなる第1の流れ;
‐二酸化炭素からなる第2の流れ;
‐水蒸気からなる第3の流れ;及び
‐少なくとも余剰の一酸化炭素、場合によっては、熱化学的平衡が原因で反応を完了できなかった水素からなる第4の流れ
に区分される。
‐ガス化リアクタ内で合成ガスを生成するために、原料のガス化を実施するガス化リアクタ(10);
‐原料のガス化リアクタ(10)で生成された合成ガスの精製を実施する精製ユニット(16);
‐精製された合成ガスのメタン化を実施するメタン化リアクタ(20);及び
‐バイオメタンを得るためのメタン化ステップ時に得られた気体混合物の仕様適合手段(30)
を備えている。
‐流れ100はバイオマス;
‐流れ101はガス化装置に注入される水蒸気;
‐流れ1はガス化装置出口のシンガス;
‐流れ2は冷却されたシンガス;
‐流れ3は脱水されたシンガス;
‐流れ102は復水;
‐流れ103は追加のWGS反応用の水蒸気;
‐流れ4は仕様への適合前のバイオメタン;
‐流れ104はCO/H2;
‐流れ105はCO2;
‐流れ106はH2O
に該当する。
この先行技術による例(図1に示したもの)では、バイオマスは、ガス化リアクタ(10)に投入され、そこでバイオマスは熱化学変換に供され、次いでガス化装置から出た合成ガス(又はシンガス)は、熱交換器(14)内を通過した後、脱水ユニット(15)内へと進入する。水蒸気の冷却及び凝縮によるかかる脱水ステップの後、精製ユニット(16)における精製ステップ(204)と、WGSリアクタ(17)における水蒸気の添加を伴うWGSステップが行われる。次いで、シンガスは、圧縮機(18)における圧縮ステップ(205)に供される。上記の方法で生成され上記の汚染物質を除去されたシンガスはメタン化リアクタ(20)に供給され、次いで、仕様への適合専用のユニット(30)で分離ステップに供される。
この本発明による実施例(図3に示したもの)では、バイオマス供給導管(100)を流動するバイオマスは、ガス化リアクタ(10)に供給され、そこで熱化学変換に供され、次いでガス化装置から出た合成ガス(又はシンガス)は、熱交換器(14)内を通過した後、脱水ユニット(15)内へと進入する。水蒸気の冷却及び凝縮による脱水ステップ(203)の後、精製ユニット(16)における精製ステップが行われる。次いで、シンガスは、圧縮機(18)における圧縮ステップ(205)に供される。上記の方法で生成され上記の汚染物質を除去されたシンガスはメタン化リアクタ(20)に供給され、次いで、仕様への適合専用のユニット(30)で分離ステップに供される。
メタン生成に基づいた方法のエネルギ効率は、以下の式:
ここで
mCH4はメタンの質量、
mbiomasseはバイオマスの質量、
PCICH4はメタンの発熱量、
PCIbiomasseはバイオマスの発熱量である。
‐ガス化によって生成される水素流れが、23.75kmol/hから27.27kmol/hに増加する;
‐シフト水蒸気流れが抑えられる(40.00kmol/h);
‐メタン化の出口において除去される水の流れが、50.57kmol/hから11.85kmol/hまで減少し、この減少分は、本方法によって消費される冷却エネルギ利得に置き換えられる;
‐水素の体積分率の仕様への適合は、メタン化リアクタの出口におけるH2/CH4比が原因で、これ以上必要とはならない複雑な操作であり本方法の効率の損失の原因であったが、これが6.3%から2.7%まで変化する(この改善は主に、メタン化リアクタ内の一酸化炭素の余剰によるものである);
‐装置出口でのバイオメタン(SNG)流れが、11.81kmol/hから13.33kmol/hまで変化し、即ち12.9%の利得となる
を得ることを可能にする。
Claims (12)
- 炭化水素系原料を原料としたバイオメタンの生成方法であって、少なくとも以下のステップ:
‐ガス化リアクタ(10)内で合成ガスを生成するための前記原料のガス化ステップ(201);
‐前記ガス化ステップ(201)の後の前記合成ガスを冷却するための熱交換ステップ(202);
‐前記熱交換ステップの後の前記冷却による復水を除去するために実施される脱水ステップ(203);
‐精製ユニット(16)内における前記ガス化ステップにより生成され前記熱交換ステップおよび前記脱水ステップにより冷却かつ脱水された前記合成ガスの精製ステップ(204);
‐メタン化リアクタ(20)内における精製された前記合成ガスのメタン化ステップ(206);
‐バイオメタンを得るための前記メタン化ステップ時に得られた前記合成ガスの仕様適合ステップ(207)であって、前記仕様適合ステップ(207)時に、少なくとも過剰な一酸化炭素からなる流れを、前記ガス化リアクタ(10)に還流させる(208)ステップ、
を連続的に含む方法。 - 前記方法は、前記合成ガスを4〜80℃の温度に冷却することを特徴とする、請求項1に記載の方法。
- 前記方法は、前記合成ガスを25〜35℃の温度に冷却することを特徴とする、請求項1に記載の方法。
- 前記炭化水素系原料はバイオマスであることを特徴とする、請求項1〜3のいずれか1項に記載の方法。
- 還流される流れは、残留水素を含有することを特徴とする、請求項1〜4のいずれか1項に記載の方法。
- 前記還流される流れは、残留メタンを含有することを特徴とする、請求項1〜5のいずれか1項に記載の方法。
- 前記ガス化リアクタ出口(10)において、前記合成ガスの温度は、600〜1000℃の範囲内となることを特徴とする、請求項1〜6のいずれか1項に記載の方法。
- 前記熱交換ステップ(202)は、前記精製ステップ(204)の前に実施されることを特徴とする、請求項7に記載の方法。
- 前記方法は、0.5〜70barの範囲内の圧力下で実施されることを特徴とする請求項1〜8のいずれか1項に記載の方法。
- 前記メタン化リアクタ出口で得られる前記気体混合物の温度は、250〜700℃の範囲内であることを特徴とする、請求項1〜9のいずれか1項に記載の方法。
- 前記仕様適合ステップの後得られる流れの温度は、周囲温度であることを特徴とする、
請求項1〜10のいずれか1項に記載の方法。 - 炭化水素系原料を原料として、請求項1〜11のいずれか1項に記載の方法を実施するためのバイオメタンの生成デバイスであって、少なくとも:
‐ガス化リアクタ内で合成ガスを生成するために、前記原料のガス化を実施するガス化リアクタ(10);
‐前記ガス化リアクタの後に設けられた前記合成ガスを冷却するための熱交換器(14);
‐前記熱交換器の後に設けられた前記冷却による復水を除去するための脱水ユニット(15);
‐前記原料の前記ガス化リアクタ(10)で生成され前記熱交換器および前記脱水ユニットにより冷却かつ脱水された前記合成ガスの精製を実施する精製ユニット(16);
‐精製された前記合成ガスのメタン化を実施するメタン化リアクタ(20);及び
‐前記バイオメタンを得るための、前記メタン化ステップ時に得られた気体混合物の仕様適合手段(30)であって、少なくとも過剰な一酸化炭素からなる流れを、前記ガス化リアクタに還流させるのに適した手段を備えている仕様適合手段、
から構成されたデバイス。
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