JP2019044238A - 合成ガス生成システム - Google Patents
合成ガス生成システム Download PDFInfo
- Publication number
- JP2019044238A JP2019044238A JP2017169984A JP2017169984A JP2019044238A JP 2019044238 A JP2019044238 A JP 2019044238A JP 2017169984 A JP2017169984 A JP 2017169984A JP 2017169984 A JP2017169984 A JP 2017169984A JP 2019044238 A JP2019044238 A JP 2019044238A
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- Prior art keywords
- cathode
- gas
- anode
- catalyst
- circulation line
- Prior art date
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Links
- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 36
- 238000003786 synthesis reaction Methods 0.000 title claims abstract description 36
- 239000003054 catalyst Substances 0.000 claims abstract description 99
- 239000007788 liquid Substances 0.000 claims abstract description 56
- 229910002091 carbon monoxide Inorganic materials 0.000 claims abstract description 36
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 33
- 239000007864 aqueous solution Substances 0.000 claims abstract description 31
- 239000000203 mixture Substances 0.000 claims abstract description 30
- 238000001514 detection method Methods 0.000 claims abstract description 27
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 72
- 239000001569 carbon dioxide Substances 0.000 claims description 36
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 36
- 239000012530 fluid Substances 0.000 claims description 30
- 238000000926 separation method Methods 0.000 claims description 21
- 238000004519 manufacturing process Methods 0.000 claims description 14
- 238000010521 absorption reaction Methods 0.000 claims description 12
- 229910003771 Gold(I) chloride Inorganic materials 0.000 claims description 9
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 9
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 9
- FDWREHZXQUYJFJ-UHFFFAOYSA-M gold monochloride Chemical compound [Cl-].[Au+] FDWREHZXQUYJFJ-UHFFFAOYSA-M 0.000 claims description 9
- 229910052760 oxygen Inorganic materials 0.000 claims description 9
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 claims description 6
- 238000011144 upstream manufacturing Methods 0.000 claims description 6
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- 101710134784 Agnoprotein Proteins 0.000 claims description 3
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- ADZWSOLPGZMUMY-UHFFFAOYSA-M silver bromide Chemical compound [Ag]Br ADZWSOLPGZMUMY-UHFFFAOYSA-M 0.000 claims description 3
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- 229910052744 lithium Inorganic materials 0.000 claims description 2
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- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 abstract description 27
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- 239000000243 solution Substances 0.000 abstract 1
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- 239000002250 absorbent Substances 0.000 description 2
- 230000002745 absorbent Effects 0.000 description 2
- 238000005341 cation exchange Methods 0.000 description 2
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
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- 239000005977 Ethylene Substances 0.000 description 1
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- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- NPYPAHLBTDXSSS-UHFFFAOYSA-N Potassium ion Chemical compound [K+] NPYPAHLBTDXSSS-UHFFFAOYSA-N 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- FKNQFGJONOIPTF-UHFFFAOYSA-N Sodium cation Chemical compound [Na+] FKNQFGJONOIPTF-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- -1 U.S. Pat. No. 5 Chemical compound 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 229910003460 diamond Inorganic materials 0.000 description 1
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- 238000001704 evaporation Methods 0.000 description 1
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- 239000000284 extract Substances 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- GPRLSGONYQIRFK-UHFFFAOYSA-N hydron Chemical compound [H+] GPRLSGONYQIRFK-UHFFFAOYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 239000011133 lead Substances 0.000 description 1
- 229910001416 lithium ion Inorganic materials 0.000 description 1
- 229910001092 metal group alloy Inorganic materials 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 229910001414 potassium ion Inorganic materials 0.000 description 1
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 239000000741 silica gel Substances 0.000 description 1
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- 239000004332 silver Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
- 229910001415 sodium ion Inorganic materials 0.000 description 1
- 238000000638 solvent extraction Methods 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 230000002123 temporal effect Effects 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- ZIBGPFATKBEMQZ-UHFFFAOYSA-N triethylene glycol Chemical compound OCCOCCOCCO ZIBGPFATKBEMQZ-UHFFFAOYSA-N 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
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- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
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Abstract
【解決手段】 CO2を含む水溶液の電気還元によってCO及びH2を生成する合成ガス生成システム1であって、隔膜3によって区画されたアノード室4及びカソード室5を有する電解装置6と、カソード室に接続され、CO2を含むカソード液を循環させるカソード側循環ライン7と、カソード側循環ラインに設けられ、カソード液にCO生成触媒を供給する触媒供給装置29と、カソード室において生成した生成ガスのCO及びH2の比を測定するガス組成検出装置35とを有し、ガス組成検出装置の検出結果に基づいて、生成ガスにおけるCOに対するH2の比を所定の目標範囲にすべく、触媒供給装置によるCO生成触媒の供給量の制御、及び電解装置によるアノード15及びカソード16間に印加する電圧の制御の少なくとも一方を実行する。
【選択図】 図1
Description
実験1では、電解装置におけるアノード及びカソード間の電流密度が、生成ガスのH2/CO比に与える影響を確認した。使用した電解装置は、容器と、容器の内室をアノード室及びカソード室に区画するアニオン交換膜と、アノード室に配置された白金メッシュ電極であるアノードと、カソード室に配置された黒鉛電極であるカソードとを有する。アノード室及びカソード室には、電解質としてKHCO3、CO生成触媒としてZn(OCOCH3)2を含む水溶液を満たした。水溶液には、二酸化炭素ガスのバブリングを常時行い、水溶液中の二酸化炭素濃度を飽和状態にした。アノード及びカソード間の電流密度が5〜40mA/cm2の所定の値となるように印加電圧を調節し、定電流を30分間流した。この間、水溶液の温度は25℃に維持した。電圧の印加開始から30分後にアノード室の生成ガスを回収し、ガスクロマトグラフィーによって組成分析を行った。
実験2では、CO生成触媒の濃度が、生成ガスのH2/CO比に与える影響を確認した。使用した電解装置は、実験1と同様である。アノード室及びカソード室には、電解質としてKHCO3、CO生成触媒としてZn(OCOCH3)2を含む水溶液を満たした。水溶液は、Zn(OCOCH3)の濃度を変化させたものを複数用意した。水溶液には、二酸化炭素ガスのバブリングを常時行い、水溶液中の二酸化炭素濃度を飽和状態にした。アノード及びカソード間の電流密度が5mA/cm2の所定の値となるように印加電圧を調節し、定電流を30分間流した。この間、水溶液の温度は25℃に維持した。電圧の印加開始から30分後にアノード室の生成ガスを回収し、ガスクロマトグラフィーによって組成分析を行った。
実験3では、生成ガスのH2/CO比の経時変化を確認した。使用した電解装置は、実験1と同様である。アノード室及びカソード室には、電解質としてKHCO3、CO生成触媒としてZnCO3を含む水溶液を満たした。水溶液には、二酸化炭素ガスのバブリングを常時行い、水溶液中の二酸化炭素濃度を飽和状態にした。アノード及びカソード間の電流密度が30mA/cm2の所定の値となるように印加電圧を調節し、定電流を100時間流した。この間、水溶液の温度は25℃に維持した。また、任意の時間においてアノード室の生成ガスを回収し、ガスクロマトグラフィーによって組成分析を行った。また、組成分析の結果、H2/CO比が1.8以上になった時点においてZnCO3を水溶液に添加した。
3 :隔膜
4 :アノード室
5 :カソード室
6 :電解装置
7 :アノード側循環ライン
8 :カソード側循環ライン
14 :電気分解槽
15 :アノード
16 :カソード
23 :電源装置
24 :制御装置
25 :カソード側気液分離装置
26 :切替弁
27 :水供給装置
28 :電解質供給装置
29 :CO生成触媒供給装置
30 :二酸化炭素吸収槽
31 :バイパスライン
32 :生成ガスライン
33 :生成ガスタンク
34 :除湿塔
35 :ガス組成検出装置
37 :固液分離装置
41 :アノード側気液分離装置
42 :水供給装置
43 :電解質供給装置
Claims (10)
- CO2を含む水溶液の電気還元によってCO及びH2を生成する合成ガス生成システムであって、
アノードを有するアノード室、カソードを有するカソード室、及び前記アノード室と前記カソード室とを区画する隔膜を有する電解装置と、
前記カソード室に接続され、CO2を含むカソード液を循環させるカソード側循環ラインと、
前記カソード側循環ラインに設けられ、前記カソード液にCO生成触媒を供給する触媒供給装置と、
前記カソード室において生成した生成ガスのCO及びH2の比を測定するガス組成検出装置とを有し、
前記ガス組成検出装置の検出結果に基づいて、前記生成ガスにおけるCOに対するH2の比を所定の目標範囲にすべく、前記触媒供給装置によるCO生成触媒の供給量の制御、及び前記電解装置による前記アノード及び前記カソード間に印加する電圧の制御の少なくとも一方を実行することを特徴とする合成ガス生成システム。 - 前記カソード側循環ラインと並列に設けられ、上流端及び下流端が前記カソード側循環ラインに接続されたバイパスラインと、
前記バイパスラインに流れる前記カソード液の流量を制御する流量制御弁と、
前記バイパスラインに設けられた固液分離装置とを更に有することを特徴とする請求項1に記載の合成ガス生成システム。 - CO2を含む水溶液の電気還元によってCO及びH2を生成する合成ガス生成システムであって、
アノードを有するアノード室、カソードを有するカソード室、及び前記アノード室と前記カソード室とを区画する隔膜を有する電解装置と、
前記カソード室に接続され、CO2を含むカソード液を循環させるカソード側循環ラインと、
前記カソード側循環ラインに設けられ、前記カソード液にCO生成触媒を供給する触媒供給装置と、
前記カソード室において生成した生成ガスのCO及びH2の比を測定するガス組成検出装置と、
前記カソード側循環ラインと並列に設けられ、上流端及び下流端が前記カソード側循環ラインに接続されたバイパスラインと、
前記バイパスラインに流れる前記カソード液の流量を制御する流量制御弁と、
前記バイパスラインに設けられた固液分離装置とを有し、
前記ガス組成検出装置の検出結果に基づいて、前記生成ガスにおけるCOに対するH2の比を所定の目標範囲にすべく、前記触媒供給装置によるCO生成触媒の供給量の制御、前記流量制御弁による前記固液分離装置に供給する前記カソード液の流量の制御及び前記電解装置による前記アノード及び前記カソード間に印加する電圧の制御の少なくとも1つを実行することを特徴とする合成ガス生成システム。 - 前記目標範囲は、COに対するH2のモル比率が0.25以上2.5以下に設定されていることを特徴とする請求項1〜請求項3のいずれか1つの項に記載の合成ガス生成システム。
- 前記CO生成触媒は、粉末、水溶液、及び懸濁液の少なくとも1つの状態で前記カソード液に供給されることを特徴とする請求項1〜請求項4のいずれか1つの項に記載の合成ガス生成システム。
- 前記CO生成触媒が、Zn、ZnO、ZnO2、ZnO3、ZnSO4、Zn(NO3)2、ZnCl2、ZnBr2、ZnI2、Zn(OCOCH3)2、Ag、AgO、Ag2O、Ag2O3、AgNO3、AgCl、AgBr、Ag(OCOCH3)、Au、AuCl、AuCl3、H[AuCl4]、AuBr3、H[AuBr4]、Au(OCOCH3)、Au(OCOCH3)3からなる群の少なくとも1つを含むことを特徴とする請求項1〜請求項5のいずれか1つの項に記載の合成ガス生成システム。
- 前記カソード液は、LiOH、NaOH、KOH、Li2CO3、Na2CO3、K2CO3、LiHCO3、NaHCO3、及びKHCO3からなる群の少なくとも1つを含むことを特徴とする請求項1〜請求項6のいずれか1つの項に記載の合成ガス生成システム。
- 前記カソード側循環ラインに設けられ、気体のCO2を前記カソード液に接触させ、前記カソード液にCO2を吸収させる二酸化炭素吸収槽を更に有することを特徴とする請求項1〜請求項7に記載の合成ガス生成システム。
- 前記カソード側循環ラインに設けられ、前記生成ガスと前記カソード液とを分離する気液分離装置を更に有することを特徴とする請求項1〜請求項8に記載の合成ガス生成システム。
- 前記カソード側循環ラインと独立して前記アノード室に接続され、アノード液を循環させるアノード側循環ラインを更に有することを特徴とする請求項1〜請求項9に記載の合成ガス生成システム。
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