JP5782400B2 - 脱硫システム、水素製造システム、燃料電池システム、燃料の脱硫方法及び水素の製造方法 - Google Patents
脱硫システム、水素製造システム、燃料電池システム、燃料の脱硫方法及び水素の製造方法 Download PDFInfo
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Description
市販のγ−アルミナ担体に、金属Ni量で8質量%の硝酸ニッケル・六水和物を、含浸法により担持し、120℃で3時間乾燥後、400℃で3時間焼成しNi/Al2O3触媒(以下、触媒前駆体A)を得た。触媒前駆体A中の酸化ニッケルの担持量は触媒前駆体A全量基準で10質量%であった。
硝酸ニッケル六水和物(市販試薬特級)272.5gと硝酸亜鉛六水和物(市販試薬特級)54.8gをイオン交換水に溶解し、2500mlとした水溶液をA液とした。炭酸ナトリウム(市販試薬特級)130.8gをイオン交換水に溶解し、市販のシリカゾル(粒径約15nm)50g(シリカ含有量15.0g)と混合、1000mlとした溶液をB液とした。A液とB液を攪拌しながら40℃にて混合し、沈殿を形成した。沈殿をイオン交換水で洗浄後、得られたケーキを粉砕し、120℃で10時間乾燥後、360℃で4時間焼成し、焼成粉100gを得た。焼成粉の組成はNiO/ZnO/SiO2=70質量%/15質量%/15質量%、残存Naは0.05質量%以下であった。得られた焼成粉を1mmφにて押出成型し、触媒前駆体Bとした。
市販のγ−アルミナ担体に、金属Cu量で26質量%の硝酸銅・三水和物を、含浸法により担持し、120℃で3時間乾燥後、400℃で3時間焼成しCu/Al2O3触媒(以下、触媒前駆体C)を得た。触媒前駆体C中の酸化銅の担持量は触媒前駆体C全量基準で10質量%であった。
触媒前駆体A6mlを固定床流通式反応管に充填し、GHSV=30h−1、400℃で6時間水素還元を施して、脱硫触媒Aを調製した。ジメチルスルフィド(DMS)を80容量ppm含みかつ酸素濃度0.5容量%のメタンガス51容量%、水素32容量%、一酸化炭素4容量%、二酸化炭素13容量%の燃料ガス(燃料ガス中の酸素濃度は0.26容量%)を、GHSV=1000h−1にて、常圧、350℃で流通させた。反応管出口の硫黄濃度を、SCD(Sulfur Chemiluminescence Detector)ガスクロマトグラフィーにより測定した。実験開始後、出口ガスのDMS濃度が0.05容量ppm以上となったところでガスの流通を止め、実験開始から実験終了までの間に脱硫触媒Aに吸着されたDSM量を算出し、脱硫性能を求めた。なお、本性能試験において、ジメチルジスルフィドは、耐久性能評価の面で通常より燃料中に高濃度含有されている。
メタンガスの酸素濃度を4.0容量%(燃料ガス中の酸素濃度は2.0容量%)に変更したこと以外は、実施例1と同様にして実験を行い、脱硫性能を求めた。
メタンガスの酸素濃度を0容量%に変更したこと以外は、実施例1と同様にして実験を行い、脱硫性能を求めた。
触媒前駆体Aにかえて触媒前駆体B6mlを固定床流通式反応管に充填し、GHSV=30h−1、400℃で6時間水素還元を施して、脱硫触媒Bを調製した。次いで、燃料ガスの水素含有量を0容量%、脱硫温度を250℃に変更したこと以外は実施例1、実施例2又は参考例1と同様にして実験を行い、脱硫性能を求めた。
燃料ガスの水素含有量を8容量%、1容量%又は0.5容量%に変更したこと以外は、実施例1と同様にして実験を行い、脱硫性能を求めた。
脱硫温度を100℃に変更したこと以外は実施例1、実施例2又は参考例1と同様にして実験を行い、脱硫性能を求めた。
触媒前駆体Aにかえて触媒前駆体C6mlを固定床流通式反応管に充填し、GHSV=30h−1、400℃で6時間水素還元を施して、脱硫触媒Cを調製したこと以外は、実施例1、実施例2又は参考例1と同様にして実験を行い、脱硫性能を求めた。
Claims (9)
- 炭化水素系燃料と、硫黄化合物と、0.1容量%〜4容量%の酸素と、1容量%〜50容量%の水素とを含む燃料組成物を後段に供給する燃料供給部と、
前記燃料供給部から供給された前記燃料組成物を、Niを含有する脱硫触媒を用いて150〜450℃で脱硫する脱硫部と、を備え、
前記脱硫触媒におけるNiの含有量が、酸化物換算で、前記脱硫触媒の全量を基準として20〜60質量%である、脱硫システム。 - 前記脱硫触媒が、Zn、Cu、Fe及びCoからなる群より選択される1種以上の金属を更に含有する、請求項1に記載の脱硫システム。
- 前記脱硫部が、前記脱硫触媒と、前記脱硫触媒の後段に具備されたZn、Cu、Fe及びCoからなる群より選択される1種以上の金属を含有する第二の脱硫触媒と、を有する、請求項1に記載の脱硫システム。
- 前記炭化水素系燃料が、メタンを80容量%以上含むガスである、請求項1〜3のいずれか一項に記載の脱硫システム。
- 請求項1〜4のいずれか一項に記載の脱硫システムと、前記脱硫部で脱硫した前記燃料組成物から水素を発生させる水素発生部と、を備える、水素製造システム。
- 請求項5に記載の水素製造システムを備える、燃料電池システム。
- 炭化水素系燃料と、硫黄化合物と、0.1容量%〜4容量%の酸素と、1容量%〜50容量%の水素とを含む燃料組成物を、Niを含有する脱硫触媒を用いて150〜450℃で脱硫する工程を備え、
前記脱硫触媒におけるNiの含有量が、酸化物換算で、前記脱硫触媒の全量を基準として20〜60質量%でる、燃料の脱硫方法。 - 前記炭化水素系燃料が、メタンを80容量%以上含むガスである、請求項7に記載の燃料の脱硫方法。
- 請求項7に記載の燃料の脱硫方法によって脱硫された前記燃料組成物を改質して水素を得る工程を備える、水素の製造方法。
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Application Number | Priority Date | Filing Date | Title |
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JP2012074668A JP5782400B2 (ja) | 2012-03-28 | 2012-03-28 | 脱硫システム、水素製造システム、燃料電池システム、燃料の脱硫方法及び水素の製造方法 |
PCT/JP2013/056498 WO2013146198A1 (ja) | 2012-03-28 | 2013-03-08 | 脱硫システム、水素製造システム、燃料電池システム、燃料の脱硫方法及び水素の製造方法 |
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