成果報告書詳細
管理番号20120000000028
タイトル*平成22年度中間年報 水素製造・輸送・貯蔵システム等技術開発 水素製造機器要素技術に関する研究開発 水素分離型リフォーマーの高耐久化・低コスト化研究開発(1)
公開日2012/2/17
報告書年度2010 - 2010
委託先名東京瓦斯株式会社
プロジェクト番号P08003
部署名新エネルギー部
和文要約和文要約等以下本編抜粋:1. 研究開発の内容及び成果等 (i)水素分離型リフォーマーシステムの耐久性向上の研究開発 (1)水素分離膜の耐久性・信頼性の検証試験 2005年から2007年まで実施した「水素安全利用等基盤技術開発事業 水素インフラに関する研究開発 高効率水素製造メンブレン技術の開発」(以下、「前事業」)にて水素製造効率81.4%を達成した40 Nm3/h級水素分離型リフォーマーシステム(図1)の運転試験を継続し、水素分離膜モジュール及びシステムの耐久性、及び長期連続運転よるシステムの運転安定性を検証し、課題抽出を行った。昨年度まで総運転時間2300時間、起動回数62回であったシステムの運転を継続し、総運転時間は4000時間、起動回数は86回となり、水素純度は99.99%を維持していることを確認した。
英文要約Title:Development of Technologies for Hydrogen Production, Delivery, and Storage Systems. Development of Elemental Technologies for Hydrogen Production Components. Research and Development for Increase of Durability and Cost Reduction of Membrane Reformer (FY2008 - FY2012) FY2010 Annual Report

Durability verification test of the 2nd 40Nm3/h-class membrane reformer system, which has achieved 81.4% HHV efficiency in hydrogen production in the previous NEDO project, was continued to clarify the issues on stable operation. The hydrogen purity was over 99.99% after 4000 h operation and 86 times starts and stops. The longest continuous operation h without any trouble increased to 810 h from 640 h, but it is clear that more improvement is required to ensure stability of the membrane reformer system.
Dismantling investigation of the most deteriorated membrane unit, which includes two membrane modules, in the membrane reformer system has been carried out to investigate the cause of the leakage from the modules after 4000 h operation. After the appearance and leakage inspection, the catalyst and membrane were investigated. Leakages from the two modules in the unit were 27.2 Ncc/min and 21.7 Ncc/min. While the catalytic activity of the catalyst is high enough, dozens of pin halls were observed in the membrane modules. Extrinsic particles were observed at the center of the most pin halls and Fe, Al, Si were detected by electron probe X-ray microanalysis (EPMA). The investigation revealed that the pin halls were caused by mainly the attachment of extrinsic particles on the membranes.
In addition to the system durability test, module-level durability test has been done with an improved unit for 13000 h. The purity of produced hydrogen was 99.99%, even after 13000 h operation. Dismantling investigation of the tested module after 13000 h operation was been carried out to investigate the cause of degradation of hydrogen purity and flux. Leakages from the two modules in the unit were 0.55 Ncc/min and non-detected (lower than 0.2 Ncc/min). The catalytic activity of the catalyst is high enough even after 13000 h operation. Only two pin halls were observed in one of the membrane modules and Fe, Al, and Si were detected by EPMA. The leakage was caused by extrinsic particles or impurities in the membrane.
Solutions for the issues on long-term stability were examined and the auxiliaries of the membrane reformer were improved. During the durability test, several auxiliaries, such as a boiler and a flare stack, were repaired and improved after their troubles, then the stability and reliability of the system has been improved.
Long-term hydrogen permeation test and reforming test were carried out with Membrane On Catalyst (MOC) modules. In the hydrogen permeation test, hydrogen permeability was maintained even after about 8000 h permeation at 550 deg C. However, leakage increased during the test. In the reforming test, the increase of leakage also turned out to be a significant issue with a MOC module.
In addition, rapid start-up tests were carried out with a MOC module and a small-scale test reformer which consists of four MOC modules. In both tests, rapid start-up within three hs and hydrogen purity over 99.99 vol % were demonstrated. However, some MOC modules in the test reformer were damaged maybe because of rapid temperature drop.
Long-term reforming test was carried out with an advanced MOC module which was developed to prevent leakage. In the reforming test, the product hydrogen purity was as high as 99.9988 vol % even after more than 1000 h reforming at 550 deg C. This result showed that durability against leakage improved dramatically in the advanced MOC module. However, the advanced MOC module still had room for improvement because it showed lower reforming performance than the original MOC module.
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