成果報告書詳細
管理番号20160000000249
タイトル*平成27年度中間年報 エネルギー・環境新技術先導プログラム 低環境負荷アンモニア製造法の研究開発
公開日2016/5/17
報告書年度2015 - 2015
委託先名国立大学法人名古屋工業大学 日揮株式会社 学校法人名古屋電気学園愛知工業大学
プロジェクト番号P14004
部署名イノベーション推進部
和文要約
英文要約Development of Environmental-friendly Ammonia Production System
Ammonia is an essential compound as a source of many chemicals. In industry, it is synthesized by the Haber–Bosch process from N2 and H2. The method, however, is accomplished under environmentally demanding conditions of high temperature and high pressure, and furthermore, the H2 gas used in the process is produced by steam reformation of fossil fuels. For a next energy generation process, it is desirable to produce NH3 from a hydrogen source derived from H2O. A number of researchers in various chemical fields have investigated conversion of N2 to NH3 under mild conditions, and transition metal complexes have been found to promote electrochemical generation of NH3 as catalysts. Among of them, Becker and co−workers reported that titanocene dichloride, Cp2TiCl2, could reduce N2 to NH3 when the controlled−potential electrolysis (CPE) is carried out at −2.2 V (vs. Ag wire) in MeOH solution containing 0.3 M LiClO4 and 0.25 M catechol. This reaction proceeds at room temperature under 1 atm using hydrogen atoms from catechol and/or MeOH, but the yield of NH3 per Cp2TiCl2 and the current efficiency were both found to be quite low, 1.45% and 0.28 %, respectively. In order to improve this reaction, we decided to carry out CPE using a solid polymer electrolyte cell (SPE cell), which is composed of a working electrode (W.E.) and a counter electrode (C.E.) separated by a proton exchange membrane. In the previously reported electrochemical synthesis of NH3 in an SPE cell, a proton was generated by oxidation of H2O at C.E., which was transferred to the W.E. to react with N2. It is advantageous that the proton originating from H2O oxidation is employed and the generated O2 is separated from the W.E. by proton exchange membrane. Thus, it is possible to use H2O as the hydrogen source.
In this project, we performed the electrochemical reduction of N2 to NH3 using a W.E. coated with Cp2TiCl2–supported ionic liquid in an SPE cell under ambient conditions, where an ionic liquid has recently been employed in a number of different research efforts, because it has several unique properties such as low volatility, an electrochemical window, high thermal and chemical stability, and electric conductivity. The problems in our system are as follows; (i) low-stability of the catalyst in the catalytic cycle, (ii) high overpotential in dinitrogen reduction, (iii) low current efficiency in the electrochemical dinitrogen reduction, and (iv) evolution of dihydrogen gas. In order to resolve these problems, we mainly investigate on the preparation of catalytically active and highly stable metal complexes, the development of high performance reaction field using the ionic liquid, and fabrication of the electrochemical reduction cells.
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