热化学硫碘循环制氢中Bunsen反应与碘化氢分解的模拟与实验研究

【作者】 刘广义；

【导师】 周俊虎； 刘建忠；

【作者基本信息】 浙江大学 ， 工程热物理， 2006， 硕士

【摘要】 当今世界，为了解决能源短缺、环境污染日益严重等问题，洁净的新能源开发已是迫在眉睫。氢能是一种洁净的能源载体，热化学循环制氢是通过一系列的化学反应在较低的温度下使水分解制取氢气的方法。本文研究了最接近工业化阶段的热化学循环——硫碘循环（SI循环）中的Bunsen反应和碘化氢分解反应。 本文首先利用FactSage软件对Bunsen反应和碘化氢分解的热力学平衡进行了模拟。研究了反应物比例、温度、压力对bunsen反应的影响，温度、压力、膜反应器和水的存在对碘化氢分解热力学平衡状态的影响，对选择Bunsen反应和碘化氢分解的条件提供了一定的参考。 其次，利用恒温型磁力搅拌器加热，使用全自动电位滴定仪滴定离子浓度，在自制的反应器上进行了HI、H₂SO₄、I₂的混合溶液的分层现象和副反应的实验，研究了不同温度、不同浓度的溶液中分层现象的出现，研究了水含量、温度和碘量对液液分离特性的影响和对副反应的影响。温度范围20-70℃。 再次，提出了碘化氢均相反应的动力学机理，利用CHEMKIN软件包对碘化氢分解动力学进行了模拟，研究了反应时间、温度和压力对碘化氢分解动力学的影响，并与热力学平衡的结果进行了对照。温度范围300-900℃。 最后，利用溶胶-凝胶法制备了5种Pt催化剂，使用XRO和氮吸附法对Pt催化剂和沸石的晶体结构和表面织构进行了表征。在管式反应器上通过电炉加热进行了碘化氢均相分解和催化分解实验，研究了不同温度下的HI分解率，比较了6种催化剂的催化效果。更多还原

【Abstract】 Drawbacks to fossil fuel utilization include limited supply and pollution. Hydrogen is a environmentally attractive transportation fuel that has the potential to replace fossile fuels. Thermochemical water-splitting is the conversion of water into hydrogen and oxygen by a series of thermally driven chemical reactions. Bunsen reaction and hydrogen iodide decomposition in IS（iodine-sulfur） cycle, the most industrialized thermochemical cycle was studied.Firstly, the thermodynamic equilibrium of Bunsen reaction and hydrogen iodide decomposition were examined. The effect of reactant ratio、 temperature and pressure on the thermodynamic equilibrium of Bunsen reaction were discussed and the effect of temperature、 pressure、 membrane reactor and vapor on the thermodynamic equilibrium of hydrogen iodide decomposition were discussed too. The results are helpful to find the proper condition of Bunsen reaction and hydrogen iodide decomposition.Secondly, separation characteristics of 2 liquid phrase and side-reactions from HI、 H₂SO₄、I₂ were investigated experimentally in operating temperature range,from 20℃ to 70℃. The effects of solution temperature 、acid concentration and iodine concentration on separation characteristics of 2 liquid phrase and side-reactions were discussed. Iodine concentration at the point where the solution starts to separate were determined.Thirdly, a dynamic model of homogeneous decomposition of hydrogen iodine were put forward and kinetic simulation of hydrogen iodine homogeneous decomposition was made on different reactive time、 temperature（range from 300°C to 900°C） and pressure.At last, 5 Pt catalysts was successfully prepared by the Sol-Gel method. The composition, microgram and pore size distribution of 6 catalysts（including 5 Pt catalysts and zeolite） are studied by the XRD and Nitrogen adsorption method. The homogeneous and catalytic decomposition of hydrogen iodine were studied experimentally with a tube type electric furnace. The conversion of hydrogen iodine was examined on different temperature.更多还原