【摘要】 介绍了固定床两段法甲烷部分氧化制合成气的新工艺 ,对在改性的La -Mn系钙钛矿催化剂上发生的甲烷低温燃烧进行了初步考察 ,比较系统地考察了温度、压力等工艺条件对两段法造气工艺的影响 ,结合本实验室的专利催化剂La2 O3 -Ni/MgAl2 O4 ,进行了两段法工艺 30 0h加压稳定性实验。结果表明 :将甲烷低温催化燃烧与部分氧化相结合 ,采用分段进氧方式的两段法工艺可使甲烷与氧气的混合更偏离爆炸极限 ,保证了安全生产。同时利用一段甲烷燃烧放出的热量将原料预热到二段反应所需的温度 ,并在二段反应器中将放热的部分氧化反应与吸热的重整反应相结合 ,可保证整个造气过程在绝热条件下操作 ,有效避免了部分氧化催化剂床层飞温。高温、加压稳定性实验表明 ,La -Mn钙钛矿贫氧催化燃烧催化剂和部分氧化催化剂La2 O3 -Ni/MgAl2 O4 催化活性稳定 ,适应长周期运行。以上这一切都表明两段法造气工艺拥有良好的工业开发前景。更多还原

【Abstract】 A novel two-stage fixed bed reactor for catalytic partial oxidation of methane to syngas was introduced. The effects of reaction conditions (such as temperature, pressure etc.) on two-stage process and on the performance of developed La-Mn perovskite-type catalyst in the complete combustion of methane were investigated. Furthermore using La 2O 3-Ni/MgAl 2O 4 partial oxidation catalyst, 300 hours stability experiment of two-stage process was finished. The results show that the introduction of O 2 in two stages can reduce the explosion danger in operation through the decrease of CH 4/O 2 ration. A portion of methane that was burned to CO 2 and H 2O in the first reactor can give out combustion heat to pre-heat the feed of the second reactor. In the second reactor, endothermic CO 2 and H 2O reforming reaction and exothermic CH 4 partial oxidation are integrated. In this way, adiabatic operation can be realized and avoid the appearance of hot spot in the second reactor. The results of the 300 hours stability test of two-stage process show that La-Mn perovskite-type catalyst and La 2O 3-Ni/MgAl 2O 4 partial oxidation catalyst all maintained high catalytic activity and good stability. All results indicate that two-stage process may be used in industry.更多还原