| CoMoSx/γ-Al2O3催化剂在还原脱硫中的吸附性能和催化活性 |
| Adsorption Properties and Catalytic Activity of CoMoSx/γ-Al2O3 Catalysts in Reduction Desulfurization |
| 作者 | 单位 | E-mail | | 刘哲男 | 北京理工大学化学与化工学院, 北京 100081 | | | 耿云峰 | 北京北大先锋科技有限公司, 北京 100080 | | | 石泉 | 北京理工大学化学与化工学院, 北京 100081 | | | 黎汉生 | 北京理工大学化学与化工学院, 北京 100081 | hanshengli@bit.edu.cn | | 史大昕 | 北京理工大学化学与化工学院, 北京 100081 | | | 吴芹 | 北京理工大学化学与化工学院, 北京 100081 | | | 赵芸 | 北京理工大学化学与化工学院, 北京 100081 | | | 冯彩虹 | 北京理工大学化学与化工学院, 北京 100081 | | | 矫庆泽 | 北京理工大学化学与化工学院, 北京 100081
北京理工大学珠海学院化工与材料学院, 珠海 519085 | |
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| 摘要: 以等体积浸渍法与原位还原硫化法相结合制备了CoMoSx/γ-Al2O3催化剂。采用X射线衍射（XRD）、扫面电子显微镜/能谱（SEM/EDS）、X射线光电子能谱（XPS）、程序升温脱附/程序升温还原/程序升温表面反应-质谱分析（TPD/TPR/TPSR-MS）对催化剂进行了表征，系统地研究了CoMoSx/γ-Al2O3催化剂的结构、表面CO和SO2的吸附-脱附行为及其表面反应特性。采用微型固定床反应器评价了CoMoSx/γ-Al2O3催化剂的催化特性。研究表明，CoMoSx/γ-Al2O3催化剂由γ-Al2O3和高分散的Co-Mo-S组成，预硫化过程中不会出现CoS2和Co9S8等硫化物。γ-Al2O3几乎不会吸附CO，CoMoSx对CO具有强吸附作用；而γ-Al2O3和CoMoSx都可以吸附SO2，但γ-Al2O3的吸附作用较弱，CoMoSx的吸附作用较强。在γ-Al2O3上会吸附微量的COS，而CoMoSx不会吸附COS。在SO2与CO的表面反应中，吸附在CoMoSx上的SO2会与CO发生反应，而吸附在γ-Al2O3上的SO2不会发生反应。在400℃时，SO2的转化率和硫单质的选择性都接近100%。 |
| 关键词: 还原脱硫 一氧化碳 二氧化硫 钴 钼 氧化铝 吸附 |
| 基金项目: |
| Abstract: CoMoSx/γ-Al2O3 catalyst was prepared by using an impregnation method combining with in-situ reduction method. In order to systematically obtain the structure of the CoMoSx/γ-Al2O3 catalyst and study the adsorption-desorption performance and the surface reactions of CO and SO2, the catalyst was characterized using X-ray diffraction (XRD), scanning electron microscope/energy dispersive spectrdmeter (SEM/EDS), X-ray photoelectron spectroscopy (XPS), temperature programmed desorption/programmed temperature reduction/temperature progra-mmed surface reaction-mass spectrometry (TPD/TPR/TPSR-MS). The catalytic performances of the CoMoSx/γ-Al2O3 catalyst were tested in a packed-bed microreactor. The results show that the CoMoSx/γ-Al2O3 catalyst was composed of γ-Al2O3 and highly dispersed Co-Mo-S. During the pre-vulcanization, no sulfides such as CoS2 and Co9S8 were formed. CO was adsorbed on CoMoSx instead of γ-Al2O3. SO2 was weakly adsorbed on γ-Al2O3 but strongly adsorbed on CoMoSx. COS was adsorbed on γ-Al2O3 with a small amount, but not adsorbed on CoMoSx. Furthermore, SO2 adsorbed on CoMoSx was active and reacted with CO adsorbed on CoMoSx, while SO2 adsorbed on γ-Al2O3 did not react. Finally, the conversion of SO2 and the selectivity of sulfur were obtained up to 100% at 400℃. |
| Keywords: reduction desulfurization carbon monoxide sulfur dioxide cobalt molybdenum alumina adsorption |
| 投稿时间：2018-08-20 修订日期：2018-10-19 |
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| 刘哲男,耿云峰,石泉,黎汉生,史大昕,吴芹,赵芸,冯彩虹,矫庆泽.CoMoSx/γ-Al2O3催化剂在还原脱硫中的吸附性能和催化活性[J].无机化学学报,2019,35(1):34-42. |
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