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作 者:熊莲[1,2] 罗彩容[1,2] 郭海军[1,2] 陈新德[1,2] 陈勇[3]
机构地区:[1]中国科学院可再生能源与天然气水合物重点实验室,广东广州510640 [2]中国科学院广州能源研究所,广东广州510640 [3]中国科学院广州分院,广东广州510640
出 处:《石油学报(石油加工)》2012年第3期470-475,共6页Acta Petrolei Sinica(Petroleum Processing Section)
基 金:中国科学院可再生能源与天然气水合物重点实验室基金项目(y107jd);广州市科技计划项目(2008Zi-D021)资助
摘 要:采用热重-差热分析(TG-DTG)、X射线衍射(XRD)、场发射扫描电镜(FE-SEM)手段对Cu-Fe-Co/SO2催化剂进行表征。将Cu-Fe-Co/SO2用于催化合成气制备增塑剂醇的反应,考察了不同工艺条件对总醇时空收率、增塑剂醇分布及CO转化率的影响。结果表明,Cu、Fe、Co 3种活性组分在SiO2载体上分散均匀,且Cu-Fe-Co/SO2的孔隙丰富,孔道结构牢固,利于增塑剂醇合成反应的进行。随着反应温度的升高,增塑剂醇质量分数逐渐降低,总醇时空收率呈现先上升后下降的趋势;反应压力增加,总醇时空收率增加,CO转化率缓慢上升,但幅度很小,增塑剂醇质量分数变化很小;当液时空速(GHSV)在3000~8000h-1范围内增加时,总醇时空收率增加,但CO转化率降低,增塑剂醇质量分数变化不明显。当T=623K、p=5.5MPa,GHSV=6000h-1时,随着合成气中H2体积分数的增加,总醇时空收率先升高后降低,增塑剂醇质量分数降低;V(H2)/V(CO)=1时,总醇时空收率最高为260.79g/(kg.h),增塑剂醇质量分数为28.79%。A prepared Cu-Fe-Co/SiO2 catalyst was characterized by TG-DTG, XRD and FE-SEM, and used to catalyze the synthesis of plasticizer alcohols. The effects of different process conditions on synthesis of plasticizer alcohols from syngas were investigated, which were judged by the time and space yield of total alcohols, the distributions of plasticizer alcohols and CO conversion. The results indicated that the three active components Cu, Fe and Co in the catalyst were dispersed uniformly on SiO2 carrier. The Cu-Fe-Co/SiO2 catalyst exhibited a wealthy and strong pore structure, which was conductive to synthesis of plasticizer alcohols. With the reaction temperature increasing, the mass fraction of plasticizer alcohols decreased gradually, and the time and space yield of total alcohols followed a trend of firstly increasing and then decreasing. The time and space yield of total alcohols and CO conversion increased slowly and slightly with the increase of reaction pressure. Little effect of reaction pressure appeared on distributions of plasticizer alcohols. With GHSV increasing from 3000 h 1 to 8000 h-1 , the time and space yield of total alcohols increased but the CO conversion decreased, and the mass fraction of plasticizer alcohols didn t change significantly. It was proved that the time and space yield of total alcohols firstly increased then decreased with the increase of hydrogen volume fraction, while reaction temperature, pressure and GHSV were 623 K, 5.5 MPa and 6000 h-1 respectively, under which and the value of V(H2)/V(CO) was 1, the time and space yield of total alcohols could reach to highest value of 260.79 g/(kg ·h) as well as the mass fraction of plasticizer alcohols was 28.79 %.
关 键 词:增塑剂醇 合成气 CO加氢 Cu-Fe-Co基催化剂
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