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合成气制备增塑剂醇的初步研究
引用本文:熊莲,罗彩容,郭海军,陈新德,陈勇.合成气制备增塑剂醇的初步研究[J].石油学报(石油加工),2012,28(3):470-475.
作者姓名:熊莲  罗彩容  郭海军  陈新德  陈勇
作者单位: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
基金项目: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:通过场发射扫描电镜(FE-SEM)、热重-差热分析(TG-DTA)、X射线衍射(XRD)等手段对Cu-Fe-Co基催化剂进行表征,考察其物性能否满足合成气制备增塑剂醇的要求。XRD结果表明Cu、Fe、Co三种金属组分在载体上分散均匀,是催化剂CO加氢反应的活性中心;TG结果表明此催化剂最佳热解温度为673K且成型后热稳定性良好,催化剂反应后积碳也比较少;SEM结果表明此催化剂具有丰富的孔隙结构,利于增塑剂醇合成反应进行。以加氢反应考察不同温度、压力、空速(GHSV)、V(H2):V(CO)等条件对催化剂催化性能的影响,重点考察合成气反应后总醇时空收率、增塑剂醇分布以及CO转化率。结果表明在563~653K范围内,随反应温度升高增塑剂醇比例从36.87%逐渐降低,总醇时空收率呈现先上升后下降的趋势,623K总醇的时空收率最高为152.01 g?(kg?h)-1;反应压力升高总醇时空收率增加,CO转化率缓慢上升但幅度很小,增塑剂醇选择性变化很小;空速3000~8000h-1范围内,随空速增加,醇的时空收率升高但CO转化率降低,对醇分布影响也较小。随合成气中H2比例增加,总醇时空收率先升高后降低,增塑剂醇选择性降低,V(H2):V(CO)=1:1时,总醇时空收率最高为260.79 g?(kg?h)-1,增塑剂醇为28.79%。

关 键 词:增塑剂醇  合成气  CO加氢  Cu-Fe-Co基催化剂  
收稿时间:2011-05-18

Study on the Synthesis of Plasticizer Alcohols From Syngas
XIONG Lian,LUO Cairong,GUO Haijun,CHEN Xinde,CHEN Yong.Study on the Synthesis of Plasticizer Alcohols From Syngas[J].Acta Petrolei Sinica (Petroleum Processing Section),2012,28(3):470-475.
Authors:XIONG Lian  LUO Cairong  GUO Haijun  CHEN Xinde  CHEN Yong
Affiliation:1. Key Laboratory of Renewable Energy and Natural Gas Hydrate, Chinese Academy of Sciences, Guangzhou 510640, China; 2. Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China; 3. Guangzhou Branch of Chinese Academy of Sciences, Guangzhou 510640, China
Abstract: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%.
Keywords:plasticizer alcohols  syngas  CO hydrogenation  Cu-Fe-Co-based catalyst
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