焦炉煤气三重整制合成气的工艺比较及催化剂改性  

Comparison of processes on tri-reforming of coke oven gas to syngas and catalysts modification

作　　者：申曙光[1] 李安琪[1] 陈攀攀[1] 赵志军[1] 

机构地区：[1]太原理工大学化学化工学院,山西太原030024

出　　处：《现代化工》2013年第5期61-65,共5页Modern Chemical Industry

基　　金：山西省科技攻关项目(20120321003-02);太原市科技发展项目(110138)

摘　　要：在固定床反应器中,对焦炉煤气H2O/O2/CO2三重整制合成气的3种工艺———非催化工艺、催化工艺和二段工艺进行了比较;同时考察了以共浸法加入助剂CaO、Co、Cu、Fe对二段工艺中催化反应性能的影响。结果表明,焦炉煤气中氢气的存在不利于甲烷的转化,但有利于二氧化碳的转化。反应温度高于800℃时,二段工艺的甲烷和二氧化碳转化率明显高于其他2种工艺,与催化工艺相比,二段工艺中焦炉煤气的空速可达6 945 h-1;碱金属氧化物CaO的加入促进了CH4和CO2的转化;助剂Cu提高了催化剂的高温活性,900℃时CH4转化率可达99.1%,CO收率可达95.5%;Fe提高了催化剂的低温活性。XRD结果表明,CaO能削弱Ni2Al4O4的特征峰,催化剂的还原性和分散性较好。The tri-reforming of coke oven gas in three processes （ non-catalytic process, catalytic process, two-stage process） is carried out to obtain an optimal process. A series of Ni-based catalysts are synthesized by adding CaO, Co, Cu and Fe promoters with an impregnation method. The influence of the addition of promoters on the catalytic performance in two-stage process is studied as well. The results show that H2 present in the feed gas results in lower CH4 conversion, but increased CO2 conversion. CH4 and CO2 conversions of two-stage process are obviously higher than those of the other two processes when the reaction temperature is above 800~C. The CH4 and COs conversion are found to be 93.4% and 61.3% at 900℃ ,respectively. Compared with the catalytic process ,the gas hourly space velocity of coke oven gas in two- stage process can reach 6 945 h^-1. The addition of CaO promotes CH4 and CO2 conversion. The Cu promoter increases the catalyst activity at high temperature and provides a CH4 conversion of 99. 1% and a CO yield of 95.5% at 900℃. The Fe promoter increases catalyst activity at low temperature. The result of XRD shows that the addition of CaO weakens the characteristic peak of Ni2Al4O4 ,and leads to the catalysts with better reducibility and dispersibility.

关 键 词：焦炉煤气 三重整 合成气 镍基催化剂 助剂 

分 类 号：TQ032[化学工程]