Fe_2O_3-CuO/ZSM-5催化剂催化低浓度瓦斯制甲醇  

Catalyzing low concentration mine gas to methanol by Fe_2O_3-CuO/ZSM-5 catalyst

作　　者：徐锋[1] 吴扬[1] 李创[1] 朱丽华[1] 

机构地区：[1]黑龙江科技大学安全工程学院,黑龙江哈尔滨150022

出　　处：《化工进展》2016年第5期1446-1451,共6页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(51374098);哈尔滨市科技创新人才研究专项资金项目(2013RFQXJ085);黑龙江省博士后科研启动基金(LBH-Q14143);黑龙江科技大学安全工程学院大项目培育基金(aq2013-2)项目

摘　　要：采用催化氧化的方法,将煤矿抽采瓦斯制成高价值的化学品或液体燃料甲醇是其综合利用的一个发展方向。寻找对瓦斯转化具有较好的催化效果,且能替代贵金属催化剂的普通催化剂是瓦斯催化氧化制甲醇的研究重点。本文以硝酸铁、硝酸铜和ZSM-5分子筛为原料,采用离子交换法制备了Fe_2O_3/ZSM-5、Cu O/ZSM-5和Fe_2O_3-Cu O/ZSM-5催化剂,并在乙酸溶剂中考察了3种催化剂催化低浓度瓦斯部分氧化合成甲醇的性能。结果表明,Fe_2O_3/ZSM-5、Cu O/ZSM-5和Fe_2O_3-Cu O/ZSM-5对瓦斯部分氧化制甲醇反应均有催化活性,但Fe_2O_3-Cu O/ZSM-5的催化效果最明显,且Fe、Cu负载量对催化剂的催化活性影响较为显著,Fe和Cu的最佳理论负载量分别为4.21%和3.22%。在Fe_2O_3-Cu O/ZSM-5(x_(Fe)=4.21%,x_(Cu)=3.22%)添加量为0.1g、乙酸溶剂用量30m L的条件下,Fe_2O_3-Cu O/ZSM-5催化甲烷体积分数为20%配制瓦斯制甲醇的最佳反应条件为初始反应压力4.0MPa、反应温度200℃、反应时间3h。The conversion of mine gas as the feedstock to produce highly valuable chemicals and liquid fuel（methanol） has become a research hot spot. Catalytic oxidation,an effective technique for activating mine gas,has received considerable attention in recent years. The research on highly efficient and cheap catalysts is critically important for catalytic oxidation of mine gas into methanol. Using ferric nitrate,copper nitrate and ZSM-5 molecular sieve as raw materials,Fe2O_3/ZSM-5,Cu O/ZSM-5 and Fe2O_3-Cu O/ZSM-5 catalysts were prepared by the ion exchange method,and their selective oxidation of low concentration mine gas to methanol were investigated in acetic acid. Results showed that Fe2O_3/ZSM-5,Cu O/ZSM-5 and Fe2O_3-Cu O/ZSM-5 all had catalytic activity for the selective oxidation of mine gas to methanol,and Fe2O_3-Cu O/ZSM-5 exhibited the most evident catalytic effect. Meanwhile,the active metal loading had significant effect on the catalytic activity of the catalyst,and theoretically the best loadings of Fe and Cu were 4.21% and 3.22%,respectively. When the addition of Fe2O_3-Cu O/ZSM-5（x_（Fe）=4.21%,x_（Cu）=3.22%） was 0.1g and the amount of acetic acid was 30 m L,the optimum reaction conditions of oxidation of mine gas（with the volume fraction of methane being 20%）to methanol catalyzed by Fe_2O_3-Cu O/ZSM-5 were： initial reaction pressure 4.0 MPa, reaction temperature 200℃ and reaction time 3h.

关 键 词：Fe2O3-CuO/ZSM-5 催化剂 部分氧化 瓦斯 甲醇 

分 类 号：O643.32[理学—物理化学]