摘要
采用自制的实验装置,开展了甲烷液相部分氧化制甲醇的研究,考察了反应溶剂、初始压力、反应温度、催化剂的种类及其用量对甲烷转化率和甲醇收率的影响。实验结果表明,游离SO3含量为50%(w)的发烟硫酸适于用做甲烷部分氧化制甲醇的反应溶剂;甲烷转化率随初始压力的升高而增大,而甲醇收率随初始压力的增加呈先增加后趋于平缓的趋势;在160～180℃内,甲烷转化率和甲醇收率均随反应温度的升高而增大;以I2为催化剂时,当I2的添加量为1 778 mg(含50%(w)SO3的发烟硫酸70 mL)时,甲烷转化率和甲醇收率最大;以V2O5为催化剂时,随V2O5添加量的增加,甲烷转化率和甲醇收率均增大,但当V2O5的添加量超过2 546 mg(含50%(w)SO3的发烟硫酸70 mL)时,V2O5添加量对提高甲醇收率的作用不明显。通过对实验数据的分析,建立了反应动力学方程。
The partial oxidation of mathane to methanol in liquid phase was studied in self-made experimental apparatus and the influences of different factors on the methane conversion and methanol yield were investigated. The results show that 50%（w） oleum is an appropriate solvent for the partial oxidation. With the increase of the initial reaction pressure, the methane conversion increases, and the methanol yield first increases and then does not change when the pressure reaches a certain value. The methane conversion and the methanol yield increase with the rise of the reaction temperature in the temperature range of 160-180 ~C. The partial oxidation can be conducted with I2 or V205 catalyst. For I2 catalyst system, the optimum I2 dosage is 1 778 mg（oleum（50%（w）SO3）70 mL）. For V2O5 catalyst system, the methane conversion and methanol yield are positively correlated with the V2O5 dosage, but the methanol yield does not change significantly with the addition of the catalyst when the addition is more than 2 546 mg（oleum（50%（w）SO3）70 mL）. A reaction kinetics model for the partial oxidation was established based on the experimental data.
出处
《石油化工》
CAS
CSCD
北大核心
2012年第10期1137-1142,共6页
Petrochemical Technology
基金
国家自然科学基金项目(51004045)
黑龙江省教育厅科学技术研究项目(12511481)
关键词
甲烷
甲醇
液相部分氧化
动力学
methane
methanol
partial oxidation in liquid phase
kinetics
