摘要
首先采用溶胶-凝胶法制备了Co-Pd/TiO_2催化剂,之后以磷钨酸为杂多酸,采用过量浸渍的方法制备了不同浓度磷钨酸改性的双金属催化剂。考察了改性催化剂对CH_4和CO_2两步梯阶转化直接合成乙醇和乙酸的催化性能,并通过XRD、NH3-TPD-MS、BET、FT-IR和XPS等技术手段对催化剂的结构、组成、比表面积和孔径分布等进行了表征。实验结果表明,以0.04mol/L磷钨酸改性的催化剂活性金属分散性好,催化剂比表面积大,这共同保障了该反应协同高效的进行。在常压、150℃的反应条件下其乙醇和乙酸的总时空速率达到10.54mg/(g·h),与未经磷钨酸改性的催化剂对比活性提高了2.55倍。
The Co-Pd/TiO2 catalysts were prepared by sol-gel method,which then were modified by impregnating them with excessive heteropoly acid of phosphotungstic acid in different concentrations.The catalytic performances of the modified catalysts for direct synthesis of ethanol and acetic acid from CH4 and CO2 by a stepwise conversion technology were investigated.XRD,NH3-TPD-MS,BET,FT-IR and XPS were used to characterize the structure,composition,specific surface area and pore diameter distribution of the catalysts.The results show that the catalyst modified by 0.04mol/L phosphotungstic acid display good dispersity of active metal and large specific surface area,which ensure the synergistic and efficient process of the reaction.Under atmospheric pressure and 150℃,over this catalyst,the total space-time yield of ethanol and acetic acid was up to 10.54mg·g^-1·h^-1,which was 2.55 times higher than that of the unmodified catalyst.
作者
宋刚
时培祥
陶诗琪
高东若
黄伟
SONG Gang;SHI Pei-xiang;TAO Shi-qi;GAO Dong-ruo;HUANG Wei(Key Laboratory of Coal Science and Technology,Ministry of Education and Shanxi Province,Institute Coal Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,China)
出处
《天然气化工—C1化学与化工》
CAS
CSCD
北大核心
2018年第6期39-46,74,共9页
Natural Gas Chemical Industry
基金
国家自然科学基金重点项目(21336006)
国家自然科学基金面上项目(21176176)
高等学校博士学科点专项(优先发展领域)(20111402130002).
