Lei Hong, Zheng Ruheng, Liu Yeping, Gao Jiacheng, Chen Xiang, Feng Xiaoliang
College of Chemical and Material Engineering, Quzhou University Quzhou 324000 China
RSC Adv. 2019 May 3;9(24):13696-13704. doi: 10.1039/c9ra00658c. eCollection 2019 Apr 30.
Hydrogenation of CO to chemicals is of great importance in the reduction of greenhouse gas emission. And the interaction and/or the boundary between Cu and ZnO played a crucial role in the performance of the Cu-ZnO catalyst for CO hydrogenation to methanol. In this work, cylindrical shaped ZnO was first synthesized controlled hydrothermal precipitation of Zn(COCH)·2HO, and Cu was further deposited on ZnO reduction in aqueous solution. Characterizations indicated that the crystallization degree of ZnO decreased with the increasing content of Cu, while the exposed surface area of Cu exhibited a volcano shaped curve. It was found that the cylindrical shaped ZnO combined Cu catalysts were active for the hydrogenation of CO, and the space time yield of methanol reached 0.50 g (g h) at H/CO = 3, 240 °C, 3.0 MPa, and 0.54 mol (g h), but the methanol selectivity decreases with the reduction of the (002) polar plane of ZnO. The conversion of CO and methanol selectivity were discussed with the detected exposed Cu surface area and the number of oxygen vacancies.
将一氧化碳加氢转化为化学品对于减少温室气体排放具有重要意义。铜与氧化锌之间的相互作用和/或界面在用于将一氧化碳加氢制甲醇的铜-氧化锌催化剂的性能中起着关键作用。在本工作中,首先通过对Zn(COCH)·2HO进行可控水热沉淀合成了圆柱形氧化锌,然后通过在水溶液中还原将铜进一步沉积在氧化锌上。表征结果表明,氧化锌的结晶度随铜含量的增加而降低,而铜的暴露表面积呈现出火山形曲线。研究发现,圆柱形氧化锌负载铜催化剂对一氧化碳加氢具有活性,在H/CO = 3、240 °C、3.0 MPa和0.54 mol (g h)条件下,甲醇的时空产率达到0.50 g (g h),但甲醇选择性随氧化锌(002)极性面的减少而降低。结合检测到的暴露铜表面积和氧空位数量对一氧化碳转化率和甲醇选择性进行了讨论。