Zhao Yinshuang, Dong Fang, Han Weiliang, Zhao Haijun, Tang Zhicheng
State Key Laboratory for Oxo Synthesis and Selective Oxidation, National Engineering Research Center for Fine Petrochemical Intermediates, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences Lanzhou 730000 PR China
University of Chinese Academy of Sciences Beijing 100039 PR China.
RSC Adv. 2018 Jan 4;8(3):1583-1592. doi: 10.1039/c7ra11676d. eCollection 2018 Jan 2.
Cu-Ce/graphene catalysts show high dispersion of metal particles and excellent activity and stability for catalytic oxidation. In this study, a hydrothermal method was used to synthesize a series of bimetallic Cu-Ce/graphene catalysts, and the effects of the proportions of Cu and Ce on CO oxidation were investigated in detail. Indispensable characterizations such as XPS, XRD, TEM, BET, and H-TPR were conducted to explore the effect of the Cu/Ce molar ratio and the metal valence on the activity and determine the structure-performance relationship. The results showed that bimetallic supported catalysts, such as 3Cu5Ce/graphene, 1Cu1Ce/graphene, and 5Cu3Ce/graphene, possessed significant catalytic activity. Especially, the 5Cu3Ce/graphene catalyst showed highest catalytic activity for CO oxidation, the value was 132 °C, and the apparent activation energy was 68.03 kJ mol. Furthermore, the stability of the 5Cu3Ce/graphene catalyst was outstanding, which could be maintained for at least 12 h. Moreover, the CeO particles were well crystalline with the size 5-9 nm in these catalysts, and the CuO nanoparticles were well dispersed on CeO and graphene. Notably, the ratio of Cu/Ce in the catalyst was higher, the interaction between the Ce species and the graphene was stronger, and the Cu species were more easily reduced; this was beneficial for the oxidation of CO.
铜铈/石墨烯催化剂对金属颗粒表现出高分散性,并且在催化氧化方面具有优异的活性和稳定性。在本研究中,采用水热法合成了一系列双金属铜铈/石墨烯催化剂,并详细研究了铜和铈的比例对一氧化碳氧化的影响。进行了XPS、XRD、TEM、BET和H-TPR等必不可少的表征,以探究铜/铈摩尔比和金属价态对活性的影响,并确定结构-性能关系。结果表明,双金属负载催化剂,如3Cu5Ce/石墨烯、1Cu1Ce/石墨烯和5Cu3Ce/石墨烯,具有显著的催化活性。特别是,5Cu3Ce/石墨烯催化剂对一氧化碳氧化表现出最高的催化活性,T90值为132℃,表观活化能为68.03kJ/mol。此外,5Cu3Ce/石墨烯催化剂的稳定性出色,可至少保持12小时。而且,在这些催化剂中,CeO颗粒结晶良好,尺寸为5-9nm,CuO纳米颗粒在CeO和石墨烯上分散良好。值得注意的是,催化剂中铜/铈的比例越高,铈物种与石墨烯之间的相互作用越强,铜物种越容易被还原;这有利于一氧化碳的氧化。