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Investigation of metal oxide additives onto Na2WO4-Ti/SiO2 catalysts for oxidative coupling of methane to value-added chemicals
Catalysis Today ( IF 5.2 ) Pub Date : 2020-04-01 , DOI: 10.1016/j.cattod.2020.03.048
Sarannuch Sringam , Phattaradit Kidamorn , Thanaphat Chukeaw , Metta Chareonpanich , Anusorn Seubsai

The oxidative coupling of methane (OCM) is a closely related reaction process involving the transformation of methane (CH4) and O2 mixtures into value-added chemicals such as ethylene and ethane (i.e. C2+). This work presents the effects of metal oxide additives into the Na2WO4-Ti/SiO2 catalyst on the performance of the OCM reaction. Several metal oxide additives—including oxides of Co, Mn, Cu, Fe, Ce, Zn, La, Ni, Zr, Cr, and V—were investigated with the Na2WO4-Ti/SiO2 catalyst. All of the catalysts were prepared using co-impregnation and the catalyst activity test was performed in a plug flow reactor at a reactor temperature range of 600–800 °C and atmospheric pressure. The physicochemical properties of the prepared catalysts relating to their catalytic activity were discussed by using the information of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM) measurements. Na2WO4-Ti/SiO2 added Mn was found to be the most active catalyst, involving shifts of binding energies of W 4f and Ti 2p toward lower binding energies. Moreover, a variety of operating conditions—including reactant- to-nitrogen gas ratio, catalyst mass, reactor temperature, and total feed flow rate—were intensively examined for the OCM reaction using the Na2WO4-Ti-Mn/SiO2 catalyst. The maximum C2+ yield was subsequently discovered at 22.09% with 62.3% C2+ selectivity and 35.43% CH4 conversion. Additionally, the stability of the Na2WO4-Ti-Mn/SiO2 catalyst was also monitored with time on stream for 24 h.



中文翻译:

Na 2 WO 4 -Ti / SiO 2催化剂上金属氧化物添加剂对甲烷氧化偶联成增值化学品的研究

甲烷的氧化偶联(OCM)是密切相关的反应过程,涉及将甲烷(CH 4)和O 2混合物转化为增值化学品,例如乙烯和乙烷(即C 2+)。这项工作提出了Na 2 WO 4 -Ti / SiO 2催化剂中金属氧化物添加剂对OCM反应性能的影响。用Na 2 WO 4 -Ti / SiO 2研究了几种金属氧化物添加剂,包括Co,Mn,Cu,Fe,Ce,Zn,La,Ni,Zr,Cr和V的氧化物催化剂。所有催化剂均采用共浸渍法制备,并在活塞流反应器中在600–800°C的反应器温度和大气压下进行催化剂活性测试。通过使用X射线衍射(XRD),X射线光电子能谱(XPS)和扫描电子显微镜(SEM)的信息,讨论了所制备催化剂的物理化学性质及其催化活性。Na 2 WO 4 -Ti / SiO 2发现添加的Mn是最具活性的催化剂,涉及W 4f和Ti 2p的结合能向较低的结合能的转变。此外,针对使用Na 2 WO 4 -Ti-Mn / SiO 2催化剂进行的OCM反应,对各种操作条件(包括反应物与氮气的比例,催化剂质量,反应器温度和总进料流速)进行了深入检查。。随后发现最大的C 2+产率为22.09%,具有62.3%的C 2+选择性和35.43%的CH 4转化率。另外,还对Na 2 WO 4 -Ti-Mn / SiO 2催化剂的稳定性进行了24小时的在线监测。

更新日期:2020-04-20
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