Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2017-07-11 , DOI: 10.1016/j.apcata.2017.07.012 Pengwei Wang , Guofeng Zhao , Ye Liu , Yong Lu
The Mn2O3-Na2WO4/SiO2 catalyst is the most promising one among the enormous catalysts for the oxidative coupling of methane (OCM) but only at above 800 °C. No doubt that lowering temperature of the OCM process is at the forefront of this catalysis field. A promising low-temperature active and selective TiO2-doped Mn2O3 Na2WO4/SiO2 catalyst, consisting of 6 wt% TiO2, 6 wt% Mn2O3, 10 wt% Na2WO4 and SiO2 in balance, is developed by solution combustion synthesis (SCS) method. This catalyst is capable of converting 20% CH4 with 70% selectivity to C2-C3 hydrocarbons even at 700 °C (catalyst bed temperature) and is stable for at least 250 h without deactivation sign, for a feed gas of 50% CH4 in air using a gas hourly space velocity of 8000 mL gcat.−1 h−1. In contrast, the non-TiO2-doped SCS catalyst is almost inactive at 700 °C whereas it can achieve reactivity (∼24% CH4 conversion and ∼74% C2-C3 selectivity) comparable to the TiO2-doped one at 800 °C. XRD and Raman results evidently reveal that the formation of MnTiO3 during the OCM process appears to be important for the low-temperature OCM activity improvement by TiO2-doping.
中文翻译:
TiO 2掺杂的Mn 2 O 3 -Na 2 WO 4 / SiO 2催化剂用于甲烷的氧化偶联:固溶燃烧合成和MnTiO 3依赖性低温活性的提高
Mn 2 O 3 -Na 2 WO 4 / SiO 2催化剂是甲烷(OCM)氧化偶联的巨大催化剂中最有前途的一种,但仅在800°C以上。毫无疑问,降低OCM工艺的温度是该催化领域的最前沿。一个有希望的低温活性和选择性的TiO 2掺杂的Mn 2 ö 3的Na 2 WO 4 /二氧化硅2催化剂,包括6重量%的TiO 2,6重量%的Mn 2 ö 3,10重量%的Na 2 WO 4和SiO 2个平衡,是通过固溶燃烧合成(SCS)方法开发的。即使在700°C(催化剂床温)下,该催化剂也能够将20%CH 4转化为C 2 -C 3烃,选择性为70%,并且对于50%的进料气,至少可稳定250h无失活迹象。使用8000 mL g cat的时空速度的空气中CH 4 。-1 小时-1。与此相反,非的TiO 2掺杂的SCS催化剂是在700℃,而它可以实现反应性(~24%CH几乎无活性的4转化率和~74%C 2 -C 3的选择性)媲美的TiO 2-在800°C时掺杂一个。XRD和拉曼结果明显表明,在OCM工艺过程中MnTiO 3的形成对于通过掺杂TiO 2改善低温OCM活性很重要。