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Atomically dispersed SrOx species on exposed {2 2 2} facets of pyrochlore La2Zr2O7 nanocrystals for boosting low-temperature oxidative coupling of methane
Fuel ( IF 6.7 ) Pub Date : 2022-10-30 , DOI: 10.1016/j.fuel.2022.126479
Tongtong Wu , Yuechang Wei , Jing Xiong , Yitao Yang , Dawei Han , Zhen Zhao , Jian Liu

The efficient catalysts of strontium oxide (SrOx) supported on exposed {2 2 2} facets of pyrochlore La2Zr2O7 nanocrystals (SrOx/LZO-Y) were elaborately synthesized by incipient wetness impregnation method. The introduction of atomically dispersed SrOx species on La2Zr2O7 surface can increase the amount of surface oxygen vacancies induced by Sr2+ substitution of La3+ cations, and the increasing of moderate surface alkaline sites are beneficial to enhance catalytic performance for oxidative coupling of methane (OCM). The SrOx/LZO-Y catalysts have super catalytic performance during low-temperature OCM reaction. SrOx/LZO-12 catalyst with the highest concentrations of O2 species exhibits the highest activity and the lowest apparent activation energy (84 kJ mol−1) during low-temperature OCM into C2H4 and C2H6 (C2) products, i.e., its CH4 conversion, selectivity and yield of C2 products at 600 °C are 30.5 %, 47.4 % and 14.5 %, respectively, and its ratio of C2H4/C2H6 products is 0.77. Based on the results of multiple experimental characterizations, the mechanism of SrOx/LZO-Y catalysts for OCM reaction is proposed: the surface alkaline active centers (O2) induced by doping of Sr ions can promote the critical step of CH4 activation significantly during low-temperature OCM reaction. It is a new strategy to develop the low-temperature and high-activity catalysts for OCM in practical application.



中文翻译:

在烧绿石 La2Zr2O7 纳米晶体的暴露 {2 2 2} 面上原子分散的 SrOx 物种用于促进甲烷的低温氧化耦合

采用初湿浸渍法精心合成了负载在烧绿石La 2 Zr 2 O 7纳米晶(SrO x /LZO-Y)外露{2 2 2}晶面上的氧化锶(SrO x )高效催化剂。在La 2 Zr 2 O 7表面引入原子级分散的SrO x物种可以增加由Sr 2+取代La 3+阳离子引起的表面氧空位的数量,而适度的表面碱性位点的增加有利于提高催化性能用于甲烷的氧化偶联 (OCM)。氧化锶  x /LZO-Y催化剂在低温OCM反应中具有超强的催化性能。SrO x /LZO-12 催化剂低温OCM 生成C 2 H 4和C 2 H 6 ( C 2 ) 产物,即其CH 4转化率、C 2产物在600℃时的选择性和收率分别为30.5 %、47.4 %和14.5 %,其比值为C 2 H 4 /C 2 H6 个产品是 0.77。基于多项实验表征结果,提出了SrO x /LZO-Y催化剂用于OCM反应的机理:Sr离子掺杂诱导的表面碱性活性中心(O 2 -)可以促进CH 4活化的关键步骤在低温OCM反应过程中显着。开发用于OCM的低温高活性催化剂在实际应用中是一种新的策略。

更新日期:2022-10-30
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