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Tuning the dimensionality of layered Srn+1Tin−xNixO3n+1 perovskite structures for improved activity in syngas generation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2018-02-12 , DOI: 10.1016/j.jcat.2018.01.015
Srikanth Dama , Seema Ghodke , Richa Bobade , Hanmant Gurav , Satyanarayana Chilukuri

Interest in perovskite type oxides is growing due to their versatile catalytic applications. A series of Ruddlesden-Popper (RP) type layered perovskite oxides Srn+1Tin−xNixO3n+1 were prepared and evaluated for their catalytic activity in steam reforming, CO2 reforming and bi-reforming of methane. These materials, prepared through citrate gel method were characterized to understand their structure and Ni reducibility. Substitution of Ni in RP phases was established through refinement of XRD powder pattern. During methane reforming, the catalytic activity increased with the order of RP phase of SrTi1−xNixO3−δ (n = ∞). TPR results show variation in Ni reducibility with the order of RP phase, while TPD-O2 study helped to estimate oxygen vacancies. These vacancies seem to influence catalytic activity during methane reforming. Transient pulse experiments show that CO2 dissociates over oxygen vacancies to give CO and oxygen, with later replenishing lattice oxygen in SrTi0.8Ni0.2O3−δ (n = ∞) phases. Highly labile oxygen vacancies generated in the bulk of SrTi0.8Ni0.2O3−δ must be migrating to the surface, helping in the removal of coke formed. Characterization of catalysts after reaction helped in better understanding of coke precursors.



中文翻译:

调整层状Sr n + 1 Ti n-x Ni x O 3n + 1钙钛矿结构的尺寸,以提高合成气产生的活性

钙钛矿型氧化物由于其广泛的催化应用而引起了人们的兴趣。制备了一系列Ruddlesden-Popper(RP)型层状钙钛矿氧化物Sr n + 1 Ti n-x Ni x O 3n + 1,并评估了它们在甲烷蒸汽重整,CO 2重整和双重整中的催化活性。通过柠檬酸盐凝胶法制备的这些材料经过表征,以了解其结构和Ni还原性。通过细化XRD粉末图案,确定了RP相中Ni的取代。甲烷重整过程中,催化活性随SrTi 1-x Ni x O3 - δRP相的增加而增加。(n =∞)。TPR结果显示Ni还原性随RP相的顺序而变化,而TPD-O 2研究有助于估计氧空位。这些空位似乎影响甲烷重整过程中的催化活性。瞬态脉冲实验表明,CO 2在氧空位上解离生成CO和氧,随后在SrTi 0.8 Ni 0.2 O3 (n =∞)相中补充晶格氧。大量SrTi 0.8 Ni 0.2 O3 -δ中产生的高度不稳定的氧空位必须迁移到表面,以帮助除去形成的焦炭。反应后催化剂的表征有助于更好地了解焦炭前体。

更新日期:2018-02-12
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