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Structural evaluation and catalytic performance of nano-Au supported on nanocrystalline Ce0.9Fe0.1O2-delta solid solution for oxidation of carbon monoxide and benzylamine

机译:纳米Ce0.9Fe0.1O2-δ固溶体上负载的纳米金对一氧化碳和苄胺氧化的结构评价和催化性能

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In this work, we systematically investigated the structure-activity performance of nanosized Au/CeO2 and Au/Ce0.9Fe0.1O2-delta catalysts, along with nanocrystalline CeO2 (a)nd Ce0.9Fe0.1O2-delta supports, for the oxidation of carbon monoxide and benzylamine. An extensive physicochemical characterization was undertaken using XRD, BET surface area, BJH analysis, TG-DTA, XPS, TEM, Raman, AAS and CHN analyses. XRD studies confirmed the formation of smaller sized Ce0.9Fe0.1O2-delta nanocrystallites due to the incorporation of Fe3+ ions into the CeO2 lattice. Interestingly, Raman analysis revealed that the addition of Au remarkably improves the structural properties of the supports, evidenced by F-2g peak shift and peak broadening, a significant observation in the present work. TEM images revealed the formation of smaller Au particles for Au/Ce0.9Fe0.1O2-delta (similar to 3.6 nm) compared with Au/CeO2 (similar to 5.3 nm), attributed to ample oxygen vacancies present on the Ce0.9Fe0.1O2-delta surface. XPS studies indicated that Au and Fe are present in metallic and +3 oxidation states, respectively, whereas Ce is present in both +4 and +3 oxidation states (confirming its redox nature). Activity results showed that the incorporation of Fe outstandingly enhances the efficacy of the Au/CeO2 catalyst for both CO oxidation and benzylamine oxidation. A 50% CO conversion was achieved at similar to 349 and 330 K for Au/CeO2 and Au/Ce0.9Fe0.1O2-delta catalysts, respectively. As well, the Au/Ce0.9Fe0.1O2-delta catalyst showed similar to 99% benzylamine conversion with similar to 100% dibenzylimine selectivity for 7 h reaction time and 403 K temperature, whereas only 81% benzylamine conversion was achieved for the Au/CeO2 sample under similar conditions. The excellent performance of the Au/Ce0.9Fe0.1O2-delta catalyst is mainly due to the existence of smaller Au particles and an improved synergetic effect between the Au and the Ce0.9Fe0.1O2-delta support. It is confirmed that the oxidation efficiency of the Au catalysts is highly dependent on the preparation method.
机译:在这项工作中,我们系统地研究了纳米Au / CeO2和Au / Ce0.9Fe0.1O2-delta催化剂以及纳米晶体CeO2(a)和Ce0.9Fe0.1O2-delta载体的结构活性,以氧化一氧化碳和苄胺。使用XRD,BET表面积,BJH分析,TG-DTA,XPS,TEM,拉曼,AAS和CHN分析进行了广泛的理化表征。 XRD研究证实,由于将Fe3 +离子掺入CeO2晶格中,形成了尺寸较小的Ce0.9Fe0.1O2-δ纳米微晶。有趣的是,拉曼分析表明,Au的添加显着改善了载体的结构性能,这是由F-2g峰位移和峰展宽所证明的,这是本工作的一项重要发现。 TEM图像显示与Au / CeO2(约5.3 nm)相比,Au /Ce0.9Fe0.1O2-δ(约3.6 nm)形成了较小的Au颗粒,这归因于Ce0.9Fe0.1O2上存在大量的氧空位-三角表面。 XPS研究表明,Au和Fe分别以金属和+3氧化态存在,而Ce分别以+4和+3氧化态存在(证实其氧化还原性质)。活性结果表明,Fe的掺入显着增强了Au / CeO2催化剂对CO氧化和苄胺氧化的功效。对于Au / CeO2和Au /Ce0.9Fe0.1O2-δ催化剂,分别以349和330 K达到50%的CO转化率。同样,Au /Ce0.9Fe0.1O2-δ催化剂在7 h反应时间和403 K温度下显示出相似的99%苄胺转化率和100%的二苄基亚胺选择性,而Au /Ce0.9Fe0.1O2-δ催化剂的转化率仅为81%相似条件下的CeO2样品。 Au /Ce0.9Fe0.1O2-δ催化剂的出色性能主要是由于存在较小的Au颗粒,以及Au与Ce0.9Fe0.1O2-δ载体之间的协同作用得到改善。证实了Au催化剂的氧化效率高度依赖于制备方法。

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