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Probing the promotional roles of cerium in the structure and performance of Cu/SiO2 catalysts for ethanol production

机译:探索铈的促销作用铜/二氧化硅催化剂的结构和性能乙醇生产

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In this contribution, the efficient hydrogenation of dimethyl oxalate (DMO) to ethanol was achieved over a series of cerium promoted Cu/SiO2 (xCe-Cu/SiO2) catalysts prepared by a urea-assisted gelation approach. As a promoter, Ce played a crucial role in improving the structure, properties and catalytic performance of the Cu/SiO2 catalysts. The structure and chemical properties of the synthesized catalysts were characterized by XRD, FT-IR, in situ XRD, TEM, STEM-EDX mapping, N2O titration, H-2-TPR, H-2-TPD, XPS, XAES, etc. The characterization results disclosed that the addition of a Ce promoter to the Cu/SiO2 catalysts remarkably increased the Cu dispersion and retarded the sintering of small-sized Cu species. The strong interaction between the Ce promoter and Cu species substantially changed the redox properties of xCe-Cu/SiO2 catalysts and made the Cu2+ species easy to reduce. In addition, the activation ability of H-2 species was significantly improved in the xCe-Cu/SiO2 catalysts, as evidenced by H-2-TPD studies. Among these synthesized catalysts, the 1Ce-Cu/SiO2 catalyst with a 1.0 wt% Ce loading exhibited the highest catalytic activity (100% DMO conversion), ethanol selectivity (91.8%) and stability. This enhancement of catalytic activity, ethanol selectivity and stability is very promising for the development of an alternative route for the production of ethanol by hydrogenation of DMO from syngas.
机译:在这个贡献,高效加氢草酸二甲酯(DMO)乙醇在一系列的铈促进了铜/二氧化矽(xCe-Cu /二氧化硅)准备的一个催化剂urea-assisted凝胶的方法。在提高Ce起到了至关重要的作用结构、性质和催化性能铜/二氧化硅催化剂。合成催化剂的化学性质通过XRD, ir、原位XRD、H-2-TPR TEM, STEM-EDX映射,一氧化二氮滴定,H-2-TPD、XPS、xa等等。结果透露,除了Ce启动子铜/二氧化硅催化剂相当增加了铜分散和迟钝烧结的小型铜物种。Ce启动子之间的相互作用和铜大大改变了氧化还原物种xCe-Cu /二氧化硅催化剂,使的属性Cu2 +物种容易减少。2物种的活化能力显著提高xCe-Cu /二氧化矽催化剂,就是明证H-2-TPD研究。这些合成的催化剂,1 ce-cu /二氧化矽催化剂1.0 wt % Ce加载展出DMO转化催化活性最高(100%),乙醇(91.8%)选择性和稳定性。提高催化活性的乙醇选择性和稳定性是很有前途的另一种途径的发展生产乙醇的DMO的加氢从合成气。

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