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Direct synthesis of higher alcohols from syngas over modified Mo2C catalysts under mild reaction conditions

机译:在轻度反应条件下,通过修饰的MO2C催化剂直接合成合成剂的较高醇

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Direct syngas conversion to higher alcohols with high selectivity under mild reaction conditions has attracted much attention but still remains a great challenge. Herein, we reported that the addition of Rh and K promoters to Mo2C (RhK/Mo2C) can significantly increase alcohols selectivity to 44.4% under a mild reaction pressure of 1 MPa. Mechanism study illustrated that interface sites between Rh and Mo2C promoted by K effectively contributed to the improved catalytic performance. The K promoter not only promoted the dispersion of Rh with a partial Rhδ+ state under working conditions but also suppressed further hydrogenation of olefins. In addition, the highly dispersed Rhδ+ species increased the concentration of non-dissociated CO* intermediates and greatly improved the coupling ability of CO and alkyl species to form alcohols. This work provides a promising strategy to design efficient heterogeneous catalysts at low pressure for higher alcohols synthesis over Mo2C-based catalysts.
机译:在轻度反应条件下,直接的合成气转化为具有高选择性的高等醇已引起了很多关注,但仍然是一个巨大的挑战。 在本文中,我们报道说,在1 MPa的轻度反应压力下,将RH和K启动子添加到MO2C(RHK/MO2C)中可以显着提高酒精的选择性至44.4%。 机理研究表明,k促进的RH和MO2C之间的界面位点有效地有助于改善催化性能。 K启动子不仅在工作条件下促进了RH与部分RHδ+状态的分散体,而且还抑制了烯烃的进一步氢化。 此外,高度分散的RHδ+物种增加了非解散的CO*中间体的浓度,并大大提高了CO和烷基物质形成酒精的耦合能力。 这项工作为在基于MO2C的催化剂上合成高压合成的高压下设计有效的异质催化剂提供了一种有希望的策略。

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