Higher alcohol synthesis (HAS) from syngas presents an effective method for obtaining clean liquid fuels and high-value chemicals. In this study, we regulated the catalytic performance by altering the dispersion of Rh on the CeO₂ support. A comprehensive understanding of the regulatory mechanism of catalytic performance and the key CO adsorption configurations was achieved through a series of characterization experiments. In reduced catalysts, Rh existed in two forms: Rh⁺ at the Rh–CeO₂ interface and Rh⁰ away from the interface. The total length of the Rh–CeO₂ interface perimeter was influenced by the size of Rh nanoparticles, thereby regulating the ratio of Rh⁰ to Rh⁺. A balanced distribution of Rh⁰ to Rh⁺ is necessary to improve the selectivity, indicating that the synthesis of higher alcohols is contingent upon the synergistic effect of Rh⁺ and Rh⁰, and the Rh⁰–Rh⁺ sites are identified as the key sites. Furthermore, we clarified the configurations of CO stably adsorbed on the Rh/CeO₂ surface under reaction conditions: Rh⁺₂H_x–(CO) and Rh⁰_2–(CO). The C–C coupling between the two adsorbed CO was found to be crucial for the production of higher alcohols.

中文翻译：

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通过金属分散控制最大化 Rh0–Rh+ 位点的数量，用于从合成气合成高级醇


从合成气合成高级醇（HAS）是获得清洁液体燃料和高价值化学品的有效方法。在这项研究中，我们通过改变Rh在CeO ₂载体上的分散来调节催化性能。通过一系列表征实验，全面了解了催化性能的调控机制和关键的CO吸附构型。在还原催化剂中，Rh以两种形式存在：Rh ⁺在Rh-CeO ₂界面处和Rh ⁰远离界面处。 Rh-CeO ₂界面周长的总长度受Rh纳米颗粒尺寸的影响，从而调节Rh ⁰与Rh ⁺的比率。 Rh ⁰到Rh ⁺的平衡分布对于提高选择性是必要的，这表明高级醇的合成取决于Rh ⁺和Rh ⁰的协同作用，并且Rh ⁰ -Rh ⁺位点被确定为关键位点。 此外，我们还阐明了在反应条件下稳定吸附在Rh/CeO ₂表面上的CO的构型：Rh ⁺ ₂ H _x –(CO)和Rh ⁰ _2- (CO)。研究发现，两个吸附的 CO 之间的 C-C 耦合对于高级醇的生产至关重要。