Catalytic Activity Enhancement on Alcohol Dehydrogenation via Directing Reaction Pathways from Single- to Double-Atom Catalysis,Journal of the American Chemical Society

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Catalytic Activity Enhancement on Alcohol Dehydrogenation via Directing Reaction Pathways from Single- to Double-Atom Catalysis
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-03-09 , DOI: 10.1021/jacs.1c12705
Ce Liu ₁ , Teng Li ₁ , Xingchao Dai ₁ , Jian Zhao ₁ , Dongcheng He _{1,

2} , Guomin Li _{1,

2} , Bin Wang ₁ , Xinjiang Cui ₁

Affiliation

To further improve the intrinsic reactivity of single-atom catalysts (SACs), the controllable modification of a single site by coordinating with a second neighboring metal atom, developing double-atom catalysts (DACs), affords new opportunities. Here we report a catalyst that features two bonded Fe–Co double atoms, which is well represented by an FeCoN₆(OH) ensemble with 100% metal dispersion, that work together to switch the reaction mechanism in alcohol dehydrogenation under oxidant-free conditions. Compared with Fe-SAC and Co-SAC, FeCo-DAC displays higher activity performance, yielding the desired products in up to 98% yields. Moreover, a broad diversity of benzyl alcohols and aliphatic alcohols convert into the corresponding dehydrogenated products with excellent yields and high selectivity. The kinetic reaction results show that lower activation energy is obtained by FeCo-DAC than that by Fe-SAC and Co-SAC. Moreover, computational studies demonstrate that the reaction path by DACs is different from that by SACs, providing a rationale for the observed enhancements.

中文翻译：

从单原子催化到双原子催化引导反应途径提高乙醇脱氢的催化活性

为了进一步提高单原子催化剂（SACs）的内在反应性，通过与第二个相邻金属原子配位对单个位点进行可控修饰，开发双原子催化剂（DACs），提供了新的机遇。在这里，我们报告了一种具有两个键合 Fe-Co 双原子的催化剂，这很好地代表了 FeCoN ₆(OH) 集合与 100% 金属分散体，它们共同作用以在无氧化剂条件下切换醇脱氢的反应机制。与 Fe-SAC 和 Co-SAC 相比，FeCo-DAC 表现出更高的活性性能，以高达 98% 的收率产生所需的产品。此外，多种苯甲醇和脂肪醇以优异的收率和高选择性转化为相应的脱氢产物。动力学反应结果表明，FeCo-DAC获得的活化能低于Fe-SAC和Co-SAC。此外，计算研究表明，DAC 的反应路径与 SAC 的反应路径不同，为观察到的增强提供了依据。

更新日期：2022-03-09

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