Efforts spanning decades toward the implementation of direct synthesis of higher alcohols from syngas have been unfruitful. Progress is hindered by insufficient understanding derived from catalyst complexity, as the need for different functionalities usually requires combining various metals, promoters, and supports. We reveal that iron becomes a remarkable catalyst when promoted by zirconia. Iron with 10 mol % ZrO achieves a space-time yield of 250 mg h g and 30% selectivity to higher alcohols at their optimized conditions, superior to reported monometallic Fe catalysts and comparable to state-of-the-art multimetallic materials. This catalyst, with an outstanding balance between performance and simplicity, was examined via X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Oxygen vacancy formation and healing in amorphous ZrO clusters enhance H and CO activation and FeC formation in contact with FeO. Activity-composition correlations suggest this FeO-FeC interface as the active phase. Promoted monometallic iron emerges as a promising platform for future generations of catalysts.

中文翻译：

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有缺陷的氧化锆促进单金属铁催化剂用于高级醇合成


数十年来从合成气直接合成高级醇的努力一直没有成果。由于对催化剂复杂性的理解不足，进展受到阻碍，因为对不同功能的需求通常需要结合各种金属、促进剂和载体。我们发现，在氧化锆的促进下，铁成为一种出色的催化剂。含有 10 mol% ZrO 的铁在优化条件下实现了 250 mg hg-1 的时空产率和 30% 的高级醇选择性，优于报道的单金属 Fe 催化剂，与最先进的多金属材料相当。通过 X 射线衍射 (XRD)、X 射线吸收光谱 (XAS) 和漫反射红外傅里叶变换光谱 (DRIFTS) 对该催化剂在性能和简单性之间具有出色的平衡。无定形 ZrO 簇中氧空位的形成和愈合增强了 H 和 CO 的活化以及与 FeO 接触的 FeC 的形成。活性-成分相关性表明该 FeO-FeC 界面为活性相。促进的单金属铁成为未来几代催化剂的有前途的平台。