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A Monodisperse ε′-(CoxFe1–x)2.2C Bimetallic Carbide Catalyst for Direct Conversion of Syngas to Higher Alcohols
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-05-06 , DOI: 10.1021/acscatal.2c01078 Zhuang Zeng 1 , Zhuoshi Li 1, 2 , Li Kang 1 , Xiaoxue Han 1 , Zouxuan Qi 1 , Shaoxia Guo 1 , Junhu Wang 3 , Alexandre Rykov 3 , Jing Lv 1 , Yue Wang 1, 2 , Xinbin Ma 1, 2
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-05-06 , DOI: 10.1021/acscatal.2c01078 Zhuang Zeng 1 , Zhuoshi Li 1, 2 , Li Kang 1 , Xiaoxue Han 1 , Zouxuan Qi 1 , Shaoxia Guo 1 , Junhu Wang 3 , Alexandre Rykov 3 , Jing Lv 1 , Yue Wang 1, 2 , Xinbin Ma 1, 2
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Higher alcohol synthesis (HAS) from syngas through nonpetroleum carbon resources is quite prospective but still challenging owing to the unsatisfactory selectivity and catalytic stability. Here, we proposed a monodisperse ε′-(CoxFe1–x)2.2C alloy carbide catalyst derived from CoxFe3–xO4 spinel oxide nanoparticles, which was applied in the HAS reaction. The Co/Fe molar ratio showed a significant impact on the evolution of active sites, and the catalyst with a Co/Fe molar ratio of 1/2 contained the highest ε′-(CoxFe1–x)2.2C content of 80.2%, which achieved the best selectivity and space time yield toward higher alcohols (HA) as high as 38.5% and 1.932 g g(Fe + Co)–1 h–1, outperforming most of the reported modified Fischer–Tropsch synthesis catalysts for HAS. Density functional theory calculations further confirmed that the formation of ε′-(CoxFe1–x)2.2C alloy carbide became more difficult when the Co/Fe ratio exceeds 1/2. It is demonstrated that the ε′-(CoxFe1–x)2.2C exhibited moderate bonding with CO, which is crucial for the balance between CO dissociation and CO insertion, thus increasing the HA selectivity. The Co1Fe2 catalyst with a robust CoFe alloy carbide structure exhibited stable catalytic performance for over 300 h because of the inhibition of phase separation and surface carbon deposition. These insights into the formation and properties of CoFe alloy carbide may provide possibilities for the development of bimetallic catalysts for HAS.
中文翻译：
用于将合成气直接转化为高级醇的单分散 ε'-(CoxFe1–x)2.2C 双金属碳化物催化剂
通过非石油碳资源从合成气合成高级醇（HAS）具有相当的前景，但由于选择性和催化稳定性不理想，仍然具有挑战性。在这里，我们提出了一种衍生自 Co x Fe 3– x O 4尖晶石氧化物纳米颗粒的单分散 ε'-(Co x Fe 1– x ) 2.2 C 合金碳化物催化剂，并将其应用于 HAS 反应。Co/Fe摩尔比对活性位点的演化有显着影响，Co/Fe摩尔比为1/2的催化剂含有最高的ε′-(Co x Fe 1- x ) 2.2C 含量为 80.2%，实现了对高级醇 (HA) 的最佳选择性和时空产率，高达 38.5% 和 1.932 gg (Fe + Co) –1 h –1，优于大多数报道的改性费托合成HAS的催化剂。密度泛函理论计算进一步证实，当Co/Fe比超过1/2时，ε'-(Co x Fe 1- x ) 2.2 C合金碳化物的形成变得更加困难。证明了ε′-(Co x Fe 1– x ) 2.2C表现出与CO的适度结合，这对于CO解离和CO插入之间的平衡至关重要，从而增加了HA的选择性。由于抑制了相分离和表面碳沉积，具有坚固的 CoFe 合金碳化物结构的 Co 1 Fe 2催化剂表现出稳定的催化性能超过 300 小时。这些对 CoFe 合金碳化物的形成和性质的见解可能为开发用于 HAS 的双金属催化剂提供可能性。
更新日期：2022-05-06
中文翻译：
用于将合成气直接转化为高级醇的单分散 ε'-(CoxFe1–x)2.2C 双金属碳化物催化剂
通过非石油碳资源从合成气合成高级醇（HAS）具有相当的前景，但由于选择性和催化稳定性不理想，仍然具有挑战性。在这里，我们提出了一种衍生自 Co x Fe 3– x O 4尖晶石氧化物纳米颗粒的单分散 ε'-(Co x Fe 1– x ) 2.2 C 合金碳化物催化剂，并将其应用于 HAS 反应。Co/Fe摩尔比对活性位点的演化有显着影响，Co/Fe摩尔比为1/2的催化剂含有最高的ε′-(Co x Fe 1- x ) 2.2C 含量为 80.2%，实现了对高级醇 (HA) 的最佳选择性和时空产率，高达 38.5% 和 1.932 gg (Fe + Co) –1 h –1，优于大多数报道的改性费托合成HAS的催化剂。密度泛函理论计算进一步证实，当Co/Fe比超过1/2时，ε'-(Co x Fe 1- x ) 2.2 C合金碳化物的形成变得更加困难。证明了ε′-(Co x Fe 1– x ) 2.2C表现出与CO的适度结合，这对于CO解离和CO插入之间的平衡至关重要，从而增加了HA的选择性。由于抑制了相分离和表面碳沉积，具有坚固的 CoFe 合金碳化物结构的 Co 1 Fe 2催化剂表现出稳定的催化性能超过 300 小时。这些对 CoFe 合金碳化物的形成和性质的见解可能为开发用于 HAS 的双金属催化剂提供可能性。
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