Choudhry Deepa, Winburn Matthew R, Sarin Suchit, Chimentão Ricardo J, Cheung Chin Li
Department of Chemistry, University of Nebraska-Lincoln, Lincoln, NE, 68588, U.S.A.
Department of Materials and Mechanical Engineering, University of Nebraska-Lincoln, Lincoln, NE, 68588, U.S.A.
ChemSusChem. 2025 Feb 16;18(4):e202400776. doi: 10.1002/cssc.202400776. Epub 2024 Nov 10.
The utilization of carbon dioxide through chemical conversion is a promising approach for the recycling of carbon resources. Despite well-developed industrial processes for CO hydrogenation to methanol, the effective use of CO as a feedstock remains challenging because of the costly requirements of high temperature and reaction pressure. In this paper, we report the methanol synthesis from CO and hydrogen using a dielectric barrier discharge (DBD) reactor under atmospheric pressure with a nickel-cerium-aluminum mixed oxide (Ni/Ce-Al MOx) catalyst. The combined use of plasma and the Ni/Ce-Al MOx catalyst was observed to yield 13.3±0.4 % of methanol, favorably compared to the 2.6±0.5 % yield of the case without catalyst. Microscopy images, selected area electron diffraction patterns, and energy-dispersive X-ray analysis confirmed the presence of fluorite-structured ceria, aluminium, nickel, and nickel oxide particles in the catalyst. The reaction mechanism for the plasma-assisted hydrogenation of CO was hypothesized to involve a carbide formation pathway due to the presence of carbide confirmed by X-ray photoelectron spectroscopic characterization.
通过化学转化利用二氧化碳是一种很有前景的碳资源循环利用方法。尽管将一氧化碳加氢制甲醇的工业工艺已经很成熟，但由于高温和反应压力的成本要求较高，有效利用一氧化碳作为原料仍然具有挑战性。在本文中，我们报道了在大气压下使用介电势垒放电（DBD）反应器和镍 - 铈 - 铝混合氧化物（Ni/Ce - Al MOx）催化剂，由一氧化碳和氢气合成甲醇的过程。观察到等离子体与Ni/Ce - Al MOx催化剂联合使用时甲醇产率为13.3±0.4%，与无催化剂情况下2.6±0.5%的产率相比更具优势。显微镜图像、选区电子衍射图谱和能量色散X射线分析证实催化剂中存在萤石结构的二氧化铈、铝、镍和氧化镍颗粒。通过X射线光电子能谱表征证实存在碳化物，据此推测等离子体辅助一氧化碳加氢的反应机理涉及碳化物形成途径。
