Transformation of syngas to valuable oxygenated products over Rh-MnOx/SiO2, Rh-Co/ZrO2 and Rh-Cu/ZrO2 catalysts

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2024-06-29 DOI:10.1016/j.apcata.2024.119852

Noora Lind, Atte Aho, Kari Eränen, Pasi Virtanen, Irina Simakova, Päivi Mäki-Arvela, Dmitry Yu. Murzin

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Abstract

The conversion of syngas into higher alcohols was examined using bimetallic Rh-Co, Rh-Cu, and multimetallic RhCuPd catalysts, all of which were supported on ZrO₂. This process was also studied using a MnOx-promoted Rh/SiO₂ catalyst. These experiments were conducted within a temperature range of 225–300 °C, under a pressure of 30 bar, and with a H₂/CO ratio of 2. The catalysts were characterized using a variety of physicochemical methods, including Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS), and Carbon Monoxide Diffuse Reflectance Infrared Fourier Transform Spectroscopy (CO DRIFTS). The Rh particle sizes in the fresh catalysts were found to be less than 3 nm. The Rh-Co catalyst supported on ZrO₂ exhibited the highest selectivity to ethanol, achieving 38 % at a CO conversion rate of 58 % at 275 °C. This catalyst also demonstrated a chain growth probability of 0.35 for alcohols. A slightly higher chain growth probability was observed with the Rh-MnOx/SiO₂ catalyst, although this also resulted in the formation of substantial amounts of acetic acid. Interestingly, this acetic acid could be converted into ketones when RhMnOx was used in conjunction with Pd/ZrO₂.

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在 Rh-MnOx/SiO2、Rh-Co/ZrO2 和 Rh-Cu/ZrO2 催化剂上将合成气转化为有价值的含氧产品

使用双金属 Rh-Co、Rh-Cu 和多金属 RhCuPd 催化剂（均以 ZrO2 为载体）研究了合成气转化为高级醇的过程。此外，还使用 MnOx 促进的 Rh/SiO2 催化剂对这一过程进行了研究。这些实验的温度范围为 225-300℃，压力为 30 巴，H2/CO 比为 2。催化剂的表征采用了多种物理化学方法，包括透射电子显微镜 (TEM)、X 射线衍射 (XRD)、X 射线光电子能谱 (XPS) 和一氧化碳漫反射红外傅立叶变换能谱 (CO DRIFTS)。发现新鲜催化剂中的 Rh 粒子尺寸小于 3 nm。以 ZrO2 为载体的 Rh-Co 催化剂对乙醇的选择性最高，在 275 °C、一氧化碳转化率为 58% 的条件下，乙醇的选择性达到 38%。这种催化剂对乙醇的链增长概率也达到了 0.35。Rh-MnOx/SiO2 催化剂的链增长概率略高，但也会形成大量乙酸。有趣的是，当 RhMnOx 与 Pd/ZrO2 结合使用时，这种醋酸可转化为酮。

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.