火焰湿浸渍Co/CeO2制备Co/CeO2的CO2甲烷化研究

IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL
ChemCatChem Pub Date : 2025-07-10 DOI:10.1002/cctc.202500679
Angelina Evtushkova, Jason M.J.J. Heinrichs, Nikolay Kosinov, Emiel J.M. Hensen
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引用次数: 0

摘要

采用湿浸渍法将Co浸渍在火焰合成的CeO2上,制备了一套不同Co负载的Co/CeO2催化剂,并进行了CO2甲烷化试验。在低Co负荷(2.5 mol.%)下,Co以Co2+离子形式存在,与CeO2强相互作用,在300℃时仍未还原。这种高度分散的Co2+ (~ 2.5 mol.%)在所有催化剂中都是恒定的。较高的Co负载(5和10 mol.%)导致分离的Co3O4纳米颗粒(~ 2-2.5 nm),在300°C时部分还原为金属Co纳米颗粒(2.5 - 3 nm)。当Co含量较低时,浸渍催化剂主要生成Co, CO2转化率较低,而Co含量≥5 mol%的催化剂有利于生成CH₄,Co和c2h是₆副产物。在CO加氢作用下,这些样品对烯烃和氧化物的选择性较高(86%),对CH₄的选择性较低。所有催化剂在CO和CO₂加氢过程中都经历了失活,这归因于CO纳米颗粒上的碳沉积。高度分散的Co2 +和小Co簇具有更强的失活抗性和Co生成选择性。氧化再生有效地去除碳沉积,恢复初始活性。这些结果突出了Co分散度和粒径对Co 2加氢过程中产物选择性和催化剂稳定性的影响。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

CO2 Methanation Of Co/CeO2 Prepared by Wetness Impregnation of Co on Flame-Synthesized CeO2

CO2 Methanation Of Co/CeO2 Prepared by Wetness Impregnation of Co on Flame-Synthesized CeO2

CO2 Methanation Of Co/CeO2 Prepared by Wetness Impregnation of Co on Flame-Synthesized CeO2

CO2 Methanation Of Co/CeO2 Prepared by Wetness Impregnation of Co on Flame-Synthesized CeO2

A set of Co/CeO2 catalysts with varying Co loading was prepared by wet impregnation of Co onto flame-synthesized CeO2 and tested in CO2 methanation. At low Co loading (2.5 mol.%), Co existed as Co2+ ions strongly interacting with CeO2, which remained unreduced at 300 °C. This population of highly dispersed Co2+ (∼2.5 mol.%) was constant across all catalysts. Higher Co loadings (5 and 10 mol.%) led to segregated Co3O4 nanoparticles (∼2–2.5 nm), which partially reduced to metallic Co nanoparticles (2.5 – 3 nm) at 300 °C. At low Co content, the impregnated catalysts mainly produced CO at a low CO2 conversion, while catalysts ≥ 5 mol% Co favored CH₄ formation with minor CO and C₂H₆ by-products. Under CO hydrogenation, these samples showed high selectivity toward olefins and oxygenates (86%) and low CH₄ selectivity. All catalysts experienced deactivation during CO and CO₂ hydrogenation, attributed to carbon deposition on Co nanoparticles. The highly dispersed Co2⁺ and small Co clusters were more resistant to deactivation and selective for CO production. Oxidative regeneration effectively removed carbon deposits and restored initial activity. These results highlight the influence of Co dispersion and particle size on product selectivity and catalyst stability during CO₂ hydrogenation.

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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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