5%Ni/CeO2-Al2O3 催化剂上的二氧化碳加氢:载体成分的影响

IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Research on Chemical Intermediates Pub Date : 2024-05-29 DOI:10.1007/s11164-024-05312-7
Amir Mosayebi, Atieh Ranjbar, Mohammad Hosein Eghbal Ahmadi
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摘要

在当前工作中,研究重点是评估 5%Ni/CeO2-Al2O3 催化剂中 CeO2 与 Al2O3 的比例对 240-400 °C 温度范围内二氧化碳加氢反应的影响。主要目的是提高转化率,同时尽量减少催化剂表面的焦炭沉积。镍是通过沉积-沉淀法掺入 CeO2-Al2O3 载体的。使用热重分析 (TGA)、X 射线衍射 (XRD)、N2 吸附/解吸、温度编程还原 (TPR)、H2-化学吸附、X 射线荧光 (XRF) 和 CHNS 分析仪等技术研究了新鲜催化剂、还原催化剂和废催化剂的各种理化性质。XRD 结果表明,在 Ni/Al2O3 催化剂中添加 CeO2 以及增加杂化载体中的铈含量对晶体结构没有明显影响。但是,催化剂的还原性、焦炭沉积和焦炭形成量、催化剂表面的焦炭结构、催化性能和热稳定性等几项性能都发生了变化。Ni/Al2O3 催化剂的 CO2 转化率在最初通电 35 小时内保持相对稳定(41.25%),表明没有明显的失活现象。相反,Ni/CeO2-Al2O3 催化剂在初始 45 小时内表现出较高的稳定性。在 400 °C 下,Ni/CeO2(50%)-Al2O3(50%)的二氧化碳转化率最高(58%),这主要归因于镍物种与载体之间较低的相互作用以及较高的还原度。在 240-400 °C 的整个温度范围内,与 Ni/Al2O3 和 Ni/CeO2 催化剂相比,Ni/CeO2-Al2O3 催化剂的甲烷选择性更高,而 CO 选择性更低。
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CO2 hydrogenation over 5%Ni/CeO2–Al2O3 catalysts: effect of supports composition

In current work, the investigation centered on assessing the impact of the CeO2 to Al2O3 ratio in a 5%Ni/CeO2–Al2O3 catalyst on the CO2 hydrogenation reaction within the temperature range of 240–400 °C. The primary aim was to achieve enhanced conversion rates, while minimizing coke deposition on the catalyst surface. Nickel was incorporated into the CeO2–Al2O3 supports via the deposition–precipitation method. The various physicochemical properties of fresh, reduced and spent catalysts were studied using techniques such as thermal gravimetric analysis (TGA), X-ray diffraction (XRD), N2 adsorption/desorption, temperature programmed reduction (TPR), H2-chemisorption, X-ray fluorescence (XRF), and CHNS analyzer. XRD results revealed that the addition of CeO2 to the Ni/Al2O3 catalyst and the increase in ceria loading in the hybrid support had no obvious effect on the crystalline structure. However, several properties including reducibility, coke deposition, and coke formation quantity, coke structure on the catalyst surface, catalytic performance, and thermal stability were altered. The CO2 conversion remained relatively stable (41.25%) up to 35 h initial on stream for Ni/Al2O3 catalyst, indicating no significant deactivation. Conversely, Ni/CeO2–Al2O3 catalyst exhibited high stability up to 45 h initial. The highest CO2 conversion (58%) was achieved with the Ni/CeO2 (50%)–Al2O3 (50%) at 400 °C, primarily attributed to a lower interaction between nickel species and the support, along with a higher reduction degree. Ni/CeO2–Al2O3 catalysts displayed higher methane selectivity and lower CO selectivity compared to both Ni/Al2O3 and Ni/CeO2 catalysts across the entire temperature range of 240–400 °C.

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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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