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镧促进的Ni/γ -Al₂O₃用于甲烷干重整的比较研究——喷雾干燥法增强镍分散及强化金属-载体相互作用

Comparative study on La-promoted Ni/γ-AlO for methane dry reforming - spray drying for enhanced nickel dispersion and strong metal-support interactions.

作者信息

Pegios N, Bliznuk V, Prünte S, Schneider J M, Palkovits R, Simeonov K

机构信息

Department of Heterogeneous Catalysis, Chemical Technology (ITMC), RWTH Aachen University Worringerweg 2 Aachen 52074 North Rhine-Westphalia Germany

Department of Electrical Energy, Metals, Mechanical Construction & Systems (EEMMeCS), Group Metals Science & Technology Tech Lane Ghent Science Park - Campus A, Technologiepark 903 B-9052 Gent Belgium.

出版信息

RSC Adv. 2018 Jan 2;8(2):606-618. doi: 10.1039/c7ra06570a.

Abstract

Dry reforming of methane (DRM) enables an efficient utilization of two abundant greenhouse gases by converting them into syngas, a versatile feedstock for chemical synthesis. Aiming for high catalyst performance and enhanced coke resistance, different preparation techniques of La-promoted Ni/γ-AlO catalysts for DRM were compared facilitating structure-performance correlations. The studied synthesis techniques comprehend incipient wetness impregnation and co-precipitation as well as alternative techniques such as spray drying. All catalysts were fully characterized before and after reaction by N-physisorption, XRD, H-TPR and STEM-EDX elemental mapping. Additionally, a thorough investigation of carbon deposits has been carried out by TGA/DSC and STEM-EDX, respectively. The different preparation techniques led generally to very different physical properties, structure, chemical species and anti-coking properties of the catalyst. However, some catalysts with similar physicochemical characteristics differed in catalytic performance and coking resistance. Superior catalytic performance could be reached for catalysts prepared by spray drying and related to excellent Ni dispersion, strong metal-support interaction and very low coke formation of only 2.7% of the catalyst weight. After 6 h time on stream only minor sintering occurred, with few Ni nanoparticles up to 10 nm.

摘要

甲烷干重整(DRM)通过将两种丰富的温室气体转化为合成气(一种用于化学合成的通用原料),实现了对它们的高效利用。为了获得高催化剂性能和增强抗积碳性能,比较了用于DRM的La促进的Ni/γ -Al₂O₃催化剂的不同制备技术,以促进结构-性能关联。所研究的合成技术包括初湿浸渍、共沉淀以及喷雾干燥等替代技术。所有催化剂在反应前后都通过N-物理吸附、XRD、H-TPR和STEM-EDX元素映射进行了全面表征。此外,分别通过TGA/DSC和STEM-EDX对碳沉积物进行了深入研究。不同的制备技术通常导致催化剂具有非常不同的物理性质、结构、化学物种和抗结焦性能。然而,一些具有相似物理化学特性的催化剂在催化性能和抗焦性方面存在差异。通过喷雾干燥制备的催化剂可实现优异的催化性能,这与出色的Ni分散性、强金属-载体相互作用以及仅为催化剂重量2.7%的极低积碳形成有关。在6小时的运行时间后,仅发生了轻微的烧结,只有少数直径达10 nm的Ni纳米颗粒。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0e68/9076903/ee075a5661a0/c7ra06570a-f1.jpg

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