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用于CO加氢反应中镍和钌催化剂的石墨烯基材料载体：性能及杂质作用的判定

Graphene-Based Material Supports for Ni- and Ru- Catalysts in CO Hydrogenation: Ruling out Performances and Impurity Role.

作者信息

Ebrahim Atakoohi Sina, Riani Paola, Spennati Elena, Savio Letizia, Vattuone Luca, De Maron Jacopo, Garbarino Gabriella

机构信息

Department of Civil, Chemical, and Environmental Engineering, University of Genova, Via Opera Pia 15, 16145, Genova, Italy.

Department of Chemistry and Industrial Chemistry, University of Genova, Via Dodecaneso 31, 16146, Genova, Italy.

出版信息

ChemSusChem. 2024 Dec 6;17(23):e202400993. doi: 10.1002/cssc.202400993. Epub 2024 Oct 10.

DOI:10.1002/cssc.202400993
PMID:39042568
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11632576/
Abstract

Laboratory-prepared Gnp using molten salt, commercial Gnp and reduced graphene oxide (rGO) have been characterized and utilized as support for CO hydrogenation catalysts. Ni- and Ru- catalysts supported over Gnp, commercial Gnp and rGO have been deeply characterized at different stages using Raman, IR, XRD, FE-SEM-EDXS, SEM-EDXS, XPS, and TEM, also addressing carbon loss before reaction and evolved species, thus allowing a better comprehension of the produced materials. Ni and Ru/rGO were inactive while Gnp-supported ones were active. Ru has been found almost completely selective toward reverse Water Gas Shift to CO, approaching the forecasted thermodynamic equilibrium at 723 K, in the tested conditions (Y~55 %), with an apparent activation energy in the range of 70-90 kJ/mol. Exhaust catalysts pointed out the presence of sulfur partially linked to the carbon matrix and partially producing the corresponding metal sulfide with the detection of surface oxidized species in the cationic form and adsorbed species as well. The metal-based nanoparticles displayed a quite narrow size distribution, confirming the promising behavior of these catalytic systems for CO utilization.

摘要

使用熔盐法在实验室制备的石墨烯纳米片（Gnp）、商用Gnp和还原氧化石墨烯（rGO）已被表征，并用作CO加氢催化剂的载体。负载在Gnp、商用Gnp和rGO上的Ni和Ru催化剂在不同阶段通过拉曼光谱、红外光谱、X射线衍射、场发射扫描电子显微镜-能谱仪（FE-SEM-EDXS）、扫描电子显微镜-能谱仪（SEM-EDXS）、X射线光电子能谱和透射电子显微镜进行了深入表征，还研究了反应前的碳损失和逸出物种，从而更好地理解所制备的材料。Ni/rGO和Ru/rGO无活性，而负载在Gnp上的催化剂具有活性。在测试条件下（Y~55 %），发现Ru几乎完全选择性地发生逆水煤气变换生成CO，在723 K时接近预测的热力学平衡，表观活化能在70-90 kJ/mol范围内。尾气催化剂表明存在部分与碳基质结合的硫，部分硫生成相应的金属硫化物，同时检测到阳离子形式的表面氧化物种和吸附物种。金属基纳米颗粒的尺寸分布相当窄，证实了这些催化体系在CO利用方面的良好性能。

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