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Design of efficient supported Pd-Co catalysts for selective hydrogenation of acetylene
Journal of Catalysis ( IF 7.3 ) Pub Date : 2024-03-06 , DOI: 10.1016/j.jcat.2024.115417
Daria V. Yurpalova , Tatyana N. Afonasenko , Igor P. Prosvirin , Andrey V. Bukhtiyarov , Larisa M. Kovtunova , Zakhar S. Vinokurov , Mikhail V. Trenikhin , Evgeny Yu. Gerasimov , Evgeny V. Khramov , Dmitry A. Shlyapin

The research is devoted to the study of active component formation in the novel Pd-Co catalysts supported on carbon material Sibunit. It was shown that 0.5 %Pd–0.5 %Co/C samples exhibit high ethylene yield in the acetylene hydrogenation process due to the presence of fcc PdCo particles. According to XRD-TPR analysis, solid solution formation begins during the reduction of samples in H at T ≥ 500 °C. Using the EXAFS, XRD and EDX it was established that H-treatment at 500 °C leads to the formation of ∼PdCo particles and an increase in the reduction temperature to 600 and 700 °C is accompanied by the enrichment of the Pd-Co-phase with cobalt to ∼PdCo and ∼PdCo compositions, respectively. The ethylene yield on Pd-Co/C catalysts reduced at 500, 600 and 700 °C is 56, 66 and 68 %, respectively, which significantly exceeds the ethylene quantity obtained on monometallic Pd/C samples (∼52 %). It is assumed that the excellent selectivity of Pd-Co/C samples treated in H at 600 and 700 °C is due to an increase in the amount of palladium atoms surrounded by cobalt and a change in the palladium electronic state (XPS).

中文翻译:

高效负载型 Pd-Co 乙炔选择性加氢催化剂的设计

该研究致力于研究碳材料 Sibunit 负载的新型 Pd-Co 催化剂中活性组分的形成。结果表明,由于存在面心立方 PdCo 颗粒,0.5%Pd–0.5%Co/C 样品在乙炔加氢过程中表现出高乙烯产率。根据 XRD-TPR 分析,在 T ≥ 500 °C 时样品在 H 中还原期间开始固溶体形成。使用 EXAFS、XRD 和 EDX 确定,500 °C 下的 H 处理会导致~PdCo 颗粒的形成,并且还原温度升高至 600 和 700 °C 伴随着 Pd-Co- 的富集。分别含有钴的~PdCo和~PdCo组合物。 Pd-Co/C 催化剂在 500、600 和 700 °C 还原时的乙烯收率分别为 56%、66% 和 68%,明显超过单金属 Pd/C 样品获得的乙烯量(~52%)。据推测,在 600 和 700 °C H 中处理的 Pd-Co/C 样品具有优异的选择性,这是由于钴包围的钯原子数量增加以及钯电子态 (XPS) 的变化。
更新日期:2024-03-06
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