Pd Catalysts Supported on Mixed Iron and Titanium Oxides in Phenylacetylene Hydrogenation: Effect of TiO2 Content in Magnetic Support Material

苯乙炔加氢中混合铁和钛氧化物负载的 Pd 催化剂:磁性载体材料中 TiO2 含量的影响

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作者:Eldar T Talgatov, Akzhol A Naizabayev, Farida U Bukharbayeva, Alima M Kenzheyeva, Raiymbek Yersaiyn, Assemgul S Auyezkhanova, Sandugash N Akhmetova, Evgeniy V Zhizhin, Alexandr R Brodskiy

Abstract

Recently, Pd catalysts supported on magnetic nanoparticles (MNPs) have attracted a great attention due to their ability of easy separation with an external magnet. Modification of MNPs is successfully used to obtain Pd magnetic catalysts with enhanced catalytic activity. In this work, we discussed the effect of titania content in TiO2/MNPs support materials on catalytic properties of Pd@TiO2/MNPs catalysts in phenylacetylene hydrogenation. TiO2/MNPs composites were prepared by simple ultrasound-assisted mixing of TiO2 and MNPs, synthesized by co-precipitation method. This was followed by deposition of palladium ions on the mixed metal oxides using NaOH as precipitant. The supports and catalysts were characterized using XRD, BET, STEM, EDX, XPS, and a SQUID magnetometer. Pd nanoparticles (5-6 nm) formed were found to be homogeneously distributed on support materials representing the well-mixed metal oxides with TiO2 content of 10, 30, 50, or 70%wt. Testing of the catalysts in phenylacetylene hydrogenation showed that their activity increased with increasing TiO2 content, and the process was faster in alkali medium (pH = 10). The hydrogenation rates of triple and double C-C bonds on Pd@70TiO2/MNPs achieved 9.3 × 10-6 mol/s and 23.1 × 10-6 mol/s, respectively, and selectivity to styrene was 96%. The catalyst can be easily recovered with an external magnet and reused for 12 runs without significant degradation in the catalytic activity. The improved catalytic properties of Pd@70TiO2/MNPs can be explained by the fact that the surface of the support is mainly composed of TiO2 particles, affecting the state and size of Pd species.

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