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Synthesis of highly dispersed Pd nanoparticles supported on multi-walled carbon nanotubes and their excellent catalytic performance for oxidation of benzyl alcohol

机译:多壁碳纳米管上负载的高分散钯纳米粒子的合成及其对苯甲醇氧化的优异催化性能

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摘要

Narrow sized and highly homogeneous dispersed Pd nanoparticles have been synthesized on nitric acid-functionalized multi-walled carbon nanotubes (CNTs) without a capping agent. The TEM images show that the extremely small Pd nanoparticles with an average size of about 1.5 nm were homogeneously dispersed on the surface of the CNTs. The characterization results indicate that the pretreatment with nitric acid not only improved the dispersion of Pd, but also enhanced the strong interaction between the Pd nanoparticles and the CNTs, thereby preventing their agglomeration and leaching in the liquid phase. On pretreatment with HNO3, it is possible to generate more acidic groups on the surface of CNTs without a significant change in textural properties. The catalytic performance of the aforementioned material was investigated for selective oxidation of benzyl alcohol. Pd/CNTs exhibits high activity (~98% conversion) and selectivity (~90%) to benzaldehyde with excellent reusability. The high activity of the catalyst was attributed to the small size, high dispersion of Pd nanoparticles and higher accessibility of reactants. A careful analysis of the kinetic data suggests that there are different sites for the disproportionation and oxidation reactions. The excellent reusability of Pd/CNT catalysts makes this material a promising candidate for selective benzyl oxidation. Further, the results of the present study show that it is possible to synthesize uniformly dispersed Pd nanoparticles on various carbon supports without a capping agent.
机译:在没有封端剂的情况下,已经在硝酸官能化的多壁碳纳米管(CNT)上合成了尺寸狭窄且高度均匀的Pd纳米颗粒。 TEM图像显示平均尺寸为约1.5nm的极小的Pd纳米颗粒均匀地分散在CNT的表面上。表征结果表明,硝酸预处理不仅改善了Pd的分散性,而且增强了Pd纳米颗粒与CNT之间的强相互作用,从而防止了它们在液相中的团聚和浸出。在用HNO3预处理时,有可能在CNT的表面上产生更多的酸性基团,而不会明显改变织构性质。研究了上述材料对苯甲醇的选择性氧化的催化性能。 Pd / CNT表现出高活性(〜98%转化率)和对苯甲醛的选择性(〜90%),具有出色的可重复使用性。催化剂的高活性归因于Pd纳米颗粒的小尺寸,高分散性和较高的反应物可及性。仔细分析动力学数据表明歧化和氧化反应存在不同的位置。 Pd / CNT催化剂极好的可重复使用性使该材料成为选择性苄基氧化的有前途的候选者。此外,本研究的结果表明,可以在没有封端剂的情况下在各种碳载体上合成均匀分散的Pd纳米颗粒。

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