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Architecture controlled PtNi@mSiO(2) and Pt-NiO@mSiO(2) mesoporous core-shell nanocatalysts for enhanced p-chloronitrobenzene hydrogenation selectivity

机译:体系结构控制的PtNi @ mSiO(2)和Pt-NiO @ mSiO(2)介孔核壳纳米催化剂可提高对氯硝基苯的加氢选择性

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Architecture controlled PtNi@mSiO(2) and Pt-NiO@mSiO(2) mesoporous core-shell nanocatalysts were synthesized for selective p-chloronitrobenzene hydrogenation to p-chloroaniline. Tetradecyl trimethyl ammonium bromide (TTAB) capped PtNi nanoparticles (NPs) were coated by SiO2 through the hydrolysis of tetraethylorthosilicate. The resultant PtNi@SiO2 core-shell NPs were calcined to remove TTAB to obtain mesoporous Pt-NiO@SiO2 core-shell nanocatalysts (Pt-NiO@mSiO(2)), which were subsequently reduced by hydrogen to form mesoporous PtNi@SiO2 core-shell nanocatalysts (PtNi@mSiO(2)). The relevant characterizations such as XRD, TEM, H-2-TPR, and BET confirm that the PtNi@mSiO(2) NPs consist of PtNi alloy nanoparticle cores and mesoporous SiO2 shells while the Pt-NiO@mSiO(2) NPs contain Pt-NiO heteroaggregate nanoparticle cores and mesoporous SiO2 shells. The catalytic results for selective hydrogenation of p-chloronitrobenzene show that the selectivity of p-chloroaniline formation over the PtNi@mSiO(2) and Pt-NiO@mSiO(2) nanocatalysts is significantly improved relative to that of control Pt@mSiO(2) nanocatalysts. Moreover, the PtNi@mSiO(2) and Pt-NiO@mSiO(2) nanocatalysts demonstrate high stability during multiple cycles of catalytic hydrogenation reactions. The enhanced catalytic performance is ascribed to the metal-metal interaction for the PtNi@mSiO(2) catalysts and metal-oxide interaction for the Pt-NiO@mSiO(2) catalysts.
机译:合成了可控制的PtNi @ mSiO(2)和Pt-NiO @ mSiO(2)介孔核-壳纳米催化剂,用于选择性对氯硝基苯加氢成对氯苯胺。通过原硅酸四乙酯的水解作用,用SiO2包覆四烷基三甲基溴化铵(TTAB)的PtNi纳米颗粒(NPs)。煅烧生成的PtNi @ SiO2核-壳NPs以去除TTAB,以获得中孔Pt-NiO @ SiO2核-壳纳米催化剂(Pt-NiO @ mSiO(2)),随后将其通过氢气还原以形成中孔PtNi @ SiO2核壳纳米催化剂(PtNi @ mSiO(2))。 XRD,TEM,H-2-TPR和BET等相关特征证明PtNi @ mSiO(2)NPs由PtNi合金纳米颗粒核和中孔SiO2壳组成,而Pt-NiO @ mSiO(2)NPs中包含Pt -NiO异质聚集纳米颗粒核和中孔SiO2壳。对氯硝基苯选择性加氢的催化结果表明,相对于对照Pt @ mSiO(2),PtNi @ mSiO(2)和Pt-NiO @ mSiO(2)纳米催化剂上对氯苯胺形成的选择性显着提高。 )纳米催化剂。此外,PtNi @ mSiO(2)和Pt-NiO @ mSiO(2)纳米催化剂在催化加氢反应的多个循环中表现出很高的稳定性。增强的催化性能归因于PtNi @ mSiO(2)催化剂的金属-金属相互作用和Pt-NiO @ mSiO(2)催化剂的金属-氧化物相互作用。

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