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Tailoring Pt-Fe2O3 Interfaces for Selective Reductive Coupling Reaction to Synthesize Imine
作者: 来源 : 时间:2016-12-09 字体<    >

The tailoring of metal-metal oxide interface has emerged as an effective way to improve the activity of heterogeneous catalysts. The traditional way to introduce metal-metal oxide interface is dispersing metal NPs on the oxide support. However, most conventional support and metal NPs are structurally non-uniform, and the structures of supported metal catalysts are not well understood. Recently, we have applied atomic layer deposition to engineer Pt-Fe3+-OH interface on multiwalled carbon nanotubes (CNTs) by selectively coating the supported Fe2O3 NPs with ultra-thin Pt shell, or depositing thin Fe2O3 films on the surface of supported Pt NPs. The catalysts with maximized ratio of Pt-Fe3+-OH interface showed high selectivity compared with the supported Pt/CNTs catalysts and the mixture of supported Pt and Fe2O3 catalysts in the one-pot synthesis of imine via tandem reductive coupling of nitrobenzene and furfural at normal temperature. The Pt-Fe3+-OH interface increased the imine selectivity by weakening the Pt-H bond and suppressing the further hydrogenation of imine. In contrast, monometallic Pt catalysts show a strong Pt-H interaction and dominant formation of amine. Further comparison revealed that the Fe2O3-Pt core-shell structure exhibited a higher TOF in the generation of imine and a better utilization of Pt than Pt-Fe2O3 core-shell structure.

We appreciate the financial support from the National Natural Science Foundation of China (21403271, 21173248 and 21403272), the Hundred Talents Program of the Chinese Academy of Sciences, the Hundred Talents Program of Shanxi Province, and the Natural Science Foundation of Shanxi Province (201411012-1 and 2015021046). This work was published in ACS CatalysisB. Zhang, X.-W. Guo, H. Liang, H. Ge, X. Gu, S. Chen, H. Yang, Y. Qin, Tailoring Pt–Fe2O3 Interfaces for Selective Reductive Coupling Reaction To Synthesize Imine, ACS Catalysis, (2016) 6560-6566)。

 

 

负载型金属催化剂是应用最为广泛的多相催化剂。金属-金属氧化物界面的组成和机构可显著影响催化剂的性能。精细调控金属-氧化物界面结构是提高多相催化剂催化性能的有效手段。传统方法多通过将金属纳米颗粒分散在氧化物载体上来形成金属-金属氧化物界面,不能在埃的尺度精细调控界面结构,难以获得界面主导的高效催化剂。原子层沉积技术(atomic layer deposition, ALD)由于其自限制特性和单原子层状的生长方式,在纳米尺度精细设计调控金属-金属氧化物界面结构有着显著的优势。最近,我们用ALD技术制备了一种新型的Fe2O3-Pt核壳结构催化剂,利用Pt超薄修饰Fe2O3纳米颗粒,在低温硝基苯加氢偶联糠醛制备亚胺反应中,其TOF和选择性显著高于同尺度的单金属Pt催化剂和氧化铁超薄修饰的Pt催化剂。进一步的研究表明,表面的Pt-Fe3+-OH界面位点弱化了Pt-H键,抑制了亚胺的过度加氢,而将Pt超薄负载在Fe2O3纳米颗粒显著提高了Pt的利用率和Pt-Fe3+-OH界面位点数目。该方法具有一定的普适性,可以用于精确调控其他金属-氧化物界面催化剂。该项目得到了国家自然科学基金(21403271, 2117324821403272)、中科院百人计划、山西省百人计划、山西省自然科学基金(201411012-1,2015021046) 等的支持。该工作发表在ACS CatalysisB. Zhang, X.-W. Guo, H. Liang, H. Ge, X. Gu, S. Chen, H. Yang, Y. Qin, Tailoring Pt–Fe2O3 Interfaces for Selective Reductive Coupling Reaction To Synthesize Imine, ACS Catalysis, (2016) 6560-6566)。

论文链接:http://pubs.acs.org/doi/abs/10.1021/acscatal.6b01756

 


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