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首页> 外文期刊>Catalysis science & technology >New multicomponent catalysts for the selective aerobic oxidative condensation of benzylamine to N-benzylidenebenzylamine
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New multicomponent catalysts for the selective aerobic oxidative condensation of benzylamine to N-benzylidenebenzylamine

机译：新的多组分催化剂，用于选择性有氧氧化降温的苄胺与N-苯二烯苯甲胺的凝聚

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Aerobic oxidative condensation of benzylamine to N-benzylidenebenzylamine was carried out on new gold-based catalysts using as support bimodal UVM-7-like mesoporous silica containing Ni and Ce (or Sn) as oxide nanodomains partially embedded inside the mesoporous UVM-7 silica walls. These nanodomains acted as effective and stable inorganic anchors favoring the nucleation, growth and stability of supported gold particles. Following the atrane method ( a "one-pot" strategy able to harmonize the hydrolytic reactivity of different heteroelements through the use of complexes containing triethanolamine-derived ligands (atranes) as precursors) the stability of the oxide nanodomains during oxidation and thermal treatments was ensured. The catalysts were prepared using a two-step synthesis in which gold was incorporated through impregnation of previously synthesized bimodal porous silicas containing different heteroelements trapped by the silica mesostructure. The versatility of the preparative approach allowed the high surface area and accessibility of mesoporous silica and also an easy and homogeneous inclusion of heteroelements in one pot. Aerobic oxidative condensation of benzylamine on these catalysts occurred selectively only with the formation of N-benzylidenebenzylamine. While selectivity was total, the productivities (mol(product) g(cat)(-1) h(-1)) varied in a wide range as a function of catalyst composition (chemical composition and atomic ratios of the constitutive support elements). The catalytic behavior was merely controlled by the size of gold particles, but the support also exerts an influence. The best results were obtained on the mesoporous Au/Ce-60-Ni-10-UVM-7 catalyst having a 0.97( wt.%) gold content ( in the form of nanoparticles of ca. 4 nm) and preserving a relatively high surface area ( 566 m(2) g(-1)) and pore volume ( 0.91 cm(3) g(-1)). The comparison with the individual or bicomponent catalysts led to the conclusion of a cooperative interaction between the catalyst components. However, gold itself exhibits a higher activity than the promoters or co-catalysts (i.e. phases containing Ni and/or Ce).
机译：苄胺对N-苯甲酰烯苯甲胺的有氧氧化凝结在新的基于黄金的催化剂上使用作为含氧和氧化物纳米域的Ni和ce（或SN）的含有NI和SN）的二型UVM-7样二孔（或Sn 。这些纳米域充当有效稳定的无机锚固剂，有利于支撑金颗粒的成核，生长和稳定性。遵循实体方法（一种“单锅”策略，能够通过使用含有三乙醇胺衍生的配体（阿特拉斯）作为前体的复合物来协调不同异质元素的水解反应性），以确保氧化物纳米构和热处理过程中的氧化物纳米构象的稳定性。使用两步合成制备催化剂，通过浸入先前合成的双峰多孔硅，其中包含含有二氧化硅介质结构的不同异质元素的浸渍，将黄金掺入。制备方法的多功能性允许介孔二氧化硅的高表面积和可访问性，并且在一个锅中也容易且均匀地包含异质元素。这些催化剂上苄胺在这些催化剂上的有氧氧化凝结仅在N-苯二烯苯甲胺的形成下才有选择性地发生。虽然选择性是总的，但生产率（Mol（product）g（cat）（-1）h（-1））在较大范围内随催化剂组成的函数而变化，催化剂组成（本构构成的化学成分和原子比率）的函数。催化行为仅由金颗粒的大小控制，但支撑也会产生影响。最好的结果是在中孔AU/CE-60-NI-10-10-UVM-7催化剂上具有0.97（wt。％）的金含量（以CA. 4 nm的纳米颗粒形式），并保留相对较高的表面面积（566 m（2）g（-1））和孔体积（0.91 cm（3）g（-1））。与个体或双成分催化剂的比较导致结论催化剂成分之间的合作相互作用。然而，黄金本身比启动子或共催化剂表现出更高的活性（即包含Ni和/或CE的相）。

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