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Construction of green nanostructured heterogeneous catalysts via non-covalent surface decoration of multi-walled carbon nanotubes with Pd(II) complexes of azamacrocycles
Journal of Catalysis ( IF 7.3 ) Pub Date : 2017-08-09 , DOI: 10.1016/j.jcat.2017.07.023
Matteo Savastano , Paloma Arranz-Mascarós , Carla Bazzicalupi , Maria Paz Clares , Maria Luz Godino-Salido , Maria Dolores Gutiérrez-Valero , Mario Inclán , Antonio Bianchi , Enrique García-España , Rafael López-Garzón

Green nanostructured heterogeneous catalysts were prepared via a bottom-up strategy. Designed ligands were synthesized joining covalently an electrondeficient pyrimidine residue and a scorpiand azamacrocycle. The desired molecular properties were easily transferred to nanostructured materials in two steps: first, exploiting their spontaneous chemisorption onto multi-walled carbon nanotubes (MWCNTs) via the pyrimidinic moiety in water at room temperature, then, taking advantage of the easy coordination of Pd(II) to the azamacrocycle in the same conditions. An evenly distribution of catalytic centres was obtained on the MWCNTs surface. Catalytic properties of these materials were assessed toward the Cu-free Sonogashira cross-coupling, leading to significant improvements in terms of yields and reaction conditions, especially when considering the possibility to maintain yields of 90%, or above, in a feasible amount of time (2 h), while working under green conditions (water, 50 °C, aerobic atmosphere). The catalysts proved to be reusable for several cycles with good yields.



中文翻译:

通过含氮杂大环的Pd(II)配合物的多壁碳纳米管的非共价表面装饰来构建绿色纳米结构的非均相催化剂

通过自下而上的策略制备了绿色纳米结构的非均相催化剂。合成设计的配体,该配体共价连接缺电子的嘧啶残基和蝎形的氮杂大环。所需的分子特性很容易通过两步转移到纳米结构材料上:首先,通过室温下水中的嘧啶部分将其自发化学吸附到多壁碳纳米管(MWCNT)上,然后利用Pd的易配位性( II)在相同条件下进行氮杂双环。在MWCNTs表面上获得了催化中心的均匀分布。对这些材料的催化性能进行了评估,以实现无铜的Sonogashira交叉偶联,从而在产率和反应条件方面取得了显着改善,尤其是考虑在绿色条件下(水,50°C,有氧气氛)工作时,在可行的时间内(2小时)保持90%或更高的产量的可能性。事实证明,该催化剂可重复使用多个周期,收率良好。

更新日期:2017-08-09
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