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Efficient photocatalytic one-pot hydrogenation and N-alkylation of nitrobenzenes/benzonitriles with alcohols over Pd/MOFs: Effect of the crystal morphology & “quasi-MOF” structure
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-06-04 , DOI: 10.1016/j.jcat.2020.05.033
Hongmei Cheng , Xingyu Long , Fengxia Bian , Chaofen Yang , Xingyan Liu , Heyan Jiang

One-pot multi-step reactions over visible-light induced catalysis feature the sustainable green process. Here, ligand structure change and 2-MI coordinated modulation were adapted to adjust the crystal size, morphology and crystalline structure of Fe-MOFs; double solvent impregnation was employed for the Pd loading; “quasi-MOF” materials with retained morphology were formed with calcination under N2. Above modified materials were employed as multifunctional photocatalysts for highly efficient one-pot hydrogenation and N-alkylation of nitrobenzenes or benzonitriles with alcohols after in situ Pd photoreduction. Photocatalytic performance was evidently affected by the Fe-MOFs crystal size, morphology, crystalline structure alteration and “quasi-MOF” construction. One-pot hydrogenation and N-alkylation of benzonitriles with alcohols was achieved with excellent catalytic performance firstly in heteroegeneous catalysis. Reaction mechanism was proposed with the assistance of in situ DRIFTS.



中文翻译:

在Pd / MOF上用醇对光催化硝基苯/苯甲腈进行光催化一锅加氢和N-烷基化:晶体形态和“准MOF”结构的影响

在可见光诱导的催化作用下的一锅多步反应具有可持续的绿色过程。在这里,配体结构的变化和2-MI协调的调制被用来调整Fe-MOFs的晶体尺寸,形态和晶体结构。Pd负载采用双溶剂浸渍。在N 2下煅烧形成具有保留形态的“准MOF”材料。上述改性材料被用作多功能光催化剂,用于原位Pd光还原后,硝基苯或苄腈与醇的高效一锅式加氢和N-烷基化。Fe-MOFs的晶体大小,形态,晶体结构改变和“准MOF”结构明显影响了光催化性能。首先在异相催化中以优异的催化性能实现了苯甲腈与醇的一锅式加氢和N-烷基化反应。在原位DRIFTS的协助下,提出了反应机理。

更新日期:2020-06-04
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