Journal of Catalysis ( IF 6.5 ) Pub Date : 2019-08-01 , DOI: 10.1016/j.jcat.2019.06.023 Yuanyuan Ma , Zhongling Lang , Jing Du , Likai Yan , Yonghui Wang , Huaqiao Tan , Shifa Ullah Khan , Yang Liu , Zhenhui Kang , Yangguang Li
Selective reduction of nitroarenes is extremely valuable in industrial chemical production. The main reduced products are usually aniline derivatives obtained using single-component noble- or transition-metal catalysts; however, other important products such as hydrazobenzene derivatives always involve in harsh conditions and multiple reaction steps. Here, we realize an unexpected switchable reduction of nitroarenes into aniline or hydrazobenzene derivatives with high yield and selectivity just by controlling the molar ratio of nitroarenes to N2H4·H2O with a nickel–tungsten carbide composite nanocatalyst loaded on carbon (Ni-WC/C). A series of control experiments and density functional theory (DFT) calculations indicate that the multiple interfaces between Ni and WC can induce a synergistic effect, significantly modulating the electronic structure of the Ni-WC/C catalyst, and endowing the catalyst with switchable selectivity and high activity for the reduction of nitroarenes by hydrogenation. This synergistic multi-interfacial catalyst may offer a new way to design and explore highly efficient and selective catalysts for the controllable reduction of nitroarenes and similar hydrogenation reactions.
中文翻译:
一种可选择性切换的多界面Ni-WC杂化催化剂,可有效还原硝基芳烃
选择性还原硝基芳烃在工业化学生产中非常有价值。主要的还原产物通常是使用单组分贵金属或过渡金属催化剂获得的苯胺衍生物。但是,其他重要的产物,例如苯衍生物,总是要在苛刻的条件下和多个反应步骤中进行。在此,仅通过控制硝基芳烃与N 2 H 4 ·H 2的摩尔比,就可以实现高产率和高选择性地将硝基芳烃意外地还原为苯胺或苯衍生物。O,负载在碳上的镍-碳化钨复合纳米催化剂(Ni-WC / C)。一系列控制实验和密度泛函理论(DFT)计算表明,Ni和WC之间的多个界面可产生协同效应,显着调节Ni-WC / C催化剂的电子结构,并使催化剂具有可切换的选择性和选择性。氢化还原硝基芳烃的高活性。这种协同的多界面催化剂可能为设计和探索高效和选择性的催化剂提供新途径,以控制硝基芳烃的还原反应和类似的氢化反应。