Center for Molecular Science and Engineering, College of Science, Northeastern University, Shenyang 110819, PR China.
College of Chemistry and Materials Science, Fujian Normal University, Fuzhou, Fujian 350007, PR China.
Int J Biol Macromol. 2024 Oct;278(Pt 3):134573. doi: 10.1016/j.ijbiomac.2024.134573. Epub 2024 Aug 30.
The utilization efficiency of palladium-based catalysts has sharply increased in many catalytic reactions. However, numerous studies have shown that preparing alloys of palladium with other metals has superior catalytic activity than pure palladium. Additionally, hierarchical porous carbon has gradually developed into an excellent carrier for loading bimetallic nanoparticles. In this study, we firstly pyrolyzed chitosan, sodium bicarbonate and nickel nitrate to create highly dispersed porous carbon materials doped with Ni NPs. The carbon materials were then grafted with silane coupling agent (APTMS) to afford them with amino groups on the surface. Taking advantage of the fact that Pd can react with Ni in spontaneous reduction reaction, Pd was deposited on the surface of Ni to produce PdNi bimetallic-loaded carbon catalysts containing amino groups. The resulting catalysts were examined by a series of characterizations and were found to have a hierarchically porous structure and large specific surface area, which increased the number of active sites of the catalysts. In comparison to other Pd catalysts, the PdNi/HPCS-NH catalysts displayed remarkable activity for Suzuki coupling reaction and hydro reduction of nitroaromatics, which exhibited a high turnover frequency value (TOF) of 37,857 h and 680.9 h, respectively. These were mainly due to the high dispersion of the PdNi NPs and the superior structure of the carriers. Moreover, the catalysts did not experience a significant decline in activity after ten cycles. All in all, this investigation has created a new approach for the fabrication of novel carriers for Pd catalysts, which is in line with the concept of green chemistry and recyclable.
钯基催化剂在许多催化反应中的利用率大幅提高。然而,许多研究表明,制备钯与其他金属的合金比纯钯具有更高的催化活性。此外,分级多孔碳已逐渐发展成为负载双金属纳米粒子的优良载体。在本研究中,我们首先通过热解壳聚糖、碳酸氢钠和硝酸镍制备了高度分散的多孔碳材料,该材料掺杂有 Ni NPs。然后,将碳材料接枝上硅烷偶联剂(APTMS),使表面带有氨基。利用 Pd 可以在自发还原反应中与 Ni 反应的事实,将 Pd 沉积在 Ni 的表面上,制备出含有氨基的 PdNi 负载型碳催化剂。通过一系列的表征对所得催化剂进行了研究,发现其具有分级多孔结构和大的比表面积,从而增加了催化剂的活性位点数量。与其他 Pd 催化剂相比,PdNi/HPCS-NH 催化剂在 Suzuki 偶联反应和硝基芳烃的加氢还原反应中表现出显著的活性,其 TOF 值分别高达 37857 h 和 680.9 h。这主要归因于 PdNi NPs 的高分散性和载体的优越结构。此外,催化剂在十次循环后活性没有明显下降。总之,这项研究为 Pd 催化剂的新型载体的制备开辟了一条新途径,符合绿色化学和可回收的理念。