State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Gansu Provincial Engineering Laboratory for Chemical Catalysis, Lanzhou University, Lanzhou 730000, PR China.
Key Laboratory of Evidence of Science and Technology Research and Application, Gansu Institute of Political Science and Law, PR China.
J Colloid Interface Sci. 2018 Jul 1;521:132-140. doi: 10.1016/j.jcis.2018.03.041. Epub 2018 Mar 14.
Nowadays, chemical catalytic methods for the treatment of organic wastes are attracting more and more research attention. In the current research, novel catalysts with palladium nanoparticles (Pd NPs) supported on the hollow mesoporous silica nanotubes (h-mSiO) were synthesized for the catalytic reduction of 4-nitrophenol (4-NP) and hydrodechlorination (HDC) of 4-chlorophenol (4-CP). The key point for the fabrication of the catalysts is that a certain thickness of the silica shell was wrapped on the multiwalled carbon nanotubes (MWNTs) or Pd/MWNTs through biphase stratification approach, and then the samples were calcined to remove the MWNTs. Thereby, h-mSiO and Pd@h-mSiO samples were obtained. The prepared materials have excellent pore structure and exhibit high specific surface areas. The reduction of 4-NP by the Pd/h-mSiO and Pd@h-mSiO catalysts showed higher TOF values than many other catalysts, and the yield of HDC of 4-CP to phenol reached 100% with a low loading of Pd in water solvent. The excellent catalytic activities of the Pd/h-mSiO and Pd@h-mSiO catalysts should attribute to the excellent connectivity of the h-mSiO which not only can increase the accessibility of the Pd active sites but also enhance the mass transfer of the reactants. It is worth mention that, there is almost no Pd NPs aggregation or losing during the reaction process, and the prepared catalysts still showed good catalytic activity and physical stability after recycling. Moreover, the catalyst shows potential for catalytic reduction of nitroarenes in a fixed bed reactor, thus could be used for continuously treat nitroarenes polluted water.
如今,用于处理有机废物的化学催化方法引起了越来越多的研究关注。在当前的研究中,合成了负载在中空介孔硅纳米管(h-mSiO)上的钯纳米颗粒(Pd NPs)的新型催化剂,用于催化还原 4-硝基苯酚(4-NP)和 4-氯苯酚(4-CP)的加氢脱氯(HDC)。制备催化剂的关键在于通过双相分层法在多壁碳纳米管(MWNTs)或 Pd/MWNTs 上包裹一定厚度的硅壳,然后将样品煅烧以去除 MWNTs。从而得到 h-mSiO 和 Pd@h-mSiO 样品。所制备的材料具有优异的孔结构,并表现出高的比表面积。由 Pd/h-mSiO 和 Pd@h-mSiO 催化剂还原 4-NP 显示出比许多其他催化剂更高的 TOF 值,并且在水溶剂中低负载量的 Pd 下,4-CP 的 HDC 产率达到 100%。Pd/h-mSiO 和 Pd@h-mSiO 催化剂的优异催化活性应归因于 h-mSiO 的优异连通性,这不仅可以增加 Pd 活性位的可及性,而且还可以增强反应物的传质。值得一提的是,在反应过程中几乎没有 Pd NPs 聚集或损失,并且在回收后,所制备的催化剂仍然表现出良好的催化活性和物理稳定性。此外,该催化剂在固定床反应器中对硝基芳烃的催化还原表现出潜力,因此可用于连续处理硝基芳烃污染的水。