A urea-functionalized ordered mesoporous polymeric nanoparticle for removing the perrhenate anion ReO as the surrogate of the particularly intractable anion radioactive pollutant TcO was demonstrated in the present study. This nanomaterial (denoted as urea-MPN) was produced for the first time by a surfactant-directed urea-phenol-formaldehyde resol oligomers self-assembly protocol under hydrothermal condition. The obtained urea-MPN possessed the uniform nanosized spherical morphology with a 3D interconnected ordered cubic mesoporous structure. Also, the urea functional groups were succefully embedded in the polymer framework without the alteration of the molecular configuration. Meanwhile, it exhibited excellent β radiation resistance up to 200 kGy dose. We employed the perrhenate anion ReO to test its potential for the removal of anionic radioactive pollutant TcO from water. Interestingly, the optimized urea-MPN nanocomposite achieved the high removal efficiency at a low concentration of 0.25 mM within a short contact time of 30 min. The control experimental results revealed that the short nanoscale pore channels and the hydrophobic mesopore surface facilitated the hydrogen-bonding interaction between the charge-diffuse ReO tetrahedral oxoanion and the urea moieties in the framework of urea-MPN, accounting for the rapid and effective removal performance in pure water. Importantly, it can selectively capture ReO in the presence of different competitive anions including NO, CO, SO, and PO. This attractive capability of this unique nanosized mesoporous polymeric sorbent will pave the way for the diverse applications in the decontamination of nuclear wastes in a more economical and sustainable manner.
A series of Pd/Ph-SBA-15 catalysts with ordered mesoporous structure are designed by using the phenyl-functionalized SBA-15 (Ph-SBA-15) as supports. These catalysts exhibit higher activity and selectivity toward biphenyl than Pd/SiO 2 , Pd/MCM-41, Pd/Ph-MCM-41 and Pd/SBA-15 in a water-medium iodobenzene Ullmann coupling reaction. The promoting effects on the activity and selectivity could be mainly attributed to the high dispersion of Pd active sites, the ordered mesoporous channels and the strong surface hydrophobocity which facilitate the diffusion and/or adsorption of organic reactant molecules, especially in aqueous media. Meanwhile, the relatively large pore channels are favorable for the coupling of iodobenzene to form biphenyl, which is much bigger than the byproduct benzene resulting from the dehalogenation of iodobenzene. The Pd/Ph-SBA-15 catalyst could be separated easily from reaction products and used repetitively several times, showing the superiority over the homogeneous catalysts for industrial applications.
A mesoporous Pd(II) organometallic catalyst is synthesized by coordinating the Pd(II) with the amine-ligand anchored on ethyl-bridged PMOs. During Barbier reaction in water as an environmentally friendly medium, the as-prepared Pd(II)-PMOs (Et) exhibits matchable catalytic activity and selectivity with the corresponding homogeneous Pd(II) catalyst and could be used repetitively for more than 5 times, which could reduce the cost and even diminish the environmental pollution from heavy metallic ions, showing a good potential in industrial applications. On one hand, the excellent catalytic performance could be attributed to the high surface area and ordered mesporous structure of the PMOs support, which ensures the higher dispersion of Pd(II) active sites and also facilitates the diffusion of reactant molecules. On the other hand, the ethyl fragments embedded in the pore walls could enlarge mesopores and also enhance surface hydrophobility of the PMOs support, which further promotes the diffusion and adsorption of organic molecules, especially in aqueous medium, leading to higher activity and selectivity.
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