Rosette-like Layered Double Hydroxides: Adsorbent Materials for the Removal of Anionic Pollutants from Water.
Kenji TamuraRina KawashiriNobuo IyiYujiro WatanabeHiroshi SakumaMasumi KamonPublished in: ACS applied materials & interfaces (2019)
Rosette-like layered double hydroxide (roseLDH) crystals with interlayer CO32- anions were synthesized by the reaction of Mg(NO3)2, Al(NO3)3, and hexamethylenetetramine (HMT) at 140 °C over 4 days. Crystals as large as 20 μm were produced when using a specific range of HMT concentrations. The substitution of CO32- interlayer ions with ClO4- or Cl- anions was achieved by the addition of perchloric acid or hydrochloric acid, respectively, to dispersion of material in methanol. The products were denoted as CO32-roseLDH, ClO4-roseLDH, and Cl-roseLDH, respectively. These LDHs were characterized using X-ray diffraction under controlled relative humidity, as well as by Fourier transform infrared spectroscopy and scanning electron microscopy. Adsorption experiment with anions such as phosphate (HPO42-) and nitrate (NO3-) was conducted by using ClO4-roseLDH and Cl-roseLDH. The results indicate that both anions were adsorbed through an ion-exchange mechanism. The maximum HPO42- adsorption capacity at equilibrium on ClO4-roseLDH was 1.6 mmol g-1 (49.6 mg P g-1), which corresponds to approximately 75% of the total positive layer charge. Cl-roseLDH showed a similar adsorption capability. Commercially available platelike LDH particles were essentially impermeable to water flow due to clogging, while the roseLDH crystals showed excellent permeability, an order of magnitude higher than that exhibited by the platelike LDH synthesized using a homogeneous precipitation method with different growth conditions. Anion adsorption during batch and flow-through test with the ClO4-roseLDH (mean particle diameter ∼ 38 μm) in a packed bed showed good uptake of HPO42- and NO3- from aqueous solutions. These results demonstrate the potential of roseLDH materials to serve as a column filler adsorbent of the hazardous anions.