Yasir A.J. Al-Hamadani

Sonocatalytical degradation enhancement for ibuprofen and sulfamethoxazole in the presence of glass beads and single-walled carbon nanotubes

Sonocatalytic degradation experiments were carried out to determine the effects of glass beads (GBs) and single-walled carbon nanotubes (SWNTs) on ibuprofen (IBP) and sulfamethoxazole (SMX) removal using low and high ultrasonic frequencies (28 and 1000kHz). In the absence of catalysts, the sonochemical degradation at pH 7, optimum power of 0.18WmL(-1), and a temperature of 15°C was higher (79% and 72%) at 1000kHz than at 28kHz (45% and 33%) for IBP and SMX, respectively. At the low frequency (28kHz) H2O2 production increased significantly, from 10μM (no GBs) to 86μM in the presence of GBs (0.1mm, 10gL(-1)); however, no enhancement was achieved at 1000kHz. In contrast, the H2O2 production increased from 10μM (no SWNTs) to 31μM at 28kHz and from 82μM (no SWNTs) to 111μM at 1000kHz in the presence of SWNTs (45mgL(-1)). Thus, maximum removals of IBP and SMX were obtained in the presence of a combination of GBs and SWNTs at the low frequency (94% and 88%) for 60min contact time; however, >99% and 97% removals were achieved for 40 and 60min contact times at the high frequency for IBP and SMX, respectively. The results indicate that both IBP and SMX degradation followed pseudo-first-order kinetics. Additionally, the enhanced removal of IBP and SMX in the presence of catalysts was because GBs and SWNTs increased the number of free OH radicals due to ultrasonic irradiation and the adsorption capacity increase with SWNT dispersion.

Aggregation kinetics of single walled carbon nanotubes influenced by the frequency of ultrasound irradiation in the aquatic environment

The colloidal stability of single-walled carbon nanotubes (SWNTs) sonicated at three different ultrasonication (US) frequencies (28, 580, and 1000kHz) were investigated under environmentally relevant conditions. In particular, correlations between surface chemistry, electrokinetic potential, interaction energy, and the aggregation kinetics of the aqueous SWNTs were studied. We observed that H2O2 production is negatively correlated with the yield of hydroxylation and carboxylation of SWNTs, which was dependent on the generation of ultrasonic energy by cavity collapse during US process. The SWNTs sonicated at relatively high US frequencies (580 and 1000kHz) aggregated rapidly in synthetic surface water, whereas alkalinity affected the stability of SWNTs insignificantly. This was because the SWNTs became less negatively charged under such conditions and were captured in deep primary energy wells, according to the Derjaguin-Landau-Verwey-Overbeek theory. Critical coagulation concentration values for the ultrasonicated SWNTs were determined to be 102mM NaCl for 28kHz, 22mM NaCl for 580kHz, and 43mM NaCl for 1000kHz. Suwannee River humic acid decreased the aggregation rate of SWNTs due to the steric hindrance, because of adsorbed macromolecules. Our findings show that the aggregate stability of SWNTs is controlled largely by a complex interplay between the evolution of surface functional groups on the SWNTs during US and solution chemistry.

Sonocatalytic degradation of carbamazepine and diclofenac in the presence of graphene oxides in aqueous solution

This research investigated the removal of carbamazepine (CBZ) and diclofenac (DCF) in water using ultrasonic (US) treatment in the absence or presence of graphene oxides (GOs). Three frequencies and three pH conditions were tested (28, 580, and 1000 kHz and 3.5, 7, and 9.5, respectively). Regarding the effects of US frequency and pH, 580 kHz and pH 3.5 were more effective at removing CBZ and DCF (>86% for CBZ and >92% for DCF) than 1000/28 kHz and pH 7/9.5 within 60 min. However, sonocatalytic removal was enhanced in the presence of GOs; more than 99% CBZ and DCF removal was achieved at 580 kHz and pH 3.5 within 40 min. The sonicated GOs were more stable at 28 kHz than at higher frequencies of 580 and 10,00 kHz. The adsorption of CBZ and DCF has increased when GOs were sonicated at 28 kHz (44% and 61%, respectively) compared with 580 kHz (34% and 52%, respectively) and 1000 kHz (18% and 39%, respectively). The negative charges of GOs increased at 28 kHz (-105.1 mV), however, it decreased at higher frequencies such as 580 kHz (-71.5 mV) and 1000 kHz (-58.6 mV), which led to increased electrostatic repulsion that increased the stability of the GO particles in water. The overall enhancement in CBZ and DCF removal was due to an increase in cavitational bubbles, which in turn led to increased production of OH• and enhanced adsorption due to dispersion (resulting from US irradiation), which caused an increase in active adsorption sites of the GOs.

Fabrication of graphene-oxide/β-Bi2O3/TiO2/Bi2Ti2O7 heterojuncted nanocomposite and its sonocatalytic degradation for selected pharmaceuticals

A graphene-oxide (GO)/β-Bi2O3/TiO2/Bi2Ti2O7 heterojuncted nanocomposite, designated as GBT, was synthesized via a two-step hydrothermal process. The sonocatalytic activity of the GBT was evaluated at several frequencies (28, 580, and 970 kHz) and compared with Bi-doped GO (GB) and Ti-doped GO (GT). Transmission electron microscopy images showed heterojuncted crystal structures of Bi and Ti on GO, and X-ray diffraction patterns verified that the crystal structures consisted of β-Bi2O3, TiO2, and Bi2Ti2O7 nanocomposites. Energy-dispersive X-ray spectroscopy revealed a higher proportion of metal on GBT surfaces compared with GB and GT surfaces. The energy band gaps of GT, GB, and GBT were 3.0, 2.8, and 2.5 eV, respectively. Two pharmaceuticals (PhACs; carbamazepine [CBZ] and acetaminophen [ACE]) were selected and treated under sonolytic conditions at frequencies of 28, 580, and 970 kHz at a power level of 180 W L-1. The selected pharmaceuticals, present at initial concentrations of 20 μM, were reduced by over 99% by ultrasonic irradiation in the presence of GBT. The 580 kHz treatment achieved the most rapid organic removal among the frequencies tested. The removal kinetic of CBZ was higher than that of ACE owing to its relatively high hydrophobicity. High sonocatalytic activity of GBT was observed through measurement of H2O2 in solution. Because of its low band gaps and high surface activity, GBT exhibited higher sonolytic activity in removing selected PhACs than GT or GB.