3D printed monoliths: From powder to an efficient catalyst for antibiotic degradation

To improve the effectiveness and durability of wastewater treatment technologies, researchers are showing a growing interest in 3D printing technology. This technology has attracted significant interest owing to its ability to fabricate challenging complex geometries using different material compositions. This manuscript is focused on the development of 3D monoliths from noncommercial filaments, i.e., a powder blend of iron oxide and polylactic acid (PLA) at 15 wt% of the former. Different monolith designs have been prepared to improve the fluid dynamics of the process, so a simple cylinder (15-Fe₃O₄@PLA) and a cylinder with double the length and an internal mesh (15-Fe₃O₄@PLA-DM) were used. These monoliths were characterized by Scanning electron microscopy (SEM), Differential scanning calorimetry (DSC) and Mössbauer spectroscopy, then used for water-based ofloxacin degradation in a continuous down-up flow configuration. Additionally, computational fluid dynamics simulations were performed to estimate the degradation rate constants and analyze the distribution of fluid velocity and pollutant concentration along the 15-Fe₃O₄@PLA-reactor. The oxidant dose was also optimized to develop the highest degradation rate. The degradation of the target pollutant for those monoliths was 55 and 82 % under optimized conditions. In addition, the 15-Fe₃O₄@PLA-DM monolith was operated for long term experiments, keeping the degradation performance at a good 67 % for up to 120 h. Finally a fixed-bed reactor was mounted with printed pellets of the mixture (15:85), Fe₃O₄:PLA, after being ground in a range of 125-200 μm. Under this setup configuration, we observed the total degradation of ofloxacin. 3D printing technology is cheap, reproducible and time saving in the development of supported catalysts in comparison with conventional deposition techniques. Moreover, the leaching of active sites on streams was largely diminished. In fact under continuous operation the leached Fe concentration is below 0.1 ppm, corroborating the good adhesion of the catalyst in the PLA support.