RESUMO
Heteroatom-doped carbon materials can effectively activate H2O2 into â¢OH during the metal-free electro-Fenton (EF) process. However, information on bifunctional catalysts for the simultaneous generation and activation of H2O2 is scarce. In this study, O- and F-doped porous carbon cathode materials (PPCs) were prepared by the direct carbonization of polyvinylidene fluoride (PVDF) for sulfamerazine (SMR) removal in a metal-free EF process. The porous structure and chemical composition of the PPCs were regulated by the carbonization temperature. PPC-6 (carbonized at 600 °C) exhibited optimal electrocatalytic performance in terms of electrochemical H2O2 generation and activation owing to its high specific surface area, mesoporous structure, and optimum fractions of doped O and F. Excellent performance of the 2e- oxygen reduction reaction was found with an H2O2 selectivity of 93.5% and an average electron transfer number of 2.13. An H2O2 accumulative concentration of 103.9 mg/L and an SMR removal efficiency of 90.1% were achieved during the metal-free EF process. PPC-6 was able to stably remove SMR over five consecutive cycles, retaining 92.6% of its original performance. Quantitative structure-activity relationship analysis revealed that doped oxygen functional groups contributed substantially to H2O2 generation, and semi-ionic C-F bonds with high electronegativity were the cause of the activation of H2O2 to â¢OH. These findings suggest that the PVDF-derived carbonaceous catalysts are feasible and desirable for metal-free EF processes.
Assuntos
Sulfamerazina , Poluentes Químicos da Água , Carbono , Polímeros de Fluorcarboneto , Peróxido de Hidrogênio/química , Metais , Oxirredução , Oxigênio/análise , Polivinil , Porosidade , Poluentes Químicos da Água/análiseRESUMO
Fenton process is the most popular for wastewater treatment among all available advanced oxidation processes (AOPs). Numerous endeavors have been devoted to improving the oxidation efficiency of Fenton reaction in terms of promoting ·OH generation, accelerating iron redox cycle and extending applicable pH range. However, in addition to oxidation, coagulation and adsorption also simultaneously occur in the Fenton process, which play important role in the removal of pollutants. Rapid progress has revealed the synergistic effects of oxidation, coagulation and adsorption in the Fenton process, providing new ideas for the treatment of complex and refractory wastewater. Based on available studies, this review is the first to systematically summarize the research progress regarding the synergistic effects of oxidation, coagulation and adsorption in the integrated Fenton-based processes for wastewater treatment. The involved mechanism of the synergistic effects in different Fenton processes (homogeneous Fenton, heterogeneous Fenton and physical field-assistant Fenton coupling process) are critically reviewed. Furthermore, special attention has been paid to the representative applications of the synergistic effects in wastewater treatment (such as industrial organic wastewater, landfill leachate and heavy metal-organic complexes, etc.), particularly focusing on the operation parameters and removal performance. Finally, a conclusion of the review and subsequently, perspectives are given for possible research directions. We believe this review can provide useful information for researchers and end-users involved in the development and application of the Fenton process in wastewater treatment.
Assuntos
Águas Residuárias , Poluentes Químicos da Água , Adsorção , Peróxido de Hidrogênio , Oxirredução , Eliminação de Resíduos LíquidosRESUMO
Recently, increasing attention has been paid to the inactivation of antibiotic resistant bacteria (ARB) during the electrochemical disinfection. However, no available information could be found on ARB inactivation in water during metal-free electrochemical disinfection. In this study, polyvinylidene fluoride (PVDF)-based carbon catalyst (PPC) was chosen as working electrode. Batch experiments were conducted to investigate key design for ARB inactivation, effects of water matrix and potential risks after the disinfection under the pre-determined conditions. The disinfection with current density at 2.25 mA/cm2 and Air/Water ratio of 10:1 was optimal with the largest ARB inactivation (5.0 log reduction for 40 min), which was in line with the profile and yield of hydrogen peroxide (H2O2) during the disinfection. Effects of water matrix analysis implied that ARB inactivation efficiencies during the disinfection in acidic solutions were better than the one in alkaline solutions, which could be due to rich CC levels on surface of PPC cathode. After the optimal disinfection, ARB counts increased slightly at the first 2 h and then tended to disappear, and there were no conjugation transfer and little transformation for target antibiotic resistance genes, indicating that potential risks could be blocked after the disinfection for 40 min. Furthermore, intermittent flow was more effective in inactivating ARB compared with continuous flow. These suggested that the application of metal-free electrochemical disinfection with PPC to inactivate ARB in water was feasible and desirable in this study.
Assuntos
Desinfecção , Purificação da Água , Antagonistas de Receptores de Angiotensina/farmacologia , Inibidores da Enzima Conversora de Angiotensina/farmacologia , Antibacterianos/farmacologia , Bactérias , Carbono/farmacologia , Peróxido de Hidrogênio/farmacologia , Águas Residuárias/microbiologia , Água/farmacologiaRESUMO
Solidification/stabilization (S/S) is an option for the treatment of electrolytic manganese residue (EMR). Basic burning raw material (BRM) could successfully solidify/stabilize EMR, though heavy metals S/S mechanism and long-term stability remain unclear. Herein, Mn2+ and NH4+ S/S behavior, hydrated BRM and S/S EMR characterization, Mn2+ long-term leaching behavior, phase and morphology changes for long-term leaching were discussed in detail to clarify these mechanisms. Mn2+ and NH4+ leaching concentrations as well as pH value in S/S EMR were respectively 0.02 mg/L, 0.68 mg/L and 8.75, meeting the regulations of Chinese standard GB 8978-1996. Long-term stability of EMR was significantly enhanced after S/S. Mn2+ leaching concentration, Mn2+ migration, Mn2+ cumulative release, Mn2+ apparent diffusion coefficient and conductivity of EMR reduced to 0.05 mg/L, 5.5 × 10-6 mg/(m2·s), ~ 9 mg/m2, 6.30 × 10-15 m2/s and 435 µs/cm. Mechanism studies showed that the hydration of BRM forms OH-, calcium silicate hydrate gels (C-S-H) and ettringite. Therefore, during S/S process, NH4+ was escaped as NH3, Mn2+ was solidified/stabilized as tephroite (Mn2SiO4), johannsenite (CaMnSi2O6) and davreuxite (MnAl6Si4O17(OH)2), and Pb2+, Cu2+, Ni2+, Zn2+ were solidified/stabilized by C-S-H and ettringite via substitution and encapsulation. This study provides a good choice for EMR long-term stable storage.
Assuntos
Metais Pesados , Eliminação de Resíduos , Eletrólise , Eletrólitos/química , Íons , Manganês/químicaRESUMO
Tissue hemodynamics, including the blood flow, oxygenation, and oxygen metabolism, are closely associated with many diseases. As one of the portable optical technologies to explore human physiology and assist in healthcare, near-infrared diffuse optical spectroscopy (NIRS) for tissue oxygenation measurement has been developed for four decades. In recent years, a dynamic NIRS technology, namely, diffuse correlation spectroscopy (DCS), has been emerging as a portable tool for tissue blood flow measurement. In this article, we briefly describe the basic principle and algorithms for static NIRS and dynamic NIRS (i.e., DCS). Then, we elaborate on the NIRS instrumentation, either commercially available or custom-made, as well as their applications to physiological studies and clinic. The extension of NIRS/DCS from spectroscopy to imaging was depicted, followed by introductions of advanced algorithms that were recently proposed. The future prospective of the NIRS/DCS and their feasibilities for routine utilization in hospital is finally discussed.