RESUMO
Peroxydisulfate (PDS) and peroxymonosulfate (PMS) could be efficiently activated by heat to generate reactive oxygen species (ROS) for the degradation of organic contaminants. However, defects including the inefficiency treatment and pH dependence of monooxidant process are prominent. In this study, synergy of heat and the PDS-PMS binary oxidant was studied for efficient triclosan (TCS) degradation and apply in rubber wastewater. Under different pH values, the degradation of TCS followed pseudo-first-order kinetics, the reaction rate constant (kobs) value of TCS in heat/PDS/PMS system increased from 1.8 to 4.4 fold and 6.8-49.1 fold when compared to heat/PDS system and heat/PMS system, respectively. Hydroxyl radicals (·OH), sulfate radicals (SO4·-) and singlet oxygen (1O2) were the major ROS for the degradation of TCS in heat/PDS/PMS system. In addition, the steady-state concentrations of ·OH/1O2 and SO4·-/·OH/1O2 increased under acidic conditions and alkaline conditions, respectively. It was concluded that the pH regulated the ROS for degradation of TCS in heat/PDS/PMS system significantly. Based on the analysis of degradation byproducts, it was inferred that the dechlorination, hydroxylation and ether bond breaking reactions occurred during the degradation of TCS. Moreover, the biological toxicity of the ten byproducts was lower than that of TCS was determined. Furthermore, the heat/PDS/PMS system is resistant to the influence of water substrates and can effectively improve the water quality of rubber wastewater. This study provides a novel perspective for efficient degradation of TCS independent of pH in the heat/PDS/PMS system and its application of rubber wastewater.
Assuntos
Triclosan , Poluentes Químicos da Água , Oxidantes/química , Águas Residuárias , Espécies Reativas de Oxigênio , Borracha , Oxirredução , Poluentes Químicos da Água/química , Peróxidos/químicaRESUMO
Biochars are being increasingly applied in soil for carbon sequestration, fertility improvement, as well as contamination remediation. Phosphoric acid (H3PO4) pretreatment is a method for biochar modification, but the mechanism is not yet fully understood. In this work, biochars and the raw biomass were treated by H3PO4 prior to pyrolysis. Due to an acid catalysis and crosslink, the micropores of the pretreated particles were much more than those without H3PO4 pretreatment, resulting in the dramatical enhancement of specific surface areas of the pretreated particles. Crystalline cellulose (CL) exhibited a greater advantage in the formation of micropores than of amorphous lignin (LG) with H3PO4 modification. The formation mechanisms of micropores were: (a) H+ from H3PO4 contributes to micropores generation via H+ catalysis process; (b) the organic phosphate bridge protected the carbon skeleton from micropore collapse via the crosslinking of phosphate radical. The sorption capacities to carbamazepine (CBZ) and bisphenol A (BPA) increased after H3PO4 modification, which is ascribed to the large hydrophobic surface areas and more abundant micropores. Overall, H3PO4 pretreatment produced biochars with large surface area and high abundance of porous structures. Furthermore, the H3PO4 modified biochars can be applied as high adsorbing material as well as P-rich fertilizer.
Assuntos
Biomassa , Carvão Vegetal , Ácidos Fosfóricos , Adsorção , Compostos Benzidrílicos/análise , Carbamazepina/análise , Carbono , Sequestro de Carbono , Fertilizantes , Interações Hidrofóbicas e Hidrofílicas , Lignina/química , Fenóis/análise , Solo/químicaRESUMO
Three soils with different tillage activities were collected and compared for their organic matter sources and degradation. Two soils (TD and TP) with human activities showed more diverse of chemicals in both free lipids and CuO oxidation products than the one (NS) without human activities. Branched alkanoic acids only accounted for less than 5% of lipids, indicating limited microbial inputs in all three investigated soils. The degradation of lignin in NS and TD was relatively higher than TP, probably because of the chemical degradation, most likely UV light-involved photodegradation. Lignin parameters obtained from CuO oxidation products confirmed that woody gymnosperm tissue (such as pine trees) may be the main source for NS, while angiosperm tissues from vascular plant may be the predominant source for the lignins in TD and TP. Analysis of BPCAs illustrated that BC in NS may be mainly originated from soot or other fossil carbon sources, whereas BC in TD and TP may be produced during corn stalk and straw burning. BC was involved in mineral interactions for TD and TP. The dynamics of organic matter needs to be extensively examined for their nonideal interactions with contaminants.
Assuntos
Agricultura , Solo/química , Carbono/química , Carbono/metabolismo , China , Cobre/química , Cromatografia Gasosa-Espectrometria de Massas , Humanos , Lignina/química , Lignina/metabolismo , Lipídeos/química , Oxirredução , Fotólise/efeitos da radiação , Raios UltravioletaRESUMO
Channels formed by membrane proteins regulate the transport of water, ions or nutrients that are essential to cells' metabolism. Recent advances in nanotechnology allow us to fabricate solid-state nanopores for transporting and analyzing biomolecules. However, uncontrollable surface properties of a fabricated nanopore cause irregular transport of biomolecules, limiting potential biomimetic applications. Here we show that a nanopore functionalized with a self-assembled monolayer (SAM) can potentially regulate the transport of a DNA molecule by changing functional groups of the SAM. We found that an enhanced interaction between DNA and a SAM-coated nanopore can slow down the translocation speed of DNA molecules and increase the DNA capture-rate. Our results demonstrate that the transport of DNA molecules inside nanopores could be modulated by coating a SAM on the pore surface. Our method to control the DNA motion inside a nanopore may find its applications in nanopore-based DNA sequencing devices.