RESUMO
A self-powered photoelectrochemical (PEC) sensor has attracted widespread attention in the field of analysis, but it is still a challenge to enhance its response signals with rational strategies. In this work, a novel self-powered PEC sensing platform was developed for the quantitative detection of gatifloxacin (GAT) based on a photofuel cell consisting of two types of ZIF-derived ZnO/Co3O4 heterojunctions as photoactive materials. Peroxymonosulfate (PMS) was first used as an electron acceptor coupled with a photofuel cell to develop a synergetic signal amplification strategy. In a dual-photoelectrode system, the PMS activation on the ZnO@Co3O4 photocathode not only accelerated electron transfer from the Co3O4@ZnO photoanode to achieve strong signal intensity but also improved the sensing sensitivity by the oxidation reaction of generated highly active radicals to GAT. Compared with the absence of electron acceptors, the introduction of PMS produced a 2-fold enhancement in the signal output performance and a more than 72-fold improvement in the signal sensitivity. For the construction of the sensing interface, a molecularly imprinted polymer was assembled on the photocathode to specifically recognize GAT. The proposed sensor exhibited a detection range of 10-1 to 105 pM with a detection limit of 0.065 pM. The proposed sensing method has the advantages of sensitivity, simplicity, reliable stability, and anti-interference ability, which opens the door to the design of high-performance self-powered PEC sensors.
Assuntos
Técnicas Biossensoriais , Cobalto , Óxidos , Peróxidos , Óxido de Zinco , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/métodos , Limite de DetecçãoRESUMO
The aging of microplastics (MPs) is extremely influenced by photochemically-produced reactive intermediates (PPRIs), which are mediated by natural photosensitive substances. Algal extracellular polymeric substances (EPS) can produce PPRIs when exposed to sunlight. Nonetheless, the specific role of EPS in the aging process of MPs remains unclear. This work systematically explored the aging process of polystyrene (PS) MPs in the EPS secreted by Chlorella vulgaris under simulated sunlight irradiation. The results revealed that the existence of EPS accelerated the degradation of PS MPs into particles with sizes less than 1 µm, while also facilitating the formation of hydroxy groups on the surface. The release rate of dissolved organic matter (DOM) from PS MPs was elevated from 0.120 mg·L-1·day-1 to 0.577 mg·L-1·day-1. The primary factor contributing to the elevated levels of DOM was humic acid-like compounds generated through the breakdown of PS. EPS accelerated the aging process of PS MPs by primarily mediating the formation of triplet excited states (3EPS*), singlet oxygen (1O2), and superoxide radicals (O2â-), resulting in indirect degradation. 3EPS* was found to have the most substantial impact. This study makes a significant contribution to advance understanding of the environmental fate of MPs in aquatic environments impacted by algal blooms.
Assuntos
Chlorella vulgaris , Poluentes Químicos da Água , Microplásticos , Plásticos , Matriz Extracelular de Substâncias Poliméricas/química , Luz Solar , Poliestirenos , Poluentes Químicos da Água/análise , Substâncias Húmicas/análiseRESUMO
Herein, ternary metal-organic frameworks (MOFs)-derived MnCoFeO with different levels of oxygen vacancies (Ov) were designed by adjusting the doping amount of Mn and employed to activate peroxymonosulfate (PMS) for sulfamethoxazole (SMX) degradation. The MnCoFeO-2 with the largest Ov content exhibited the highest SMX degradation efficacy. Almost 100% of SMX was removed within 5 min using the MnCoFeO-2/PMS system. The reaction rate constant (kobs) was 1.7321 min-1, which was 4.1 times that of CoFeO (0.4195 min-1). Both the SO4â¢- and 1O2 were the dominant reactive oxygen species. Significantly, the relationship among Ov, radical pathways, and non-radical pathways was explored for the first time. The results showed that Ov could regulate the radical pathways by promoting the adsorption of PMS onto MnCoFeO-2. Ov was positively correlated with 1O2 (P < 0.05) and facilitated the direct electron transfer. The superior catalytic activity of MnCoFeO was attributed to the Fe, Co, Mn active sites, Lewis basic sites and Ov in MnCoFeO. Mn(II) not only contributed to the formation of Ov, but also facilitated the reduction of Fe(III). Additionally, Ov was mainly concentrated near the low-valent metal ions, thus the synergistic effect between the metal active sites and Ov promoted the activation of PMS.
Assuntos
Estruturas Metalorgânicas , Poluentes Químicos da Água , Compostos Férricos , Oxigênio , Peróxidos/química , Espécies Reativas de Oxigênio , Sulfametoxazol/química , Poluentes Químicos da Água/químicaRESUMO
Here, we studied seasonal variation of effluent organic matter (EfOM), based on molecular weight distribution and fluorescent components, during the traditional anaerobic/anoxic/oxic (A2O) wastewater treatment processes. Microbial community structure and effect of temperature on some isolated pure strains were analyzed to explain the related mechanism. Results showed that the anaerobic process played a key role in EfOM removal by removing building blocks, low molecular weight (LMW) neutrals, biopolymers, and protein-related substances (C4 and C5), thus determining the fate of EfOM during the A2O processes. On the other hand, humic substances, LMW neutrals, large molecular-sized hydrophobic humic-like compounds (C3), and aromatic proteins (C4) were generated during the anoxic process in summer and winter. Proteobacteria (Gamma-, Beta-, and Alpha-proteobacteria) and Bacteroidetes constituted over 50% of the sludge community. Temperature was found to be positively correlated with the generation of soluble microbial products (SMP) based on the performance of the mixture of isolated Herbaspirillum sp. (Beta-proteobacteria) and Pseudomonas sp. (Gamma-proteobacteria). Through comprehensive analysis of the co-action of Proteobacteria and temperature, we proposed the Synergetic Effect of Temperature and Proteobacteria as a possible mechanism of the seasonal variation of EfOM. These findings are important for understanding the fate of EfOM during the wastewater treatment processes and therefore be helpful for better EfOM control.