RESUMEN
Atom-site catalysts, especially for graphitic carbon nitride-based catalysts, represents one of the most promising candidates in catalysis membrane for water decontamination. However, unravelling the intricate relationships between synthesis-structure-properties remains a great challenge. This study addresses the impacts of coordination environment and structure units of metal central sites based on Mantel test, correlation analysis, and evolution of metal central sites. An optimized unconventional oxygen doping cooperated with Co-N-Fe dual-sites (OCN Co/Fe) exhibits synergistic mechanism for efficient peroxymonosulfate activation, which benefits from a significant increase in charge density at the active sites and the regulation in the natural population of orbitals, leading to selective generation of SO4 â¢-. Building upon these findings, the OCN-Co/Fe/PVDF composite membrane demonstrates a 33 min-1 ciprofloxacin (CIP) rejection efficiency and maintains over 96% CIP removal efficiency (over 24 h) with an average permeance of 130.95 L m-2 h-1. This work offers a fundamental guide for elucidating the definitive origin of catalytic performance in advance oxidation process to facilitate the rational design of separation catalysis membrane with improved performance and enhanced stability.
RESUMEN
Organic polymers hold great potential in photocatalysis considering their low cost, structural tailorability, and well-controlled degree of conjugation for efficient electron transfer. Among the polymers, Schiff base networks (SNWs) with high nitrogen content have been noticed. Herein, a series of SNWs is synthesized based on the melamine units and dialdehydes with different bonding sites. The chemical and structural variation caused by steric hindrance as well as the related photoelectric properties of the SNW samples are investigated, along with the application exploration on photocatalytic degradation and energy production. The results demonstrate that only SNW-o based on o-phthalaldehyde responds to visible light, which extends to over 550 nm. SNW-o shows the highest tetracycline degradation rate of 0.02516 min-1, under 60-min visible light irradiation. Moreover, the H2O2 production of SNW-o is 2.14 times higher than that of g-C3N4. The enhanced photocatalytic activity could be ascribed to the enlarged visible light adsorption and intramolecular electron transfer. This study indicates the possibility to regulate the optical and electrical properties of organic photocatalysts on a molecular level, providing an effective strategy for rational supramolecular engineering to the applications of organic materials in photocatalysis.
Asunto(s)
Peróxido de Hidrógeno , Bases de Schiff , Luz , Antibacterianos , PolímerosRESUMEN
In recent years, using semiconductor photocatalysts for antibiotic contaminant degradation under visible light has become a hot topic. Herein, a novel and ingenious cadmium-doped graphite phase carbon nitride (Cd-g-C3N4) photocatalyst was successfully constructed via the thermal polymerization method. Experimental and characterization results revealed that cadmium (Cd) was well doped at the g-C3N4 surface and exhibited high intercontact with g-C3N4. Additionally, the introduction of cadmium significantly improved the photocatalytic activity, and the optimum degradation efficiency of tetracycline (TC) reached 98.1%, which was exceeded 2.0 times that of g-C3N4 (43.9%). Meanwhile, the Cd-doped sample presented a higher efficiency of electrical conductivity, light absorption property, and photogenerated electron-hole pair migration compared with g-C3N4. Additionally, the quenching experiments and electron spin-resonance tests exhibited that holes (h+), hydroxyl radicals (â¢OH), superoxide radicals (â¢O2-) were the main active species involved in TC degradation. The effects of various conditions on photocatalytic degradation, such as pH, initial TC concentrations, and catalyst dosage, were also researched. Finally, the degradation mechanism was elaborated in detail. This work gives a reasonable point to synthesizing high-efficiency and economic metal-doped photocatalysts.
Asunto(s)
Grafito , Antibacterianos/química , Cadmio , Catálisis , Grafito/química , Luz , Nitrilos , Compuestos de Nitrógeno , Superóxidos , Tetraciclina/químicaRESUMEN
MOF-derived multi-metal nanomaterials are attracting numerous attentions in widespread applications such as catalysis, sensors, energy storage and conversion, and environmental remediation. Compared to the monometallic counterparts, the presence of foreign metal is expected to bring new physicochemical properties, thus exhibiting synergistic effect for enhanced performance. MOFs have been proved as a good platform for the fabrication of polymetallic nanomaterials with requisite features. Herein, various design strategies related to constructing multi-metallic nanomaterials from MOFs are summarized for the first time, involving metal nodal substitution, seed epitaxial growth, ion-exchange strategy, guest species encapsulation, solution impregnation and combination with extraneous substrate. Afterwards, the recent advances of multi-metallic nanomaterials for electrocatalytic applications, including oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), are systematically discussed. Finally, a personal outlook on the future trends and challenges are also presented with hope to enlighten deeper understanding and new thoughts for the development of multi-metal nanomaterials from MOFs.
Asunto(s)
Estructuras Metalorgánicas , Nanoestructuras , Catálisis , Estructuras Metalorgánicas/química , Metales , Nanoestructuras/química , Oxígeno/química , Estudios ProspectivosRESUMEN
Organic semiconductors have been recognized as a new generation of photocatalysts for pollutants degradation and energy production. Herein, organic heterojunction (TpMa/CN) consisting of carbon nitride and ß-ketoenamine-based covalent organic framework is fabricated via a controllable self-assembly approach. The as-prepared TpMa/CN heterojunctions show enlarged visible-light absorption. The optimum TpMa/CN-5 photocatalyst achieves the highest photocatalytic activity towards tetracycline degradation, and its photocatalytic degradation rate is improved by 2.3 and 4.3 times than TpMa and CN, respectively. As a multifunctional photocatalyst, TpMa/CN-5 sample also shows remarkable photocatalytic activity for hydrogen peroxide production (880.494 µM h-1), which is 49 times higher than that of CN. Experimental and theoretical investigations indicate that a built-in electric field is formed at the interface of composite, which enables an accelerated charge transfer and separation. This work develops an effective strategy to design difunctional photocatalyst and deciphers the electronic properties and mechanisms of g-C3N4-based organic photocatalysts, which spurs further interests for organic heterojunction photocatalysts in the future.
Asunto(s)
Estructuras Metalorgánicas , Tetraciclina , Catálisis , Luz , SemiconductoresRESUMEN
To develop efficient catalysts is one of the major ways to solve the energy and environmental problems. Spinel ferrites, with the general chemical formula of MFe2O4 (where M = Mg2+, Co2+, Ni2+, Zn2+, Fe2+, Mn2+, etc.), have attracted considerable attention in catalytic research. The flexible position and valence variability of metal cations endow spinel ferrites with diverse physicochemical properties, such as abundant surface active sites, high catalytic activity and easy to be modified. Meanwhile, their unique advantages in regenerating and recycling on account of the magnetic performances facilitate their practical application potential. Herein, the conventional as well as green chemistry synthesis of spinel ferrites is reviewed. Most importantly, the critical pathways to improve the catalytic performance are discussed in detail, mainly covering selective doping, site substitution, structure reversal, defect introduction and coupled composites. Furthermore, the catalytic applications of spinel ferrites and their derivative composites are exclusively reviewed, including Fenton-type catalysis, photocatalysis, electrocatalysis and photoelectro-chemical catalysis. In addition, some vital remarks, including toxicity, recovery and reuse, are also covered. Future applications of spinel ferrites are envisioned focusing on environmental and energy issues, which will be pushed by the development of precise synthesis, skilled modification and advanced characterization along with emerging theoretical calculation.
RESUMEN
Antibiotic residues in soil may cause potential risks to human health and soil ecosystems. To avoid these potential risks, comprehensive study of the adsorption, transport and biodegradation of antibiotics in soil is very imperative. This review provided current views about the most recent studies, which have been conducted toward the adsorption, transport and biodegradation of antibiotics in soil. The influencing factors affecting the adsorption behaviors of antibiotics in soil, including the antibiotics properties (e.g., molecular structure, hydrophobicity, polarity, polarizability, and spatial configuration) and the soil characteristics (e.g., soil type, soil pH, coexisting ions, and soil organic matter), were discussed. The effects of fertilizer colloids, porous media, and pH of soil on the transport behaviors of antibiotics were analyzed. The biodegradation of antibiotics in soil were also highlighted by investigating the effects of soil microbiome, soil pH, soil temperature, and interactions between antibiotics. Prospects of antibiotics adsorption, transport and biodegradation were also proposed.
Asunto(s)
Contaminantes del Suelo , Suelo , Adsorción , Antibacterianos , EcosistemaRESUMEN
As a widely used antibiotic, tetracycline has a huge hidden danger to human health. Municipal sludge rich in organic substances has the potential to produce biochar. In this work, the municipal sludge biochar from solid waste was modified by the alkali-acid binding method, and tetracycline was efficiently removed from the aqueous solution, the adsorption removal efficiency reached to 86% at initial concentration of 200â¯mg/L. The activation energy was determined by analyzing the adsorption kinetics at different temperatures and tetracycline concentrations. The results showed that tetracycline adsorption on modified biochar was endothermic reaction. Presenting the Langmuir-Freundlich model, adsorption site energy distributions was reckoned. The average adsorption site energy and corresponding standard deviation of the adsorption site energy distribution were deduced emphatically to inquiry the strength of tetracycline adsorption on modified biochar and the adsorption site heterogeneity. The method proposed of research further proves that modified biochar from sewage sludge remove tetracycline from contaminated water has great potential, and exploration of tetracycline adsorption mechanisms by quantifying average site energy. The results and methods of this work can be transferred to study water treatment systems.
RESUMEN
In this study, the oxidized multiwalled carbon nanotube (O-MWCNTs) was obtained by a simple method, and investigated by various techniques (SEM, TEM, FT-IR, XPS and zeta potential) for the removal of pefloxacin and Cu(II). The mutual effects of their adsorption onto O-MWCNTs were comprehensively clarified with sole and binary systems with adsorption kinetics, sorption thermodynamic and sorption isotherm models. The results indicated that there are site enhancement and competition of pefloxacin and Cu(II) on O-MWCNTs. According to mechanism investigation on the adsorption of pefloxacin and Cu(II) by XPS analysis, pH impact study, electrostatic interaction and π-π interactions, the low concentration of Cu(II)/pefloxacin could act as a bridge between pefloxacin/Cu(II) and O-MWCNTs, which significantly enhances the adsorption of pefloxacin/Cu(II). This study provided effective method and valuable reference for the elimination of pefloxacin/Cu(II) from aquatic environments.
RESUMEN
Persulfate is the latest oxidant which is being used increasingly for the remediation of groundwater and soil contaminated with organic compounds. It is of great significant to offer readers a general summary about different methods of activating persulfate, mainly including heat-activated, metal ions-activated, UV-activated, and alkaline-activated. Meanwhile, in addition to persulfate concentration as an influencing factor for persulfate oxidation process, selected information like temperature, anions, cations, pH, and humic acid are presented and discussed. The last section focuses on the advantages of different activated persulfate processes, and the suggestions and research needs for persulfate-based advanced oxidation in the remediation of polluted groundwater and soil.
RESUMEN
Selenium (Se) contamination in surface and ground water in numerous river basins has become a critical problem worldwide in recent years. The exposure to Se, either direct consumption of Se or indirectly may be fatal to the human health because of its toxicity. The review begins with an introduction of Se chemistry, distribution and health threats, which are essential to the remediation techniques. Then, the review provides the recent and common removal techniques for Se, including reduction techniques, phytoremediation, bioremediation, coagulation-flocculation, electrocoagulation (EC), electrochemical methods, adsorption, coprecipitation, electrokinetics, membrance technology, and chemical precipitation. Removal techniques concentrate on the advantages, drawbacks and the recent achievements of each technique. The review also takes an overall consideration of experimental conditions, comparison criteria and economic aspects.
Asunto(s)
Selenio , Contaminantes del Suelo , Biodegradación Ambiental , Humanos , Suelo , AguaRESUMEN
A significant amount of antimony (Sb) enters into the environment every year because of the wide use of Sb compounds in industry and agriculture. The exposure to Sb, either direct consumption of Sb or indirectly, may be fatal to the human health because both antimony and antimonide are toxic. Firstly, the introduction of Sb chemistry, distribution and health threats are presented in this review, which is essential to the removal techniques. Then, we provide the recent and common techniques to remove Sb, including adsorption, coagulation/flocculation, membrane separation, electrochemical methods, ion exchange and extraction. Removal techniques concentrate on the advantages, drawbacks, economical efficiency and the recent achievements of each technique. We also take an overall consideration of experimental conditions, comparison criteria, and economic aspects.