RESUMO
Creating efficient catalysts for simultaneous H2O2 generation and pollutant degradation is vital. Piezocatalytic H2O2 synthesis offers a promising alternative to traditional methods but faces challenges like sacrificial reagents, harsh conditions, and low activity. In this study, we introduce a cobalt-loaded ZnO (CZO) piezocatalyst that efficiently generates H2O2 from H2O and O2 under ultrasonic (US) treatment in ambient aqueous conditions. The catalyst demonstrates exceptional performance with ~50.9% TOC removal of phenol and in situ generation of 1.3 mM H2O2, significantly outperforming pure ZnO. Notably, the CZO piezocatalyst maintains its H2O2 generation capability even after multiple cycles, showing continuous improvement (from 1.3 mM to 1.8 mM). This is attributed to the piezoelectric electrons promoting the generation of dynamic defects under US conditions, which in turn promotes the adsorption and activation of oxygen, thereby facilitating efficient H2O2 production, as confirmed by EPR spectrometry, XPS analysis, and DFT calculations. Moreover, the CZO piezocatalysts maintain outstanding performance in pollutant degradation and H2O2 production even after long periods of inactivity, and the deactivated catalyst due to metal ion dissolution could be rejuvenated by pH adjustment, offering a sustainable solution for wastewater purification.
RESUMO
The growing consumption of drugs of abuse together with the inefficiency of the current wastewater treatment plants toward their presence has resulted in an emergent class of pollutants. Thus, the development of alternative approaches to remediate this environmental threat is urgently needed. Microrobots, combining autonomous motion with great tunability for the development of specific tasks, have turned into promising candidates to take on the challenge. Here, hybrid urchin-like hematite (α-Fe2O3) microparticles carrying magnetite (Fe3O4) nanoparticles and surface functionalization with organic ß-cyclodextrin (CD) molecules are prepared with the aim of on-the-fly encapsulation of illicit drugs into the linked CD cavities of moving microrobots. The resulting mag-CD microrobots are tested against methamphetamine (MA), proving their ability for the removal of this psychoactive substance. A dramatically enhanced capture of MA from water with active magnetically powered microrobots when compared with static passive CD-modified particles is demonstrated. This work shows the advantages of enhanced mass transfer provided by the externally controlled magnetic navigation in microrobots that together with the versatility of their design is an efficient strategy to clean polluted waters.
Assuntos
Ciclodextrinas , Metanfetamina , Poluentes Químicos da Água , Metanfetamina/química , Ciclodextrinas/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação , Magnetismo , Robótica , Purificação da Água/métodos , Compostos Férricos/químicaRESUMO
The waste management and water purification are daunting environmental challenges. Biochar, a carbonaceous material prepared from diverse organic waste (agricultural, household residues and municipal sewage sludge) has garnered substantial attention due to its excellent attributes, including carbon content, cation exchange efficacy, ample specific surface area, and structural robustness. Thus, the present review comprehensively analyzes bio waste-derived biochar with a particular emphasis on water remediation applications. This article primarily delves into various strategies for modifying biochar, elucidating the underlying mechanisms behind these modifications and their potential for bolstering pollutant removal efficiency. Furthermore, it addresses the impact of functionalization on both biochar stability and cost for commercialization. Lastly, the article outlines key developments, SWOT analysis, and future prospects, offering insights into the practical execution of biochar applications at a larger scale. Therefore, this article paves the way for future research to deepen the understanding of modified biochar with mechanisms for exploring water remediation applications in a more sustainable manner.
Assuntos
Poluentes Ambientais , Recuperação e Remediação Ambiental , Gerenciamento de Resíduos , Carvão Vegetal , Esgotos , SoloRESUMO
In recent years, extensive research endeavors are being undertaken for synthesis of an efficient, economic and eco-friendly cerium oxide nanoparticles (CeO2 NPs) using plant extract mediated greener approach. A number of medicinal plants and their specific parts (flowers, bark, seeds, fruits, seeds and leaves) have been found to be capable of synthesizing CeO2 NPs. The specific key phytochemical constituents of plants such as alkaloids, terpenoids, phenolic acids, flavones and tannins can play significant role as a reducing, stabilizing and capping agents in the synthesis of CeO2 NPs from their respective precursor solution of metal ions. The CeO2 NPs are frequently using in diverse fields of science and technology including photocatalytic degradation of dyes, antibiotics as well as antimicrobial applications. In this review, the mechanism behind the green synthesis CeO2 NPs using plant entities are summarized along with discussion of analytical results from characterization techniques. An overview of CeO2 NPs for water remediation application via photocatalytic degradation of dyes and antibiotics are discussed. In addition, the mechanisms of antimicrobial efficacy of CeO2 NPs and current challenges for their sustainable application at large scale in real environmental conditions are discussed.
Assuntos
Anti-Infecciosos , Cério , Nanopartículas Metálicas , Nanopartículas , Antibacterianos/química , Corantes , Nanopartículas/química , Cério/química , Plantas , Nanopartículas Metálicas/químicaRESUMO
Herbicide contamination in aquatic systems has become a global concern due to their long- term persistence, accumulation and health risks to humans. Paraquat, a widely used and cost-effective nonselective herbicide, is frequently applied in agricultural fields for pest control. Consequently, the removal of paraquat from contaminated water is crucial. This research presents a sustainable and environmentally benign method for paraquat removal from aqueous system by integrating wetland plants (Eichhornia crassipes) with biochar derived from melamine-modified palm kernel shells. The prepared biochar was characterized by using various analytical techniques. The effectiveness of biochar in enhancing phytoremediation was evaluated through a series of experiments, showing significant paraquat removal efficiencies of 99.7, 98.3, and 82.8% at different paraquat concentrations 50, 100, and 150 mg L-1, respectively. Additionally, present study examined the impact of biochar on the growth of E. crassipes, highlighting its potential to reduce the toxic effects of paraquat even present at higher concentrations. The paraquat removal mechanism was elucidated, focusing on the synergistic role of biochar adsorption and phytoremediation capability of E. crassipes. This innovative approach is an effective, feasible, sustainable and eco-friendly technique that can contribute to the development of advanced and affordable water remediation processes for widespread application.
The novelty of this study lies in the implementation of combined approach by phytoremediation with biochar modified with melamine. This study highlighted synergistic integration of two concurrent systems. The biochar generated from waste palm kernel shells played a pivotal role in facilitating the plants' survival and resilience against the paraquat toxicity, rather than succumbing to its deleterious effects. This research delineates a robust methodology for the elimination of emerging pollutants, offering researchers a platform to make pioneering advancements in this scientific field for sustainable future.
RESUMO
Self-propelled nanomotors represent a promising class of adaptable and versatile technologies with broad applications in the realms of biomedicine and environmental remediation. Herein, we report a biocatalytic nanomotor based on a covalent-organic framework (COF) that demonstrates intelligent and switchable motion triggered by a blue-to-red light switch. Consequently, when exposed to blue light, the nanomotor significantly enhances the removal of contaminants in aqueous solutions due to its elevated mobility. Conversely, it effectively deactivates its motion and contaminant removal upon exposure to red light. This study explores the heterogeneous assembly strategy of the COF-based nanomotor and its light-controlled propulsion performance and provides a novel strategy for the regulation of movement, offering valuable insights for the design and practical applications of nanomotors.
RESUMO
The laccase mediator system (LMS) with a broad substrate range has attracted much attention as an efficient approach for water remediation. However, the practical application of LMS is limited due to their high solubility, poor stability and low reusability. Herein, the bimetallic Cu/ZIFs encapsulated laccase was in-situ grown in poly(vinyl alcohol) (PVA) polymer matrix. The PVA-Lac@Cu/ZIFs hydrogel was formed via one freeze-thawing cycle, and its catalytic stability was significantly improved. The mediator was further co-immobilized on the hydrogel, and this hierarchically co-immobilized ABTS/PVA-Lac@Cu/ZIFs hydrogel could avoid the continuous oxidation reaction between laccase and redox mediators. The co-immobilized LMS biocatalyst was used to degrade malachite green (MG), and the degradation rate was up to 100 % within 4 h. More importantly, the LMS could be recycled synchronously from the dye solutions and reused to degrade MG multiple times. The degradation rate remained above 69.4 % after five cycles. Furthermore, the intermediate products were detected via liquid chromatography-mass spectrometry, and the potential degradation pathways were proposed. This study demonstrated the significant potential of utilizing the MOF nanocrystals and hydrogel as a carrier for co-immobilized LMS, and the effective reuse of both laccase and mediator was promising for laccase application in wastewater treatment.
Assuntos
Enzimas Imobilizadas , Lacase , Enzimas Imobilizadas/química , Enzimas Imobilizadas/metabolismo , Lacase/química , Lacase/metabolismo , Hidrogéis/química , Corantes de Rosanilina/químicaRESUMO
Quiescent batch experiments were conducted to evaluate the influences of Cl-, F-, HCO3-, HPO42-, and SO42- on the reactivity of metallic iron (Fe0) for water remediation using the methylene blue (MB) method. Strong discoloration of MB indicates high availability of solid iron corrosion products (FeCPs). Tap water was used as an operational reference. Experiments were carried out in graduated test tubes (22 mL) for up to 45 d, using 0.1 g of Fe0 and 0.5 g of sand. Operational parameters investigated were (i) equilibration time (0-45 d), (ii) 4 different types of Fe0, (iii) anion concentration (10 values), and (iv) use of MB and Orange II (O-II). The degree of dye discoloration, the pH, and the iron concentration were monitored in each system. Relative to the reference system, HCO3- enhanced the extent of MB discoloration, while Cl-, F-, HPO42-, and SO42- inhibited it. A different behavior was observed for O-II discoloration: in particular, HCO3- inhibited O-II discoloration. The increased MB discoloration in the HCO3- system was justified by considering the availability of FeCPs as contaminant scavengers, pH increase, and contact time. The addition of any other anion initially delays the availability of FeCPs. Conflicting results in the literature can be attributed to the use of inappropriate experimental conditions. The results indicate that the application of Fe0-based systems for water remediation is a highly site-specific issue which has to include the anion chemistry of the water.
Assuntos
Poluentes Químicos da Água , Purificação da Água , Ferro , Água , Ânions , Poluentes Químicos da Água/análise , Purificação da Água/métodosRESUMO
Environmental electrochemistry and water resource recovery are covered in this review. The study discusses the growing field's scientific basis, methods, and applications, focusing on innovative remediation tactics. Environmental electrochemistry may solve water pollution and extract resources. Electrochemical methods may effectively destroy or convert pollutants. This method targets heavy metals, organic compounds, and emerging water contaminants such as pharmaceuticals and microplastics, making it versatile. Environmental electrochemistry and resource recovery synergize to boost efficiency and sustainability. Innovative electrochemical methods can extract or synthesise metals, nutrients, and energy from wastewater streams, decreasing treatment costs and environmental effect. The study discusses electrocoagulation, electrooxidation, and electrochemical advanced oxidation processes and their mechanics and performance. Additionally, it discusses current electrode materials, reactor designs, and process optimisation tactics to improve efficiency and scalability. Resource recovery in electrochemical remediation methods is also examined for economic and environmental feasibility. Through critical examination of case studies and techno-economic evaluations, it explains the pros and cons of scaling up these integrated techniques. This study covers environmental electrochemistry and resource recovery's fundamental foundations, technology advances, and sustainable water management consequences.
Assuntos
Poluentes Químicos da Água , Poluentes Químicos da Água/química , Águas Residuárias/química , Técnicas Eletroquímicas , Metais Pesados/químicaRESUMO
Endophytic microorganisms contribute significantly to water bioremediation by enhancing pollutant degradation and supporting aquatic plant health and resilience by releasing bioactive compounds and enzymes. These microorganisms inhabit plant tissues without causing disease or any noticeable symptoms. Endophytes effectively aid in eliminating contaminants from water systems. Nanoparticles serve as potent enhancers in bioremediation processes, augmenting the efficiency of pollutant degradation by increasing surface area and bioavailability, thereby improving the efficacy and rate of remediation. Their controlled nutrient release and ability to stabilize endophytic colonization further contribute to the enhanced and sustainable elimination of contaminated environments. The synergistic effect of endophytes and nanoparticles in water remediation has been widely explored in recent studies, revealing compelling outcomes. Water pollution poses significant threats to human health, ecosystems, and economies; hence, the sixth global goal of the Sustainable Development Agenda 2030 of the United Nations aims to ensure the availability and sustainable management of water resources, recognizing their crucial importance for current and future generations. Conventional methods for addressing water pollution exhibit several limitations, including high costs, energy-intensive processes, the production of hazardous by-products, and insufficient effectiveness in mitigating emerging pollutants such as pharmaceuticals and microplastics. Noticeably, there is an inability to effectively remove various types of pollutants, thus resulting in incomplete purification cycles. Nanoparticle-enhanced water bioremediation offers an innovative, eco-friendly alternative for degrading contaminants. A growing body of research has shown that integrating endophytic microorganisms with nanoparticles for water bioremediation is a potent and viable alternative. This review examines the potential of using endophytic microorganisms and nanoparticles to enhance water remediation, exploring their combined effects and applications in water purification. The paper also provides an overview of synthetic methods for producing endophyte-nanoparticle composites to optimize their remediation capabilities in aqueous environments. The final section of the review highlights the constraints related to integrating endophytes with nanoparticles.
Assuntos
Biodegradação Ambiental , Endófitos , Nanopartículas , Nanopartículas/química , Endófitos/metabolismo , Purificação da Água/métodos , Poluentes Químicos da Água , HumanosRESUMO
We modified C3-symmetric benzene-1,3,5-tris-amide (BTA) by introducing flexible linkers in order to generate an N-centered BTA (N-BTA) molecule. The N-BTA compound formed gels in alcohols and aqueous mixtures of high-polar solvents. Rheological studies showed that the DMSO/water (1:1, v/v) gels were mechanically stronger compared to other gels, and a similar trend was observed for thermal stability. Powder X-ray analysis of the xerogel obtained from various aqueous gels revealed that the packing modes of the gelators in these systems were similar. The stimuli-responsive properties of the N-BTA towards sodium/potassium salts indicated that the gel network collapsed in the presence of more nucleophilic anions such as cyanide, fluoride, and chloride salts at the MGC, but the gel network was intact when in contact with nitrate, sulphate, acetate, bromide, and iodide salts, indicating the anion-responsive properties of N-BTA gels. Anion-induced gel formation was observed for less nucleophilic anions below the MGC of N-BTA. The ability of N-BTA gels to act as an adsorbent for hazardous anionic and cationic dyes in water was evaluated. The results indicated that the ethanolic gels of N-BTA successfully absorbed methylene blue and methyl orange dyes from water. This work demonstrates the potential of the N-BTA gelator to act as a stimuli-responsive material and a promising candidate for water purification.
RESUMO
Electronic waste (e-waste) is one of the fastest-growing waste streams in the world and Europe is classified as the first producer in terms of per capita amount. To reduce the environmental impact of e-waste, it is important to recycle it. This work shows the possibility of reusing glassy substrates, derived from the MW-assisted acidic leaching of Waste Printed Circuit Boards (WPCBs), as an adsorbent material. The results revealed an excellent adsorption capability against methylene blue (MB; aqueous solutions in the concentration range 10-5 M-2 × 10-5 M, at pH = 7.5). Comparisons were performed with reference samples such as activated carbons (ACs), the adsorbent mostly used at the industrial level; untreated PCB samples; and ground glass slides. The obtained results show that MW-treated WPCB powder outperformed both ground glass and ground untreated PCBs in MB adsorption, almost matching AC adsorption. The use of this new adsorbent obtained through the valorization of e-waste offers advantages not only in terms of cost but also in terms of environmental sustainability.
RESUMO
The metal intoxication and its associated adverse effects to humans have led to the research for development of water treatment technologies from pollution hazards. Therefore, development of cheaper water remediation technologies is more urgent than ever. Clays and clay minerals are naturally occurring, inexpensive, non-toxic materials possessing interesting chemical and physical properties. As a result of interesting surface properties, these have been developed as efficient absorbent in water remediation. Recently, clay-polymer nanocomposites have provided a cost-effective technological platform for removing contaminants from water. Covering research advancements from past 25 years, this review highlights the developments in clay-polymer nanocomposites and their advanced technical applications are evaluated with respect to the background and issues in remediation of toxic metals and organic compounds from water. The extensive analysis of literature survey of more than two decades suggests that future work need to highlight on advancement of green and cost-effective technologies. The development of understanding of the interaction and exchange between toxin and clay-polymer composites would provide new assembly methods of nanocomposites with functional molecules or nanomaterials need to be extended to increase the detection and extraction limit to parts per trillion.
Assuntos
Argila , Nanocompostos , Polímeros , Poluentes Químicos da Água , Purificação da Água , Nanocompostos/química , Argila/química , Polímeros/química , Purificação da Água/métodos , Poluentes Químicos da Água/análise , Silicatos de Alumínio/químicaRESUMO
Efficient spontaneous molecular oxygen (O2) activation is an important technology in advanced oxidation processes. Its activation under ambient conditions without using solar energy or electricity is a very interesting topic. Low valence copper (LVC) exhibits theoretical ultrahigh activity toward O2. However, LVC is difficult to prepare and suffers from poor stability. Here, we first report a novel method for the fabrication of LVC material (P-Cu) via the spontaneous reaction of red phosphorus (P) and Cu2+. Red P, a material with excellent electron donating ability and can directly reduce Cu2+ in solution to LVC via forming Cu-P bonds. With the aid of the Cu-P bond, LVC maintains an electron-rich state and can rapidly activate O2 to produce ·OH. By using air, the ·OH yield reaches a high value of 423 µmol g-1 h-1, which is higher than traditional photocatalytic and Fenton-like systems. Moreover, the property of P-Cu is superior to that of classical nano-zero-valent copper. This work first reports the concept of spontaneous formation of LVC and develops a novel avenue for efficient O2 activation under ambient conditions.
Assuntos
Cobre , Peróxido de Hidrogênio , Peróxido de Hidrogênio/química , Fósforo , Oxirredução , OxigênioRESUMO
Converting biomass into biochar (BC) as a functional biocatalyst to accelerate persulfate activation for water remediation has attracted much attention. However, due to the complex structure of BC and the difficulty in identifying the intrinsic active sites, it is essential to understand the link between various properties of BC and the corresponding mechanisms promoting nonradicals. Machine learning (ML) recently demonstrated significant potential for material design and property enhancement to help tackle this problem. Herein, ML techniques were applied to guide the rational design of BC for the targeted acceleration of nonradical pathways. The results showed a high specific surface area, and O% values can significantly enhance nonradical contribution. Furthermore, the two features can be regulated by simultaneously tuning the temperatures and biomass precursors for efficient directed nonradical degradation. Finally, two nonradical-enhanced BCs with different active sites were prepared based on the ML results. This work serves as a proof of concept for applying ML in the synthesis of tailored BC for persulfate activation, thereby revealing the remarkable capability of ML for accelerating bio-based catalyst development.
Assuntos
Carvão Vegetal , Poluentes Químicos da Água , Oxirredução , Carvão Vegetal/química , Catálise , Temperatura , Poluentes Químicos da Água/análiseRESUMO
Harmful cyanobacterial blooms and the released microcystins (MCs) caused serious environmental and public health concerns to drinking water safety. Photo-oxidation is an appealing treatment option and alternative to conventional flocculation and microbial antagonists, but the performances of current photosensitizers (either inorganic or organic) are unsatisfactory. Here, a polythiophene photosensitizer (PT10) with both high yield of reactive oxygen species (ROS) production (mainly 1O2, ΦΔ = 0.51, > 8 h continuous generation) and moderate photostability was used as a powerful algaecide to inhibit Microcystis aeruginosa. Due to the positive charge of PT10, the algal cells were quickly flocculated, followed by efficient inactivation in 4 h under white light irradiation (96.7%, 10 mW/cm2). Meanwhile, PT10 was self-immolated in about 6 h. Upon biosafety evaluation with adult zebrafish, the low toxicity of PT10 and the degradation products of PT10 and algae (early logarithmic growth stage) were confirmed. In addition, microcystin-LR (MC-LR), a toxic microcystin that will be released during the destruction of the algal cells, was also degraded. Therefore, PT10-based photoinactivation of M. aeruginosa featured both high performance and low secondary pollution. In real-world aquatic systems, PT10 was confirmed to be capable of sunlight-assisted inactivation of M. aeruginosa and prevent algal blooms, thus making it appealing for environmental remediation.
Assuntos
Cianobactérias , Microcystis , Animais , Luz Solar , Peixe-Zebra , Cianobactérias/metabolismo , Microcystis/metabolismo , Microcistinas/metabolismo , Proliferação Nociva de AlgasRESUMO
The continuous electron supply for oxidant decomposition-induced reactive oxygen species (ROS) generation is the main contributor for the long-standing micropollutant oxidation in the iron-based advanced oxidation processes (AOPs). Herein, as a new class of co-catalysts, metal borides with dual active sites and preeminent conductive performance can effectively overcome the inherent drawback of Fenton-like reactions by steadily donating electrons to inactive Fe(III). Among the metal borides, tungsten boride (WB) exhibits a significant co-catalytic performance run ahead of common heterogeneous co-catalysts and exceptionally high stability. Based on qualitative and semi-quantitative tests, the hydroxyl radical, sulfate radical, and iron(IV)-oxo complex are all produced in the WB/Fe(III)/PDS system and Fe(IV)-induced methyl phenyl sulfoxide decomposition is up to 72%. Moreover, the production efficiency of ROS and relative proportions of radical and nonradical pathways change with various experimental conditions (dosages of PDS, WB, and solution pH) and water matrices. The rate-determining step of Fe(II) regeneration is greatly accelerated resulting from the synergetic effect between exposed metallic reactive sites and nonmetallic boron with reductive properties of WB. In addition, the self-dissolution of surface tungsten oxide and boron oxide leads to a renovated surface for sustainable Fe(III) reduction in long-term operations. Our discovery provides an efficient and sustainable strategy in the field of enhanced AOPs for water remediation.
Assuntos
Boro , Compostos Férricos , Compostos Férricos/química , Espécies Reativas de Oxigênio , Peróxido de Hidrogênio/química , Ferro/química , Metais , Oxirredução , ÁguaRESUMO
The conversion of agricultural waste into high-value carbon products has been an attractive area in waste management strategy. This study highlighted the synthesis and effectiveness of green pea peels (GPP), green pea biochar (GPBC), and nano-ferromagnetic green pea biochar (NFGPBC) by the ferrous/ferric co-precipitation synthesis method for eliminating cationic dyes molecules from solutions. The morphological, physicochemical, and structural properties of GPP, GPBC, and NFGPBC were approved by Scanning Electron Microscopy (SEM), Transmission Emission Microscopy (TEM), Energy Dispersive X-ray (EDX), Bruneau Emmett Teller (BET), Fourier Transform Infrared spectroscopy (FTIR), and X-ray Diffraction (XRD) techniques. Vibrating Sample Magnetometry (VSM) analysis confirmed the NFGPBC magnetization performance. The capacity of each adsorbent for methylene blue removal was evaluated at various parameters of material dosage (50-250 mg/150 mL), pH (2-12), initial concentration (50-250 mg/L), contact time (0-90 min) and temperature (20-60 °C). The three developed adsorbent materials GPP, GPBC, and NFGPBC, possessed reasonable BET surface areas of 0.6836, 372.54, and 147.88 m2g-1, and the corresponding monolayer adsorption capacities of 163.93, 217.40, and 175.44 mg/g, respectively. The superior performances of GPBC and NFGPBC were due to their increased surface area compared with the parent green pea peels (GPP). The results from adsorption kinetics studies of all prepared materials were pseudo-second-order and Elovich kinetics models. The thermodynamic parameters exhibited MB sorption's favorability, spontaneity, and endothermic nature. The NFGPBC material experienced Vander Waal forces, electrostatic interaction, hydrogen bonding, and hydrophobic interactions as predominant modes of the solid-liquid interaction. The regeneration, recycling, and reusability of the synthesized GPP, GPBC, and NFGPBC performed at five adsorption cycles revealed that NFGPBC demonstrated excellent cyclical performances attaining a minimum 8.9% loss in capacity due to paramagnetic properties. Thus, NFGPBC is a green, efficient, and eco-friendly material recommended for large-scale production and application in wastewater.
Assuntos
Azul de Metileno , Poluentes Químicos da Água , Pisum sativum , Descontaminação , Carvão Vegetal/química , Adsorção , Cinética , Poluentes Químicos da Água/química , Concentração de Íons de Hidrogênio , Espectroscopia de Infravermelho com Transformada de FourierRESUMO
Arsenic (As(V))-contaminated water is a major global threat to human health and the ecosystem because of its enormous toxicity, carcinogenicity, and high distribution in water streams. Thus, As(V) removal in the environmental samples has received considerable attention. Till now, numerous metal-organic framework materials have been used for the As(V) removal from the aqueous medium, but low As(V) removal and instability of the adsorbents have severely cut off their practical applications. In this study, a ferrocene-encapsulated zeolitic imidazolate framework-67 (Fc-ZIF-67) material was synthesized for As(V) removal from an aqueous solution at neutral pH using a simple solution mixing process. The ferrocene encapsulation provides water-stable and structural defects to ZIF-67. Furthermore, the ferrocene molecule and imidazole linker can enhance As(V) adsorption via both chemisorption and physisorption. The novel Fc-ZIF-67 adsorbent exhibited superior As(V) adsorption performance with an adsorption capacity of 63.29 mg/g at neutral pH. The Langmuir and Freundlich isotherm models were also used to analyze adsorption behavior.
Assuntos
Arsênio , Poluentes Químicos da Água , Purificação da Água , Zeolitas , Humanos , Zeolitas/química , Ecossistema , Metalocenos , Água/química , Adsorção , Poluentes Químicos da Água/química , Cinética , Concentração de Íons de HidrogênioRESUMO
The present work entails the synthesis of thermally modified graphitic carbon nitride (GCN) using a two-step thermal treatment procedure and its subsequent use in the photocatalytic reduction of toxic pollutants such as rhodamine B dye (RhB) and chromium (VI) (Cr(VI)) from aquatic environments. The as-synthesised exfoliated GCN (GCNX) is characterised by X-ray diffraction (XRD) analysis, Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDS), Brunauer-Emmett-Teller analysis (BET), diffuse reflectance spectroscopy (DRS), photoluminescence spectroscopy (PL), field emission scanning electron microscopy (FESEM), and transmission electron microscopy (TEM). These characterisations helped to elucidate the phase formation, chemical structure, composition, surface area, optical properties, and morphology of the sample. With assistance from a visible light source, GCNX can degrade RhB dye within 30 min in the presence of hydrogen peroxide (H2O2) and reduce Cr(VI) to Cr(III) in under 2 h in the presence of formic acid (FA/HCOOH). Variations in different catalytic parameters, including catalyst amount, pH of the solution, initial RhB or Cr(VI) concentration, and variation in H2O2 or FA concentration, are performed to inspect their effects on the photodegradation activity of GCNX. Moreover, the GCNX catalyst exhibits impressive stability and reusability. A thorough statistical evaluation follows the response surface methodology to understand the complex interaction between the factors contributing to the catalytic activity. The band alignment of differently functionalised GCN blocks in their pristine form and their H2O2/FA-adsorbed states is investigated using first-principles calculations to provide a further understanding of the RhB and Cr(VI) reduction mechanisms. The modified GCN can thus be effectively employed as a low-cost material for removing contamination from aquatic environments.