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The widespread application of nanotechnology inevitably leads to an increased release of engineered nanoparticles (ENPs) into the environment. Due to their specific physicochemical properties, ENPs may interact with other contaminants and exert combined effects on the microbial community and metabolism of anaerobic digestion (AD), an important process for organic waste reduction, stabilization, and bioenergy recovery. However, the complicated interactions between ENPs and other contaminants as well as their combined effects on AD are often overlooked. This review therefore focuses on the co-occurrence of ENPs and cocontaminants in the AD process. The key interactions between ENPs and cocontaminants and their combined influences on AD are summarized from the available literature, including the critical mechanisms and influencing factors. Some sulfides, coagulants, and chelating agents have a dramatic "detoxification" effect on the inhibition effect of ENPs on AD. However, some antibiotics and surfactants increase the inhibition of ENPs on AD. The reasons for these differences may be related to the interactive effects between ENPs and cocontaminants, changes of key enzyme activities, adenosine triphosphate (ATP) levels, reactive oxygen species (ROS) production, and microbial communities. New scientific opportunities for a better understanding of the coexistence in real world situations are converging on the scale of nanoparticles.
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Nanopartículas , Anaerobiose , Nanopartículas/química , Nanotecnologia , Espécies Reativas de OxigênioRESUMO
The photothermal process has attracted considerable attention in water treatment due to its advantages of low energy consumption and high efficiency. In this respect, photothermal materials play a crucial role in the photothermal process. Particularly, carbonaceous materials have emerged as promising candidates for this process because of exceptional photothermal performance. While previous research on carbonaceous materials has primarily focused on photothermal evaporation and sterilization, there is now a growing interest in exploring the potential of photothermal effect-assisted advanced oxidation processes (AOPs). However, the underlying mechanism of the photothermal effect assisted by carbonaceous materials remains unclear. This review aims to provide a comprehensive review of the photothermal process of carbonaceous materials in water treatment. It begins by introducing the photothermal properties of carbonaceous materials, followed by a discussion on strategies for enhancing these properties. Then, the application of carbonaceous materials-based photothermal process for water treatment is summarized. This includes both direct photothermal processes such as photothermal evaporation and sterilization, as well as indirect photothermal processes that assisted AOPs. Meanwhile, various mechanisms assisted by the photothermal effect are summarized. Finally, the challenges and opportunities of using carbonaceous materials-based photothermal processes for water treatment are proposed.
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Future renewable energy supply and green, sustainable environmental development rely on various types of catalytic reactions. Copper single-atom catalysts (Cu SACs) are attractive due to their distinctive electronic structure (3d orbitals are not filled with valence electrons), high atomic utilization, and excellent catalytic performance and selectivity. Despite numerous optimization studies are conducted on Cu SACs in terms of energy conversion and environmental purification, the coupling among Cu atoms-support interactions, active sites, and catalytic performance remains unclear, and a systematic review of Cu SACs is lacking. To this end, this work summarizes the recent advances of Cu SACs. The synthesis strategies of Cu SACs, metal-support interactions between Cu single atoms and different supports, modification methods including modification for carriers, coordination environment regulating, site distance effect utilizing, and dual metal active center catalysts constructing, as well as their applications in energy conversion and environmental purification are emphatically introduced. Finally, the opportunities and challenges for the future Cu SACs development are discussed. This review aims to provide insight into Cu SACs and a reference for their optimal design and wide application.
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Photocatalysis is currently a hot research field, which provides promising processes to produce green energy sources and other useful products, thus eventually benefiting carbon emission reduction and leading to a low-carbon future. The development and application of stable and efficient photocatalytic materials is one of the main technical bottlenecks in the field of photocatalysis. Perovskite has excellent performance in the fields of photocatalytic hydrogen evolution reaction (HER), oxygen evolution reaction (OER), carbon dioxide reduction reaction (CO2RR), organic synthesis and pollutant degradation due to its unique structure, flexibility and resulting excellent photoelectric and catalytic properties. The stability problems caused by perovskite's susceptibility to environmental influences hinder its further application in the field of photocatalysis. Therefore, this paper innovatively summarizes and analyzes the existing methods and strategies to improve the stability of perovskite in the field of photocatalysis. Specifically, (i) component engineering, (ii) morphological control, (iii) hybridization and encapsulation are thought to improve the stability of perovskites while improving photocatalytic efficiency. Finally, the challenges and prospects of perovskite photocatalysts are discussed, which provides constructive thinking for the potential application of perovskite photocatalysts.
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Poluentes Ambientais , Iodo , Compostos de Cálcio , Catálise , Fontes Geradoras de EnergiaRESUMO
Composting has made it practicable to dispose electrolytic manganese residues (EMR) in a less toxic way, nevertheless, the decomposition and the loss of nitrogen is a critical issue. This study aimed to investigate the role of Phanerochaete chrysosporium (PC) inoculation on nitrogen migration and promotion of decomposing organic matter (OM), as well as the effect on bacterial community structure during EMR composting. The results exhibited that nitrogen loss tallied with the first-order kinetic model. PC inoculation increased the relative microbial abundance of Firmicutes, which improved the efficiency of nitrogen nitrification and OM degradation, and increased the germination index and total nitrogen content by 13.8% and 2.95 g/kg, respectively. Moreover, aromatic benzenes replaced heteropolysaccharides, alcohols and ethers as the main components of OM in fertilizer, leading up to a more stable humus structure. This study provides a rationale and a novel perspective on the resource and nutrient conservation of EMR-contaminated soils.
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As a rising branch of advanced oxidation processes, persulfate activation has attracted growing attention. Unlike catalysts that have been widely studied, the selection of persulfate is previously overlooked. In this study, the affecting factors of persulfates were studied. The effect of target pollutant properties on superior persulfate species (the species with a higher degradation efficiency) was investigated by multiwalled carbon nanotube (MWCNT)/persulfate catalytic systems. Innovatively, the EHOMO (or vertical ionization potential (VIP)) value of the target pollutant was proposed to be an index to judge the superior persulfate species, and the threshold is VIP= 6.397-6.674 eV, EHOMO= -8.035â¼- 7.810 eV, respectively. To be specific, when the VIP of phenolic compounds is higher (or EHOMO of phenolic compounds is lower) than the threshold, the catalytic performance of peroxymonosulfate would be higher than that of peroxydisulfate. Moreover, the effects of coexisting cations on peroxydisulfate superior species were further investigated. It was illustrated that the hydrated cation radius of coexisting cations would influence the pollutant degradation efficiency under some circumstances. This study provides a new approach to improve the cost of persulfate activation systems and promotes the underlying downstream application of persulfate activation systems.
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Single-atom catalysts (SACs) for photocatalytic hydrogen peroxide (H2 O2 ) generation are researched but it is still challenging to obtain high H2 O2 yields. Herein, graphite carbon nitride (FeSA /CN) confined single Fe atoms with N/O coordination is prepared, and FeSA /CN shows high H2 O2 production via oxalic acid and O2 activation. Under visible light illumination, the concentration of H2 O2 generated by FeSA /CN can achieve 40.19 mM g-1 h-1 , which is 10.44 times higher than that of g-C3 N4 . The enhanced H2 O2 generation can be attributed to the formation of metal-organic complexes and rapid electron transfer. Moreover, the O2 activation of photocatalysts is revealed by 3,3',5,5'-tetramethylbenzidine oxidation. The results display that the O2 activation capacity of FeSA /CN is higher than that of g-C3 N4 , which facilitates the formation of H2 O2 . Finally, density functional theory calculation demonstrates that O2 is chemically adsorbed on Fe atomic sites. The adsorption energy of O2 is enhanced from -0.555 to -1.497 eV, and the bond length of OO is extended from 1.235 to 1.292 Å. These results exhibit that the confinement of single Fe atoms can promote O2 adsorption and activation. Finally, the photocatalytic mechanism is elaborated, which provides a deep understanding for SACs-catalyzed H2 O2 generation.
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Due to the synergistic effects of biochar and compost/composting, the combined application of biochar and compost (biochar-compost) has been recognized as a highly promising and efficient method of soil improvement. However, the willingness to apply biochar-compost for soil improvement is still low compared to the use of biochar or compost alone. This paper collects data on the application of biochar-compost in several problem soils that are well-known and extensively investigated by agronomists and scientists, and summarizes the effects of biochar-compost application in common problem soils. These typical problem soils are classified based on three different characteristics: climatic zones, abiotic stresses, and contaminants. The improvement effect of biochar-compost in different soils is assessed and directions for further research and suggestions for application are made. Generally, biochar-compost mitigates the high mineralization rate of soil organic matter, phosphorus deficiency and aluminum toxicity, and significantly improves crop yields in most tropical soils. Biochar-compost can help to achieve long-term sustainable management of temperate agricultural soils by sequestering carbon and improving soil physicochemical properties. Biochar-compost has shown positive performance in the remediation of both dry and saline soils by reducing the threat of soil water scarcity or high salinity and improving the consequent deterioration of soil conditions. By combining different mechanisms of biochar and compost to immobilize or remove contaminants, biochar-compost tends to perform better than biochar or compost alone in soils contaminated with heavy metals (HMs) or organic pollutants (OPs). This review aims to improve the practicality and acceptability of biochar-compost and to promote its application in soil. Additionally, the prospects, challenges and future directions for the application of biochar-compost in problem soil improvement were foreseen.
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Compostagem , Metais Pesados , Poluentes do Solo , Solo/química , Poluentes do Solo/análise , Metais Pesados/análise , Carvão Vegetal/químicaRESUMO
Over the last decades, advanced oxidation processes (AOPs) have been widely used in surface and ground water pollution control. The heterogeneous electro-Fenton (EF) process has gained much attention due to its properties of high catalytic performance, no generation of iron sludge, and good recyclability of catalyst. As of October 2022, the cited papers and publications of EF are around 1.3 × 10-5 and 3.4 × 10-3 in web of science. Among the AOP techniques, the contaminant removal efficiencies by EF process are above 90% in most studies. Current reviews mainly focused on the mechanism of EF and few reviews comprehensively summarized heterogeneous catalysts and their applications in wastewater treatment. Thus, this review focuses on the current studies covering the period 2012-2022, and applications of heterogeneous catalysts in EF process. Two kinds of typical heterogeneous EF systems (the addition of solid catalysts and the functionalized cathode catalysts) and their applications for organic contaminants degradation in water are reviewed. In detail, solid catalysts, including iron minerals, iron oxide-based composites, and iron-free catalysts, are systematically described. Different functionalized cathode materials, containing Fe-based cathodes, carbonaceous-based cathodes, and heteroatom-doped cathodes, are also reviewed. Finally, emphasis and outlook are made on the future prospects and challenges of heterogeneous EF catalyst for wastewater treatments.
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Poluentes Químicos da Água , Água , Esgotos , Minerais , Catálise , Peróxido de Hidrogênio , Poluentes Químicos da Água/análise , OxirreduçãoRESUMO
Biochar has been frequently used as a persulfate (PS) activator due to its attractive properties, but dissolved organic matter (DOM) derived from the noncarbonized part of biochar has received less attention, not to mention its specific role and impact in biochar/PS systems. In this study, wheat straw, municipal sludge, and swine bone were selected as the representative feed stocks of biochar. Subsequently, these three types of biochar were adopted to explore the roles of DOM in biochar/PS systems. Although the composition and amount of DOM derived from different biochar were discrepant, they exhibited similar effect in biochar/PS systems. To be specific, the pore-clogging effect of DOM on biochar suppressed the adsorption capacity and catalytic performance of the three biochar. Furthermore, the removal of DOM decreased the environmental risk of these biochar/PS systems and enhanced the stability of the involved biochar. With respect to the variation in degradation mechanism, the removal of DOM increased the proportion of electron transfer pathway in unison, but the diminution in the roles of O2⢯ and 1O2 was more remarkable in bone-derived-biochar/PS systems. Additionally, the toxicity test illustrated that the leakage and accumulation of DOM were toxic to Chlorella sp., and the DOM from sludge-derived-biochar presented the highest toxicity. Overall, this study analyzes the roles of DOM derived from different biochar in biochar/PS systems and evaluates their environmental risk, which contributes to a comprehensive understanding of the fate of DOM derived from biochar.
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Chlorella , Matéria Orgânica Dissolvida , Esgotos , Carvão VegetalRESUMO
As one of the tactics to produce reactive oxygen radicals, the Fenton-like process has been widely developed to solve the increasingly severe problem of environmental pollution. However, establishing advanced mediators with sufficient stability and activity for practical application is still a long-term objective. Herein, we proposed a facile strategy through polymeric carbon nitride (pCN) in-situ growth single cobalt atom for efficient degradation of antibiotics by peroxymonosulfate (PMS) activation. X-ray absorption spectroscopy and high-angle annular dark field-scanning transmission electron microscopy prove the single cobalt atoms are successfully anchored on pCN. Moreover, extended X-ray absorption fine structure analysis shows that the embedded cobalt atoms are constructed by covalently forming the Co-N bond and Co-O bond, which endow the single-atom cobalt catalyst with high stability. Experiment results indicate that the prepared single-atom cobalt catalyst can be used for efficient PMS activation catalytic degradation of tetracycline with a high degradation rate of 98.7 % in 60 min. And the CoN/O sites with single cobalt atoms serve as the active site for generating active radical species (singlet oxygen) from PMS activation. This work may expand the strategy for constructing single-atom catalysts and extend its application for the advanced oxidation process.
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Gold (Au) nanoparticles supported on certain platforms display highly efficient activity on nitroaromatics reduction. In this study, steam-activated carbon black (SCB) was used as a platform to fabricate Au/SCB composites via a green and simple method for 4-nitrophenol (4-NP) reduction. The obtained Au/SCB composites exhibit efficient catalytic performance in reduction of 4-NP (rate constant kapp = 2.1925 min-1). The effects of SCB activated under different steam temperature, Au loading amount, pH, and reaction temperature and NaBH4 concentration were studied. The structural advantages of SCB as a platform were analyzed by various characterizations. Especially, the result of N2 adsorption-desorption method showed that steam activating process could bring higher surface area (from 185.9689 to 249.0053 m2/g), larger pore volume (from 0.073268 to 0.165246 cm3/g), and more micropore for SCB when compared with initial CB, demonstrating the suitable of SCB for Au NP anchoring, thus promoting the catalytic activity. This work contributes to the fabrication of other supported metal nanoparticle catalysts for preparing different functional nanocomposites for different applications.
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Ouro , Nanopartículas Metálicas , Catálise , Carvão Vegetal , Ouro/química , Nanopartículas Metálicas/química , Nitrofenóis/química , Fuligem , VaporRESUMO
In this study, CuCo layered double hydroxide/biochar composite (CuCo LDH/BC) was prepared and employed for activating H2O2 to degrade ciprofloxacin (CIP), a common fluroquinolone antibiotic detected in water environment. The as-synthesized catalysts were also comprehensively characterized to study the physiochemical properties. For the catalytic activity, the degradation rate of CuCo LDH/BC to CIP was approximately 1.5 times higher than that of CuCo LDH. The improved catalytic activity can be ascribed to the synergistic effect between CuCo LDH and BC, such as more functional groups, accelerated electron transfer, and varied charge distribution. Meanwhile, CuCo LDH/BC/H2O2 could degrade CIP efficiently in a wider pH range comparing with CuCo LDH/H2O2, and the efficiency was approximately 84.7% at neutral pH within 90 min. The generation of OH, O2- and 1O2 in CuCo LDH/BC/H2O2 system were then verified by electron spin resonance (ESR) technology. The quenching experiments indicated that both non-radical pathway (1O2) and radical pathway (OH, O2-) led to CIP degradation, in which O2- and 1O2 made major contribution. Then, the intermediate products of CIP during catalytic reaction were monitored by high-performance liquid chromatography-mass spectrometry (HPLC-MS), and the environmental risk of these degradation intermediates was tested through seed germination experiments. This study tends to provide valuable information for LDH/BC application in heterogeneous Fenton-like reaction.
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Carvão Vegetal , Peróxido de Hidrogênio , Carvão Vegetal/química , Ciprofloxacina , Peróxido de Hidrogênio/química , Hidróxidos/químicaRESUMO
Peroxymonosulfate (PMS)-based advanced oxidation processes for wastewater treatment have received extensive attention in the past years. Here, a novel Mn, Ce co-modified g-C3N4 (MnCe-CN) composite was successfully synthesized by one-step pyrolysis for activating PMS. The physical and chemical characterization of MnCe-CN/PMS was conducted, indicating that Mn and Ce were evenly distributed on g-C3N4 and existed in the form of Mn-N structure and CeO2, respectively. The MnCe-CN/PMS system could effectively degrade pollutants such as acetaminophen (ACT), methylparaben (MeP), p-nitrophenol (PNP), and 2,4-dichlorophenol (2,4-DCP). Among them, 2,4-DCP could be rapidly degraded, reaching 100% within 30 min. The masking experiments and electrochemical testing results revealed that 2,4-DCP was degraded via superoxide radicals (O2Ë-), singlet oxygen (1O2), and electron transfer path. The cyclic experiments and real water treatment experiments testified that the oxidative system had excellent stability and applicability. This study provides a facile synthetic method to fabricate bimetallic co-modified g-C3N4 for the enhancement of PMS activation.
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Peróxidos , Oxigênio Singlete , Oxirredução , Peróxidos/química , SuperóxidosRESUMO
The increasingly serious pollution of antibiotics brings an enormous threat to the ecological environment and human health. Graphite phase carbon nitride (g-C3N4), as a popular photocatalytic material, is widely used in photocatalytic degradation of antibiotics in water. In order to make up for the shortage of g-C3N4 monomer, CeO2/N-doped g-C3N4 (CeNCN) composite photocatalysts co-modified with nitrogen doping and CeO2 loading were designed and synthesized with the idea of expanding visible light absorption and promoting photogenerated carrier separation. CeNCN exhibits excellent photodegradation performance, the removal rate of tetracycline reached 80.09% within 60 min, which is much higher than that of g-C3N4 (CN) and N-doped g-C3N4 (NCN); and the quasi-first-order degradation rate constant is 0.0291, which is 7.86 and 2.29 times higher than CN and NCN. Electron spin resonance and free radical trapping experiments confirmed that h+, O2- and OH are the active substances in the photocatalytic system. After 5 cycles, the degradation efficiency of tetracycline still exceeds 75%, which indicates that CeNCN has good stability. This work proves that N-doping and CeO2 loading can effectively broaden the photoresponse range of g-C3N4, facilitate the separation of photogenerated electron-hole pairs, and provide a reference for the construction of g-C3N4-based photocatalyst with high-efficiency photodegradation activity.
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Grafite , Antibacterianos , Catálise , Cério , Humanos , Luz , Nitrogênio , Compostos de Nitrogênio , TetraciclinaRESUMO
Recently, photo-Fenton technology has been widely used to degrade tetracycline (TC) because of its great efficiency and wide application range. Herein, Fe-Ni layered double hydroxides (FeNi-LDH)/Ti3C2 photo-Fenton system was constructed in this study. The results showed the introduction of Ti3C2 solved some problems of FeNi-LDH such as poor conductivity, easy aggregation, and high recombination rate of photoelectron. Benefiting from these advantages, FeNi-LDH/Ti3C2 exhibited excellent TC removal rate of 94.7% while pure FeNi-LDH was only 54%. Besides, FeNi-LDH/Ti3C2 possessed strong pH tolerance (2-11) and the removal efficiency was still up to 82% after the four-cycle experiment. Furthermore, the quenching experiments revealed the reaction mechanism, where âOH and ·O2- were the primary active radicals for degrading TC. Last, the results of the simulated wastewater treatment and the inorganic ion interference tests showed that FeNi-LDH/Ti3C2 possessed practical application potential. In brief, this study shows that FeNi-LDH/Ti3C2 can offer a certain theoretical basis for the actual development of hydrotalcite in heterogeneous photo-Fenton systems.
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Titânio , Água , Catálise , Peróxido de Hidrogênio , Hidróxidos , TetraciclinaRESUMO
With the increasing serious water pollutions, an increasing interest has given for the nanocomposites as environmental catalysts. To date, noble metals-based nanocomposites have been extensively studied by researchers in environmental catalysis. In detail, serving as key functional parts, noble metals are usually combined with other nanomaterials for rationally designing nanocomposites, which exhibit enhanced catalytic properties in pollutants removal. Noble metals in the nanocomposites possess tailored properties, thus playing different important roles in catalytic oxidation reactions for pollutants removal. To motivate the research and elaborate the progress of noble metals, this review (i) summarizes advanced characterization techniques and rising technology of theoretical calculation for evaluating noble metal, and (ii) classifies the roles according to their disparate mechanism in different catalytic oxidation reactions. Meanwhile, the enhanced mechanism and influence factors are discussed. (iii) The conclusions, facing challenges and perspectives are proposed for further development of noble metals-based nanocomposites as environmental catalysts.
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Poluentes Ambientais , Nanoestruturas , Catálise , Metais , OxirreduçãoRESUMO
Recently, persulfate (PS) activation system has grown up as a primary branch of advanced oxidation processes, and biochar has been recognized as a potential nonmetal material in this field. However, few studies have focused on the corresponding relationship between actives sites on biochar and active species in AOPs. To pave this way, similar biochar (obtained from different pyrolysis temperature) with different functional structures were involved. In this study, biochar derived from swine bone (BBC) was applied in PS activation system to degrade acetaminophen (ACT). The results showed that both radical and non-radical pathway worked in the PS/BBCs systems, and the degradation rate (from 0.1042 to 0.4364â¯min-1) climbed with the increase of pyrolysis temperature (from 700 to 900⯰C). To probe into the corresponding relationship between functional structure and active species, the effect of pyrolysis temperature on functional structure was analyzed. It came out that 1) defects could act as active sites for various active species; 2) persistent free radicals could do favor to the generation of 1O2 and O2-; 3) hydroxyapatite in swine bone only served as hard templet for the porous structure. ACT degradation process was measured by Liquid chromatograph-mass spectrometer, and Scendesmus obliquus was applied to investigate the toxicity of PS/BBCs system. It illustrated that the existence of SO4- mainly contributed to the generation of high toxic intermediates (such as biphenyl and diphenyl ether) in the PS/BBCs system. Furthermore, the enhancement of adsorption capacity would mitigate the toxicity of PS/BBCs systems to some extent.
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Acetaminofen , Carvão Vegetal , Acetaminofen/toxicidade , Adsorção , Animais , Domínio Catalítico , SuínosRESUMO
The use of antibiotics for beings is a most significant milestone in present era. However, owing to the excessive use, a large amount of antibiotics accumulated in water, leading to serious pollution. An efficient method is urgently needed to treat the antibiotics pollution. Photo-Fenton process is a green method with utilizing solar energy. Catalyst is important. This work combines manganese ferrite MnFe2O4 and MoS2 to synthesize MnFe2O4-MoS2 (FMG) composite as the catalyst of photo-Fenton process, which shows good performance on tetracycline antibiotics degradation. Light intensity exhibits positive correlation with the catalytic activity. h+, â¢OH and 1O2 participate in tetracycline degradation. h+ plays a key role in tetracycline removal. â¢OH has a little impact on tetracycline removal, but it has a great impact on the mineralization ability of this photo-Fenton process. Additionally, cycling experiments confirm the stability of FMG. And owing to its magnetism, FMG can be easily recycled by external magnetic field. This photo-Fenton process over FMG with utilizing the synergism of MnFe2O4 and MoS2 is a promising method for antibiotics pollution treatment.
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Antibacterianos , Molibdênio , Catálise , Compostos Férricos , Compostos de Manganês , TetraciclinaRESUMO
In the present study, an innovative carbon self-doped g-C3N4 (CCN) loaded with ultra-low CeO2 (0.067-0.74 wt%) composite photocatalyst is successfully synthesized via a facile one-pot hydrothermal and calcination method. The CeO2/CCN exhibits superior photocatalytic performance for tetracycline degradation (78.9% within 60 min), H2O2 production (151.92 µmol L-1 within 60 min), and Cr(VI) reduction (99.5% within 40 min), which much higher than that of g-C3N4, CCN, CeO2, and CeO2/g-C3N4. The enhanced photocatalytic performance is originated from the fact that the doping of C can efficaciously broaden the utilization range of solar light and improve the reduction ability of photogenerated electrons. Meanwhile, the ultra-low loading of CeO2 can effectually promote the migration of photogenerated electrons and enhance the specific surface area. Besides, the experiments of pH effect and cycle ability indicate that CeO2/CCN has excellent durability and stability. Finally, the photocatalytic mechanism of CeO2/CCN is systematically discussed. This work proves that combining element doping and semiconductor coupling is a promising strategy to design high-efficiency g-C3N4-based photocatalysts.