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The influences of the positive Fe3+ and the negative Cr2O72- on the tetracycline (TC) photodegradation by N-doped dissolved black carbon (NDBC) have been investigated in this work. A series of samples (NDBC300, NDBC400 and NDBC500) have been extracted from the corresponding biochar. NDBC400 has the best photodegradation performance (79%) for TC under visible light irradiation. Adding Cr2O72- and Fe3+ can reduces TC photodegradation efficiency into 37% and 53%, respectively. This maybe from that Cr2O72- has stronger interaction with NDBC400 than Fe3+ since it can quench more fluorescence intensity of NDBC400 than Fe3+. Furthermore, Cr2O72- can reduce the steady-state concentration of 3NDBC400*, 1O2 and â¢OH, whereas Fe3+can just reduce the steady-state concentration of 3NDBC400* and increase the concentration of â¢OH. This may explain why Cr2O72- has stronger inhibit performance of TC photodegradation by NDBC400 than Fe3+. The band structures of NDBC400, NDBC400-Fe3+ and NDBC400-Cr2O72- are constructed. And the VB of NDBC400-Fe3+ has a stronger ability to produce â¢OH than NDBC400. In summary, coupling interaction and band structure characterization of NDBC400, NDBC400-Fe3+ and NDBC400-Cr2O72- can explain well why Cr2O72 has stronger inhibition effect than Fe3+ and Fe3+ can increase the concentration of â¢OH. This work provides a deep insight for the photochemical behavior of dissolved black carbon and the transformation behavior of the co-existed metal ions and antibiotics.
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The misuse and inevitable release of antibiotics can cause significant harm to both human health and the environment, and the use of polymeric semiconductors for photodegradation of antibiotics in aqueous environments is one of the most effective strategies to alleviate the current dilemma. Nevertheless, the inherently high exciton binding energy (Eb) and low photogenerated carrier transfer efficiency for most photocatalysts results in unsatisfactory photodegradation performance. Hence, this work proposes a donor polarization strategy to regulate the exciton dissociation of conjugated microporous polymers (CMPs) by minimizing their Eb. Results exhibited that the introduction of the strong donor unit 3,4-ethylenedioxythiophene (EDOT) not only reduces the Eb and effectively promotes exciton dissociation, but also broadens the visible light absorption of CMP. Among them, EdtTz-CMP with the lowest Eb (99 meV) delivered an efficiency of 94.6% in photocatalytic degradation of tetracycline (TC) with in 90 min, significantly higher than those of its analogues. This work provides a viable approach to design CMPs by tuning the intrinsic dipole of the donor for efficient environmental purification.
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Degradation of polyolefin (PE) plastic by a traditional chemical method requires a high pressure and a high temperature but generates complex products. Here, sulfur vacancy-rich ZnIn2S4 and hydroxy-rich ZnIn2S4 were rationally fabricated to realize photocatalytic degradation of PE in an aqueous solution under mild conditions. The results reveal that the optimized photocatalyst could degrade PE into CO2 and CO, and PE had a weight loss of 84.5% after reaction for 60 h. Systematic experiments confirm that the synergetic effect of hydroxyl groups and S vacancies contributes to improve the photocatalytic degradation properties of plastic wastes. In-depth investigation illustrates that the active radicals attack (h+ and â¢OH) weak spots (C-H and C-C bonds) of the PE chain to form CO2, which is further selectively photoreduced to CO. Multimodule synergistic tandem catalysis can further improve the utilization value of plastic wastes; for example, product CO2/CO in the plastic degradation process can be converted in situ into HCOOH by coupling with electrocatalytic technology.
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Exploring high-performance photocatalysts still remains a big challenge due to poor charge separation efficiency. Herein, we prepare a novel anatase/rutile TiO2-Ag3PO4 hollow photocatalyst (A/R-TiO2-Ag3PO4) for addressing this challenge. Microstructural characterization and photoelectric measurements confirm that the synergy of hollow structure and dual-heterojunction can provide abundant active sites and boost efficient charge separation through dual-pathway charge transfer mechanism. The A/R-TiO2-Ag3PO4 photocatalyst exhibits the highest photocurrent density (15.25 µA cm-2), which is 8.4 and 5.2 times than that of A-TiO2-Ag3PO4 (1.82 µA cm-2) and P25-Ag3PO4 (2.93 µA cm-2), respectively. Photo-degradation experiment shows that A/R-TiO2-Ag3PO4 presents a high degradation percentage (98.7 %) of thiamethoxam (THX) within 30 min, which is 1.45 and 1.23 times than that of A-TiO2-Ag3PO4 (68.1 %) and P25-Ag3PO4 (80.7 %), respectively. Furthermore, the degradation percentage of THX by A/R-TiO2-Ag3PO4 is as high as 96.4 % after seven successive cycles, indicating excellent cycling stability. Therefore, this work provides a new insight into exploring other high-performance photocatalysts by combining hollow structure and dual-heterojunction.
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Tylosin tartrate, a macrolide antibiotic, is one of a class of emerging contaminants that have been detected in natural bodies of water since they are not easily removed by conventional treatment processes. In this study, the direct and indirect photodegradation of tylosin tartrate was analyzed to understand the role of reactive oxygen species and organic matter that may be present in surface waters. While direct photolysis caused negligible degradation (k = (9.4 ± 1.8) × 10-5 s-1), the addition of 0.4 M hydrogen peroxide (k = (2.18 ± 0.01) × 10-4 s-1) or usage of the photo-Fenton process (k = (2.96 ± 0.02) × 10-4 s-1) resulted in greater degradation. The degradation was maximized by combining tylosin tartrate with an experimentally determined optimal concentration of humic acid (15 mg/L), which readily produced singlet oxygen and increased the overall degradation (k = 1.31 ± 0.05) × 10-3 s-1) by means of indirect photolysis. Absolute pseudo-first-order bimolecular reaction rate constants for tylosin tartrate were measured with singlet oxygen [(4.7936 ± 0.0001) × 105 M-1 s-1] and hydroxyl radical [(5.2693 ± 0.0002) × 109 M-1 s-1] using competition kinetics, and when combined with data on concentration of the reactive oxygen species, showed that the hydroxyl radical makes a contribution to the degradation that is approximately eleven orders of magnitude greater than singlet oxygen.
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This research addresses the scalable and inexpensive synthesis of α-Fe2O3via hydrothermal method without any precipitating agent as well as the enhancement of solar driven photocatalytic and H2 production through doping different chromium proportions. Competency of α-Fe2O3, both pure and doped with chromium, to function as photocatalyst was evaluated by its interaction with multiple dyes, which was real-time monitored utilizing (Internet of Things) IoT technique. By adding chromium, the rate of deterioration increased substantially from 15 to 94% for TB under sunlight in a remarkably brief 20 min by employing a very small amount of Cr0.8Fe1.2O3 (0.3 g/L), as evidenced by high degree of mineralization i.e. 85% and LC-HRMS. Also, the rapid breakdown of Trypan Blue (TB) was indicated by BOD5/COD ratio. Moreover, Cr-doped α-Fe2O3 displays excellent H2 production (~ 132 µmol h-1 g-1) as compared to α-Fe2O3. This work highlights the potential utilization of Cr-doped α-Fe2O3 for the purification of industrial waste water and green energy harvesting.
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Water pollution seriously affects the development of society and human life. There are various kinds of pollutants, including soluble pollutants and insoluble floaters on the water surface. Herein, the photocatalyst semiconductor BiOCl and superhydrophobic functional particles Mg(OH)2 were deposited on the surfaces of canvas and polyester felt to construct superhydrophobic canvas and polyester felt. The contact angles of the synthetic superhydrophobic canvas and polyester felt were measured as 152° and 155.3°, respectively. The selective adsorption of hexadecane was achieved using the wetting difference between the surface of water and pollutants floating on the surface. For dissolved pollutants, the surface wettability needed to be changed with the help of ethanol. The degradation efficiencies were all greater than 90%, demonstrating the versatility of the synthetic superhydrophobic canvas and polyester felt.
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Halophenols are toxic and persistent pollutants in water environments which poses harm to various organisms. Due to their high stability and long residence time, ultraviolet radiation, heavy metals and oxidizing agents have been largely adopted on treating these compounds. However, these treatment methods could pose toxicity or hazardous risks to the marine environment and plant operators. In this study, a water-soluble porphyrin photocatalyst was synthesized and introduced for halophenol treatment using UV-free LED white light. The porphyrin catalyst is a macrocyclic ring consisting of pyrroles linked with methine bridges, the highly conjugated ring provided the superior functionality of visible light absorption. Surprisingly, over 99 % degradation of halophenols and over 90 % dehalogenation have been achieved without metal chelation, even higher than those of transition metal porphyrins with inclusion of Fe3+, Zn2+, Cu2+, Co2+, Ni2+, and Mn2+. Ring-opening reactions were confirmed with the formation of carboxylic acids; dicarboxylic acids like acrylic acid, and malonic acid; while fumaric acid was the main product. Total organic carbon results indicated no CO2 produced during the reaction. Triplet absorbance and scavenger studies also indicated that singlet oxygen and conduction band electrons are the main radical species for halophenol degradation. The 100-fold singlet emission quenching over triplet absorption quenching indicated that the excited electrons tend to be transferred via singlet state. This concept brings along new approaches detoxifying halophenol-related wastewater without UV, metals and other additives, which is more environmentally-friendly and sheds light to the conversion of toxic materials into useful chemical precursors.
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Designing efficient dual-functional catalysts for photocatalytic oxygen reduction to produce hydrogen peroxide (H2O2) and photodegradation of dye pollutants is challenging. In this work, we designed and fabricated an S-scheme heterojunction (g-C3N4/ZnO composite photocatalyst) via one-pot calcination of a mixture of ZIF-8 and melamine in the KCl/LiCl molten salt medium. The KCN/ZnO composite produced 4.72 mM of H2O2 within 90 min under illumination (with AM 1.5 filter), which is almost 1.3 and 7.8 times than that produced over KCN and ZnO, respectively. Simultaneously, the KCN/ZnO also showed excellent photodegradation performance for the dye pollutants (Rhodamine B, RhB), with a removal rate of 92 % within 2 h. The apparent degradation rate constant of RhB over KCN/ZnO was approximately 5-8 times that of KCN and ZnO. In the photocatalytic process, photo-generated holes and superoxide radicals are the main active species. Oxygen (O2) was mainly reduced to produce H2O2 via a two-electron (2e-) pathway with superoxide radicals as intermediates and the 2e- oxygen reduction reaction selectivity of KCN/ZnO was close to 69.82 %. Photo-generated holes are mainly responsible for the degradation of RhB. Compared with pure KCN and ZnO, the enhanced photocatalytic activity of the KCN/ZnO composite is mainly attributed to the following aspects: 1) larger specific surface area and pore volume is beneficial to expose more active sites; 2) stronger light harvesting ability and red-shifted absorption edge bestow the compound a stronger light utilization efficiency; 3) the construction of S-scheme heterostructure between KCN and ZnO improve the photogenerated electron-hole pairs separation ability and bestow photogenerated carriers a higher redox potential.
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The photodegradation of macroplastics in the marine environment remains poorly understood. Here, we investigated the weathering of commercially available plastics (tabs 1.3 × 4.4 × 0.16 cm), including high-density polyethylene, low-density polyethylene, polypropylene, polystyrene, and polycarbonate, in seawater under laboratory-simulated ultraviolet A radiation for 3-9 months, equivalent to 25-75 years of natural sunlight exposure without considering other confounding factors. After the exposure, the physical integrity and thermal stability of the tabs remained relatively intact, suggesting that the bulk polymer chains were not severely altered despite strong irradiation, likely due to their low specific surface area. In contrast, the surface layer (â¼1 µm) of the tabs was highly oxidized and eroded after 9 months of accelerated weathering. Several antioxidant additives were identified in the plastics through low temperature pyrolysis coupled with gas chromatography/mass spectrometry (Pyr-GC/MS) analysis. The Pyr-GC/MS results also revealed many new oxygen-containing compounds formed during photodegradation, and these compounds indicated the dominance of chain scission reactions during weathering. These findings highlight the strong resistance of industrial macroplastics to weathering, emphasizing the need for a broader range of plastics with varying properties and sizes to accurately estimate plastic degradation in the marine environment.
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Plásticos , Rayos Ultravioleta , Fotólisis , Agua de Mar/química , Cromatografía de Gases y Espectrometría de Masas , Luz SolarRESUMEN
Methylisothiazolinone (MIT) and Benzisothiazolinone (BIT) are two widely used non-oxidizing biocides of isothiazolinones. Their production and usage volume have sharply increased since the pandemic of COVID-19, inevitably leading to more release into water environment. However, their photochemical behaviors in water environment are still unclear. Therefore, this study investigated photodegradation properties of MIT and BIT in natural water under simulated sunlight. The results demonstrated that direct photolysis was mainly responsible for their photodegradation which occurred through their excited singlet states rather than triplet states. The quantum yields of MIT and BIT photodegradation were 11 - 13.6 × 10-4 and 2.43 - 5.79 × 10-4, respectively. pH had almost no effect on the photodegradation of MIT, while the photodegradation of BIT was significantly promoted under alkaline condition due to abundance of BIT in its deprotonated form (BIT-N-). Cl-, NO3- and dissolved organic matter (DOM) in natural water inhibited the photodegradation of both MIT and BIT, with the light screening effect of DOM being the most significantly inhibitory factor. The addition of other isothiazolinones, which possibly coexisted with MIT and BIT in actual condition, slightly inhibited the photodegradation of MIT and BIT. The estimated half-life under natural sunlight at a 30°N latitude was estimated to be approximately 1.1 days. The photodegradation pathways of MIT and BIT are similar, primarily initiated from the ring-opening at the N-S bond, with Frontier electron densities (FED) calculations suggesting the likelihood of oxidation and ·OH addition reactions at the O, N, and S sites. While the photodegradation products exhibited significantly reduced acute toxicity compared to their parent compounds, they nonetheless posed substantial chronic toxicity. These insights are vital for assessing the ecological impacts of MIT and BIT in aquatic environments.
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Innovative and efficient strategies are urgently needed for wastewater treatment and environmental remediation. The photocatalytic degradation properties of photo-responsive nanomaterials (NMs) have become a prime candidate due to their low negative impact and photo-adjustability. Photocatalytic NMs vary in their degradation of different pollutants depending on the type of synthetic material, excitation light source, and physicochemical properties. Essentially, photocatalytic NMs excited by light produce reactive oxygen species (ROS) or metal ions that can degrade complex structure pollutants. Therefore, this review summarises the recent advances of photocatalytic NMs in the environmental application within the last 3 years, focusing on the development schemes, structural analyses, photocatalytic mechanisms, and the degradation effects of dyes, antibiotics, pesticides, phenolic compounds, metals, hormones, and other contaminants. The limitations and future directions are also explained. This review hopes to provide a possible pathway for the subsequent development of novel and efficient photocatalytic NMs to cope with complex and variable polluted environments.
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Near UV and visible light photodegradation can target therapeutic proteins during manufacturing and storage. While the underlying photodegradation pathways are frequently not well-understood, one important aspect of consideration is the formulation, specifically the formulation buffer. Citrate is a common buffer for biopharmaceutical formulations, which can complex with transition metals, such as Fe(III). In an aqueous solution, the exposure of such complexes to light leads to the formation of the carbon dioxide radical anion (â¢CO2-), a powerful reductant. However, few studies have characterized such processes in solid formulations. Here, we show that solid citrate formulations containing Fe(III) lead to the photochemical formation of â¢CO2-, identified through DMPO spin trapping and HPLC-MS/MS analysis. Factors such as buffers, the availability of oxygen, excipients, and manufacturing processes of solid formulations were evaluated for their effect on the formation of â¢CO2- and other radicals such as â¢OH.
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Aniones , Dióxido de Carbono , Compuestos Férricos , Luz , Fotólisis , Rayos Ultravioleta , Dióxido de Carbono/química , Aniones/química , Compuestos Férricos/química , Tampones (Química) , Cromatografía Líquida de Alta Presión/métodos , Ácido Cítrico/química , Química Farmacéutica/métodos , Espectrometría de Masas en Tándem/métodos , Excipientes/química , Radicales Libres/químicaRESUMEN
Photodegradation of microplastics (MPs) induced by sunlight plays a crucial role in determining their transport, fate, and impacts in aquatic environments. Dissolved black carbon (DBC), originating from pyrolyzed carbon, can potentially mediate the photodegradation of MPs owing to its potent photosensitization capacity. This study examined the impact of pyrolyzed wood derived DBC (5 mg C/L) on the photodegradation of polystyrene (PS) MPs in aquatic solutions under UV radiation. It revealed that the photodegradation of PS MPs primarily occurred at the benzene ring rather than the aliphatic segments due to the fast attack of hydroxyl radical (â¢OH) and singlet oxygen (1O2) on the benzene ring. The photosensitivity of DBC accelerated the degradation of PS MPs, primarily attributed to the increased production of â¢OH, 1O2, and triplet-excited state DBC (3DBC*). Notably, DBC-mediated photodegradation was related to its molecular weight (MW) and chemical properties. Low MW DBC (<3 kDa) containing more carbonyl groups generated more â¢OH and 1O2, accelerating the photodegradation of MPs. Nevertheless, higher aromatic phenols in high MW DBC (>30 kDa) scavenged â¢OH and generated more O2â¢-, inhibiting the photodegradation of MPs. Overall, this study offered valuable insights into UV-induced photodegradation of MPs and highlighted potential impacts of DBC on the transformation of MPs.
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Dissolved organic matter (DOM) can affect the transformation of pollutants through photosensitization, but most current research focuses on hydrophilic pollutants, making it such that less attention is paid to hydrophobic pollutants. In this paper, the effect and action mechanism of coexisting DOM on the photodegradation of decachlorobiphenyl (PCB-209) on suspended particles collected from the Yellow River were systematically investigated in a heterogeneous system using DOM standards and model compounds. Through molecular probe experiments, mass spectrometry analysis and theoretical calculations, we found that the excited triplet state of DOM (3DOM*) could excite PCB-209 to undergo dechlorination reaction. Due to the different modes of electron transition, the presence of carbonyl groups decreased the energy of 3DOM*, whereas the electron-donating groups made the energy of 3DOM* higher. DOM containing phenolic hydroxyl groups led to a higher steady-state concentration of â¢OH, and DOM containing phenyl ketone structures had a stronger ability to produce â¢O2-. Compared with aqueous â¢OH, â¢O2- produced from hydrophobic microregions could react more readily with PCB-209. This study deepens the understanding of the role of different functional groups of DOM in the photosensitized transformation of hydrophobic compounds.
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Fotólisis , Bifenilos Policlorados/química , Contaminantes Químicos del Agua/químicaRESUMEN
Parabens are classified as emerging contaminants in global waters, and the ubiquitous emergence of their high-risk chlorinated products generated from chlorine-based wastewater disinfection has attracted increasing attention. However, rather limited information is available on their photofate after discharging into surface waters, and their degradation behavior after solar-based engineering water treatment is unclear. Herein, the reactivity of four chlorinated parabens with different photochemically produced reactive intermediates was measured. Quantitative contribution analysis in abating such compounds showed the dominance of direct photolysis in sunlit natural freshwaters. Introducing a technical solar/peroxymonosulfate (PMS) system could greatly improve the removal of chlorinated parabens. The economic analysis suggested that chlorinated parabens exhibited a minimum value of economic input as 93.41-158.04 kWh m-3 order-1 at 0.543-0.950 mM PMS. The high-resolution mass spectrometry analysis of the degradation products suggested that dechlorination, hydroxylation, and ester chain cleavage were the dominant transformation pathways during photolysis and solar/PMS treatment. Furthermore, the in silico prediction indicated severe aquatic toxicity of certain products but enhanced biodegradability. Overall, this investigation filled a knowledge gap on the reactivity of chlorinated parabens with diverse reactive transients and their quantitative contributions to the photolysis and solar/PMS treatment of emerging micropollutants in water.
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Photodegradation of drug substances leads to the formation of known and unknown degradation products. These unknown degradation products interfere and give erroneous results because of absorption on analytical wavelengths. This interference could be eliminated using the correction of irrelevant absorbancies. This study is based on the application of linear and non-linear correction of irrelevant absorption for the determination of methylcobalamin (MC) and hydroxocobalamin in the photolytic degradation assisted by ascorbic acid (AH2). MC follows first-order degradation kinetics and the rate of degradation (kobs) ranges from 1.99-2.34 × 10-2, min-1 at pH 2.0-12.0. The second-order rate constants (k2) for the photochemical interaction of MC and AH2 are in the range of 17.9-60.3 × 10-2 M-1, min-1 (acidic region) and 10.3-24.6 × 10-2 M-1, min-1 (alkaline region). The k2-pH profile was found to be bell-shaped and the maximum rate of degradation in the presence of AH2 is at pH 5.0 (60.3 × 10-2 M-1, min-1) due to the protonation of MC. However, in alkaline pH, the rate of photodegradation decreases due to the ionization form of AH2 which is AH- species.
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In this work, polyvinylidene fluoride (PVDF) intercalated CuFe layered double hydroxides (LDH) membranes were fabricated and investigated for UV-LED/persulfate degradation of methylene blue (MB), crystal violet (CV), methyl orange (MO), and Eriochrome black T (EBT) dyes from water. The PVDF-CuFe membrane exhibited improved heterogeneity, surface functionality (CuO, Fe-O, Cu-O-Fe), surface roughness, and hydrophilicity. The process parameters were optimized by response surface methodology, and maximum MB removal (100%) was achieved within 45.22-178.5 min at MB concentration (29.45-101.93 mg/L), PP concentration (0.5-2.41 g/L) and catalyst dosage (1.84-1.95 g/L). The degradation kinetics was well described by a pseudo-first-order model (R2=0.982) and fast reaction rate (0.029-0.089/min). The MB dye degradation mechanism is associated with HOâ¢/SO4â¢- reactive species generated by Fe3+/Fe2+ or Cu2+/Cu+ in PVDF-CuFe membrane and PP dissociation. The PVDF-CuFe membrane demonstrated excellent recyclability performance with a 12% reduction after five consecutive cycles. The catalytic membrane showed excellent photocatalytic degradation of crystal violet (100%), methyl orange (79%), and Eriochrome black T (60%). The results showed that UV-LED/persulfate-assisted PVDF-CuFe membranes can be used as a recyclable catalyst for the effective degradation of dye-contaminated water streams.
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The bottom contact in perovskite solar cells (PSCs) is easy to cause deep trap states and severe instability issues, especially under maximum power point tracking (MPPT). In this study, sodium gluconate (SG) is employed to disperse tin oxide (SnO2) nanoparticles (NPs) and regulate the interface contact at the buried interface. The SG-SnO2 electron transfer layer (ETL) enabled the deposition of pinhole-free perovskite films in ambient air and improved interface contact by bridging effect. SG-SnO2 PSCs achieved an impressive power conversion efficiency (PCE) of 25.34% (certified as 25.17%) with a high open-circuit voltage (VOC) exceeding 1.19 V. The VOC loss is less than 0.34 V relative to the 1.53 eV bandgap, and the fill factor (FF) loss is only 2.02% due to the improved contact. The SG-SnO2 PSCs retained around 90% of their initial PCEs after 1000 h operation (T90 = 1000 h), higher than T80 = 1000 h for the control SnO2 PSC. Microstructure analysis revealed that light-induced degradation primarily occurred at the buried holes and grain boundaries and highlighted the importance of bottom-contact engineering.
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The objective of this study is to develop an efficient, easily recoverable membrane-based photocatalyst for removing organic pollutants from aqueous solutions. This study documents the effective synthesis of a novel composite photocatalyst comprising WO3/g-C3N4(WCN) loaded onto cellulose acetate (CA). The physicochemical properties of the synthesized nanocomposites were validated using a range of techniques, including Fourier transform infrared spectroscopy, x-ray diffraction, scanning electron microscopy (SEM), energy-dispersive x-ray spectroscopy, and UV-visible diffuse reflectance spectroscopy. SEM analysis revealed that the WCN particles exhibited a well-decorated arrangement on the CA surface in the form of spherical particles. The successfully synthesized film was utilized as a potential adsorbent for removing organic pollutants such as Rhodamine B (Rh-B) and Methylene blue (MB) from aqueous solutions under UV light illumination. The results showcased the significant potential of the WCN@CA nanocomposite, achieving a remarkable 83% and 85% efficiency in eliminating Rh-B and MB. The pseudo-first-order kinetic models were found to be appropriate for both dye adsorption onto the WCN@CA nanocomposite. The WCN@CA catalyst, capable of being reused five times without significant loss of efficiency, shows great potential for decomposing toxic organic pollutants. The novelty of this work lies in the innovative combination of WCN with CA, resulting in a highly efficient and reusable photocatalyst for environmental remediation.