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1.
J Environ Sci (China) ; 148: 437-450, 2025 Feb.
Article in English | MEDLINE | ID: mdl-39095178

ABSTRACT

For environmental applications, it is crucial to rationally design and synthesize photocatalysts with positive exciton splitting and interfacial charge transfer. Here, a novel Ag-bridged dual Z-scheme Ag/g-C3N4/CoNi-LDH plasmonic heterojunction was successfully synthesized using a simple method, with the goal of overcoming the common drawbacks of traditional photocatalysts such as weak photoresponsivity, rapid combination of photo-generated carriers, and unstable structure. These materials were characterized by XRD, FT-IR, SEM, TEM UV-Vis/DRS, and XPS to verify the structure and stability of the heterostructure. The pristine LDH, g-C3N4, and Ag/g-C3N4/CoNi-LDH composite were investigated as photocatalysts for water remediation, an environmentally motivated process. Specifically, the photocatalytic degradation of tetracycline was studied as a model reaction. The performance of the supports and composite catalyst were determined by evaluating both the degradation and adsorption phenomenon. The influence of several experimental parameters such as catalyst loading, pH, and tetracycline concentration were evaluated. The current study provides important data for water treatment and similar environmental protection applications.


Subject(s)
Nanocomposites , Photolysis , Silver , Water Pollutants, Chemical , Water Purification , Nanocomposites/chemistry , Water Pollutants, Chemical/chemistry , Water Purification/methods , Silver/chemistry , Catalysis , Nitriles/chemistry , Nitrogen Compounds/chemistry , Adsorption , Graphite
2.
J Environ Sci (China) ; 148: 614-624, 2025 Feb.
Article in English | MEDLINE | ID: mdl-39095194

ABSTRACT

The overuse of antibiotics and antitumor drugs has resulted in more and more extensive pollution of water bodies with organic drugs, causing detrimental ecological effects, which have attracted attention towards effective and sustainable methods for antibiotics and antitumor drug degradation. Here, the hybrid nanomaterial (g-C3N4@Fe/Pd) was synthesized and used to remove a kind of both an antibiotic and antitumor drug named mitoxantrone (MTX) with 92.0% removal efficiency, and the MTX removal capacity is 450 mg/g. After exposing to the hybrid material the MTX aqueous solution changed color from dark blue to lighter progressively, and LC-UV results of residual solutions show that a new peak at 3.0 min (MTX: 13.2 min) after removal by g-C3N4@Fe/Pd appears, with the simultaneous detection of intermediate products indicating that g-C3N4@Fe/Pd indeed degrades MTX. Detailed mass spectrometric analysis suggests that the nuclear mass ratio decreased from 445.2 (M+1H) to 126.0 (M+1H), 169.1 (M+1H), 239.2 (M+1H), 267.3 (M+1H), 285.2 (M+1H), 371.4 (M+1H) and 415.2 (M+1H), and the maximum proportion (5.63%) substance of all degradation products (126.0 (M+1H)) is 40-100 times less toxic than MTX. A mechanism for the removal and degradation of mitoxantrone was proposed. Besides, actual water experiments confirmed that the maximum removal capacity of MTX by g-C3N4@Fe/Pd is up to 492.4 mg/g (0.02 g/L, 10 ppm).


Subject(s)
Graphite , Metal Nanoparticles , Mitoxantrone , Palladium , Water Pollutants, Chemical , Mitoxantrone/chemistry , Water Pollutants, Chemical/chemistry , Graphite/chemistry , Metal Nanoparticles/chemistry , Palladium/chemistry , Iron/chemistry , Catalysis , Nitrogen Compounds/chemistry , Antineoplastic Agents/chemistry
3.
J Environ Sci (China) ; 149: 188-199, 2025 Mar.
Article in English | MEDLINE | ID: mdl-39181633

ABSTRACT

Photocatalytic disinfection is an eco-friendly strategy for countering bacterial pollution in aquatic environments. Numerous strategies have been devised to facilitate the generation of reactive oxygen species (ROS) within photocatalysts, ultimately leading to the eradication of bacteria. However, the significance of the physical morphology of photocatalysts in the context of sterilization is frequently obscured, and the progress in the development of physical-chemical synergistic sterilization photocatalysts has been relatively limited. Herein, graphitic carbon nitride (g-C3N4) is chemically protonated to expose more sharp edges. PL fluorescence and EIS results indicate that the protonation can accelerate photogenerated carrier separation and enhance ROS production. Meanwhile, the sharp edges on the protonated g-C3N4 facilitate the physical disruption of cell walls for further promoting oxidative damage. Protonated C3N4 demonstrated superior bactericidal performance than that of pristine g-C3N4, effectively eliminating Escherichia coli within 40 minutes under irradiation. This work highlights the significance of incorporating physical and chemical synergies in photocatalyst design to enhance the disinfection efficiency of photocatalysis.


Subject(s)
Disinfection , Nitriles , Nitriles/chemistry , Disinfection/methods , Catalysis , Escherichia coli/drug effects , Reactive Oxygen Species , Graphite/chemistry , Sterilization/methods , Nitrogen Compounds/chemistry
4.
J Environ Sci (China) ; 150: 657-675, 2025 Apr.
Article in English | MEDLINE | ID: mdl-39306437

ABSTRACT

The uncontrolled release of antibiotics into the environment would be extremely harmful to human health and ecosystems. Therefore, it is in urgent need to monitor the environment and promote the detection and degradation of antibiotics to the relatively harmless by-products to a feasible extent. Graphitic carbon nitride (g-C3N4) is a non-metallic n-type semiconductor that can be used for the antibiotic detection and degradation due to its easy synthesis process, excellent chemical stability and unique optical properties. Unfortunately, the utilization of visible light, electron-hole recombination and electron conductivity have hindered its potential applications in the fields of photocatalytic degradation and electrochemical detection. Although previous publications have highlighted the diverse modification methods for the g-C3N4-based materials, the underlying structure-performance relationships of g-C3N4, especially for the detection and degradation of antibiotics, remains to be further explored. In view of this, the current review centered on the recent progress in the modification techniques of g-C3N4, the detection and degradation of antibiotics using the g-C3N4-based materials, as well as the potential antibiotic degradation mechanisms of the g-C3N4-based materials. Additionally, the underlying applications of the g-C3N4-based materials for antibiotic detection and degradation were also prospected. This review would provide a valuable research foundation and the up-to-date information for the g-C3N4-based materials to combat antibiotic pollution in the environment.


Subject(s)
Anti-Bacterial Agents , Graphite , Nitrogen Compounds , Graphite/chemistry , Anti-Bacterial Agents/analysis , Anti-Bacterial Agents/chemistry , Nitrogen Compounds/chemistry , Nitrogen Compounds/analysis , Environmental Monitoring/methods , Nitriles/chemistry , Nitriles/analysis
5.
ACS Appl Bio Mater ; 7(9): 6306-6312, 2024 Sep 16.
Article in English | MEDLINE | ID: mdl-39236263

ABSTRACT

Structure engineering is of great importance to enhance the carrier separation efficiency of multiphoton absorption (MPA) materials for near-infrared (NIR) light-driven reactive oxygen species (ROS) generation. In this study, the MPA-responsive potassium/cyano group-functionalized graphitic carbon nitride was investigated, demonstrating charge redistribution and improved carrier separation efficiency by density functional theory calculations and experimental results. With various types of boosted ROS generation under UV-vis or NIR-II light irradiation, the potassium/cyano group-functionalized graphitic carbon nitride could achieve efficient multiphoton photodynamic therapy after reducing the particle size. This study developed a simple strategy to manipulate charge distribution for booting NIR light-activated ROS generation in efficient multiphoton photodynamic therapy.


Subject(s)
Biocompatible Materials , Graphite , Infrared Rays , Materials Testing , Nitrogen Compounds , Particle Size , Reactive Oxygen Species , Graphite/chemistry , Reactive Oxygen Species/metabolism , Reactive Oxygen Species/chemistry , Nitrogen Compounds/chemistry , Biocompatible Materials/chemistry , Photosensitizing Agents/chemistry , Photosensitizing Agents/pharmacology , Humans , Photochemotherapy , Nitriles/chemistry
6.
Mikrochim Acta ; 191(10): 581, 2024 09 07.
Article in English | MEDLINE | ID: mdl-39243346

ABSTRACT

To meet the needs of developing efficient extractive materials alongside the evolution of miniaturized sorbent-based sample preparation techniques, a mesoporous structure of g-C3N4 doped with sulfur as a heteroatom was achieved utilizing a bubble template approach while avoiding the severe conditions of other methods. In an effort to increase the number of adsorption sites, the resultant exfoliated structure was then modified with thymol-coumarin NADES as a natural sorbent modifier, followed by introduction into a nylon 6 polymer via an electrospinning process. X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, field-emission scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), and Brunauer-Emmett-Teller (BET) surface area analysis validated S-doped g-C3N4 and composite production. The prepared electrospun fiber nanocomposite, entailing satisfactory processability, was then successfully utilized as a sorbent in on-chip thin film micro-solid-phase extraction of non-steroidal anti-inflammatory drugs (NSAIDs) from saliva samples prior to liquid chromatography-tandem mass spectrometry (LC-MS/MS) analysis. Utilizing a chip device, a thin film µ-SPE coupled with LC-MS/MS analysis yielded promising outcomes with reduced sample solution and organic solvents while extending lifetime of a thin film sorbent. The DES-modified S-doped g-C3N4 amount in electrospun was optimized, along with adsorption and desorption variables. Under optimal conditions, selected NSAIDs were found to have a linear range of 0.05-100.0 ng mL-1 with an R2 ≥ 0.997. The detection limits were ranged between 0.02 and 0.2 ng mL-1. The intra-day and inter-day precisions obtained were less than 6.0%. Relative recoveries were between 93.3 and 111.4%.


Subject(s)
Anti-Inflammatory Agents, Non-Steroidal , Deep Eutectic Solvents , Graphite , Limit of Detection , Nanofibers , Saliva , Tandem Mass Spectrometry , Saliva/chemistry , Tandem Mass Spectrometry/methods , Graphite/chemistry , Nanofibers/chemistry , Humans , Adsorption , Anti-Inflammatory Agents, Non-Steroidal/analysis , Porosity , Deep Eutectic Solvents/chemistry , Chromatography, Liquid/methods , Nitrogen Compounds/chemistry , Solid Phase Microextraction/methods , Solid Phase Extraction/methods
7.
Molecules ; 29(17)2024 Sep 04.
Article in English | MEDLINE | ID: mdl-39275040

ABSTRACT

Graphitic carbon nitride (g-C3N4, CN) has emerged as a promising photocatalytic material due to its inherent stability, antibacterial properties, and eco-friendliness. However, its tendency to aggregate and limited dispersion hinder its efficacy in practical antibacterial applications. To address these limitations, this study focuses on developing a composite hydrogel coating, in which sodium alginate (SA) molecules interact electrostatically and through hydrogen bonding to anchor CN, thereby significantly improving its dispersion. The optimal CN loading of 35% results in a hydrogel with a tensile strength of 120 MPa and an antibacterial rate of 99.87% within 6 h. The enhanced mechanical properties are attributed to hydrogen bonding between the -NH2 groups of CN and the -OH groups of SA, while the -OH groups of SA facilitate the attraction of photogenerated holes from CN, promoting carrier transfer and separation, thereby strengthening the antibacterial action. Moreover, the hydrogel coating exhibits excellent antibacterial and corrosion resistance capabilities against Pseudomonas aeruginosa on 316L stainless steel (316L SS), laying the foundation for advanced antimicrobial and anticorrosion hydrogel systems.


Subject(s)
Alginates , Anti-Bacterial Agents , Graphite , Hydrogels , Pseudomonas aeruginosa , Alginates/chemistry , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Pseudomonas aeruginosa/drug effects , Hydrogels/chemistry , Hydrogels/pharmacology , Graphite/chemistry , Graphite/pharmacology , Nitrogen Compounds/chemistry , Nitrogen Compounds/pharmacology , Corrosion , Microbial Sensitivity Tests , Coated Materials, Biocompatible/chemistry , Coated Materials, Biocompatible/pharmacology , Hydrogen Bonding , Stainless Steel/chemistry
8.
Sensors (Basel) ; 24(17)2024 Sep 09.
Article in English | MEDLINE | ID: mdl-39275755

ABSTRACT

The most frequently used sulfonamide is sulfamethazine (SMZ) because it is often found in foods made from livestock, which is hazardous for individuals. Here, we have developed an easy, quick, selective, and sensitive analytical technique to efficiently detect SMZ. Recently, transition metal oxides have attracted many researchers for their excellent performance as a promising sensor for SMZ analysis because of their superior redox activity, electrocatalytic activity, electroactive sites, and electron transfer properties. Further, Cu-based oxides have a resilient electrical conductivity; however, to boost it to an extreme extent, a composite including two-dimensional (2D) graphitic carbon nitride (g-C3N4) nanosheets needs to be constructed and ready as a composite (denoted as g-C3N4/Cu2Y2O5). Moreover, several techniques, including X-ray diffraction analysis, scanning electron microscopy analysis, energy-dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, and Raman spectroscopy were employed to analyze the composites. The electrochemical measurements have revealed that the constructed g-C3N4/Cu2Y2O5 composites exhibit great electrochemical activity. Nevertheless, the sensor achieved outstanding repeatability and reproducibility alongside a low limit of detection (LOD) of 0.23 µM, a long linear range of 2 to 276 µM, and an electrode sensitivity of 8.86 µA µM-1 cm-2. Finally, the proposed GCE/g-C3N4/Cu2Y2O5 electrode proved highly effective for detection of SMZ in food samples, with acceptable recoveries. The GCE/g-C3N4/Cu2Y2O5 electrode has been successfully applied to SMZ detection in food and water samples.


Subject(s)
Copper , Electrochemical Techniques , Food Analysis , Graphite , Sulfamethazine , Electrochemical Techniques/methods , Graphite/chemistry , Sulfamethazine/analysis , Sulfamethazine/chemistry , Copper/chemistry , Copper/analysis , Food Analysis/methods , Nitrogen Compounds/chemistry , Limit of Detection , Electrodes , Food Contamination/analysis , Water/chemistry , Reproducibility of Results
9.
Sci Rep ; 14(1): 21488, 2024 09 14.
Article in English | MEDLINE | ID: mdl-39277597

ABSTRACT

Graphite carbon nitride (g-C3N4) is a two-dimensional nano-sheet with electronic properties, which shows unique characteristics with high chemical and thermal stability in its structure. The functionalization of these compounds through covalent bonding is an important step towards significantly improving their properties and capabilities. To achieve this goal, a novel strategy for the covalent functionalization of Fe3O4@g-C3N4 with thiamine hydrochloride (vitamin B1) via cyanuric chloride (TCT), which is a divalent covalent linker, was presented. The efficiency of Fe3O4@gC3N4@Thiamine as a heterogeneous organic catalyst in the synthesis of spirooxindole-pyran derivatives and 2-amino-4H-pyran under solvent-free conditions was evaluated and the yields of high-purity products were presented. In addition, easy recycling and reuse for seven consecutive cycles without significant reduction in catalytic activity are other features of this catalyst. Moreover, the performance of the prepared sorbent in the microextraction technique (herein, magnetic solid phase extraction) was studied. The tebuconazole was selected as the target analyte. The target analyte was extracted and determined by HPLC-UV. Under the optimum condition, the linear range of the method (LDR) was estimated in the range of 0.2-100 µg L-1 (the coefficient of determination of 0.9962 for tebuconazole). The detection limit (LOD) of the method for tebuconazole was calculated to be 0.05 µg L-1. The limit of quantification (LOQ) of the method was also estimated to be 0.16 µg L-1. In order to check the precision of the proposed method, the intra-day and inter-day relative standard deviations (RSD%) were calculated, which were in the range of 1.5- 2.8%. The method was used for the successful extraction and determination of tebuconazole in tomato, cucumber, and carrot samples.


Subject(s)
Graphite , Thiamine , Triazoles , Catalysis , Triazoles/chemistry , Triazoles/analysis , Graphite/chemistry , Thiamine/chemistry , Thiamine/analysis , Food Contamination/analysis , Food Analysis/methods , Heterocyclic Compounds/chemistry , Heterocyclic Compounds/chemical synthesis , Nitrogen Compounds/chemistry , Solid Phase Microextraction/methods , Carbon Compounds, Inorganic/chemistry
10.
ACS Appl Mater Interfaces ; 16(34): 45049-45062, 2024 Aug 28.
Article in English | MEDLINE | ID: mdl-39141582

ABSTRACT

Heavy metals are crucial carcinogenic agents threatening the environment and living habituates. Among them, arsenic (As) is an important metalloid that is categorized as a group I toxic carcinogen. Roxarsone (RX) is an organoarsenic antibiotic compound primarily used as a veterinarian drug and growth promoter for poultry animals. The extensive usage of RX increased the accumulation of As in living beings and the ecosystem. Therefore, we have prepared an electrochemical sensor based on 3D bismuth oxybromide with 2D selenium-doped graphitic carbon nitride (BOB/SCN) electrocatalyst for the rapid detection of RX. The elemental and structural details were thoroughly investigated with several spectroscopic techniques. The electrochemical properties were measured by impedance and voltammetric measurements. The electrocatalytic behavior toward the RX was estimated with different voltammetric methods. Therefore, our BOB/SCN-based electrochemical sensor demonstrated a low detection limit (2.3 nM), low quantification value (7.7 nM), optimal sensitivity (0.675 µA µM-1 cm-2), and good linear ranges (0.01-77 and 77-857 µM). Additionally, this sensor showed good electrochemical performance and was applied to monitor the RX in various real samples with remarkable recoveries. Based on these results, our BOB/SCN sensor is a promising electrochemical platform for determining RX.


Subject(s)
Bismuth , Electrochemical Techniques , Graphite , Roxarsone , Selenium , Graphite/chemistry , Electrochemical Techniques/methods , Catalysis , Selenium/chemistry , Bismuth/chemistry , Roxarsone/analysis , Roxarsone/chemistry , Animals , Nitrogen Compounds/chemistry , Limit of Detection , Nitriles/chemistry
11.
Chemosphere ; 364: 143198, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39209037

ABSTRACT

The occurrence of xenobiotic pollutants in the aquatic environment troubling the present and future generation. Persistent Organic Pollutants (POPs) is one such class of xenobiotic that was dominant in that category. In the present paper, a competent visible light driven heterojunction photocatalyst combining Bismuth niobate and g-C3N4 was developed for the effective removal of Bisphenol A (BPA), a notable POP. Before constructing the heterostructure the calcination temperature for bismuth niobate synthesis was optimised for achieving most proficient photocatalysis. A phase change in the crystal structure of bismuth niobate was apparent. The Bi3NbO7 at 300-500 °C transformed to Bi5Nb3O15 at 600-700 °C and to orthorhombic BiNbO4 at 900 °C as the temperature was enhanced. With the increment in the temperature the light absorbance of the materials enhanced in UV and reduced in visible light. Thus, the bismuth niobate obtained by calcining at 500 °C demonstrated highest BPA removal under sunlight was chosen for heterojunction construction. After the heterojunction construction with g-C3N4 the crystal lattice strain was observed to be reduced for all composites, and a greater mobility of charge carriers was observed within the composite. The presence of either of the materials resulted in a different band structure and thus Type II and Z-scheme pathway was inferred. A commendable photocatalytic activity was observed for B1.5G and BG1.5 under sunlight and LED light respectively. Hight amount of g-C3N4 in the BG1.5 resulted in maximum absorbance in LED light. Superoxide radicals (*O2-) radicals were observed as major radicals for B1.5G composite, whereas both *O2- and holes (h+) were the major radicals in case of BG1.5.


Subject(s)
Benzhydryl Compounds , Bismuth , Light , Niobium , Phenols , Benzhydryl Compounds/chemistry , Bismuth/chemistry , Phenols/chemistry , Catalysis , Niobium/chemistry , Water Pollutants, Chemical/chemistry , Graphite/chemistry , Nitrogen Compounds/chemistry , Nitriles/chemistry , Persistent Organic Pollutants/chemistry , Photolysis
12.
Chemosphere ; 364: 143178, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39214404

ABSTRACT

The synthesis of sulfur-doped exfoliated graphitic carbon nitride (S-gCN) photocatalyst was achieved by the implementation of a two-step calcination technique. The XRD results revealed that all the fabricated photocatalytic materials were crystalline in nature. The inclusion of 5% sulfur in gCN led to a conspicuous escalation in the surface area of photocatalyst, rising from 10.294 to 61.185 m2g⁻1. Morphological scrutiny of the samples using FE-SEM revealed that pristine gCN exhibited tightly stacked small nanosheets, whereas inclusion of sulfur and exfoliation resulted in generation of loosely distributed large nanosheet. Furthermore, the inclusion of sulfur also induced a shift in the energy band gap (Eg) from 2.81 eV to 2.63 eV, making it felicitous for investigation as proficient visible light photocatalyst. Additionally, the photoluminescence photo-induced charge carrier recombination behavior revealed a reduced peak intensity for 5% S-gCN compared to other synthesized compositions. This observation can be directly linked to the minimized electron-hole pairs recombination during photocatalysis, underscoring its superior photocatalytic performance. Our findings revealed that the 5% S-gCN photocatalyst exhibit the most promising attributes, it degraded Tetracycline drug, Chlorpyrifos pesticide and Eriochrome Black T dye under visible light irradiation almost ∼4 times more efficiently than pristine gCN. Additionally, exceptional visible light photocatalytic antibacterial efficacy was also perceived by 5% S-gCN against S. aureus bacteria. Overall, the present research sheds light on how doping and exfoliation interact to modify the structure and catalytic properties of gCN, paving the way for the development of outstanding performance, visible light-responsive efficient photocatalysts for environmental restoration.


Subject(s)
Anti-Bacterial Agents , Graphite , Light , Sulfur , Sulfur/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/pharmacology , Catalysis , Graphite/chemistry , Nitrogen Compounds/chemistry , Photolysis , Photochemical Processes , Tetracycline/chemistry , Tetracycline/pharmacology , Water Pollutants, Chemical/chemistry , Nitriles/chemistry , Nitriles/pharmacology
13.
J Mater Chem B ; 12(37): 9364-9374, 2024 Sep 25.
Article in English | MEDLINE | ID: mdl-39188219

ABSTRACT

The detrimental effects of widespread pesticide application on the health of living organisms highlight the urgent need for technological advancements in monitoring pesticide residues at trace levels. This study involves the synthesis of a distinctive sensing material, KL@Ni@g-C3N4, which comprises nanocomposites of graphitic carbon nitride with Kraft lignin and nickel. The prepared samples were characterized using FT-IR, PXRD, TEM, SEM, and EDX techniques. The KL@Ni@g-C3N4 nanocomposite was drop-cast on a graphite electrode. Subsequently, this fabricated electrode was used to detect cypermethrin (CYP) residues in drinking water. The redox properties of the fabricated sensors were evaluated using electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). The limit of detection (LOD) of the fabricated sensor was determined to be 0.026 µg mL-1, which is below the maximum residual limits of CYP in the environment (0.5 µg mL-1) and within the acceptable range for food products (∼0.05 to 0.2 µg mL-1). Therefore, this study proposes a promising alternative to conventional methods for detecting pesticides in drinking water.


Subject(s)
Drinking Water , Electrodes , Graphite , Lignin , Nanocomposites , Nickel , Pesticides , Pyrethrins , Pyrethrins/analysis , Nanocomposites/chemistry , Graphite/chemistry , Drinking Water/analysis , Nickel/chemistry , Nickel/analysis , Lignin/chemistry , Lignin/analysis , Pesticides/analysis , Water Pollutants, Chemical/analysis , Electrochemical Techniques , Nitrogen Compounds/chemistry , Nitriles/chemistry , Nitriles/analysis , Nitriles/toxicity , Limit of Detection , Surface Properties
14.
Anal Chim Acta ; 1320: 342985, 2024 Sep 01.
Article in English | MEDLINE | ID: mdl-39142767

ABSTRACT

BACKGROUND: There is widespread interest in the design of portable electrochemical sensors for the selective monitoring of biomolecules. Dopamine (DA) is one of the neurotransmitter molecules that play a key role in the monitoring of some neuronal disorders such as Alzheimer's and Parkinson's diseases. Facile synthesis of the highly active surface interface to design a portable electrochemical sensor for the sensitive and selective monitoring of biomolecules (i.e., DA) in its resources such as human fluids is highly required. RESULTS: The designed sensor is based on a three-dimensional phosphorous and sulfur resembling a g-C3N4 hornet's nest (3D-PS-doped CNHN). The morphological structure of 3D-PS-doped CNHN features multi-open gates and numerous vacant voids, presenting a novel design reminiscent of a hornet's nest. The outer surface exhibits a heterogeneous structure with a wave orientation and rough surface texture. Each gate structure takes on a hexagonal shape with a wall size of approximately 100 nm. These structural characteristics, including high surface area and hierarchical design, facilitate the diffusion of electrolytes and enhance the binding and high loading of DA molecules on both inner and outer surfaces. The multifunctional nature of g-C3N4, incorporating phosphorous and sulfur atoms, contributes to a versatile surface that improves DA binding. Additionally, the phosphate and sulfate groups' functionalities enhance sensing properties, thereby outlining selectivity. The resulting portable 3D-PS-doped CNHN sensor demonstrates high sensitivity with a low limit of detection (7.8 nM) and a broad linear range spanning from 10 to 500 nM. SIGNIFICANCE: The portable DA sensor based on the 3D-PS-doped CNHN/SPCE exhibits excellent recovery of DA molecules in human fluids, such as human serum and urine samples, demonstrating high stability and good reproducibility. The designed portable DA sensor could find utility in the detection of DA in clinical samples, showcasing its potential for practical applications in medical settings.


Subject(s)
Dopamine , Electrochemical Techniques , Dopamine/analysis , Dopamine/urine , Humans , Electrochemical Techniques/methods , Electrochemical Techniques/instrumentation , Nitrogen Compounds/chemistry , Limit of Detection , Sulfur/chemistry , Electrodes , Biosensing Techniques/methods , Graphite/chemistry , Phosphorus/chemistry , Surface Properties
15.
Phys Chem Chem Phys ; 26(32): 21677-21687, 2024 Aug 14.
Article in English | MEDLINE | ID: mdl-39091182

ABSTRACT

In recent years, great progress has been made on the study of nanozymes with enzyme-like properties. Here, bimetallic Fe and Ni nanoclusters were anchored on the nanosheets of nitrogen-rich layered graphitic carbon nitride by one-step pyrolysis at high temperature (Fe/Ni-CN). The loading content of Fe and Ni on Fe/Ni-CN is as high as 8.0%, and Fe/Ni-CN has a high specific surface area of 121.86 m2 g-1. The Fe/Ni-CN can effectively oxidize 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of H2O2, and exhibits efficient peroxidase-like activity, leading to a 17.2-fold increase compared to pure graphitic carbon nitride (CN). Similar to the natural horseradish peroxidase (HRP), the Fe/Ni-CN nanozyme follows catalytic kinetics. The Michaelis-Menten constant (Km) value of the Fe/Ni-CN nanozyme for TMB is about 8.3-fold lower than that for HRP, which means that the Fe/Ni-CN nanozyme has better affinity for TMB. In addition, the catalytic mechanism was investigated by combination of free radical quenching experiments and density-functional theory (DFT) calculations. The results show that the high peroxidase-like activity is due to the easy adsorption of H2O2 after bimetal loading, which is conducive to the production of hydroxyl radicals. Based on the extraordinary peroxidase-like activity, the colorimetric detection of p-phenylenediamine (PPD) was constructed with a wide linear range of 0.2-30 µM and a low detection limit of 0.02 µM. The sensor system has been successfully applied to the detection of residual PPD in real dyed hair samples. The results show that the colorimetric method is sensitive, highly selective and accurate. This study provides a new idea for the efficient enhancement of nanozyme activity and effective detection of PPD by a bimetallic synergistic strategy.


Subject(s)
Colorimetry , Graphite , Iron , Nickel , Nitrogen Compounds , Phenylenediamines , Graphite/chemistry , Phenylenediamines/chemistry , Colorimetry/methods , Nitrogen Compounds/chemistry , Nickel/chemistry , Iron/chemistry , Hydrogen Peroxide/analysis , Hydrogen Peroxide/chemistry , Nitriles/chemistry , Limit of Detection , Catalysis , Benzidines/chemistry
16.
Sci Rep ; 14(1): 19123, 2024 08 18.
Article in English | MEDLINE | ID: mdl-39155360

ABSTRACT

An environmentally friendly, versatile multicomponent reaction for synthesizing isoxazol-5-one and pyrazol-3-one derivatives has been developed, utilizing a freshly prepared g-C3N4·OH nanocomposite as a highly efficient catalyst at room temperature in aqueous environment. This innovative approach yielded all the desired products with exceptionally high yields and concise reaction durations. The catalyst was well characterized by FT-IR, XRD, SEM, EDAX, and TGA/DTA studies. Notably, the catalyst demonstrated outstanding recyclability, maintaining its catalytic efficacy over six consecutive cycles without any loss. The sustainability of this methodology was assessed through various eco-friendly parameters, including E-factor and eco-score, confirming its viability as a green synthetic route in organic chemistry. Additionally, the gram-scale synthesis verifies its potential for industrial applications. The ten synthesized compounds were also analyzed via a PASS online tool to check their several pharmacological activities. The study is complemented by in silico molecular docking, pharmacokinetics, and molecular dynamics simulation studies. These studies discover 5D as a potential candidate for drug development, supported by its favorable drug-like properties, ADMET studies, docking interaction, and stable behavior in the protein binding cavity.


Subject(s)
Isoxazoles , Molecular Docking Simulation , Nanocomposites , Pyrazolones , Nanocomposites/chemistry , Pyrazolones/chemistry , Pyrazolones/chemical synthesis , Pyrazolones/pharmacokinetics , Isoxazoles/chemistry , Isoxazoles/pharmacokinetics , Graphite/chemistry , Catalysis , Molecular Dynamics Simulation , Nitriles/chemistry , Nitrogen Compounds/chemistry , Nitrogen Compounds/chemical synthesis
17.
ACS Biomater Sci Eng ; 10(8): 4645-4661, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-39086282

ABSTRACT

Graphite carbon nitride (g-C3N4) is a two-dimensional conjugated polymer with a unique energy band structure similar to graphene. Due to its outstanding analytical advantages, such as relatively small band gap (2.7 eV), low-cost synthesis, high thermal stability, excellent photocatalytic ability, and good biocompatibility, g-C3N4 has attracted the interest of researchers and industry, especially in the medical field. This paper summarizes the latest research on g-C3N4-based composites in various biomedical applications, including therapy, diagnostic imaging, biosensors, antibacterial, and wearable devices. In addition, the application prospects and possible challenges of g-C3N4 in nanomedicine are also discussed in detail. This review is expected to inspire emerging biomedical applications based on g-C3N4.


Subject(s)
Biosensing Techniques , Graphite , Nitrogen Compounds , Graphite/chemistry , Humans , Nitrogen Compounds/chemistry , Biocompatible Materials/chemistry , Animals , Nitriles/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/pharmacology , Wearable Electronic Devices , Nanomedicine/methods
18.
Environ Res ; 260: 119779, 2024 Nov 01.
Article in English | MEDLINE | ID: mdl-39142459

ABSTRACT

Lanthanum nickelate (LaNiO3), known for its high visible-light absorption, is a promising photocatalyst for water purification. However, the low conduction band position and high photogenerated carrier complexation rate of pure LaNiO3 limit its photocatalytic activity. To address this issue, we investigated the synergistic effects of doping and constructing heterojunctions. A La0.9Sr0.1NiO3 (20%)/g-C3N4 (L2CN8) heterojunction was successfully created. In addition, various characterisation techniques were then employed to analyse the structure-performance relationships of these heterojunction photocatalysts in degrading organic dyes. Results revealed that at a 10% Sr doping level, the oxygen vacancy content was 0.68, which is significantly higher than that of LaNiO3 (0.05). The increased number of oxygen vacancies enhanced the electron capture ability and improved the separation efficiency of photogenerated carriers. Furthermore, the optimised L2CN8 (20 mg) achieved 81.2% and 73.8% removal of methylene blue (50.0 mL, 10 mg L-1) and tetracycline (50.0 mL, 10 mg L-1) under simulated visible-light irradiation (λ > 420 nm). Furthermore, an active species capture experiment confirmed the significant role of superoxide radicals (·O2-) in the degradation process. Based on these experimental findings, we proposed a rational Z-type charge transfer mechanism. This study holds great importance for water pollution control and environmental protection.


Subject(s)
Lanthanum , Light , Water Pollutants, Chemical , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/analysis , Catalysis , Lanthanum/chemistry , Nickel/chemistry , Methylene Blue/chemistry , Photolysis , Photochemical Processes , Nitrogen Compounds/chemistry , Tetracycline/chemistry , Nitriles/chemistry , Graphite
19.
Int J Mol Sci ; 25(16)2024 Aug 14.
Article in English | MEDLINE | ID: mdl-39201528

ABSTRACT

Graphitic carbon nitride (g-C3N4)-based photocatalysts have garnered significant interest as a promising photocatalyst for hydrogen generation under visible light, to address energy and environmental challenges owing to their favorable electronic structure, affordability, and stability. In spite of that, issues such as high charge carrier recombination rates and low quantum efficiency impede its broader application. To overcome these limitations, structural and morphological modification of the g-C3N4-based photocatalysts is a novel frontline to improve the photocatalytic performance. Therefore, we briefly summarize the current preparation methods of g-C3N4. Importantly, this review highlights recent advancements in crafting high-performance g-C3N4-based photocatalysts, focusing on strategies like elemental doping, nanostructure design, bandgap engineering, and heterostructure construction. Notably, sophisticated doping techniques have propelled hydrogen production rates to a 104-fold increase. Ingenious nanostructure designs have expanded the surface area by a factor of 26, concurrently extending the fluorescence lifetime of charge carriers by 50%. Moreover, the strategic assembly of heterojunctions has not only elevated charge carrier separation efficiency but also preserved formidable redox properties, culminating in a dramatic hundredfold surge in hydrogen generation performance. This work provides a reliable and brief overview of the controlled modification engineering of g-C3N4-based photocatalyst systems, paving the way for more efficient hydrogen production.


Subject(s)
Graphite , Hydrogen , Nitrogen Compounds , Photochemical Processes , Hydrogen/chemistry , Catalysis , Graphite/chemistry , Nitrogen Compounds/chemistry , Light , Nanostructures/chemistry
20.
Luminescence ; 39(9): e4873, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39192766

ABSTRACT

In this study, we present the development and analysis of electrochemical sensors utilizing graphitic carbon nitride copper-tungsten nanoparticles (g-C3N4 @Cu-W Nps) capped with various cationic surfactants of differing chain lengths and counter ions. The fabricated nanoparticles underwent thorough characterization to assess their morphological, structural, and compositional attributes, revealing their uniformity, spherical morphology, and monoclinic crystal phases. Subsequently, these nanoparticles were employed in the fabrication of electrochemical sensors for hydrazine detection. A comprehensive comparison of the electrochemical responses, evaluated via cyclic voltammetry, was conducted between sensors utilizing bare nanoparticles and those capped with surfactants.


Subject(s)
Copper , Dopamine , Electrochemical Techniques , Graphite , Metal Nanoparticles , Copper/chemistry , Dopamine/analysis , Dopamine/chemistry , Metal Nanoparticles/chemistry , Graphite/chemistry , Nitrogen Compounds/chemistry , Hydrazines/chemistry , Particle Size
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