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A novel dual Z-scheme BiOBr/NH 2 -MIL-101(Fe)/g-C 3 N 4 (BNG) heterojunction was constructed via a simple two-step solvothermal process. NH 2 -MIL-101(Fe) nanoparticles and BiOBr microspheres were uniformly deposited on the surface of g-C 3 N 4 . The prepared BNG exhibited significantly enhanced photocatalytic performance for tetracycline (TC) degradation compared to single catalyst. The optimized BNG-19 composite (with 19% NH 2 -MIL-101(Fe)/g-C 3 N 4 ) achieved 92.38% degradation of TC within 75 min under visible light, which was 2.47, 1.78, and 1.84 times higher than that of pure g-C 3 N 4 , NH 2 -MIL-101(Fe), and BiOBr, respectively. Moreover, the composite exhibited excellent stability with 82.4% removal efficiency after five cycles. The enhanced photocatalytic performance was attributed to the synergistic dual Z-scheme charge transfer mechanism, which was directly evidenced by in-situ irradiated XPS showing opposite directional shifts of Bi 4f (positive) and Fe 2p/N 1s (negative). This unique charge transfer pathway effectively promoted the separation of photogenerated carriers, with •OH and •O 2 ⁻ identified as the dominant reactive species. This work provides a new strategy for constructing g-C 3 N 4 -based dual Z-scheme heterostructures with direct mechanistic evidence for efficient environmental remediation.
Developing high-performance anti-fouling ultrafiltration membranes is essential for treating shale gas wastewater (SGW), addressing its severe membrane fouling issues. This study reports the fabrication of polyvinylidene fluoride (PVDF)/PVDF-graft-poly(ethylene glycol) methyl ether methacrylate (PVDF-g-PEGMA) blended hollow fiber membranes via non-solvent induced phase separation for direct treatment of SGW. The influences of the copolymer doping ratio on microstructure, chemical composition, and hydrophilicity were systematically investigated. The addition of PVDF-g-PEGMA contributed to a favorable membrane morphology and significantly improved hydrophilicity. The 20 wt% PVDF-g-PEGMA modified membrane achieved a 64.4% increase in pure water flux while retaining over 95.9% rejection for both humic acid and bovine serum albumin. More importantly, in long-term filtration of SGW, the modified membrane demonstrated a stable permeation flux of ~30.4 L·m −2 ·h −1 , surpassing the performance of the unmodified membrane by 300% and reducing the cost of water treatment for unit flux by 17.6%. Analysis based on the extended Dragun-Landau-Verwey-Overbeek theory indicated that the incorporation of PVDF-g-PEGMA effectively reduced the attractive interaction energy between the membrane and pollutants. These results demonstrate that the PVDF-g-PEGMA blending modification not only significantly enhanced membrane permeability and anti-fouling performance under challenging real wastewater conditions but also achieved sustained flux and superior anti-fouling behavior during lab-scale SGW operation, thereby enabling water reuse with reduced maintenance demand.
Photocatalysis, as a novel technique, has been widely used for antibiotic pollution remediation in wastewater. In the processes of degradation and removal of antibiotics, the impact of photocatalysts on microenvironment is very important but remains poorly understood. In the present study, the effect of typical photocatalyst g-C3N4 (Graphitic carbon nitride) on microbial community was investigated in two sediment types (riverbed sediment and pig-farm sediment) polluted by tetracycline (TC) in central southern China. The riverbed sediment and pig farm sediment samples were respectively exposed to g-C3N4 (25, 75, 125 mg⋅kg–1) and TC (60, 120, 180 mg⋅L–1) treatments alone or combination for 30 days, respectively. The bacterial community and antibiotic resistance genes (ARGs) of the treated sediments were analyzed by Illumina sequencing and metagenomic sequencing. Studies had shown that: TC, g-C3N4, and TC/g-C3N4 have significant effects on the changes of microbial communities and components in riverbed sediment, but they do not exist in pig farm sediment. The most alterations of microbial taxa were Acidobacteriota, Actinobacteriota, and Desulfobacterota in riverbed sediment, and Elusimicrobiota in the pig farm sediment under various treatments. Through network analysis, it was found that the distribution of microorganisms in the pig farm sediment is more complex and more stable. The addition of g-C3N4 reduced the absolute abundance of ARGs in the two examined sediments, but not significantly changed their relative abundance of ARGs. The g-C3N4 application was beneficial to the removal of TC residues and to the prevention of the generation and transmission of ARGs in sediments. Our results suggested that g-C3N4 was a suitable photocatalyst with excellent application prospect for the removal of TC residues and the control of ARGs in environment.
Loading co-catalysts are an effective strategy to break the confinement of bulk carbon nitride in photocatalysis . Employing this strategy, N-doped g-C 3 N 4 decorated with CoS x was successfully prepared through a photochemical synthesis route. The optimum hydrogen evolution performance of N-CN-CoS x -4 was 1757 μmol g −1 h −1 under visible light irradiation . Superior interfacial carrier transfer properties and improved light absorption of N-CN-CoS x -4 could elucidate its better photocatalytic activity . This research offers a reference for the construction of high-efficiency, stable and low-priced photocatalysts .
Herein, we report a stable catalyst with Ru single atoms anchored on a one-dimensional carbon fiber@graphitic carbon nitride hierarchy, by assembling wet wipes composed of fiber-derived carbon fiber (CF), melamine-derived graphitic carbon nitride (g-C3N4) and RuCl3 before NaBH4 reduction. The atomically dispersed Ru species (3.0 wt%) are tightly attached via N-coordination provided by exterior g-C3N4 nanosheets, and further stabilized by the interior mesoporous CF. The obtained CF@g-C3N4–Ru SAs catalyst can be cycled six times without notable leaching of Ru or loss of GVL yield in the acidic media. This catalyst is more stable than Ru nanoparticles supported on CF@g-C3N4, as well as Ru single atoms anchored on CF and g-C3N4, and proves to be one of the most efficient metal catalysts for aqueous LA hydrogenation to γ-valerolactone (GVL). The isolated Ru atoms by strong N-coordination, and their enhanced electron/mass transfer afforded by the one-dimensional hierarchy, can be responsible for the excellent durability of CF@g-C3N4–Ru SAs under harsh reaction conditions.Keywords:Ru single atom;one-dimensional hierarchy;levulinic acid;γ-valerolactone;stability
g-C3N4/Ag3PO4/TiO2nanocomposite materials were loaded onto a polyvinylidene fluoride (PVDF) membrane using a phase inversion method to obtain a photocatalytic flat membrane for dye removal. The morphology, structure, and photocatalytic activity of the g-C3N4/Ag3PO4/TiO2nanoparticles and composite membrane were evaluated. The g-C3N4/Ag3PO4/TiO2/PVDF membrane exhibited superior morphology, hydrophilic properties, and antifouling performance compared with the raw PVDF membrane. Four-stage filtration was performed to evaluate the self-cleaning and antifouling capacity of the g-C3N4/Ag3PO4/TiO2/PVDF membrane. Upon irradiating the composite membrane with visible light for 30 min, its irreversible fouling resistance (Rir) was low (9%), and its flux recovery rate (FRR) was high (71.0%) after five filtration cycles. The removal rate of rhodamine B (RhB) from the composite membrane under visible light irradiation reached 98.1% owing to the high photocatalytic activity of the membrane, which was superior to that of raw PVDF membrane (42.5%). A mechanism of photocatalytic composite membranes for RhB degradation was proposed. Therefore, this study is expected to broaden prospects in the field of membrane filtration technology.Keywords:g-C3N4/Ag3PO4/TiO2nanocomposite;photocatalytic membrane;self-cleaning;membrane fouling;dye
A novel phosphorus and oxygen co-doped graphitic carbon nitride (sheetP-O-CNSSA) photocatalyst was successfully synthesized and applied for H2evolution under visible light. In the synthesis process ofsheetP-O-CNSSA, the supramolecular complex was developed by the self-assembly and copolymerization reaction among melamine, cyanuric acid (CA) and trithiocyanuric acid (TCA) to act as g-C3N4precursors, while (NH4)2HPO4was applied as P and O precursors for element doping. The chemical structures, morphologies, and optical properties of thesheetP-O-CNSSAwere characterized by a series of measurements, i.e., XRD, FT-IR, SEM, TEM, UV-vis DRS, and PL. The results suggested that the introduction of P and O elements could enhance the separation and migration efficiency of photogenerated electrons and holes in the energy band of g-C3N4. The photocatalytic tests over Erythrosin B (EB) sensitizedsheetP-O-CNSSAindicated that the hydrogen evolution was greatly enhanced compared with other catalysts and non-sensitizedsheetP-O-CNSSAunder visible light irradiation. Finally, a possible dye-sensitized photocatalysis mechanism was also proposed on the basis of the as-obtained results.Keywords:P-O-co-doped g-C3N4;self-assembly;dye sensitization;hydrogen evolution
Flexibility and self-cleaning are the main research hot-spots in the development of plasma substrates for practical applications in Surface-enhanced Raman scattering (SERS) at present. In this study, a flexible composite Au@Ag/ultrathin g-C 3 N 4 /Graphene (AUG) film based on PDMS film was reported and used as a highly sensitive SERS substrate for the detection of rhodamine 6G (R6G) molecules. The Au@Ag nanosphere array formed by self-assembly provided dense hot-spots, the ultrathin g-C 3 N 4 enabled the composite to possess excellent photocatalytic ability, and the graphene enhanced SERS detection and photocatalytic performance while improving the stability of the composite film . The results showed that the AUG flexible composite film had a detection limit of 10 −12 M for R6G molecules. After 10 photocatalytic cycles of testing, the composite film maintained 83 % of SERS activity. Benefiting from the graphene covering the surface, the composite films showed only a 5 % decrease in SERS detection performance after 30 days of storage in air. The facile fabrication process of AUG composite film enables it to be an outstanding candidate for the flexible, inexpensive, and stable wearable SERS sensing systems.
Sialylated immunoglobulin G (IgG) is a kind of glycoproteins in breast milk with the property of anti-inflammation. Our previous work showed that sialylated IgG could significantly promote the growth of Bifidobacterium in the gut microbiota of healthy volunteers. Nevertheless, whether sialylated IgG can benefit patients with inflammatory bowel disease (IBD) as prebiotics remains unclear. Therefore, its prebiotic effect on the gut microbiota of IBD patients was investigated by in vitro fermentation in this study. The results showed that sialylated IgG could significantly enhance the diversity, richness and composition of gut microbiota in IBD samples compared with non-sialylated IgG. In detail, sialylated IgG not only improved the growth of three common genera ( Romboutsia , Prevotella and Akkermansia ) with low relative abundance in IBD samples but also increased the genera ( Bifidobacterium , Actinomyces , Atopobium and Citrobacter ) with low relative abundance both in healthy and IBD fecal samples. Correspondingly, the contents of short-chain fatty acids for fermentation group of fecal sample from IBD patients with sialylated IgG as the carbon source were higher than those for fermentation group of fecal sample from IBD patients with non-sialylated IgG as the carbon source. In addition, the metabolic pathway results confirmed that sialylated IgG upregulated the functional genes related to hydrolysis , absorption and utilization of carbohydrates . The transcriptome sequencing results further showed that sialylated IgG could induce particular gene expression of Bifidobacterium bifidum to modulate the gut microbiota of IBD patients. Thus, as a kind of natural dietary component, sialylated IgG has potential applications in treating IBD.
A novel g-C 3 N 4 nanosheets (g-C 3 N 4 NSs)-assisted upconversion fluorescent aptasensor was proposed for Staphylococcus aureus ( S. aureus ) detection by adopting hybridization chain reaction (HCR) as a sensitizer. Two hairpin (H1 and H2) structured DNA probes were engineered predicated on the partial complementary sequence (cDNA) of S. aureus aptamer and modified on the exterior of the upconversion nanoparticles (UCNPs), respectively. The presence of S. aureus initiated the HCR system and activated H1 and H2 probes to form a double-helix away from the g-C 3 N 4 NSs vicinity. This led to the decrease in peroxidase-like activity (PA) of the g-C 3 N 4 NSs and corresponding fluorescence recovery proportional to the concentration of S. aureus (10-10 6 cfu mL −1 ). The method was applied to real food samples with acceptable recoveries (91.1–101.6%) and further validated by traditional plate counting method (p > 0.05).
Photocatalytic CO 2 reduction reaction (CO 2 RR) is an effective mean to address the current environmental and energy issues. As a kind of typical photocatalyst, g-C 3 N 4 possesses lots of advantages (i.e . , facile synthesis, visible-light response, and high stability) in CO 2 reduction. However, the poor capacity of CO 2 capture and rapid recombination of photo-generated electron and hole, both hinder the further development of g-C 3 N 4 for CO 2 RR. Herein, we developed a template co-pyrolysis strategy to prepare C–NH x -rich ( x = 1 or 2) g-C 3 N 4 , to increase the CO 2 binding and the subsequent photocatalytic CO 2 reduction efficiency. Specifically, organic molecules with multiple imino groups were used as additives to co-pyrolyze with urea. These additives can act as templates to facilitate the formation of g-C 3 N 4 with abundant C–NH x groups, which effectively improved the capacity of CO 2 capture. Meanwhile, the capacity of light absorption and the separation of photo-generated electron and hole were also optimized. As a result, the obtained C–NH x -rich g-C 3 N 4 showed greatly enhanced photocatalytic activity for CO 2 RR, over 74-fold higher than that of g-C 3 N 4 conventionally prepared. This work provides a new avenue for optimizing the g-C 3 N 4 -based photocatalysts for CO 2 RR.
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