Search Results (127)

Constructing a heterojunction is considered one of the most effective strategies for enhancing photocatalytic activity. Herein, we employ Ta₃N₅ and tubular graphitic carbon nitride (TCN) to construct a Ta₃N₅/TCN van der Waals heterojunction via electrostatic self-assembly for enhanced photocatalytic H₂ production. SEM and TEM results show that Ta₃N₅ particles (~300 nm in size) are successfully anchored onto the surface of TCN. The light absorption capability of the Ta₃N₅/TCN heterojunction is between those of Ta₃N₅ and TCN. The strong interaction between Ta₃N₅ and TCN with different energy structures (Fermi levels) by van der Waals force renders the formation of an interfacial electric field to drive the separation and transfer of photogenerated charge carriers in the Ta₃N₅/TCN heterojunction, as evidenced by the photoluminescence (PL) and photoelectrochemical (PEC) characterization results. Consequently, the optimal Ta₃N₅/TCN heterojunction exhibits a remarkable H₂ production rate of 12.73 mmol g⁻¹ h⁻¹ under visible light irradiation, which is 3.3 and 16.8 times those of TCN and Ta₃N₅, respectively. Meanwhile, the cyclic experiment demonstrates excellent stability of the Ta₃N₅/TCN heterojunction upon photocatalytic reaction. Notably, the photocatalytic performance of 15-TaN/TCN outperforms the most previously reported CN-based and Ta₃N₅-based heterojunctions for H₂ production. This work provides a new avenue for the rational design of CN-based van der Waals heterojunction photocatalysts with enhanced photocatalytic activity. Full article

The electrochemical reduction of carbon monoxide (COER) offers a promising route for generating value-added multi-carbon (C₂₊) products, such as ethanol, but achieving high catalytic performance remains a significant challenge. Herein, we performed comprehensive density functional theory (DFT) computations to evaluate CO-to-ethanol conversion on single metal atoms anchored on graphitic carbon nitride (TM/g–CN). We showed that these metal atoms stably coordinate with edge N sites of g–CN to form active catalytic centers. Screening 20 TM/g–CN candidates, we identified V/g–CN and Zn/g–CN as optimal catalysts: both exhibit low free-energy barriers (<0.50 eV) for the key ^*CO hydrogenation steps and facilitate C–C coupling via an Eley–Rideal mechanism with a negligible kinetic barrier (~0.10 eV) to yield ethanol at low limiting potentials, which explains their superior COER performance. An analysis of d-band centers, charge transfer, and bonding–antibonding orbital distributions revealed the origin of their activity. This work provides theoretical insights and useful guidelines for designing high-performance single-atom COER catalysts. Full article

Visible-light-driven photocatalytic hydrogen production is one of the ideal green technologies for solar-to-chemical energy conversion. Carbon nitride (C₃N₄, CN) has been attracting extensive attention for its suitable band structure and stability, but the efficiency of photocatalytic hydrogen evolution is low due to insufficient visible-light absorption and rapid charge recombination. Herein, we develop a novel (F, K)-co-doped CN (FKCN) catalyst via a facile thermal polymerization approach using KOH-modified melamine and NH₄F as the dopant precursors. The FKCN catalyst demonstrates broadened light absorption, significantly enhanced charge separation, and excellent cyclic stability. And the optimal F_(0.15)K₍₆₎CN catalyst achieves a hydrogen evolution rate of as high as 3101.5 μmol g⁻¹ h⁻¹ (12-fold that of pristine CN) under visible-light irradiation (λ ≥ 420 nm), which is among the best element-doped CN photocatalysts. This work highlights the effectiveness of a multi-element doping strategy in designing CN-based photocatalysts for efficient hydrogen evolution. Full article

Heterogeneous photocatalysis has emerged in recent years as a promising and sustainable decontamination method. However, several drawbacks limit the effective usage of this process up to date, such as photocatalysts’ limited properties, difficulty in modifying and improving their properties, as well as the environmental impact and cost associated with the use of the metals on which conventional photocatalysts are based. Graphitic carbon nitride (gCN), a new carbon-based photocatalyst, offers the possibility of easy modification and improvement of their properties. There are several strategies to improve the properties of these derivatives, such as increasing the surface area (modifying morphology into 0D, 1D, 2D, or porous structures), increasing the absorption in the visible (doping), and improving the separation and mobility of photogenerated charges (introducing defects, vacancies, functional groups, and doping). In this review, a compilation of these modifications, the associated improvements in its properties, and its derivatives was carried out with focus on the degradation of emerging pollutants (EPs). The property modifications enhance their behavior and efficiency of degradation, all in a cheaper and more sustainable way. Thus, improved gCN derivatives offer real possibilities for the upscaling of heterogeneous photocatalytic processes as an effective alternative for decontaminating water bodies. Full article

The development of photothermal-assisted photocatalytic systems with broad-spectrum solar utilization and high charge separation efficiency remains a critical challenge for antibiotic degradation. Herein, we report novel black g-C₃N₄ (BCN) materials synthesized via a one-step thermal copolymerization strategy using C/N precursors and tetrachlorofluorescein. After the introduction of tetrachlorofluorescein, the color of the sample changes, which gives BCN enhanced light absorption and a significant photothermal effect for poorly heating-assisted photocatalysis. The synergistic coupling of photothermal and photocatalytic processes enabled the optimal BCN-U sample to achieve exceptional degradation efficiency (89% within 120 min) for a typical antibiotic (e.g., tetracycline) under an LED lamp as the visible light source, outperforming conventional yellow g-C₃N₄ (YCN-U) by a factor of 1.37. Mechanistic studies revealed that the photothermal effect facilitates carrier separation via thermal-driven electron excitation while accelerating reactive oxygen species (•OH and •O₂⁻) generation. The synergistic interplay between photocatalysis and photothermal effects, which improved mass transfer, ensures robust stability, which provides new insights into designing dual-functional carbon nitride-based materials for sustainable environmental remediation. Full article

We combined atomistic simulations and experiments to assess the photocatalytic potential of the rutile phase of ${\mathrm{TiO}}_2$ combined with phenyl-modified carbon nitride (PhCN). Density Functional Tight Binding (DFTB) calculations predict favorable adhesion properties and type-II band alignment, crucial for efficient charge separation between PhCN and rutile TiO₂ surfaces. These theoretical predictions are validated experimentally: structural (XRD and Raman) and optical characterizations confirm the successful formation of a PhCN/rutile hybrid and indicate beneficial electronic interactions. Importantly, photocatalytic tests under visible light reveal significant degradation activity, confirming that the computationally predicted synergistic effects render the PhCN/rutile system a promising, potentially greener alternative to traditional anatase-based photocatalysts. Full article

With the annual increase in carbon emissions and the warming of the global temperature, it is imperative to accelerate the construction of a green, low-carbon, circular economic system. The photocatalytic reduction of CO₂ can convert the emitted CO₂ into valuable carbonaceous products, which is of great significance for alleviating the global CO₂ emission problem. In this study, the literature on the “photocatalytic reduction of CO₂” from two Chinese and foreign databases was used as the analysis sample. From the perspective of net present value, nitride-based catalysts were selected as the research object. An in-depth analysis of the costs and economic benefits of the nitride-based photocatalytic reduction of CO₂ was carried out, considering four factors: catalyst efficiency, light conditions, discount rate, and depreciation period. The analysis results show that with a project duration of 10 years and a discount rate of 10%, the net present values of all the catalysts are negative, indicating that from an economic perspective, investment projects using general catalysts to reduce CO₂ are not feasible under current conditions. However, it is worth noting that when the light conditions are changed and sunlight is used as the light source, the net present values corresponding to the Ta₃N₅/Bi and NiOx/Ta₃N₅ catalysts have turned positive, showing a certain economic feasibility. When the yield is increased to 2.64 times and 6.15 times of the original values, the net present values corresponding to the T-CN/ZIS (refers to ZnIn₂S₄ (ZIS) nanosheets grown in situ on tubular g-C₃N₄ microtubes (T-CNs)) catalyst and the Ta₃N₅ cuboid catalyst turn positive, and only the net present value of the g-C₃N₄/Bi₂O₂[BO₂(OH)] catalyst remains negative. Full article

The removal of polychlorinated dibenzo-p-dioxins (PCDDs) via advanced oxidation processes (AOPs) poses a significant challenge due to their high toxicity and chemical stability. In this study, a series of well-dispersed cobalt nanoparticles supported on carbon nitrides (xCoCNs) was synthesized to activate peroxymonosulfate (PMS) for 2,8-dichlorodibenzo-p-dioxin (2,8-DCDD) degradation under visible light. The catalysts prepared were characterized using SEM, XPS, photoluminescence (PL), and UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS). Among them, 2CoCN with an optimal Co content exhibited the highest photocatalytic efficiency, achieving 90.5% degradation of 2,8-DCDD within 160 min under visible light/persulfate oxidation (Vis+PMS+2CoCN system). Compared with other catalysts, 2CoCN exhibited superior optical performance and a narrower bandgap, enabling efficient excitation under visible light (Vis). Notably, all xCoCNs demonstrated pH adaptability, achieving complete degradation of 2,8-DCDD under neutral conditions (pH = 7) without additional acid/alkali adjustment. Through rigorous free radical capture experiments, it was demonstrated that SO₄^•−, ^•OH and ¹O₂ were the primary reactive oxygen species (ROS) in the Vis+PMS+2CoCN system. The catalyst exhibited excellent reusability, with stable activity retained over five cycles. Based on these findings, degradation pathways and mechanisms of 2,8-DCDD in the 2CoCN+Vis+PMS system were proposed. This study presents an effective approach for PCDD abatement in wastewater treatment applications. Full article

The use of solar energy to convert CO₂ into value-added chemicals is a promising sustainable development strategy. In this study, a black graphitic carbon nitride (CN-B) photocatalyst was fabricated through a single-step calcination process, employing phloxine B and urea as the precursor materials. The catalysts were characterized using TEM, XRD, FTIR, XPS and so on. The amount of prepolymer phloxine B was 25 mg, 35 mg and 45 mg, respectively, and the obtained samples were CN-B-0.025, CN-B-0.035 and CN-B-0.045. All samples were used for visible-catalyzed CO₂ reduction. The experimental findings indicate that the CO evolution rate of the optimal photocatalyst CN-B-0.035 reaches 27.56 μmol g_cat.⁻¹ h⁻¹. This value is nine-fold higher than that of pure CN, which has a CO evolution rate of 3.22 μmol g_cat.⁻¹ h⁻¹. The excellent photocatalytic reduction performance is due to the following factors: Firstly, the exceedingly thin nanosheet structure of the catalyst enhances the velocity of the charge transfer, and transmission electron microscopy (TEM) analysis shows that the nanosheet thickness of the catalyst CN-B is significantly thinner. Secondly, the light absorption capacity of the catalyst is enhanced. The absorbance of CN-B increases significantly in the ultraviolet region and extends to the near-infrared region, as shown with UV diffuse reflection spectroscopy. Finally, the photothermal effect of CN-B causes the catalyst temperature to rise rapidly from 20 °C to 131 °C within 120 s, which further promotes photogenerated carrier separation. This research offers a novel approach to the development of photocatalysts aimed at the photothermal-assisted photocatalytic conversion of CO₂. Full article

Sulfur hexafluoride (SF₆), the strongest greenhouse gas, has great challenges in degradation because of its stable structure, posing significant environmental concerns. Photocatalysis offers an environmentally friendly, low-energy solution, but the fluoride deposition on catalysts reduces their activity, thus limiting their large-scale application. To prevent catalyst fluoride poisoning, we report a thin-layer graphitic carbon nitride (CN) material loaded with MoO_x (CNM) that resists fluoride deposition for long-term SF₆ degradation. By combining molecular structure design and nanostructure regulation, we construct a photocatalyst with enhanced charge carrier mobility and reduced transport distances. We find that the CNM exhibits a high specific surface area, increased contact between reactants and active sites, and efficient electron–hole separation due to the Mo-N bonds, achieving an SF₆ degradation efficiency of 1.73 mmol/g after one day due to the prolonged catalytic durability of the catalyst, which is eight times higher than pristine g-C₃N₄ (0.21 mmol/g). We demonstrate the potential of CNMs for low-energy, high-efficiency SF₆ degradation, offering a new approach to mitigate the environmental impact of this potent greenhouse gas. We envision that this study will inspire further research into advanced photocatalytic materials for environmental remediation, contributing to global efforts in combating climate change. Full article

Graphite-phase carbon nitride (CN) has the advantages of high stability, non-toxicity, and harmlessness in degrading antibiotic pollutants in water. How to achieve the reduction of its electron-hole complexation efficiency as well as the improvement of its recyclability, while at the same time ensuring these advantages, is the focus of this paper. In this study, modified magnetic particles selected from coal gasification slag were used as carriers, which were compounded with CN and then subjected to a simple roasting process to obtain composite magnetic photocatalysts (MCN) with different ratios. The introduction of porous magnetic carriers increased the specific surface area of MCN, provided more active sites, and effectively improved the migration ability and redox capacity of CN carriers. Among them, 50% MCN showed excellent photodegradation performance, and the removal rate of tetracycline reached 82% within 60 min, which was much higher than that of CN. 50% MCN has a saturated magnetisation intensity of 1.55 emu·g⁻¹, which can be regenerated after recycling using a magnetic field, and the degradation efficiency of tetracycline is still more than 70% after five cycles, indicating that 50% MCN has good stability. This work demonstrates that magnetic gasification slag as a modified carrier can effectively promote the separation of photogenerated electron-hole pairs of graphite-phase carbon nitride, which provides a reference for the resourceful utilisation of coal gasification slag, as well as for the construction of g-C₃N₄-based photocatalysts with highly efficient and stable photodegradation activity. This work exemplifies how waste-derived materials can advance photocatalyst design, addressing both efficiency and sustainability challenges in water treatment. Full article

The periodical distribution of N and C atoms in carbon nitride (CN) not only results in localized electrons in each tri-s-triazine unit, but oxidation and reduction sites are in close contact spatially, resulting in severe carrier recombination. Herein, the hydrothermal method was first employed to synthesize carbon nitride (HCN), and then picolinamide (Pic) molecules were introduced at the edge of the carbon nitride so that the photo-generated electrons of the whole structure of the carbon nitride system were transferred from the center to the edge, which effectively promoted the separation of photo-generated carriers and inhibited the recombination of carriers in the structure. The introduced picolinamide not only changed the π-conjugated structure of the entire system but also acted as an electron-withdrawing group to promote charge transfer. The photocatalytic hydrogen evolution rate (HER) of the optimized HCN-Pic-1:1 sample could reach 918.03 μmolg⁻¹ h⁻¹, which was 11.8 times higher than that of the HCN, and the performance also improved. Full article

The peroxymonosulfate (PMS)-assisted photocatalytic process has shown considerable potential for the treatment of wastewater. g-C₃N₄-based catalysts are widely applied to eliminate organic pollutants in wastewater. However, the bulk catalyst prepared by dicyandiamide has the drawback of a low surface area (10 m²/g), while the porous catalyst prepared by urea suffers from a low catalyst yield based on urea (3.5%). To address these challenges, a porous V-doped carbon nitride (V/CN) was designed through one-step thermal polymerization using urea and dicyandiamide as the carbon nitride precursor and NH₄VO₃ as the V precursor. When the ratio of urea to dicyandiamide was 10:1, the yield of V/CN was improved, while it maintained a rich porous structure with a specific surface area (64.6 m²/g). The synergetic effect of V doping and nanosheet and hollow tubular structures facilitated the separation of photogenerated carriers, leading to boosting the photocatalytic activity of g-C₃N₄ in the PMS system. V/CN(10:1) could completely degrade CBZ within 20 min, exhibiting an equivalent catalytic efficiency comparable to that of V/CN prepared by urea (V/UCN), while markedly surpassing both V/DCN and CN prepared by urea alone (UCN) in performance. This study presents an economical and effective approach for the photocatalytic degradation of pharmaceutical pollutants in aquatic environments. Full article

The photocatalytic CO₂ reduction (PCR) into value-added fuels offers a promising solution to energy shortages and the greenhouse effect, thanks to the mild conditions and environmental sustainability. However, the activation of CO₂ is challenging because of the thermodynamic stability and chemical inertness of CO₂ molecules, which significantly restricts the efficiency of PCR. Cobalt carbonate hexahydrate (CCH), known for its excellent CO₂ adsorption and activation properties, faces challenges like poor electron–hole separation and photoresponse. To address these issues, graphitic carbon nitride (CN) as a “pseudo-sensitizer” was introduced into the system by an in situ heterojunction synthesis strategy to produce CCH/CN photocatalyst, where Co–N bonds formed between CCH and CN enhance charge carrier migration and lower interfacial resistance. The CCH/CN catalyst achieved a CO production rate of 19.65 μmol g⁻¹ h⁻¹, outperforming CCH, CN, and a mechanically mixed sample (Mix) by 7.74, 2.31, and 1.77 times, respectively. This work demonstrates an effective strategy for designing heterojunction catalysts to improve visible light utilization and charge transfer for efficient CO₂ reduction. Full article

Photodynamic therapy (PDT) holds considerable promise for advancing anticancer treatment, owing to its precision and minimally invasive nature. In this study, we successfully synthesized a series of titanium carbide (Ti₃C₂, TC)/graphitic carbon nitride (g-C₃N₄, CN) nanocomposite through a synergistic approach combining electron beam irradiation and 2D/2D composite formation. According to the results, 1TC/200-CN (1TC, which TC was 1, referred to the mass ratio; 200-CN, which CN was 200 kGy, referred to the irradiation metering) displayed a 94% degradation rate of methylene blue (10 mg/L) in 100 min. Furthermore, the proliferation rate of CAL-27 cells was suppressed to just 23.3% at a concentration of 320 μg/mL of 1TC/200-CN. Notably, the group treated with this concentration exhibited the largest residual scratch area, accompanied by a notable decrease in mitochondrial membrane potential. These enhanced effects were attributed to the efficient transfer of electron-hole pairs facilitated by the TC/CN composite. Our findings not only contribute to the development of efficient and stable nanocomposites for PDT applications but also provide valuable insights into the utilization of nanomaterials in the biomedical field, thereby paving the way for potential breakthroughs in cancer treatment. Full article