Search Results (1,559)

Carbon monoxide (CO) is a major toxic gas emitted from vehicle exhaust, industrial processes, and incomplete fuel combustion, posing serious environmental and health risks. Catalytic oxidation of CO into less harmful CO₂ is an effective strategy to reduce these emissions. In this study, we investigated the catalytic performance of platinum (Pt) single atoms doped on C₃N monolayers with various vacancy defects, including single carbon (C_V) and nitrogen (N_V) vacancies, using density functional theory (DFT) calculations. Our results demonstrate that Pt@N_V-C₃N exhibited the most favorable catalytic properties, with the highest O₂ adsorption energy (−3.07 eV). This performance significantly outperforms Pt atoms doped at other vacancies. It can be attributed to the strong binding between Pt and nitrogen vacancies, which contributes to its excellent resistance to Pt aggregation. CO oxidation on Pt@N_V-C₃N proceeds via the Eley–Rideal (ER2) mechanism with a low activation barrier of 0.41 eV for the rate-determining step, indicating high catalytic efficiency at low temperatures. These findings suggest that Pt@N_V-C₃N is a promising candidate for CO oxidation, contributing to developing cost-effective and environmentally sustainable catalysts. The strong binding of Pt atoms to the nitrogen vacancies prevents aggregation, ensuring the stability and durability of the catalyst. The kinetic modeling further revealed that the ER2 mechanism offers the highest reaction rate constants over a wide temperature range (273–700 K). The low activation energy barrier also facilitates CO oxidation at lower temperatures, addressing critical challenges in automotive and industrial pollution control. This study provides valuable theoretical insights for designing advanced single-atom catalysts for environmental remediation applications. Full article

Fibrate pharmaceuticals (fibrates), as a widespread class of emerging contaminants, pose potential risks to both ecological systems and human health. The photocatalytic system based on nitrogen (N) and fluorine (F) co-doped TiO₂ nanotube arrays (NF-TNAs) provides a renewable solution for fibrate pharmaceutical removal from water, powered by inexhaustible sunlight. In this study, the degradation of two typical fibrates, i.e., bezafibrate (BZF) and ciprofibrate (CPF), under simulated sunlight irradiation through NF-TNAs were investigated. The photocatalytic degradation of BZF/CPF was achieved through combined radical and non-radical oxidation processes, while the generation and reaction mechanisms of associated reactive oxygen species (ROS) were examined. Electron paramagnetic resonance detection and quenching tests confirmed the existence of h⁺, •OH, O₂^•−, and ¹O₂, with O₂^•− playing the predominant role. The transformation products (TPs) of BZF/CPF were identified through high-resolution mass spectrometry analysis combined with quantum chemical calculations to elucidate the degradation pathways. The influence of co-existing ions and typical natural organic matters (NOM) on BZF/CPF degradation were also tested. Eventually, the ecological risk of BZF/CPF transformation products was assessed through quantitative structure–activity relationship (QSAR) modeling, and the results showed that the proposed photocatalytic system can largely alleviate fibrate toxicity. Full article

Ultra-fine-grained bainitic (UFGB) steels offer excellent mechanical properties, which can be further improved by applying diamond-like carbon (DLC) coatings. However, poor adhesion between the coating and substrate remains a key limitation. Since the steel’s microstructure degrades at high temperatures, enhancing adhesion without heating the substrate is essential. This study investigates surface hardening combined with simultaneous nitrogen and hydrogen doping during the Radio Frequency Chemical Vapor Deposition (RFCVD) process to improve coating performance. Varying gas compositions were tested to assess their effects on coating properties. Nitrogen incorporation decreased hardness from 12 GPa to 9 GPa but improved adhesion, while hydrogen limited damage after coating failure. Optimizing the gas mixture led to enhanced adhesion and wear resistance. Raman and X-ray photoelectron spectroscopy (XPS) analyses confirmed that the optimized coatings had the highest sp³ bond content and elevated nitrogen levels. While both hardness and adhesion contributed to wear resistance, no direct link to coating thickness was found. Overall, co-doping with nitrogen and hydrogen is an effective approach to improve adhesion and wear resistance without requiring high processing temperatures or complex equipment. Full article

100 nm thick TiO₂/TiN bilayers with varying thickness ratios were deposited via reactive sputtering of a Ti target in controlled oxygen and nitrogen atmospheres. Post-deposition annealing in air at 600 °C was performed to induce nitrogen diffusion through the oxygen-deficient TiO₂ layer. The resulting changes in morphology and chemical environment were investigated in detail using transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and UV-Vis spectroscopy. Detailed TEM and XPS analyses have confirmed nitrogen diffusion across the TiO₂ layer, with surface nitrogen concentration and the ratio of interstitial to substitutional nitrogen dependent on the TiO₂/TiN mass ratio. Optical studies demonstrated modifications in optical constants and a reduction of the effective bandgap from 3.2 eV to 2.6 eV due to new energy states introduced by nitrogen doping. Changes in surface free energy induced by nitrogen incorporation showed a correlation to nitrogen doping sites on the surface, which had positive effects on overall photocatalytic activity. Photocatalytic activity, assessed through methylene blue degradation, showed enhancement attributed to nitrogen doping. Additionally, deposition of a 5 nm gold layer on the annealed sample enabled investigation of synergistic effects between nitrogen doping and gold incorporation, resulting in further improved photocatalytic performance. These findings establish the TiO₂/TiN bilayer as a versatile platform for supporting thin gold films with enhanced photocatalytic properties. Full article

In this study, lanthanum–nitrogen co-doped titanium dioxide (La-N-TiO₂) thin films were fabricated using Ion Beam Assisted Deposition (IBAD) and subjected to accelerated ultraviolet (UV) aging experiments to systematically investigate the impact of co-doping on the films’ resistance to UV aging. X-ray diffraction (XRD) analysis revealed that La-N co-doping inhibits the phase transition from anatase to rutile, significantly enhancing the phase stability of the films. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) characterizations indicated that co-doping increased the density and surface uniformity of the films, thereby delaying the expansion of cracks and increase in roughness induced by UV exposure. Energy-dispersive X-ray spectroscopy (EDS) results confirmed the successful incorporation of La and N into the TiO₂ lattice, enhancing the chemical stability of the films. Contact angle tests demonstrated that La-N co-doping markedly improved the hydrophobicity of the films, inhibiting the rapid decay of hydrophilicity during UV aging. After three years of UV aging, the co-doped films maintained high structural integrity and photocatalytic performance, exhibiting excellent resistance to UV aging. These findings offer new insights into the long-term stability of photovoltaic self-cleaning materials. Full article

Aloin, a kind of active phenolic component, is sourced from Aloe vera. Recently, the determination of aloin has received enormous attention, owing to its positive performance (including anti-tumor, antibacterial, detoxification, liver protection, anti-stomach damage, and skin protection activities) and painful side effects (increased carcinogenicity caused by excessive use of aloin) impacting human health. This investigation was inspired by the good fluorescence properties of carbon dots (CDs); CD-based sensors have aroused a great deal of interest due to their excellent sensitivity and selectivity. Thus, it is of great significance to develop novel CD-based sensors for aloin determination. Herein, N,F-CDs were designed and synthesized through a convenient hydrothermal strategy; the synthesized N,F-CDs possessed good fluorescence performance and a small particle size (near 4.3 nm), which demonstrated the successful preparation of N,F-CDs. The resulting N,F-CDs possessed a large Stokes shift and could emit a highly stable green fluorescence. The fluorescence of the N,F-CDs could be effectively quenched by aloin through the inner filter effect. Furthermore, the synthesis procedure was easy to operate. Finally, the N,F-CD-coated test strips were fabricated and combined with a miniaturized fluorimeter for the fluorescence detection of aloin via the inner filter effect for the first time. The N,F-CD-coated test strips were fabricated and used for the fluorescence sensing of aloin, and the results were compared with a typical ultraviolet (UV) method. The N,F-CD-coated test strips exhibited high recovery (96.9~106.1%) and sensitivity (31.8 nM, n = 3), good selectivity, low sample consumption (1 μL), high speed (5 min), good stability, and anti-interference properties. The results indicate that N,F-CD-coated test strips are applicable for the quantitative determination of aloin in bovine serum, orange juice, and urine samples. Full article

The efficient depolymerization of lignin has become a key challenge in the preparation of high-value-added chemicals. Graphitic carbon nitride (g-C₃N₄)-based photocatalytic system shows potential due to its mild and green characteristics over other depolymerization methods. However, its inherent defects, such as a wide band gap and rapid carrier recombination, severely limit its catalytic performance. In this paper, a g-C₃N₄ modification strategy of K⁺ doping and surface alkalinization is proposed, which is firstly applied to the photocatalytic depolymerization of the lignin β-O-4 model compound (2-phenoxy-1-phenylethanol). K⁺ doping is achieved by introducing KCl in the precursor thermal polymerization stage to weaken the edge structure strength of g-C₃N₄, and post-treatment with KOH solution is combined to optimize the surface basic groups. The structural/compositional evolution of the materials was analyzed by XRD, FTIR, and XPS. The morphology/element distribution was visualized by SEM-EDS, and the optoelectronic properties were evaluated by UV–vis DRS, PL, EIS, and transient photocurrent (TPC). K⁺ doping and surface alkalinization synergistically regulate the layered structure of the material, significantly increase the specific surface area, introduce nitrogen vacancies and hydroxyl functional groups, effectively narrow the band gap (optimized to 2.35 eV), and inhibit the recombination of photogenerated carriers by forming electron capture centers. Photocatalytic experiments show that the alkalinized g-C₃N₄ can completely depolymerize 2-phenoxy-1-phenylethanol with tunable product selectivity. By adjusting reaction time and catalyst dosage, the dominant product can be shifted from benzaldehyde (up to 77.28% selectivity) to benzoic acid, demonstrating precise control over oxidation degree. Mechanistic analysis shows that the surface alkaline sites synergistically optimize the C_β-O bond breakage path by enhancing substrate adsorption and promoting the generation of active oxygen species (·OH, ·O₂⁻). This study provides a new idea for the efficient photocatalytic depolymerization of lignin and lays an experimental foundation for the interface engineering and band regulation strategies of g-C₃N₄-based catalysts. Full article

Electrocatalytic urea oxidation reaction (UOR) is a promising dual-purpose approach for hydrogen production and wastewater treatment, addressing critical energy and environmental challenges. However, conventional anode materials often suffer from limited active sites and high charge transfer resistance, restricting UOR efficiency. To overcome these issues, a novel NiP@PNC/NF electrocatalyst was developed via a one-step thermal annealing process under nitrogen, integrating nickel phosphide (NiP) with phosphorus and nitrogen co-doped carbon nanotubes (PNCs) on a nickel foam (NF) substrate. This design enhances catalytic activity and charge transfer, achieving current densities of 50 mA cm⁻² at 1.34 V and 100 mA cm⁻² at 1.43 V versus the reversible hydrogen electrode (RHE). The electrode’s high electrochemical surface area (235 cm²) and double-layer capacitance (94.1 mF) reflect abundant active sites, far surpassing NiP/NF (48 cm², 15.8 mF) and PNC/NF (39.5 cm², 12.9 mF). It maintains exceptional stability, with only a 16.3% performance loss after 35 h, as confirmed by HR-TEM showing an intact nanostructure. Our single-step annealing technique provides simplicity, scalability, and efficient integration of NiP nanoparticles inside a PNC matrix on nickel foam. This method enables consistent distribution and robust substrate adhesion, which are difficult to attain with multi-step or more intricate techniques. Full article

5-Hydroxymethylfurfural (HMF) is a versatile platform molecule with the potential to replace many fossil fuel derivatives. It can be obtained through the dehydration of carbohydrates. In this study, we present a simple and cost-effective microwave-assisted method for producing HMF. This method involves the use of readily available sucrose as a substrate and glucose-derived bifunctional hydrochars as carbocatalysts. These catalysts were produced via hydrothermal carbonisation using thiourea and urea as nitrogen and sulphur sources, respectively, to introduce Brønsted acidic and basic sites into the materials. Using a microwave reactor, we found that the S, N-doped hydrochars were active in sucrose dehydration in water. Catalytic results showed that HMF yield depended on the balance between acidic and basic sites as well as the types of S and N species present on the surfaces of these hydrochars. The best-performing catalyst achieved an encouraging HMF yield of 37%. The potential of N, S-co-doped biochar as a green solid catalyst for various biorefinery processes was demonstrated. A simple kinetic model was developed to elucidate the kinetics of the main reaction pathways of this cascade process, showing a very good fit with the experimental results. The calculated rate constants revealed that reactions with a 5% sucrose loading exhibited significantly higher fructose dehydration rates and produced fewer side products than reactions using a more diluted substrate. No isomerisation of glucose into fructose was observed in an air atmosphere. On the contrary, a limited rate of isomerisation of glucose into fructose was recorded in an oxygen atmosphere. Therefore, efforts should focus on achieving a high glucose-to-fructose isomerisation rate (an intermediate reaction step) to improve HMF selectivity by reducing humin formation. Full article

The simultaneous generation of hydrogen fuel and wastewater remediation via electrocatalytic urea oxidation has emerged as a promising approach for sustainable energy and environmental solutions. However, the practical application of this process is hindered by the limited active sites and high charge-transfer resistance of conventional anode materials. In this work, we introduce a novel CoP@P, N-CNTs/NF electrocatalyst, fabricated through a facile one-step thermal annealing technique. Comprehensive characterizations confirm the successful integration of CoP nanoparticles and phosphorus/nitrogen co-doped carbon nanotubes (P, N-CNTs) onto nickel foam, yielding a unique hierarchical structure that offers abundant active sites and accelerated electron transport. As a result, the CoP@P, N-CNTs/NF electrode achieves outstanding urea oxidation reaction (UOR) performance, delivering current densities of 158.5 mA cm⁻² at 1.5 V and 232.95 mA cm⁻² at 1.6 V versus RHE, along with exceptional operational stability exceeding 50 h with negligible performance loss. This innovative, multi-element-doped electrode design marks a significant advancement in the field, enabling highly efficient UOR and energy-efficient hydrogen production. Our approach paves the way for scalable, cost-effective solutions that couple renewable energy generation with effective wastewater treatment. Full article

Substitutional doping of fullerenes represents a significant category of heterofullerenes. Due to the vast number of isomers, confirming the ground state structure poses considerable challenges. In this study, we generated isomers of C_60−nB_n and C_60−nN_n with n ranging from 2 to 12. To avoid overlooking the ground state structures, we applied specific filtering rules: no adjacent nitrogen (N) or boron (B) atoms are allowed, and substitutions in meta-positions within pentagons are prohibited when the substitution number n exceeds nine. Approximately 15,000 isomers across various values of n within the range of 2 to 12 for B and N substituted fullerenes were selected and optimized using density functional theory (DFT) calculations, forming our dataset. We developed a Graph Neural Network (GNN) that aggregates both topological connections and its dual graph with ring types as input information to predict their binding energies. The GNN achieved high accuracy, reaching a root mean square error (RMSE) of 1.713 meV. Furthermore, it operates efficiently; indeed, it can predict over six thousand isomers per second on an eight-core PC. Several predicted stable structures were further optimized by DFT to confirm their ground state configurations. The energy cutoffs of each composition were determined through statistical simulations to ensure that the selected ground state structures possess high confidence levels. Notably, new lower-energy structures have been discovered for boron-substituted fullerenes with substitution number ranging from seven to twelve and nitride-substituted fullerenes with substitution number ranging from seven to eleven. Full article

This study aimed to investigate the kinetic properties of methylene blue adsorption on carbon cryogel samples and nitrogen-doped and nitrogen-and-sulfur-co-doped carbon cryogel. Nitrogen and sulfur were incorporated into the carbon structure to enhance surface, electronic and textural properties. Methylene blue, a widely utilized dye in the textile industry, has become one of the most commonly detected substances in water systems. Experimental data were fitted with four kinetic models and showed excellent fits with the linear pseudo-second-order model. The results indicated that doping with nitrogen and sulfur did not significantly affect the adsorption of methylene blue. Full article

To address mass transport limitations in carbon nanofiber membrane electrodes for overall water splitting, a self-supporting nitrogen-doped hollow carbon nanofiber membrane embedded with Co/Co₂P heterojunctions (Co/Co₂P-NCNFs-H) was fabricated via continuous coaxial electrospinning. The architecture features uniform hollow channels (200–250 nm diameter, 30–50 nm wall thickness) and a high specific surface area (254 m² g⁻¹), as confirmed by SEM, TEM, and BET analysis. The Co/Co₂P heterojunction was uniformly dispersed on nitrogen-doped hollow carbon nanofibers through electrospinning, leverages interfacial electronic synergy to accelerate charge transfer and optimize the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). Electrochemical tests demonstrated exceptional catalytic activity, achieving current densities of 100 mA cm⁻² at ultralow overpotentials of 405.6 mV (OER) and 247.9 mV (HER) in 1.0 M KOH—surpassing most reported transition metal catalysts for both half-reactions. Moreover, the electrode exhibited robust long-term stability, maintaining performance for nearly 20 h at 0.6 V (vs. Ag/AgCl) (OER) and over 250 h at −1.5 V (vs. Ag/AgCl) (HER), attributed to the mechanical integrity of the hollow architecture and strong metal–carbon interactions. This work demonstrates that integrating hollow nanostructures (enhanced mass transport) and heterojunction engineering (optimized electronic configurations) creates a scalable strategy for designing efficient bifunctional catalysts, offering significant promise for sustainable hydrogen production via water electrolysis. Full article

The fundamental chemistries and electronic structures of platinum catalysts over nitrogen-doped carbon supports were examined to determine the subtle yet important roles graphitic defect-based and pyridinic defect-based nitrogen defects have in stabilizing platinum. These roles address and extend previously gathered incomplete knowledge of how combinations of graphitic defect and pyridinic defect affect the local electronic structure, leading to a greater unified understanding of platinum stability. A theoretical study was designed where different atomically sized platinum clusters were investigated over seven different nitrogen defect combinations on graphene carbon support. Differently sized platinum clusters offered parametric insights into the differences in metal–support interactions. Full article

Developing efficient and durable electrocatalysts for the alkaline hydrogen evolution reaction (HER) is crucial for sustainable hydrogen production. Herein, we report a novel RuP₂/Mn₂P₂O₇ heterojunction anchored on a three-dimensional nitrogen and phosphorus co-doped porous carbon (RuP₂/Mn₂P₂O₇/NPC) framework as a high-performance HER catalyst, synthesized via a controlled pyrolysis–phosphidation strategy. The heterostructure achieves uniform dispersion of ultrafine RuP₂/Mn₂P₂O₇ heterojunctions with well-defined interfaces. Furthermore, phosphorus doping restructures the electronic configuration of Mn and Ru species at the RuP₂/Mn₂P₂O₇ heterointerface, enabling enhanced catalytic activity through the accelerated electron transfer and kinetics of the HER. This RuP₂/Mn₂P₂O₇/NPC catalyst exhibits exceptional HER activity with 1 M KOH, requiring only 69 mV of overpotential to deliver 10 mA·cm⁻² and displaying a small Tafel slope of 69 mV·dec⁻¹, rivaling commercial 20% Pt/C. Stability tests reveal negligible activity loss over 48 h, underscoring the robustness of the heterostructure. The RuP₂/Mn₂P₂O₇ heterojunction demonstrates markedly reduced overpotentials for the electrochemical HER process, highlighting its enhanced catalytic efficiency and improved cost-effectiveness compared to the conventional catalytic systems. This work establishes a strategy for designing a transition metal phosphide heterostructure through interfacial electronic modulation, offering broad implications for energy conversion technologies. Full article