Insights on the efficiency and contribution of single active species in photocatalytic degradation of tetracycline: Priority attack active sites, intermediate products and their toxicity evaluation.

Photocatalysis has been proven to be an excellent technology for treating antibiotic wastewater, but the impact of each active species involved in the process on antibiotic degradation is still unclear. Therefore, the S-scheme heterojunction photocatalyst Ti3C2/g-C3N4/TiO2 was successfully synthesized using melamine and Ti3C2 as precursors by a one-step calcination method using mechanical stirring and ultrasound assistance. Its formation mechanism was studied in detail through multiple characterizations and work function calculations. The heterojunction photocatalyst not only enabled it to retain active species with strong oxidation and reduction abilities, but also significantly promoted the separation and transfer of photo-generated carriers, exhibiting an excellent degradation efficiency of 94.19 % for tetracycline (TC) within 120 min. Importantly, the priority attack sites, degradation pathways, degradation intermediates and their ecological toxicity of TC under the action of each single active species (·O2-, h+, ·OH) were first positively explored and evaluated through design experiments, Fukui function theory calculations, HPLC-MS, Escherichia coli toxicity experiments, and ECOSAR program. The results indicated that the preferred attack sites of ·O2- on TC were O20, C7, C11, O21, and N25 atoms with high f+ value. The toxicity of intermediates produced by ·O2- was also lower than those produced by h+ and ·OH.

Adsorption-enhanced photocatalytic property of Ag-doped biochar/g-C3N4/TiO2 composite by incorporating cotton-based biochar.

In this study, the biochar obtained from waste cotton fibers was introduced into the Ag-doped g-C3N4/TiO2 hybrid composite through a facile one-step hydrothermal process. The morphology, elemental composition, crystal structure, microstructure, specific surface area, chemical bonding state, energy band structure, and separation efficiency of photoinduced charge carriers of the resultant composite were examined using scanning electron microscope, energy dispersive X-ray spectrometer, X-ray diffractometer, transmission electron microscope, surface area analyzer, X-ray photoelectron spectroscope, Ultraviolet-visible spectrophotometer, ultraviolet photoelectron spectroscope, and photoluminescence spectroscope. The adsorption isotherms, kinetics and thermodynamics of the biochar, Ag-doped g-C3N4/TiO2 and Ag-doped biochar/g-C3N4/TiO2 were evaluated using the model methyl orange dye. The photoacatalytic degradation of the model pollutants including methyl orange, methylene blue, congo red, and tetracycline hydrochloride and the photocatalytic reduction of Cr(VI) ions were also assessed under visible light. Experimental results indicated that the photocatalytic property of the Ag-doped biochar/g-C3N4/TiO2 was significantly enhanced through the adsorption enhancement compared with the Ag-doped g-C3N4/TiO2. This was due to the uniform doping of multi-scale porous biochar with g-C3N4 nanosheet, Ag and TiO2 nanoparticles. The adsorptive enhancement induced by the biochar resulted in the narrowed band gap, suitable electronic energy band structure, and fast separation of photoinduced charge carriers of the Ag-doped biochar/g-C3N4/TiO2, which was probably due to the coexistence of multi-valence Ti+4/+3 and Ag0/+1 species and oxygen-containing groups of biochar. The major reactive species of the Ag-doped biochar/g-C3N4/TiO2 were 1O2 and h+. The MO dye adsorption onto the Ag-doped biochar/g-C3N4/TiO2 followed the Langmuir isotherm model, pseudo-first-order and pseudo-second-order kinetic models, and the adsorption process was an endothermic reaction with entropy reduction effects. As such, the Ag-doped biochar/g-C3N4/TiO2 exhibited a promising application for the treatment of wastewater containing multi-pollutants especially organic dyes and heavy metal ions.

Synergistic adsorption and kinetic studies of heterostructured g-C3N4/TiO2 nano-photocatalyst under visible light for enhanced CO2 reduction.

Graphitic carbon nitride (g-C3N4) and titanium dioxide (TiO2) were synthesized using sol-gel and ultrasonic impregnation technique followed by calcination for photocatalytic CO2 reduction. The nano-photocatalysts were analyzed for their morphological, structural, and optical characteristics. Scanning electron microscopy (SEM) revealed the presence of spherical and layered sheet-like nanoparticles, as well as the occurrence of minor aggregations. The ultraviolet-visible spectroscopy (UV-vis) revealed that g-C3N4 has good photocatalytic properties with a medium band gap (2.7 eV), and TiO2 has high charge transfer potentials, robust oxidation properties, and high band gap (3.20 eV). However, the larger band gap makes it unresponsive in the visible light spectrum. In order to circumvent this constraint, a hybrid heterostructured g-C3N4/TiO2 catalyst with different compositions, viz., 1:1, 1:2, and 2:1, were fabricated using the ultrasonic impregnation technique followed by calcination process. The optical band gap of g-C3N4/TiO2 nanocomposite shows a red shift towards 2.85 eV from 3.20 eV for bare TiO2, inferring enhanced absorption in the visible light region. Further, the photocatalytic experiments were performed using visible light sources for all the catalysts. The g-C3N4/TiO2 (2:1) reported higher photocatalytic activity due to its reduced crystallite size of 12.94 nm which were investigated using X-ray diffraction analysis (XRD) and lower band gap of 2.85 eV. The study infers that hybrid photocatalyst enhances the visible light absorption, electron-hole (e - /h +) pair separation rate, and photocatalytic reduction of CO2. In addition, two adsorption models Langmuir and Freundlich were used and adsorption kinetic data were fitted to pseudo-first-order reaction for all the five catalysts. The adsorption isotherm of CO2 by g-C3N4/TiO2 (2:1) well fitted by the Freundlich adsorption equation. On the basis of adsorption magnitude (n) values (1.74), it was found that the interaction between CO2 molecules and g-C3N4/TiO2 occurs according to the chemisorption mechanism. The kinetic study infers that the highest value of apparent rate constant (kapp) was exhibited by g-C3N4/TiO2 (2:1), which indicates that the products predominate at equilibrium.

Spatial Separation of Cocatalysts on Z-Scheme Organic/Inorganic Heterostructure Hollow Spheres for Enhanced Photocatalytic H2 Evolution and In-Depth Analysis of the Charge-Transfer Mechanism.

A Z-scheme heterojunction with spatially separated cocatalysts is proposed for overcoming fundamental issues in photocatalytic water splitting, such as inefficient light absorption, charge recombination, and sluggish reaction kinetics. For efficient light absorption and interfacial charge separation, Z-scheme organic/inorganic heterojunction photocatalysts are synthesized by firmly immobilizing ultrathin g-C3 N4 on the surface of TiO2 hollow spheres via electrostatic interactions. Additionally, two cocatalysts, Pt and IrOx , are spatially separated along the Z-scheme charge-transfer pathway to enhance surface charge separation and reaction kinetics. The as-prepared Pt/g-C3 N4 /TiO2 /IrOx (PCTI) hollow sphere photocatalyst exhibits an exceptional H2 evolution rate of 8.15 mmol h-1 g-1 and a remarkable apparent quantum yield of 24.3% at 330 nm in the presence of 0.5 wt% Pt and 1.2 wt% IrOx cocatalysts on g-C3 N4 and TiO2 , respectively. Photoassisted Kelvin probe force microscopy is used to systematically analyze the Z-scheme charge-transfer mechanism within PCTI. Furthermore, the benefits of spatially separating cocatalysts in the PCTI system are methodically investigated in comparison to randomly depositing them. This work adequately demonstrates that the combination of a Z-scheme heterojunction and spatially separated cocatalysts can be a promising strategy for designing high-performance photocatalytic platforms for solar fuel production.

Constructing Z-scheme g-C3N4/TiO2 heterostructure for promoting degradation of the hazardous dye pollutants.

The use of dyes and segments has increased widely in recent years, but it poses a serious health risk to ecosystems. In this work, TiO2 and two-dimensional g-C3N4 nanosheets (g-CN) were fabricated through co-precipitation and thermal polymerization technique, respectively. The g-CN-TiO2 photocatalyst (1: 3, 2: 2, 3: 1) in various weight percentages was prepared using a simple impregnation process. The photocatalytic behaviour of the g-CN, TiO2 NPs, and different weight percentages of g-CN-TiO2 photocatalyst was evaluated against methylene blue (MB) dye under UV-visible light illumination. Compared to pristine and other weight percentages of the g-CN-TiO2 nanocomposite, the optimized g-CN-TiO2 nanocomposite (3:1) showed promoted performance against MB dye. The enriched catalytic efficiency can be accredited to the low amount of TiO2 nanoparticles deposited on gCN nanosheets, possibly due to the boosted transport properties of the electron-hole pairs. The enriched photocatalytic behaviour can be attributed to the development of the Z-scheme system between TiO2 and g-CN. The current study is an outstanding demonstration of the development of maximum catalytic efficiency for destroying hazardous chemical dyes.

Degradation of sulfamethoxazole and antibiotic resistance genes from surface water in the photocatalyst-loading bionic ecosystems.

The behavior and removal of sulfamethoxazole (SMX) and 3 typical corresponding antibiotic resistance genes (ARGs) including sul1, sul2, sul3, and 16S rDNA in surface water were investigated in the photocatalyst-loading bionic ecosystems (PCBEs). Synthesized composite photocatalyst g-C3N4/TiO2 showing higher catalytic activity than Fe/g-C3N4/TiO2 was selected in the PCBEs. Five PCBEs, i.e., A-the control (without bionic grass or photocatalyst), B-bionic grass loaded with 4.12 g/m2 g-C3N4/TiO2, C-bionic grass loaded with 8.25 g/m2 g-C3N4/TiO2, D-bionic grass loaded with 12.37 g/m2 g-C3N4/TiO2, and E-bionic grass loaded with 16.5 g/m2 g-C3N4/TiO2 were constructed and operated in a medium-scale running cyclical flume. SMX could be photolyzed efficiently by g-C3N4/TiO2 with an optimal unit load on the bionic grass of 12.37 g/m2. 3-amino-5-methylisooxazole and p-aminobenzene sulfonamide were selected as main intermediates through the analyses of SMX degradation mechanisms and pathways, and detected in the aqueous phase and bionic grass. The intermediates were higher in the underwater part of the bionic grass than the above-water part. The overall removal of SMX ranged from 31.7 % to 82.3 % in 5 PCBEs, and the removal of sul1and sul2 were 0.2 %- 62.9 % in the aqueous phase and 8.4 %-63.2 % in the sediment. PCBE D might be the best construction when SMX and ARGs' removal was considered comprehensively. Moreover, the microbial structures showed Proteobacteria as the most dominant bacterial species had a relative abundance of 22.2 %-26.6 % and 33.4 %-68.2 % in the aquatic phase and sediment respectively, illustrating that the removal of the antibiotic and ARGs was bound up with the variations of dominant bacteria in the ecosystems. The findings illustrated that ecosystems with bionic grass and photocatalysts could be a promising technology for the removal of typical antibiotics and ARGs from surface water.

Microwave Synthesis of Visible-Light-Activated g-C3N4/TiO2 Photocatalysts.

The preparation of visible-light-driven photocatalysts has become highly appealing for environmental remediation through simple, fast and green chemical methods. The current study reports the synthesis and characterization of graphitic carbon nitride/titanium dioxide (g-C3N4/TiO2) heterostructures through a fast (1 h) and simple microwave-assisted approach. Different g-C3N4 amounts mixed with TiO2 (15, 30 and 45 wt. %) were investigated for the photocatalytic degradation of a recalcitrant azo dye (methyl orange (MO)) under solar simulating light. X-ray diffraction (XRD) revealed the anatase TiO2 phase for the pure material and all heterostructures produced. Scanning electron microscopy (SEM) showed that by increasing the amount of g-C3N4 in the synthesis, large TiO2 aggregates composed of irregularly shaped particles were disintegrated and resulted in smaller ones, composing a film that covered the g-C3N4 nanosheets. Scanning transmission electron microscopy (STEM) analyses confirmed the existence of an effective interface between a g-C3N4 nanosheet and a TiO2 nanocrystal. X-ray photoelectron spectroscopy (XPS) evidenced no chemical alterations to both g-C3N4 and TiO2 at the heterostructure. The visible-light absorption shift was indicated by the red shift in the absorption onset through the ultraviolet-visible (UV-VIS) absorption spectra. The 30 wt. % of g-C3N4/TiO2 heterostructure showed the best photocatalytic performance, with a MO dye degradation of 85% in 4 h, corresponding to an enhanced efficiency of almost 2 and 10 times greater than that of pure TiO2 and g-C3N4 nanosheets, respectively. Superoxide radical species were found to be the most active radical species in the MO photodegradation process. The creation of a type-II heterostructure is highly suggested due to the negligible participation of hydroxyl radical species in the photodegradation process. The superior photocatalytic activity was attributed to the synergy of g-C3N4 and TiO2 materials.

Light-Activated Interface Charge-Alternating Interaction on an Extended Gate Photoelectrode: A New Sensing Strategy for EGFET-Based Photoelectrochemical Sensors.

Integration of extended gate field-effect transistors (EGFET) and photoelectrochemical (PEC) measurement to construct highly sensitive sensors is an innovative research field that was proven feasible by our previous work. However, it remains a challenge on how to adjust the interaction between the extended gate and the analyte and study its influence on EGFET-based PEC sensors. Herein, a new sensing strategy was proposed by a mutual electrostatic interaction. Three-dimensional TiO2 and g-C3N4 core-shell heterojunction on flexible carbon cloth (TCN) was designed as the extended sensing gate. Tetracycline (TC) was also used as a model analyte, and it contains electron-donating groups (-NH2 and -OH) with negative charge. The designed TCN-extended sensing gate was negatively charged in the dark by introducing carbon vacancies with oxygen doping in the g-C3N4 shell, while it was positively charged under illustration due to the aggregation of photogenerated holes on the surface. Therefore, a light-activated PEC sensing platform for the sensitive and selective determination of tetracycline (TC) was demonstrated. Such a PEC sensor exhibited wide linear ranges within 100 pM to 1 µM and 1-100 µM with a low detection limit of 0.42 pM. Furthermore, the sensing platform possessed excellent selectivity, good reproducibility, and stability. The proposed sensing strategy in this work can expand the paradigm for developing a light-regulated FET-based PEC sensor by mutual electrostatic interaction, and we believe that this work will offer a new perspective for the design of interface interaction in PEC devices.

In situ synthesis of g-C3N4/TiO2 heterojunction by a concentrated absorption process for efficient photocatalytic degradation of tetracycline hydrochloride.

The construction of heterojunctions between semiconductors is a preferred route to improve overall photocatalytic activity. In this work, a facile and feasible method was innovatively developed to one-step prepare g-C3N4/TiO2 heterojunctions via an absorption-calcination process using nitrogen and titanium precursors directly. This method can effectively avoid interfacial defects and establish a tight interfacial connection between g-C3N4 and TiO2. The resultant g-C3N4/TiO2 composites exhibited prominent photodegradation efficiency for tetracycline hydrochloride (TC-HCl) under visible light and simulated-sunlight irradiation. The optimal g-C3N4/TiO2 composite (urea content of 4 g) showed the highest photocatalytic efficiency, which can degrade 90.1% TC-HCl under simulated-sunlight irradiation within 30 min, achieving 3.9 and 2 times increases compared to pure g-C3N4 and TiO2, respectively. Besides, photodegradation pathways based on the role of active species ·O2- and ·OH were identified, indicating that a direct Z-scheme heterojunction was formed over the g-C3N4/TiO2 photocatalyst. The enhanced photocatalytic performance can be attributed to the close-knit interface contact and the formation of Z-scheme heterojunction between g-C3N4 and TiO2, which can accelerate the photo-induced charge carrier separation, broaden the spectra absorption range, and retain a higher redox potential. This one-step synthesis method may provide a new strategy for the construction of Z-scheme heterojunction photocatalysts consisting of g-C3N4 and TiO2 for environmental remediation and solar energy utilization.

Robust self-cleaning membrane with superhydrophilicity and underwater superoleophobicity for oil-in-water separation.

The discharge of oily wastewater has increased dramatically and will bring serious environmental problems. In this work, a self-cleaning and anti-fouling g-C3N4/TiO2/PVDF composite membrane was fabricated via the layer-by-layer approach. The surface of as-prepared composite membrane displayed a superhydrophilic and underwater superoleophobic behavior under irradiation with visible light. Also, upon irradiation with visible light, the fabricated g-C3N4/TiO2/PVDF composite membrane displayed enhanced permeation flux and improved oil removal efficiency as a result of the generation of hydroxyl free radicals during the photocatalytic filtration process. Significantly, irradiation with visible light remarkably improved reusability of the composite membrane by initiating photocatalytic decomposition of deposited oil foulants, which enabled removal of over 99.75% of oils, thus reaching a nearly 100% flux recovery ratio. Furthermore, the g-C3N4/TiO2/PVDF composite membrane exhibited great anti-fouling behavior in photocatalysis-assisted filtration. The mechanistic study revealed that underwater superhydrophobicity and the generation of free hydroxyl radicals jointly contributed to membrane anti-fouling. The greatest advantages of this g-C3N4/TiO2/PVDF composite membrane are that not only does it degrades the oil pollutants, but it also makes the membrane less vulnerable to fouling.

Ultrasensitive photoelectrochemical biosensor for DNA 5-methylcytosine analysis based on co-sensitization strategy combined with bridged DNA nanoprobe.

Altered DNA methylation in the form of 5-methylcytosine (5-mC) patterns is correlated with disease diagnosis, prognosis, and treatment response. Therefore, accurate analysis of 5-mC is of great significance for the diagnosis of diseases. Here, an efficient enhanced photoelectrochemical (PEC) biosensor was designed for the quantitative analysis of DNA 5-mC based on a cascaded energy level aligned co-sensitization strategy coupling with the bridged DNA nanoprobe (BDN). Firstly, Au nanoparticle/graphite phase carbon nitride/titanium dioxide (AuNPs/g-C3N4@TiO2) nanocomposite was synthesized through in situ growth of AuNPs on g-C3N4@TiO2 surface as a matrix to provide a stable background signal. Next, BDN with a high mass transfer rate synthesized from a pair of DNA tetrahedral as nanomechanical handles was used as a capture probe to bind to the target sequence. The polydopamine nanosphere was applied to load with CdTe QDs (PDANS-CdTe QDs) as a photocurrent label of 5-mC antibodies. When the 5-mC existed, a large number of PDANS-Ab-CdTe QDs were introduced to the electrode surface, the formed CdTe QDs/AuNPs/g-C3N4@TiO2 co-sensitive structure could effectively enhance the electron transfer capability and photocurrent response rate due to the effective cascade energy level arrangement, leading to a significantly enhanced photocurrent signal. The proposed PEC biosensor manifested a wide range from 10-17 M to 10-7 M and a detection limit of 2.2 aM. Meanwhile, the excellent performance indicated the practicability of the designed strategy, thus being capable of the clinical diagnosis of 5-mC.

A promising catalytic solution of NO reduction by CO using g-C3N4/TiO2: A DFT study.

The direct catalytic reduction of nitric oxide (NO) by carbon monoxide (CO) to form harmless N2 and CO2 is an ideal strategy to simultaneously remove both these hazardous gases. To investigate the feasibility of using graphitic carbon nitride/titanium dioxide (g-C3N4/TiO2) to catalyze the NO reduction by CO, we systematically explore the effect of the interfacial coupling between g-C3N4 and TiO2 on the photo-induced carrier separation, the light absorption, and the surface reaction for the NO reduction by using density functional theory. The g-C3N4/TiO2 is predicted to have a better photocatalytic activity for NO reduction than g-C3N4, due to the enhanced light absorption intensity and the accelerated separation of the photo-excited electron-hole pairs. By comparing the reaction routes on g-C3N4/TiO2 and g-C3N4, the results indicate that the introduction of TiO2 can keep the surface reaction process intact with the NO dissociation (N2O formation) being the rate-determining (crucial) step. Moreover, TiO2 can facilitate the desorption of NO reduction products, avoiding the deactivation of g-C3N4. This work shows that the composition of TiO2 into g-C3N4 provides a promising catalyst in NO reduction by CO.

Photoelectrochemical water oxidation over TiO2 nanotubes modified with MoS2 and g-C3N4.

TiO2 nanotube arrays (TNAs) have been studied for photoelectrochemical (PEC) water splitting. However, there are two major barriers of TNAs, including a low photo-response and the fast charge carrier recombination in TNAs, leading to poor photocatalytic efficiency. Through a comparison of MoS2/TNAs and g-C3N4/TNAs, it was found that TNAs modified with MoS2 and g-C3N4 exhibited a current density of, respectively, 210.6 and 139.6 µA·cm-2 at an overpotential of 1.23 V vs RHE, which is 18.2 and 12 times higher than that of pure TNAs under the same conditions. The stability of the MoS2/TNAs heterojunction is higher than that of g-C3N4/TNAs.

Recent progress in g-C3N4, TiO2 and ZnO based photocatalysts for dye degradation: Strategies to improve photocatalytic activity.

Water contamination by dyes is a matter of concern for human health and the environment. Various methods (membrane separation, coagulation and adsorption) have been explored to remove/degrade dyes. However, now the exploitation of semiconductor assisted materials using renewable solar energy has emerged as a potential candidate to resolve the issue. Although, single component photocatalysts (ZnO, TiO2, ZrO2) were experimented, due to their low efficiency and stability due to the high recombination rate electron-hole pair and inefficient visible light absorption, composites of semiconductor materials are being used. Semiconductor heterojunction systems are developed by coupling two or more semiconductor components. The synergistic effect of their properties, such as adsorption and improved charge carrier migration, is observed to increase overall stability. This review covers recent progress in advanced nanocomposite materials based on g-C3N4, TiO2 and ZnO used as photocatalysts with details of enhancing the photocatalytic properties by heterojunctions, crystallinity and doping. The conclusion at the end displays a summary, research gaps and future outlook. A holistic analysis of recent progress to demonstrate the efficient heterojunctions for photodegradation with optimal conditions, this review will be helpful for the development of efficient heterostructured systems for photodegradation. This review covers references from the year 2017-2020.

Enhancement of Cr(VI) removal efficiency via adsorption/photocatalysis synergy using electrospun chitosan/g-C3N4/TiO2 nanofibers.

Chitosan/g-C3N4/TiO2 (CS/CNT) nanofibers were fabricated by electrospinning technique for Cr(VI) removal through the adsorption and photocatalytic processes. The effects of crucial factors in the adsorption process including contact time (0-1440 min), pH (1-7), initial concentration of Cr(VI) (20-800 mg/L) were investigated. The photocatalytic experiment was executed in a photochemical reactor with an 800 W xenon lamp to simulate visible light. In adsorption process, at pH = 2, the adsorption capacities of chitosan (CS) nanofibers, CS/CNT10:1 (CS : g-C3N4/TiO2 = 10:1) nanofibers and CS/CNT5:1 nanofibers were 20.8, 165.3 and 68.9 mg/g, respectively, suggesting the addition of g-C3N4/TiO2 (CNT) could notably enhance the acid resistance of CS and widen its practical application. Under visible-light irradiation, the removal efficiency of Cr(VI) using CS/CNT nanofibers was appreciably improved, which was about 50 % higher than that of pure adsorption, indicating that the CS/CNT nanofibers exhibited the effective synergistic effect of adsorption and photocatalysis.

TiO2 Nanowires with Doped g-C3N4 Nanoparticles for Enhanced H2 Production and Photodegradation of Pollutants.

With the rapid consumption of fossil fuels, along with the ever-increasing environmental pollution, it is becoming a top priority to explore efficient photocatalysts for the production of renewable hydrogen and degradation of pollutants. Here, we fabricated a composite of g-C3N4/TiO2 via an in situ growth method under the conditions of high-temperature calcination. In this method, TiO2 nanowires with a large specific surface area could provide enough space for loading more g-C3N4 nanoparticles to obtain C3N4/TiO2 composites. Of note, the g-C3N4/TiO2 composite could effectively photocatalyze both the degradation of several pollutants and production of hydrogen, both of which are essential for environmental governance. Combining multiple characterizations and experiments, we found that the heterojunction constructed by the TiO2 and g-C3N4 could increase the photocatalytic ability of materials by prompting the separation of photogenerated carriers. Furthermore, the photocatalytic mechanism of the g-C3N4/TiO2 composite was also clarified in detail.

Hybrid multifunctional core/shell g-C3N4@TiO2 heterojunction nano-catalytic for photodegradation of organic dye and pharmaceutical compounds.

The pyrolysis of melamine was an effective one-pot method for preparing a nanostructured multifunctional photocatalytic based on core/shell g-C3N4@TiO2 heterojunction. Various techniques entirely characterized these materials: X-ray diffraction (XRD) proved to enhance the as-prepared materials' crystallinity through the variation of dislocation, strain, and crystallite size with TiO2 loading. The stacked layered/sheet-like with a smooth surface of the as-prepared samples have been shown via scanning electron microscopy (SEM). Diffuse reflectance spectroscopy (DRS) showed an apparent decrease in the energy bandgap for these nanocomposites with TiO2 loading. All the prepared materials were subjected to visible photocatalytic applications under the same conditions. The dye model (Methylene Blue, MB), and antibiotic model (Amoxicillin, AMO), was photodegraded using the as-prepared nanocomposites under visible light irradiation. In the recombination reduction among TiO2 and g-C3N4 interfaces, g-C3N4 has been effectively utilized as a matrix. Our findings proved that g-C3N4@TiO2 photocatalysts exhibited superior photocatalytic performance. CNT-5 of 2.58 eV bandgap had a higher activity of 99.7 in 50 min for MB and 100% in 20 min for AMO than the other represented photocatalysts in this work. The migration of photogenerated electrons from a g-C3N4 to TiO2 via heterojunction among them as g-C3N4 (1 0 1) removes the electrons accumulated on (1 0 1) of TiO2, improve the photodegradation efficiency. Therefore, the increase in photocatalytic reaction rates, recycling, and the sample's photostability can be considered the result of successful interactions among the TiO2 and g-C3N4 systems. The suggested photodegradation mechanism of MB and AMO was discussed in detail and compared with previously reported work. Therefore, the photodegradation rate of MB and AMO via CNT-5 composite is 6 and 3 times, respectively, higher than that of g-C3N4 under simulated solar irradiation. This research creates a new perspective on the production of nanocomposite materials in the area of treatment of pharmaceutical and dye contaminants.

Noble Metal-Free TiO2-Coated Carbon Nitride Layers for Enhanced Visible Light-Driven Photocatalysis.

Composites of g-C3N4/TiO2 were one-step prepared using electron impact with dielectric barrier discharge (DBD) plasma as the electron source. Due to the low operation temperature, TiO2 by the plasma method shows higher specific surface area and smaller particle size than that prepared via conventional calcination. Most interestingly, electron impact produces more oxygen vacancy on TiO2, which facilitates the recombination and formation of heterostructure of g-C3N4/TiO2. The composites have higher light absorption capacity and lower charge recombination efficiency. g-C3N4/TiO2 by plasma can produce hydrogen at a rate of 219.9 µmol·g-1·h-1 and completely degrade Rhodamine B (20mg·L-1) in two hours. Its hydrogen production rates were 3 and 1.5 times higher than that by calcination and pure g-C3N4, respectively. Electron impact, ozone and oxygen radical also play key roles in plasma preparation. Plasma has unique advantages in metal oxides defect engineering and the preparation of heterostructured composites with prospective applications as photocatalysts for pollutant degradation and water splitting.

Facile Construction of All-Solid-State Z-Scheme g-C3N4/TiO2 Thin Film for the Efficient Visible-Light Degradation of Organic Pollutant.

The increasing discharge of dyes and antibiotic pollutants in water has brought serious environmental problems. However, it is difficult to remove such pollutants effectively by traditional sewage treatment technologies. Semiconductor photocatalysis is a new environment-friendly technique and is widely used in aqueous pollution control. TiO2 is one of the most investigated photocatalysts; however, it still faces the main drawbacks of a poor visible-light response and a low charge-separation efficiency. Moreover, powder photocatalyst is difficult to be recovered, which is another obstacle limiting the practical application. In this article, g-C3N4/TiO2 heterojunction is simply immobilized on a glass substrate to form an all-solid-state Z-scheme heterojunction. The obtained thin-film photocatalyst was characterized and applied in the visible-light photodegradation of colored rhodamine B and tetracycline hydrochloride. The photocatalytic performance is related to the deposited layers, and the sample with five layers shows the best photocatalytic efficiency. The thin-film photocatalyst is easy to be recovered with stability. The active component responsible for the photodegradation is identified and a Z-scheme mechanism is proposed.

Synergistic degradation of acid orange 7 dye by using non-thermal plasma and g-C3N4/TiO2: Performance, degradation pathways and catalytic mechanism.

In order to harness the full capability of ultraviolet and visible light in the dielectric barrier discharge induced non-thermal plasma (DBD-NTP) process, g-C3N4/TiO2 catalysts were prepared and utilized in this process. Synergistic degradation of acid orange 7 (AO7) dye by DBD-NTP and g-C3N4/TiO2 was conducted, and the performance, degradation pathways and synergistic catalytic mechanism were investigated. The results showed that the degradation rate of AO7 in the DBD-NTP and g-C3N4-15/TiO2 process increased by 39.1% compared with that in the single DBD-NTP process at 12 min discharge time. At 20 W input power, initial concentration of AO7 was 5 mg/L, catalytic dosage was 0.5 g/L, initial pH value was 10.0 and air flow rate was 52 L/h, the degradation rate of AO7 reached 100.0% after 12 min discharge time. Higher discharge power and initial concentration of AO7 inhibited AO7 degradation, whereas increasing the air flow rate and initial pH value of the solution promoted AO7 degradation. The degradation pathways of AO7 consisted of azo structure destruction, ring opening reaction, hydroxylation, carboxylation and mineralization reaction. The results of radical trapping experiment showed that O2-, h+, OH, O3 and H2O2 were the main reactive species for AO7 degradation in the DBD-NTP and g-C3N4-15/TiO2 process. The Z-scheme photocatalytic mechanism for the g-C3N4/TiO2 catalyst was proposed.