Unveiling Competitive Adsorption in TiO2 Photocatalysis through Machine-Learning-Accelerated Molecular Dynamics, DFT, and Experimental Methods.

The efficient harnessing of solar power for water treatment via photocatalytic processes has long been constrained by the challenge of understanding and optimizing the interactions at the photocatalyst surface, particularly in the presence of nontarget cosolutes. The adsorption of these cosolutes, such as natural organic matter, onto photocatalysts can inhibit the degradation of pollutants, drastically decreasing the photocatalytic efficiency. In the present work, computational methods are employed to predict the inhibitory action of a suite of small organic molecules during TiO2 photocatalytic degradation of para-chlorobenzoic acid (pCBA). Specifically, tryptophan, coniferyl alcohol, succinic acid, gallic acid, and trimesic acid were selected as interfering agents against pCBA to observe the resulting competitive reaction kinetics via bulk and surface phase reactions according to Langmuir-Hinshelwood adsorption dynamics. Experiments revealed that trimesic and gallic acids were most competitive with pCBA, followed by succinic acid. Density functional theory (DFT) and machine learning interatomic potentials (MLIPs) were used to investigate the molecular basis of these interactions. The computational findings showed that while the type of functional group did not directly predict adsorption affinity, the spatial arrangement and electronic interactions of these groups significantly influenced adsorption dynamics and corresponding inhibitory behavior. Notably, MLIPs, derived by fine-tuning models pretrained on a vastly larger dataset, enabled the exploration of adsorption behaviors over substantially longer periods than typically possible with conventional ab initio molecular dynamics, enhancing the depth of understanding of the dynamic interaction processes. Our study thus provides a pivotal foundation for advancing photocatalytic technology in environmental applications by demonstrating the critical role of molecular-level interactions in shaping photocatalytic outcomes.

Robust Photocatalytic MICROSCAFS® with Interconnected Macropores for Sustainable Solar-Driven Water Purification.

Advanced oxidation processes, including photocatalysis, have been proven effective at organic dye degradation. Tailored porous materials with regulated pore size, shape, and morphology offer a sustainable solution to the water pollution problem by acting as support materials to grafted photocatalytic nanoparticles (NPs). This research investigated the influence of pore and particle sizes of photocatalytic MICROSCAFS® on the degradation of methyl orange (MO) in aqueous solution (10 mg/L). Photocatalytic MICROSCAFS® are made of binder-less supported P25 TiO2 NPs within MICROSCAFS®, which are silica-titania microspheres with a controlled size and interconnected macroporosity, synthesized by an adapted sol-gel method that involves a polymerization-induced phase separation process. Photocatalytic experiments were performed both in batch and flow reactors, with this latter one targeting a proof of concept for continuous transformation processes and real-life conditions. Photocatalytic degradation of 87% in 2 h (batch) was achieved, using a calibrated solar light simulator (1 sun) and a photocatalyst/pollutant mass ratio of 23. This study introduces a novel flow kinetic model which provides the modeling and simulation of the photocatalytic MICROSCAFS® performance. A scavenger study was performed, enabling an in-depth mechanistic understanding. Finally, the transformation products resulting from the MO photocatalytic degradation were elucidated by high-resolution mass spectrometry experiments and subjected to an in silico toxicity assessment.

Enhanced Co-Adsorption of Alcohols and Amines for Visible Light Driven Oxidative Condensation Using Iron-Based MOF.

Imines are essential intermediates in organic transformations, and is generally produced by dehydrogenative condensation of alcohols and amines with the assist of specialized catalysts and additives. Heterogeneous photocatalysis provides a sustainable platform for such process without the using of toxic oxidants, yet a functionalized photocatalyst with optimized co-adsorption of reactants needs to be developed to promote the stoichiometric oxidative condensation under ambient conditions. Here, we show that benzyl alcohol and aniline adsorb non-interferingly on the Fe node and the linker sites of the MIL-53(Fe) metal organic frameworks (MOFs), respectively. The co-adsorption of both reactants barely influences the reduction of molecular oxygen to generate oxygen radicals, resulting in efficient formation of benzaldehyde under visible light. Additionally, the weak adsorption of water together with surface acidity of the MIL-53(Fe) promote a rapid condensation of benzaldehyde with aniline and the depletion of generated water, achieving an efficient C-N bond creation for a wide range of substrates.

A Comparison of RML Prion Inactivation Efficiency by Heterogeneous and Homogeneous Photocatalysis.

Prions are proteinaceous pathogens responsible for a variety of devastating diseases in mammals, including scrapie in sheep and goats, chronic wasting disease in cervids, and Creutzfeldt-Jakob disease (CJD) in humans. They are characterized by their exceptional persistence to common inactivation procedures. This applies to all possible sources of prion contamination as prions may be present in the tissues and biological fluids of infected individuals. Hence, efficient prion inactivation procedures are still being sought to minimize the risk of intra- or inter-species transmission. In the past, photocatalytic treatment has been proven to be capable of efficiently oxidizing and inactivating prions. In the present study, the efficacy of homogeneous photo-Fenton-based photocatalysis as well as heterogeneous photocatalysis with TiO2 in reducing RML mouse scrapie infectivity was evaluated. Prion inactivation was assessed by means of a bioassay, and the results were confirmed by in vitro experiments. While the prion infectivity of the RML mouse scrapie was reduced after treatment with the photo-Fenton reagent, the heterogeneous photocatalytic treatment of the same prion strain completely eliminated prion infectivity.

Unveiling the Role of Water in Heterogeneous Photocatalysis of Methanol Conversion for Efficient Hydrogen Production.

Water molecules, which act as both solvent and reactant, play critical roles in photocatalytic reactions for methanol conversion. However, the influence of water on the adsorption of methanol and desorption of liquid products, which are two essential steps that control the performance in photocatalysis, has been well under-explored. Herein, we reveal the role of water in heterogeneous photocatalytic processes of methanol conversion on the platinized carbon nitride (Pt/C3N4) model photocatalyst. In situ spectroscopy techniques, isotope effects, and computational calculations demonstrate that water shows adverse effects on the adsorption of methanol molecules and desorption processes of methanol oxidation products on the surface of Pt/C3N4, significantly altering the reaction pathways in photocatalytic methanol conversion process. Guided by these discoveries, a photothermal-assisted photocatalytic system is designed to achieve a high solar-to-hydrogen (STH) conversion efficiency of 2.3 %, which is among the highest values reported. This work highlights the important roles of solvents in controlling the adsorption/desorption behaviours of liquid-phase heterogeneous catalysis.

Detailed Insight into Photocatalytic Inactivation of Pathogenic Bacteria in the Presence of Visible-Light-Active Multicomponent Photocatalysts.

The use of heterogeneous photocatalysis in biologically contaminated water purification processes still requires the development of materials active in visible light, preferably in the form of thin films. Herein, we report nanotube structures made of TiO2/Ag2O/Au0, TiO2/Ag2O/PtOx, TiO2/Cu2O/Au0, and TiO2/Cu2O/PtOx obtained via one-step anodic oxidation of the titanium-based alloys (Ti94Ag5Au1, Ti94Cu5Pt1, Ti94Cu5Au1, and Ti94Ag5Pt1) possessing high visible light activity in the inactivation process of methicillin-susceptible S. aureus and other pathogenic bacteria-E. coli, Clostridium sp., and K. oxytoca. In the samples made from Ti-based alloys, metal/metal oxide nanoparticles were formed, which were located on the surface and inside the walls of the NTs. The obtained results showed that oxygen species produced at the surface of irradiated photocatalysts and the presence of copper and silver species in the photoactive layers both contributed to the inactivation of bacteria. Photocatalytic inactivation of E. coli, S. aureus, and Clostridium sp. was confirmed via TEM imaging of bacterium cell destruction and the detection of CO2 as a result of bacteria cell mineralization for the most active sample. These results suggest that the membrane ruptures as a result of the attack of active oxygen species, and then, both the membrane and the contents are mineralized to CO2.

Synthesis and characterization of TiO2-based supported materials for industrial application and recovery in a pilot photocatalytic plant using chemometric approach.

In this contribution, the performance of powdered titanium dioxide (TiO2)-based photocatalysts was evaluated in a pilot photocatalytic plant for the degradation of different dyes, with an investigated volume of 1 L and solar simulated light as irradiation source. Five different samples, synthesized in our laboratories, were tested in the pilot plant, each consisting of TiO2 nanoparticles (NPs) coupled with a different material (persistent luminescent material and semiconductor material) and treated in different thermal conditions. All synthesized samples have been subjected to X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller analysis (BET), and transmission electron microscopy (TEM) characterization, to shed light on the influence of introducing other materials on titania characteristics. To study and evaluate the significance of the parameters affecting the process in the pilot plant, a chemometric approach was applied, by selecting a mathematical model (D-Optimal) to simultaneously monitor a large number of variables (i.e., 7), both qualitative and quantitative, over a wide range of levels. At the same time, the recovery of the synthesized photocatalysts was studied following a novel promising recuperation method, i.e., annulling the surface charge of the suspended samples by reaching the isoelectric point (pHPZC) of each sample, for the quantitative precipitation of TiO2 nanoparticles.

A comprehensive review on the boosted effects of anion vacancy in the heterogeneous photocatalytic degradation, part I: Focus on sulfur, nitrogen, carbon, and halogen vacancies.

The greenest environmental remediation way is the photocatalytic degradation of organic pollutants. However, limited photocatalytic applications are due to poor sunlight absorption and photogenerated charge carriers' recombination. These limitations can be overcome by introducing anion vacancy (AV) (O, S, N, C, and Halogen) defects in semiconductors that enhance light harvesting, facilitate charge separation, modulate electronic structure, and produce reactive radicals. In continuing part A of this review, in this part, we summarized the recent AVs' research, including S, N, C, and halogen vacancies on the boosted photocatalytic features of semiconductor materials, like metal oxides/sulfides, oxyhalides, and nitrides in detail. Also, we outline the recently developed AV designs for the photocatalytic degradation of organic pollutants. The AV creating and analysis methods and the recent photocatalytic applications and mechanisms of AV-mediated photocatalysts are reviewed. AV engineering photocatalysts' challenges and development prospects are illustrated to get a promising research direction.

Progress on mechanism and efficacy of heterogeneous photocatalysis coupled oxidant activation as an advanced oxidation process for water decontamination.

The rising debate on the dilemma of photocatalytic water treatment technologies has driven researchers to revisit its prospects in water decontamination. Nowadays, heterogeneous photocatalysis coupled oxidant activation techniques are intensively studied due to their dual advantages of high mineralization and high oxidation efficiency in pollutant degradation. This paved a new way for the development of solar-driven oxidation technologies. Previous reviews focused on the advances in one specific coupling technique, such as photocatalytic persulfate activation and photocatalytic ozonation, but lack a consolidated understanding of the synergy between photocatalytic oxidation and oxidant activation. The synergy involves the migration of photogenerated carriers, radical reaction, and the increase in oxidation rate and mineralization. This review systematically summarizes the fundamentals of activation mechanism, advanced characterization techniques and synergistic effects of coupling techniques for water decontamination. Besides, specific cases that lead researchers astray in revealing mechanisms and assessing synergy are critically discussed. Finally, the prospects and challenges are put forward to further deepen the research on heterogeneous photocatalytic activation of oxidants. This work provides a consolidated view of the existing heterogeneous photocatalysis coupled oxidant activation techniques and inspires researchers to develop more promising solar-driven technologies for water decontamination.

CsPbBr3 Perovskite Nanocrystals for Photocatalytic [3+2] Cycloaddition.

Visible-light-induced halide-exchange between halide perovskite and organohalide solvents has been studied in which photoinduced electron transfer from CsPbBr3 nanocrystals (NCs) to dihalomethane solvent molecules produces halide anions via reductive dissociation, followed by a spontaneous anion-exchange. Photogenerated holes in this process are less focused. Here, for CsPbBr3 in dibromomethane (DBM), we discover that Br radical (Br⋅) is a key intermediate resulting from the hole oxidation. We successfully trapped Br⋅ with reported methods and found that Br⋅ is continuously generated in DBM under visible light irradiation, hence imperative for catalytic reaction design. Continuous Br⋅ formation within this halide-exchange process is active for photocatalytic [3+2] cycloaddition for vinylcyclopentane synthesis, a privileged scaffold in medicinal chemistry, with good yield and rationalized diastereoselectivity. The NC photocatalyst is highly recyclable due to Br-based self-healing, leading to a particularly economic and neat heterogeneous reaction where the solvent DBM also acts as a co-catalyst in perovskite photocatalysis. Halide perovskites, notable for efficient solar energy conversion, are demonstrated as exceptional photocatalysts for Br radical-mediated [3+2] cycloaddition. We envisage such perovskite-induced Br radical strategy may serve as a powerful chemical tool for developing valuable halogen radical-involved reactions.

Sol-gel and Pechini niobium modified: synthesis, characterization and application in the 2,4-D herbicide degradation.

In this work, a comparison was made between the synthesis of niobium-based materials (Nb2O5), both in terms of material characterization and catalytic performance. The methods used were chemical mixtures: modified sol-gel and Pechini. The materials were calcined at different temperatures (753, 873 and 993K) and characterized by the following techniques: photoacousticspectroscopy (PAS), zero charge point (pHPZC), scanning electron microscopy (SEM/EDS), thermogravimetric analysis (TGA/DTG) and X-ray diffraction (XRD). The photocatalytic process was carried out to evaluate the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) under UV radiation (250 W mercury vapor lamp) and different experimental conditions. In addition, to better understand the influence of parameters such as pH, catalyst concentration (0.2, 0.5 and 0.8 g L-1) and calcination temperature, a Design of Experiments (DoE) was used. The results indicated that despite having similar structures and phases in the XRD analysis, the morphology presents two distinct surfaces, due to the preparation method. Differences in the synthesis method affected the catalytic activity in the parameters studied. Although the zero charge point values are close (6.18-6.36), we observed differences in the band gap depending on the calcination temperature. In the optimal condition studied, the catalyst prepared by the sol-gel method obtained the best results.

Enhancement in photocatalytic selectivity of TiO2-based nano-catalyst through molecular imprinting technology.

Improvement in the photocatalytic selectivity is imperative for the effective and efficient utilization of catalysts. In this study, a molecularly imprinted polymer-coated iron-doped titanium dioxide (Fe-TiO2@MIP) nanocomposite was successfully synthesized by precipitation polymerization while using RB-19 as a template. The synthesized nanocomposites (Fe-TiO2@MIP and Fe-TiO2@NIP) were characterized by Fourier transform infrared spectroscopy (FT-IR), atomic force microscopy (AFM), field emission scanning electron microscopy (FESEM) with energy dispersive X-ray (EDX), X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-EMMETT-Teller (BET), and UV-visible spectrophotometry. The optimized binding experiments revealed a high imprinting factor of 5.0 for RB-19. The catalytic degradation efficiency and selectivity of Fe-TiO2@MIP enhanced to almost complete degradation of RB-19 from 70% for the parent Fe-TiO2 and 76% for Fe-TiO2@NIP. An outstanding degradation selectivity of RB-19 was achieved compared to other competitive dyes. Finally, the analysis of the non-degraded and degraded RB-19 by ESI-MS revealed the presence of different intermediates that fits well with the proposed degradation mechanism. The study opens new possibilities of selective photo-degradation of targeted contaminants that may ultimately lead to efficient use of photocatalysts.

g-C3N4/graphene oxide/SnFe2O4 ternary composite for the effective sunlight-driven photocatalytic degradation of methylene blue.

A broadly used dye, methylene blue (MB), adversely impacts human health and water resources, which triggers efficient methods for its elimination. Semiconductor-based heterogeneous photocatalysis is an environmentally friendly approach that effectively degrades organic pollutants. The purpose of the current work is to elucidate and validate the application of a promising g-C3N4/GO/SnFe2O4 (CGS) composite for the environmental remediation of methylene blue dye. The ternary CGS composite has been synthesized using a solvothermal approach. The fabricated composites were analyzed through FTIR, XRD, SEM/EDX, UV-VIS spectroscopy, TEM, and XPS. The photoactivity of composites and affecting parameters (pH, H2O2 dosage, composite amount, initial dye concentration, and irradiation time) were observed in sunlight illumination. The optimal conditions for photocatalytic degradation were pH = 5, photocatalyst dosage = 30 mg/100 mL, H2O2 dosage = 6 mM, and initial dye concentration (IDC) of 10 ppm employing ternary CGS composite, and MB dye was degraded effectively within 1 h. Ninety-eight percent degradation efficacy was attained by employing ternary CGS composite under the optimized conditions. Scavenging analysis suggested that •OH radicals were the key reactive oxygen species (ROS) responsible for the photodegradation of MB dye. Furthermore, the CGS nanocomposite exhibited outstanding recyclability of 84% after five consecutive runs, demonstrating its potential for use in practical applications, particularly pollutant removal.

Improvement of the photocatalytic activity of ZnO thin films doped with manganese.

In the herein report, we synthesized ZnO thin films doped with manganese (Mn). We studied the impact of Mn doping loads (1 %, 3 %, 5 % wt.) on physicochemical properties of the compounds. Furthermore, we presented the photocatalytic efficiency in removal of methylene blue dye. The structural assay indicated ZnO conserve the wurtzite crystalline structure after dopant insertion. Furthermore, the crystalline size of catalysts was reduced after dopant incorporation. The SEM analysis showed a change in surface morphology after modification of ZnO thin films. Furthermore, Raman spectroscopy verified the Mn insertion inside the ZnO lattice. After the doping process, band gap was reduced by 16 %, in comparison to bare ZnO. After the photocatalytic test, the doped catalysts showed better performance than bare ZnO in removing MB. The best test showed a kinetics constant value of 2.9 × 10-3 min-1 after 120 min of visible irradiation. Finally, the Mn(5 %):ZnO thin film was suitable after five degradation cycles, and the degradation process efficiency was reduced by 32%.

A high-purity gas-solid photoreactor for reliable and reproducible photocatalytic CO2 reduction measurements.

Reactions between a gas phase and a solid material are of high importance in the study of alternative ways for energy conversion utilizing otherwise useless carbon dioxide (CO2). The photocatalytic CO2 reduction to hydrocarbon fuels like e.g., methane (CH4) is such a potential candidate process converting solar light into molecular bonds. In this work, the design, construction, and operation of a high-purity gas-solid photoreactor is described. The design aims at eliminating any unwanted carbon-containing impurities and leak points, ensuring the collection of reliable and reproducible data in photocatalytic CO2 reduction measurements. Apart from the hardware design, a detailed experimental procedure including gas analysis is presented, allowing newcomers in the field of gas-solid CO2 reduction to learn the essential basics and valuable tricks. By performing extensive blank measurements (with/without sample and/or light) the true performance of photocatalytic materials can be monitored, leading to the identification of trends and the proposal of possible mechanisms in CO2 photoreduction. The reproducibility of measurements between different versions of the here presented reactor on the ppm level is evidenced.

Hydrothermal Synthesis of Heterostructured g-C3N4/Ag-TiO2 Nanocomposites for Enhanced Photocatalytic Degradation of Organic Pollutants.

In this study, heterostructured g-C3N4/Ag-TiO2 nanocomposites were successfully fabricated using an easily accessible hydrothermal route. Various analytical tools were employed to investigate the surface morphology, crystal structure, specific surface area, and optical properties of as-synthesized samples. XRD and TEM characterization results provided evidence of the successful fabrication of the ternary g-C3N4/Ag-TiO2 heterostructured nanocomposite. The heterostructured g-C3N4/Ag-TiO2 nanocomposite exhibited the best degradation efficiency of 98.04% against rhodamine B (RhB) within 180 min under visible LED light irradiation. The g-C3N4/Ag-TiO2 nanocomposite exhibited an apparent reaction rate constant 13.16, 4.7, and 1.33 times higher than that of TiO2, Ag-TiO2, and g-C3N4, respectively. The g-C3N4/Ag-TiO2 ternary composite demonstrated higher photocatalytic activity than pristine TiO2 and binary Ag-TiO2 photocatalysts for the degradation of RhB under visible LED light irradiation. The improved photocatalytic performance of the g-C3N4/Ag-TiO2 nanocomposite can be attributed to the formation of an excellent heterostructure between TiO2 and g-C3N4 as well as the incorporation of Ag nanoparticles, which promoted efficient charge carrier separation and transfer and suppressed the rate of recombination. Therefore, this study presents the development of heterostructured g-C3N4/Ag-TiO2 nanocomposites that exhibit excellent photocatalytic performance for the efficient degradation of harmful organic pollutants in wastewater, making them promising candidates for environmental remediation.

A Review on the Use of Metal Oxide-Based Nanocomposites for the Remediation of Organics-Contaminated Water via Photocatalysis: Fundamentals, Bibliometric Study and Recent Advances.

The improper disposal of toxic and carcinogenic organic substances resulting from the manufacture of dyes, drugs and pesticides can contaminate aquatic environments and potable water resources and cause serious damage to animal and human health and to the ecosystem. In this sense, heterogeneous photocatalysis stand out as one effective and cost-effective water depollution technique. The use of metal oxide nanocomposites (MON), from the mixture of two or more oxides or between these oxides and other functional semiconductor materials, have gained increasing attention from researchers and industrial developers as a potential alternative to produce efficient and environmentally friendly photocatalysts for the remediation of water contamination by organic compounds. Thus, this work presents an updated review of the main advances in the use of metal oxide nanocomposites-based photocatalysts for decontamination of water polluted by these substances. A bibliometric analysis allowed to show the evolution of the importance of this research topic in the literature over the last decade. The results of the study also showed that hierarchical and heterogeneous nanostructures of metal oxides, as well as conducting polymers and carbon materials, currently stand out as the main materials for the synthesis of MON, with better photocatalysis performance in the degradation of dyes, pharmaceuticals and pesticides.

Plasmonic photocatalytic degradation of tebuconazole and 2,4-dichlorophenoxyacetic acid by Ag nanoparticles-decorated TiO2 tracked by SERS analysis.

Chemical oxidation technologies have been notably used for the mineralization of organic pollutants from aqueous effluents, been especially relevant for the degradation of pesticides. In this context, both tebuconazole (TEB) and 2,4-dichlorophenoxyacetic acid (2,4-D) pesticides were photodegraded by a combined catalyst of TiO2 and silver nanoparticles irradiated by UV-A light (λmax = 368 nm), and the experiments were tracked by surface-enhanced Raman scattering (SERS) spectroscopy. For 2,4-D, the degradation of about 70% was observed after almost 200 min, while for TEB, a decrease of 80% of the initial concentration was observed after approximately 100 min. The SERS monitoring allowed the proposal of some by-products, such as oxidized aliphatic chain and triazole from TEB besides glycolic, glyoxylic and dihydroxyacetic acids from 2,4-D. Their toxicities were predicted through ECOSAR software, verifying that most of them were not harmful to populations of fish, Daphnia and green algae. Thus, the performed oxidative process was efficient in the photodecomposition of TEB and 2,4-D pesticides, inclusive in terms of the decreasing of the toxicity of contaminated effluents.

Effective Activation of Strong C-Cl Bonds for Highly Selective Photosynthesis of Bibenzyl via Homo-Coupling.

Carbon-carbon (C-C) coupling of organic halides has been successfully achieved in homogeneous catalysis, while the limitation, e.g., the dependence on rare noble metals, complexity of the metal-ligand catalylst and the poor catalyst stability and recyclability, needs to be tackled for a green process. The past few years have witnessed heterogeneous photocatalysis as a green and novel method for organic synthesis processes. However, the study on C-C coupling of chloride substrates is rare due to the extremely high bond energy of C-Cl bond (327 kJ mol-1 ). Here, we report a robust heterogeneous photocatalyst (Cu/ZnO) to drive the homo-coupling of benzyl chloride with high efficiency, which achieves an unprecedented high selectivity of bibenzyl (93 %) and yield rate of 92 % at room temperature. Moreover, this photocatalytic process has been validated for C-C coupling of 10 benzylic chlorides all with high yields. In addition, the excellent stability has been observed for 8 cycles of reactions. With detailed characterization and DFT calculation, the high selectivity is attributed to the enhanced adsorption of reactants, stabilization of intermediates (benzyl radicals) for the selective coupling by the Cu loading and the moderate oxidation ability of the ZnO support, besides the promoted charge separation and transfer by Cu species.

One-step calcination synthesis of 2D/2D g-C3N4/WS2 van der Waals heterojunction for visible light-induced photocatalytic degradation of pharmaceutical pollutants.

It is well-documented that accumulation of pharmaceutically active compounds (PhACs), such as antibiotics, in aquatic ecosystems is a prominent environmental hazard. Herein, a series of 2D materials-based heterojunctions, conceptualized based on the integration of graphitic carbon nitride (g-C3N4) with tungsten disulfide (WS2), was fabricated through a facile one-step calcination process, and systematically evaluated for eliminating tetracycline (TC) and sulfamethoxazole (SMX) from aqueous matrices. The microstructure, optical properties, and surface chemistry of the as-prepared composites were examined with a range of microscopy and spectroscopy techniques. In comparison with pristine g-C3N4 or bare WS2, the g-C3N4/WS2 material, with optimal WS2 loading, showed significantly improved photocatalytic activity, towards degradation of TC (84%) and SMX (96%), under visible light. Free radical scavenging experiments revealed that superoxide anions and hydroxyl radicals were predominantly responsible for the rapid breakdown of the PhACs. In addition, the dissociation intermediates and residues were identified and the plausible photocatalytic degradation pathways of TC and SMX over the as-constructed 2D/2D heterojunction were discussed. Further, the photocatalysis end products were non-toxic, as inferred via the resazurin cell viability assay, employing Escherichia coli as a model organism. Most importantly, the 2D/2D g-C3N4/WS2 architecture was structurally resilient and exhibited a fairly stable cycling performance for persistent usage in wastewater treatment. The outcomes of this study testify that 2D/2D heterojunction of g-C3N4 fragments and WS2 nanosheets holds great promise for destroying antibiotics or their metabolites, usually present in wastewaters.