Circumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects.

Artificial photosynthesis using carbon nitride (g-C3N4) holds a great promise for sustainable and cost-effective H2O2 production, but the high carrier recombination rate impedes its efficiency. To tackle this challenge, we propose an innovative method involving multispecies iodine mediators (I-/I3-) intercalation through a pre-photo-oxidation process using potassium iodide (suspected deteriorated "KI") within the g-C3N4 framework. Moreover, we introduce an external electric field by incorporating cationic methyl viologen ions to establish an auxiliary electron transfer channel. Such a unique design drastically improves the separation of photo-generated carriers, achieving an impressive H2O2 production rate of 46.40 mmol g-1 h-1 under visible light irradiation, surpassing the most visible-light H2O2-producing systems. Combining various advanced characterization techniques elucidates the inner photocatalytic mechanism, and the application potential of this photocatalytic system is validated with various simulation scenarios. This work presents a significative strategy for preparing and applying highly efficient g-C3N4-based catalysts in photochemical H2O2 production.

Tailoring the selective generation of oxidative organic radicals for toxic-by-product-free water decontamination.

Peracetic acid (PAA) is emerging as a versatile agent for generating long-lived and selectively oxidative organic radicals (R-O•). Currently, the conventional transition metal-based activation strategies still suffer from metal ion leaching, undesirable by-products formation, and uncontrolled reactive species production. To address these challenges, we present a method employing BiOI with a unique electron structure as a PAA activator, thereby predominantly generating CH3C(O)O• radicals. The specificity of CH3C(O)O• generation ensured the superior performance of the BiOI/PAA system across a wide pH range (2.0 to 11.0), even in the presence of complex interfering substances such as humic acids, chloride ions, bicarbonate ions, and real-world water matrices. Unlike conventional catalytic oxidative methods, the BiOI/PAA system degrades sulfonamides without producing any toxic by-products. Our findings demonstrate the advantages of CH3C(O)O• in water decontamination and pave the way for the development of eco-friendly water decontaminations based on organic peroxides.

2D/2D heterojunctions for rapid and self-cleaning removal of antibiotics via visible light-assisted peroxymonosulfate activation: Efficiency, synergistic effects, and applications.

Developing eco-friendly and efficient technologies for treating antibiotic wastewater is crucial. Traditional methods face challenges in incomplete removal, high costs, and secondary pollution. Heterogeneous peroxymonosulfate (PMS) activation assisted by visible light shows promise, but suitable activators remain a huge challenge. Here, we synthesized cost-effective carbon nitride/bismuth bromide oxide (CN/BiOBr) heterojunctions. Such a heterojunction achieved rapid PMS activation, achieving over 90.00% tetracycline (TC) removal only within 1 min (kobs of 2.23 min-1), surpassing previous systems by nearly 1-2 orders of magnitude and even remarkably superior to the popular single-atom catalysts. The system exhibited self-cleaning properties, maintaining activity after 8 cycles and stability across a wide pH range (3.01 to 9.03). Quenching experiments and theoretical calculations elucidated the exclusive •O2- species involvement and removal pathways. Eco-toxicity assessment and total organic carbon results confirmed simultaneous degradation, detoxification, and mineralization. This system also showed excellent resistance to environmental factors, e.g., coexisting anions, varying pH, and water sources, and demonstrated potential in coking and medical wastewater purification. This study presents a novel technique for rapidly decontaminating antibiotic wastewater through visible light-assisted PMS activation and introduces innovative bionic catalytic oxidation combining light and darkness for practical applications.

The attenuating effect of fermented soymilk on DSS-induced colitis in mice by suppressing immune response and modulating gut microbiota.

Fermented soymilk (FSM) as a new plant-based yoghurt has attracted attention for its nutritional and health benefits. The aim of this research is to explore the effect of consuming FSM before and during inflammatory bowel disease (IBD) on intestinal immune response, and to assess whether fermentation and sucrose can improve the anti-inflammatory activity of soymilk (SM) and FSM, and finally clarify their effect on the gut microbiota and levels of short-chain fatty acids (SCFAs). Consuming FSM in advance can effectively alleviate weight loss and bloody stools in mice with colitis and is associated with a 27% colon length repair rate. It can also prevent spleen and liver enlargement, inhibit immune response and oxidative stress, and increase the expression of the tight junction protein occludin gene (60%). Meanwhile, intaking FSM during IBD reduced weight loss, prevented liver damage, and repaired colon injury. In addition, fermentation enhance the inhibitory effects of FSM on colitis, whereas adding 3% sucrose to FSM had no effect on its intervention in colitis. Analysis of the composition of the gut microbiota in mice showed that the intake of FSM reduced the relative abundance of the pathogenic bacteria Parasutterella, Turicibater, and Bacteroide by 75%, 62%, and 50%, respectively, and increased the relative abundance of the beneficial bacteria Akkermansiaceae, Lachnospiraceae, Alloprevotella, and Dubosella by 28%, 50%, 80%, and 63%, respectively. It further restored the levels of SCFAs in the mouse intestine. The results provide a scientific basis for FSM as a natural anti-inflammatory food that can improve inflammatory intestinal microbiota imbalance and promote gut health.

Embedding electronic perpetual motion into single-atom catalysts for persistent Fenton-like reactions.

In our quest to leverage the capabilities of the emerging single-atom catalysts (SACs) for wastewater purification, we confronted fundamental challenges related to electron scarcity and instability. Through meticulous theoretical calculations, we identified optimal placements for nitrogen vacancies (Nv) and iron (Fe) single-atom sites, uncovering a dual-site approach that significantly amplified visible-light absorption and charge transfer dynamics. Informed by these computational insights, we cleverly integrated Nv into the catalyst design to boost electron density around iron atoms, yielding a potent and flexible photoactivator for benign peracetic acid. This exceptional catalyst exhibited remarkable stability and effectively degraded various organic contaminants over 20 cycles with self-cleaning properties. Specifically, the Nv sites captured electrons, enabling their swift transfer to adjacent Fe sites under visible light irradiation. This mechanism accelerated the reduction of the formed "peracetic acid-catalyst" intermediate. Theoretical calculations were used to elucidate the synergistic interplay of dual mechanisms, illuminating increased adsorption and activation of reactive molecules. Furthermore, electron reduction pathways on the conduction band were elaborately explored, unveiling the production of reactive species that enhanced photocatalytic processes. A six-flux model and associated parameters were also applied to precisely optimize the photocatalytic process, providing invaluable insights for future photocatalyst design. Overall, this study offers a molecule-level insight into the rational design of robust SACs in a photo-Fenton-like system, with promising implications for wastewater treatment and other high-value applications.

pH-Driven Efficacy of the Ferrate(VI)-Peracetic Acid System in Swift Sulfonamide Antibiotic Degradation: A Deep Dive into Active Species Evolution and Mechanistic Insights.

In the realm of wastewater treatment, the power of ferrate (Fe(VI)) and peracetic acid (PAA) as oxidants stands out. But their combined might is where the enhancement truly lies. Their collaborative effect intensifies, but the underlying mechanics, especially across varying pH levels and pollutant types, still lurks in obscurity. Our study delved into the sophisticated oxidation interplay among Fe(VI)-PAA, Fe(VI)-H2O2, and standalone Fe(VI) systems. Notably, at a pH of 9.0, boasting a kinetic constant of ∼0.127 M-1·s-1, the Fe(VI)-PAA system annihilated the pollutant sulfamethoxazole, outpacing its counterparts by a staggering 48.73-fold when compared to the Fe(VI)-H2O2 system and 105.58-fold when using Fe(VI) individually. The behavior of active species─such as the dynamic •OH radicals and high-valent iron species (Fe(IV)/Fe(V))─shifted with pH variations, leading to distinct degradation pathways. Our detailed exploration pinpoints the behaviors of certain species across pH levels from 3.0 to 9.0. In more acidic environments, the •OH species proved indispensable for the system's reactivity. Conversely, as the pH inclined, degradation was increasingly steered by high-valent iron species. This intensive probe demystifies Fe(VI) interactions, deepening our understanding of the capabilities of the Fe(VI)-centered system and guiding us toward cleaner water solutions. Importantly, pH value, often underappreciated, holds the reins in organic wastewater decontamination. Embracing this key player is vital as we strategize for more expansive systems in upcoming ventures.

Corrosion and Erosion Wear Behaviors of HVOF-Sprayed Fe-Based Amorphous Coatings on Dissolvable Mg-RE Alloy Substrates.

To suppress the corrosion and erosion wear of dissolvable magnesium alloy ball seats in wellbores, Fe-based amorphous coatings were deposited on dissolvable Mg-RE alloy substrates, and their microstructure, corrosion behavior, and erosion wear behavior were studied. The thickness of Fe-based amorphous coatings on dissolvable Mg-RE alloy substrates can reach 1000 µm without any cracks, and their porosity and amorphous contents are 0.79% and 86.8%, respectively. Although chloride ions will damage the compactness and protective efficacy of passive films, Fe-based amorphous coatings still maintain low corrosion current density (3.31 µA/cm2) and high pitting potential (1 VSCE) in 20 wt% KCl solution. Due to their higher hardness, the erosion wear resistance of Fe-based amorphous coatings is about 4.16 times higher than that of dissolvable Mg-RE alloy substrates when the impact angle is 30°. Moreover, the erosion rates of Fe-based amorphous coatings exhibit a nonlinear relationship with the impact angle, and the erosion rate reaches the highest value when the impact angle is 60°. The erosion wear mechanisms of Fe-based AMCs vary with the impact angles, including cutting, delamination, splat fracture, and deformation wear. This work can provide effective guidance for the corrosion and wear protection of plugging tools made from dissolvable magnesium alloy.

Effects of Temperature and Pressure on Corrosion Behavior of HVOF-Sprayed Fe-Based Amorphous Coating on the Mg-RE Alloy for Dissolvable Plugging Tools.

To retard the degradation of the magnesium alloys for dissolvable ball seats, Fe-based amorphous coatings were deposited on dissolvable Mg-RE alloy substrates using high velocity oxygen-fuel spraying technology. The results show that the Fe-based amorphous coatings possess low porosity (0.82%) and high amorphous contents (91.4%) and their corrosion resistance decreases with the increase of temperature or pressure. However, with the help of Fe-based amorphous coatings, the degradation time of dissolvable Mg-RE alloy has been significantly prolonged. In particular, the service life of coated Mg-RE alloy exceeds 360 h at temperatures below 50 °C and reaches 87 h at 120 °C and 80 atm. Under high temperature and high pressure, the compactness of passive films decreases and the chemical activities of ions and metal elements increase, leading to the degradation of corrosion resistance of Fe-based amorphous coatings. In long-term corrosion, the crystallized splats are prone to corrosion because of the multiphase structures. The corroded crystallized splats are connected to the inevitable pores by the corroded intersplat regions, resulting in the formation of corrosion channels and the corrosion failure of coatings. This study provides a useful guidance for the corrosion protection of dissolvable plugging tools made of magnesium alloys.

Orientated construction of visible-light-assisted peroxymonosulfate activation system for antibiotic removal: Significant enhancing effect of Cl.

Antibiotic contaminants can migrate over long distances in the water, thus possibly causing severe detriment to the environment and even potential harm to human health. Heterogeneous activation of peroxymonosulfate (PMS) assisted by visible light is an emerging and promising technology for the purification of such wastewater. This study designed an ultra-efficient and stable PMS activator (FeCN) to restore the typical antibiotic-polluted water under harsh conditions. About 90.94% of sulfamethoxazole (SMX) was degraded in 35 min in the constructed FeCN+PMS/vis system, and the reaction rate constant was nearly 50-fold higher than direct photocatalysis. Electron spin resonance, quenching experiments, LC/MS technique, eco-toxicity assessment, and density functional theory validated that the SMX removal was dominated by the attack of h+, •O2- and 1O2 on the active atoms of SMX molecules with high Fukui index, presenting as a simultaneous degradation and detoxification process. Such a visible-light-assisted PMS activation system also had good resistance to the environmental water bodies and a broad spectrum in the degradation of various pollutants. In particular, Cl- (50 mM) could significantly accelerate the removal of SMX with a 32.6-fold increase in catalytic activity, and the mineralization efficiency could reach 56.6% under identical conditions. Moreover, this Cl- containing system excluded the degradation products of disinfection by-products, and such a system was also versatile for different contaminants. This work demonstrates the feasibility of the FeCN+PMS/vis system for the remediation of antibiotic-contaminated wastewater in the presence and absence of Cl-, and also highlights their great potential in WWTPs.

Antioxidant properties of fermented soymilk and its anti-inflammatory effect on DSS-induced colitis in mice.

Lactic acid-fermented soymilk as a new plant-based food has aroused extensive attention because of its effects on nutrition and health. This study was conducted to delve into the antioxidative and anti-inflammatory activities of lactic acid-fermented soymilk. To elucidate the key factors that affect the antioxidant properties of fermented soymilk, the strains and preparation process were investigated. Findings show that the fermented soymilk prepared using hot-water blanching method (BT-80) demonstrated a better antioxidant activity than that using conventional method (CN-20). Besides, a huge difference was observed among the soymilks fermented with different strains. Among them, the YF-L903 fermented soymilk demonstrated the highest ABTS radical scavenging ability, which is about twofold of that of unfermented soymilk and 1.8-fold of that of L571 fermented soy milk. In vitro antioxidant experiments and the analysis of H2O2-induced oxidative damage model in Caco-2 cells showed that lactic acid-fermentation could improve the DPPH radical scavenging ability, ABTS radical scavenging ability, while reducing the content of reactive oxygen species (ROS) and malondialdehyde (MDA) in Caco-2 cells induced by H2O2, and increasing the content of superoxide dismutase (SOD). Consequently, cells are protected from the damage caused by active oxidation, and the repair ability of cells is enhanced. To identify the role of fermented soymilk in intestinal health, we investigate its preventive effect on dextran sodium sulfate-induced colitis mouse models. Results revealed that the fermented soymilk can significantly improve the health conditions of the mice, including alleviated of weight loss, relieved colonic injury, balanced the spleen-to-body weight ratio, reduced the disease index, and suppressed the inflammatory cytokines and oxidant indexes release. These results suggest that YF-L903 fermented soymilk is a promising natural antioxidant sources and anti-inflammatory agents for the food industry. We believe this work paves the way for elucidating the effect of lactic acid-fermented soymilk on intestinal health, and provides a reference for the preparation of fermented soymilk with higher nutritional and health value.

High-Performance HVOF-Sprayed Fe-Based Amorphous Coating on LA141 Magnesium Alloy via Optimizing Oxygen Flow and Kerosene Flow.

To solve the problem of poor corrosion and wear resistance of Mg-Li alloys, Fe-based amorphous coatings were prepared by high velocity oxygen-fuel spraying technology (HVOF) on the LA141 magnesium alloy substrate with a Ni60 intermediate layer. The microstructure and performance of Fe-based amorphous coatings with different oxygen flow and kerosene flow were characterized and analyzed. The results demonstrate that there is an optimal oxygen/kerosene ratio where the porosity of Fe-based amorphous coating is the lowest. Moreover, the amorphous content increases with the decrease in the oxygen/kerosene ratio. In particular, when the oxygen flow is 53.8 m3/h and the kerosene flow is 26.5 L/h, the Fe-based amorphous coating possesses the lowest porosity (0.87%), the highest hardness (801 HV0.1), the highest bonding strength (56.9 MPa), and an excellent corrosion and wear resistance. Additionally, it can be seen that the Fe-based amorphous coating is composed of amorphous splats and amorphous oxides, but the Ni60 intermediate layer exhibits an amorphous and crystalline multi-phase structure. The high bonding strength of the coating is attributed to the low porosity of Fe-based amorphous coating and the localized metallurgical bonding between different layers. Finally, the mechanisms on corrosion and wear of Fe-based amorphous coatings are also discussed.