Dual-molecular targeting nanomedicine upregulates synergistic therapeutic efficacy in preclinical hepatoma models.

Advanced hepatocellular carcinoma (HCC) is one of the most challenging cancers because of its heterogeneous and aggressive nature, precluding the use of curative treatments. Sorafenib (SOR) is the first approved molecular targeting agent against the mitogen-activated protein kinase (MAPK) pathway for the noncurative therapy of advanced HCC; yet, any clinically meaningful benefits from the treatment remain modest, and are accompanied by significant side effects. Here, we hypothesized that using a nanomedicine platform to co-deliver SOR with another molecular targeting drug, metformin (MET), could tackle these issues. A micelle self-assembled with amphiphilic polypeptide methoxy poly(ethylene glycol)-block-poly(L-phenylalanine-co-l-glutamic acid) (mPEG-b-P(LP-co-LG)) (PM) was therefore designed for combinational delivery of two molecular targeted drugs, SOR and MET, to hepatomas. Compared with free drugs, the proposed, dual drug-loaded micelle (PM/SOR+MET) enhanced the drugs' half-life in the bloodstream and drug accumulation at the tumor site, thereby inhibiting tumor growth effectively in the preclinical subcutaneous, orthotopic and patient-derived xenograft hepatoma models without causing significant systemic and organ toxicity. Collectively, these findings demonstrate an effective dual-targeting nanomedicine strategy for treating advanced HCC, which may have a translational potential for cancer therapeutics. STATEMENT OF SIGNIFICANCE: Treatment of advanced hepatocellular carcinoma (HCC) remains a formidable challenge due to its aggressive nature and the limitations inherent to current therapies. Despite advancements in molecular targeted therapies, such as Sorafenib (SOR), their modest clinical benefits coupled with significant adverse effects underscore the urgent need for more efficacious and less toxic treatment modalities. Our research presents a new nanomedicine platform that synergistically combines SOR with metformin within a specialized diblock polypeptide micelle, aiming to enhance therapeutic efficacy while reducing systemic toxicity. This innovative approach not only exhibits marked antitumor efficacy across multiple HCC models but also significantly reduces the toxicity associated with current treatments. Our dual-molecular targeting approach unveils a promising nanomedicine strategy for the molecular treatment of advanced HCC, potentially offering more effective and safer treatment alternatives with significant translational potential.

Simultaneous decomplexation of Pb-EDTA and elimination of free Pb ions by MoS2/H2O2: Mechanisms and applications.

The critical challenge of effectively removing Pb-EDTA complexes and Pb(II) ions from wastewater is pivotal for environmental remediation. This research introduces a cutting-edge bulk-MoS2/H2O2 system designed for the simultaneous decomplexation of Pb-EDTA complexes and extraction of free Pb(II) ions, streamlining the process by eliminating the need for subsequent treatment stages. The system exhibits outstanding efficiency, achieving 98.1% decomplexation of Pb-EDTA and 98.6% removal of Pb. Its effectiveness is primarily due to the generation of reactive oxygen species, notably •OH and O2•- radicals, facilitated by bulk-MoS2 and H2O2. Key operational parameters such as reagent dosages, Pb(II): EDTA molar ratios, solution pH, and the presence of coexisting ions were meticulously evaluated to determine their impact on the system's performance. Through a suite of analytical techniques, the study confirmed the disruption of Pb-O and Pb-N bonds, further elucidating the decomplexation process. It also underscored the synergistic role of bulk-MoS2's adsorption properties and the formation of PbMoO4-like precipitates in enhancing Pb elimination. Demonstrating the bulk-MoS2/H2O2 system as a robust, one-step solution that meets stringent Pb emission standards, this study provides in-depth insights into the removal mechanisms of Pb-EDTA, affirming its potential for broader application in wastewater treatment practices.

Efficient remediation of mercury-contaminated groundwater using MoS2 nanosheets in an in situ reactive zone.

Mercury contamination in groundwater is a serious global environmental issue that poses threats to human and environmental health. While MoS2 nanosheets have been proven promising in removing Hg from groundwater, an effective tool for in situ groundwater remediation is still needed. In this study, we investigated the transport and retention behavior of MoS2 nanosheets in sand column, and employed the formed MoS2in situ reactive zone (IRZ) for the remediation of Hg-contaminated groundwater. Breakthrough test revealed that high flow velocity and MoS2 initial concentration promoted the transport of MoS2 in sand column, while the addition of Ca ions increased the retention of MoS2. In Hg removal experiments, the groundwater flow velocity did not influence the Hg removal capacity due to the fast reaction rate between MoS2 and Hg. With an optimized MoS2 loading, MoS2IRZ effectively reduced the Hg effluent concentration down to <1 µg/L without apparent Hg remobilization. Additionally, flake-like MoS2 employed in this study showed much better Hg removal performance than flower-like and bulk MoS2, as well as other reported materials, with the Hg removal capacity a few to tens of times higher than those materials. These results suggest that MoS2 nanosheets have the potential to be an efficient IRZ reactive material for in situ remediation of Hg in contaminated groundwater.

Impact of different fracture types in the pyriform buttress area on nasal airway function.

INTRODUCTION: Fractures in the pyriform buttress area adversely affect facial appearance and nasal airway patency. Nasal airway function has received less attention than aesthetic problems in the literature. This retrospective study classified the different fracture types in this area and determined their impact on nasal airway function. MATHODS: Three-dimensional computed tomography images of patients with fractures in the pyriform buttress area were analyzed to identify the exact fracture pattern. The nasal airway functions were evaluated and compared between patients with different fracture patterns using acoustic rhinometry, rhinomanometry, and the nasal obstruction symptom evaluation scale. RESULTS: Overall, 47 patients, including 16 with type I fractures (high fracture line; group I), 16 with type II fractures (intermediate fracture line; group II), and 15 with type III fractures (low fracture line; group III), were included in the study. The mean minimal cross-sectional area (MCA), total nasal inspiratory resistance (Tri) and total nasal expiratory resistance (Tre) of group I were 0.51 ± 0.06 cm2, 1.67 ± 0.11 kPa L-1 s-1, and 1.66 ± 0.12 kPa L-1 s-1, respectively; those of group II were 0.48 ± 0.07 cm2, 1.89 ± 0.15 kPa L-1 s-1, and 1.88 ± 0.14 kPa L-1 s-1, respectively; and those of group III were 0.36 ± 0.04 cm2, 1.94 ± 0.21 kPa L-1 s-1, and 2.01 ± 0.34 kPa L-1 s-1, respectively. The nasal obstruction symptom evaluation (NOSE) scale scores for groups I, II, and III were 7.188, 9.813, and 13.27, respectively. CONCLUSION: Therefore, the severity of the nasal airway obstruction depends on the displacement of the fractured bones in patients with fractures in the pyriform buttress area. The most profound nasal obstruction occurs in patients with the lowest fracture line.

Application of fluorescence lifetime imaging microscopy to monitor glucose metabolism in pancreatic islets in vivo.

Glucose stimulated insulin secretion is mediated by glucose metabolism via oxidative phosphorylation generating ATP that triggers membrane depolarization and exocytosis of insulin. In stressed beta cells, glucose metabolism is remodeled, with enhanced glycolysis uncoupled from oxidative phosphorylation, resulting in the impaired glucose-mediated insulin secretion characteristic of diabetes. Relative changes in glycolysis and oxidative phosphorylation can be monitored in living cells using the 3-component fitting approach of fluorescence lifetime imaging microscopy (FLIM). We engrafted pancreatic islets onto the iris to permit in vivo FLIM monitoring of the trajectory of glucose metabolism. The results show increased oxidative phosphorylation of islet cells (∼90% beta cells) in response to hyperglycemia; in contrast red blood cells traversing the islets maintained exclusive glycolysis as expected in the absence of mitochondria.

Clinical effect of endovascular repair of complex aortic lesions using optimized Octopus surgery.

Objective: Complex aortic lesions, especially those involving branches of the visceral artery, remain a challenge to treat. A single-center study using the Octopus technique to evaluate the safety and short-term effects of endovascular repair of complex aortic lesions was reported and documented. Methods: The data of six cases who underwent optimized Octopus surgery in our center from August 2020 to February 2022 were analyzed retrospectively. The choice of operation scheme, operation time, operation complications, and follow-up data were analyzed among them. Results: The average age of the six patients undergoing optimized Octopus surgery was 55.1 ± 17.2 years. Two cases were diagnosed as pararenal aortic aneurysms; four cases were aortic dissection involving the visceral artery. All cases achieved technical success; all visceral arteries were reconstructed as planned. A total of 17 visceral arteries were planned to be reconstructed; five celiac arteries were embolized. Three cases of gutter endoleak were found during the operation without embolization but with follow-up observation. There were two cases of slight damage to renal function and two cases of perioperative death. Other complications, such as intestinal ischemia and spinal cord ischemia, did not occur. Follow-up ranged from 6 months to 30 months. One patient died of gastrointestinal bleeding 6 months after the operation. At the 6 months follow-up, computed tomographic angiography showed that all internal leaks had disappeared. The patency rate of the visceral artery was 100%, and no complications, such as stent displacement and occlusion, occurred during the follow-up period. Conclusion: With fenestrated and branched stent grafts technology not widely available, and off label use not a viable option, Octopus technology for treating complex aortic lesions should be considered. The Octopus technique is an up-and-coming surgical method, but we should recognize its operation difficulty, operation-related complications, and long-term prognosis. We should pay attention to and continue to optimize Octopus technology.

Synergistic Effects of Organic Ligands and Visible Light on the Reductive Dissolution of CeO2 Nanoparticles: Mechanisms and Implications for the Transformation in Plant Surroundings.

Cerium oxide (CeO2) nanoparticles are one of the most important engineered nanomaterials with demonstrated applications in industry. Although numerous studies have reported the plant uptake of CeO2, its fate and transformation pathways and mechanisms in plant-related conditions are still not well understood. This study investigated the stability of CeO2 in the presence of organic ligands (maleic and citric acid) and light irradiation. For the first time, we found that organic ligands and visible light had a synergistic effect on the reductive dissolution of CeO2 with up to 30% Ce releases after 3 days, which is the highest release reported so far under environmental conditions. Moreover, the photoinduced dissolution of CeO2 in the presence of citrate was much higher than that in maleate, which are adsorbed on the surface of CeO2 through inner-sphere and outer-sphere complexation, respectively. A novel ligand-dependent photodissolution mechanism was proposed and highlighted: upon electron-hole separation under light irradiation, the inner-sphere complexed citrate is more capable of consuming the hole, prolonging the life of electrons for the reduction of Ce(IV) to Ce(III). Finally, reoxidation of Ce(III) by oxygen was observed and discussed. This comprehensive work advances our knowledge of the fate and transformation of CeO2 in plant surroundings.

Human descending aorta injury caused by brucellosis: A case report.

BACKGROUND: Brucellosis is one of the most common zoonotic diseases in the world. Although cardiovascular complications of human brucellosis account for only 3% of morbidity, they are the leading cause of death. Peripheral vascular disease due to brucellosis is rare and under-reported in the literature. CASE PRESENTATION: Two patients with previous brucellosis, both of whom had been treated with anti-brucellosis, were admitted to vascular surgery for thoracic aortic ulcer and abdominal aortic pseudoaneurysm, respectively, with positive IgG antibody to brucellosis and negative IgM antibody to brucellosis, tube agglutination test, and blood culture. These 2 patients were successfully treated with aortic stent-graft implantation and followed up for 8 and 10 weeks without complications. CONCLUSIONS: Chronic damage to human blood vessels by brucellosis may not disappear with brucellosis treatment, and peripheral blood vessels should be examined annually in people previously diagnosed with brucellosis. Clinicians in related departments should pay attention to peripheral vascular complications of brucellosis.

Dual role of soil-derived dissolved organic matter in the sulfamethoxazole oxidation by manganese dioxide.

Manganese dioxide (MnO2) can mediate organic pollutant oxidation in aquatic environments, which has been reported to be inhibited or promoted by dissolved organic matter (DOM) in different studies. It remains unresolved why conflicting results have been observed and whether such results depend on the type and concentration of DOM. Here, we used three types of well-characterized DOM derived from soil heated at 50, 250, or 400 °C (DOM_50, DOM_250, and DOM_400, respectively) to evaluate the impacts of DOM type and concentration and environmental pH on MnO2-mediated oxidation of sulfamethoxazole, a widely detected and ecotoxic emerging pollutant. We observed that the degradation rate of sulfamethoxazole was possibly promoted by DOM_250 (pH 6‒8), while it was generally inhibited by DOM_50 and DOM_400. Furthermore, it was initially inhibited and then promoted with increasing DOM concentrations and was consistently less inhibited at a higher pH. The inter-DOM variations of sulfamethoxazole degradation could be explained by the more enriched polyphenolics in DOM_250 than in DOM_50 and DOM_400, whereas the weak promoting effect of DOM_400 indicates that high DOM aromaticity may not necessarily promote pollutant degradation. Our results reconcile the debate on the role of DOM in the oxidation of sulfamethoxazole by MnO2 and highlight the decisiveness of the molecular composition and concentration of DOM and the reaction pH in the overall promoting or inhibiting role of DOM.

Treatment of abdominal aortic pseudoaneurysm caused by brucellosis with endovascular aneurysm repair.

Peripheral vascular disease caused by brucellosis is rarely seen around the world; thus, it is easily ignored by patients and doctors, leading to a lack of corresponding screening and delayed comprehensive treatment. Currently, there is no standard or guideline for diagnosing and treating peripheral arterial disease caused by brucellosis. From June 2021 to December 2022, four cases of abdominal aortic pseudoaneurysm caused by brucellosis disease were treated with endovascular aneurysm repair This study reported treatment results as follows and reviewed the incidence, treatment, and prognosis of abdominal aortic pseudoaneurysm caused by brucellosis.

Efficacy of IAPP suppression in mouse and human islets by GLP-1 analogue conjugated antisense oligonucleotide.

Insulin resistance is the major risk factor for Type 2 diabetes (T2D). In vulnerable individuals, insulin resistance induces a progressive loss of insulin secretion with islet pathology revealing a partial deficit of beta cells and islet amyloid derived from islet amyloid polypeptide (IAPP). IAPP is co-expressed and secreted with insulin by beta cells, expression of both proteins being upregulated in response to insulin resistance. If IAPP expression exceeds the threshold for clearance of misfolded proteins, beta cell failure occurs exacerbated by the action of IAPP toxicity to compromise the autophagy lysosomal pathway. We postulated that suppression of IAPP expression by an IAPP antisense oligonucleotide delivered to beta cells by the GLP-1 agonist exenatide (eGLP1-IAPP-ASO) is a potential disease modifying therapy for T2D. While eGLP1-IAPP-ASO suppressed mouse IAPP and transgenic human IAPP expression in mouse islets, it had no discernable effects on IAPP expression in human islets under the conditions studied. Suppression of transgenic human IAPP expression in mouse islets attenuated disruption of the autophagy lysosomal pathway in beta cells, supporting the potential of this strategy.

Singlet oxygen generation in light-assisted peroxymonosulfate activation by carbon nitride: Role of elevated crystallinity.

Carbon nitride (CN) is an emerging 2D non-metal semiconductor material that could be used in photocatalysis and advanced oxidation processes (AOPs) for pollutants degradation. The radical-induced degradation by CN in photocatalysis or photo-assisted AOPs was widely reported in previous studies. Nevertheless, how the non-radical degradation by CN materials could be achieved under irradiation is neither well understood nor controlled. In this work, crystalline carbon nitride (CCN) was synthesized via a facile molten-salt method, and used to activate peroxymonosulfate (PMS) under visible light (>420 nm) to selectively and efficiently degrade tetracycline (TC). Compared to the traditional polymeric carbon nitride (PCN), CCN was found to be a superior PMS activator with the assistance of visible light, which was ascribed to the increased crystallinity of CN tri-s-triazine units and the increased number of catalytic sites, thereby optimizing the photoelectric properties. The activation performance could be further improved by copper loading, with TC degradation rate nearly six times more than that of PCN. EPR trapping and quenching tests showed that singlet oxygen (1O2) was the dominant reactive oxygen species in the CCN/PMS/visible light system, attributing to the increased graphitic N sites and formation of electron-deficient C in C-N bonding between neighboring tri-s-triazine units upon crystallinity elevation in CCN. In contrast to the conventional radical-based photocatalysis and AOP processes, the visible light-assisted non-radical AOP degradation was highlighted for the selectivity and the remarkable resistance to the impacts of background inorganic anions or natural organic matter (up to 10 mg/L) in the actual water matrix. This work revealed the 1O2 generation mechanism by CN-based materials under the joint assistance of visible light illumination and crystallinity elevation, and its excellent removal performance demonstrates the great potential of CCN-based materials in the practical wastewater treatment.

Redispersion mechanisms of 2D nanosheets: combined role of intersheet contact and surface chemistry.

Redispersion behavior recovers the important features of nanomaterials and thus holds great promise for exciting applications of nanomaterials in different fields. In contrast to the redispersion of nanoparticles, which is mainly determined by surface chemistry, the redispersion of 2D nanosheets could be more complicated and is not well understood. In the present study, the redispersion behavior of 2D NMs was investigated by selecting representative nanosheets, MoS2, graphene oxide and their derivatives with both experimental methods and molecular dynamics (MD) simulations. The good agreement between experiments and MD simulations suggested that the redispersion in response to surface chemistry was regulated by the alignment configurations of the nanosheets. More importantly, we revealed that the difference in the hydrophilicity properties is responsible for the distinctive separation distances of the 1T and 2H MoS2 nanosheets. Appropriately adjusting the alignment configuration of the nanosheets can alter the effect of surface hydrophilicity on the redispersion behavior. Based on these fundamental findings, we identified three distinctive zones for the redispersion tendency of the 2D nanosheets with different surface hydrophilicity, Hamaker constants and intersheet contacts. As one of the implications, the results serve as a prescreening for the stability of the 2D restacking-based membrane. For the first time, the study systematically reported the interplay of intersheet configuration and surface chemistry in the redispersion of nanosheets, which provides a theoretical foundation for the processing and applications of 2D nanomaterials.

Redispersion Behavior of 2D MoS2 Nanosheets: Unique Dependence on the Intervention Timing of Natural Organic Matter.

The aggregation-redispersion behavior of nanomaterials determines their transport, transformation, and toxicity, which could be largely influenced by the ubiquitous natural organic matter (NOM). Nonetheless, the interaction mechanisms of two-dimensional (2D) MoS2 and NOM and the subsequent influences on the redispersion behavior are not well understood. Herein, we investigated the redispersion of single-layer MoS2 (SL-MoS2) nanosheets as influenced by Suwannee River NOM (SRNOM). It was found that SRNOM played a decisive role on the redispersion of MoS2 2D nanosheets that varied distinctly from the 3D nanoparticles. Compared to the poor redispersion of MoS2 aggregates in the absence or post-addition of SRNOM to the aggregates, co-occurrence of SRNOM in the dispersion could largely enhance the redispersion and mobility of MoS2 by intercalating into the nanosheets. Upon adsorption to SL-MoS2, SRNOM enhanced the hydration force and weakened the van der Waals forces between nanosheets, leading to the redispersion of the aggregates. The SRNOM fractions with higher molecular mass imparted better dispersity due to the preferable sorption of the large molecules onto SL-MoS2 surfaces. This comprehensive study advances current understanding on the transport and fate of nanomaterials in the water system and provides fresh insights into the interaction mechanisms between NOM and 2D nanomaterials.

Late evening snack and oral amino acid capsules improved respiratory quotient and Fischer ratio in patients with alcoholic liver cirrhosis.

INTRODUCTION AND OBJECTIVES: Appropriate nutritional support may improve energy metabolism in alcoholic liver cirrhosis (ALC) patients. We explored the effect of a late evening snack (LES) and oral amino acid (OAA) capsules on energy metabolism and the Fischer ratio in ALC. PATIENTS AND METHODS: Ninety-one ALC patients were enrolled and randomly divided into three groups: 31 patients in the LES and OAA group, 32 in the LES group, and 28 controls. Respiratory quotient (RQ), carbohydrate oxidation rate (CHO%), fat oxidation rate (FAT%), serum isoleucine and the Fischer ratio were measured at baseline and at months 1, 3, and 6 of follow-up. RESULTS: The RQ in the LES and OAA group was 0.79 ± 0.06, 0.80 ± 0.04, 0.82 ± 0.04, and 0.82 ± 0.04 at baseline and at months 1, 3, and 6 of follow-up, respectively. These values were significantly higher than those in the LES group (P < 0.05). The RQ in the LES group was significantly higher than that in the control group at month 1 and month 6 (P < 0.05). CHO% in the LES and OAA group was significantly increased and FAT% was significantly decreased at month 3 of follow-up (P < 0.05). In the LES and OAA group, serum isoleucine and the Fischer ratio were markedly increased compared with the LES group and control group (P < 0.05). CONCLUSIONS: LES can significantly increase the RQ in ALC. LES and OAA were more effective than LES alone in improving serum isoleucine and the Fischer ratio.

[Application of 3D printed nasal vestibular support in the treatment of anterior nostril stenosis].

Objective:To evaluate the efficacy of 3D printed nasal vestibular support on the recovery of nasal ventilation function and nostril shape after nostril stenosis treatment. Methods:Thirty-eight patients with unilateral traumatic nasal vestibular stenosis were selected and treated with 3D printed nasal vestibular support after operation. Subjective evaluation indicators, objective nostril local morphological and structural parameters, and nasal airflow dynamics parameters by numerical simulation were used. To evaluate the nostril morphological and nasal functional recovery after treatment. Results:The subjective nasal congestion and nostril symmetry satisfaction VAS scores of the patients after nasal vestibular support treatment were improved to varying degrees compared with those before surgery; The nostril morphological parameters showed that the Δlong-axis ratio and Δ î€Œshort-axis ratio were significantly decreased after nasal vestibular support therapy （0.09±0.09 and 0.16±0.13） compared with those before surgery（0.21±0.20 and 0.28±0.21） respectively（P<0.01）. And the cross-sectional area of the nasal valve on the stenotic side nasal cavity increased from（0.40±0.27） cm² before operation to （0.71±0.26） cm² after treatment（P<0.01）; The nasal resistance on the stenosis side nasal cavity also decreased from （0.036±0.024） Pa·s/mL before operation to （0.022±0.008） Pa. s/mL after treatment（P<0.01）, and the total nasal resistance was decreased from （0.033±0.02） Pas/mL before operation to （0.021±0.007）Pa. s/mL after treatment（P<0.01） ; It also showed that NWE（nasal warming efficiency） and NHE（nasal humidification efficiency） on the stenotic side nasal cavity were significantly decreased after nasal vestibular support therapy（[95.92±2.8]% and [94.55±4.17]%） compared with those before surgery （[97.94±1.97 ]% and [96.19±2.94]%） respectively（P<0.01）. Conclusion:The 3D printed nasal vestibular support for postoperative support treatment on patients with anterior nostril stenosis can reflect the advantages of personalized treatment and allow patients to obtain satisfactory results, and the use of individually designed 3D printed nasal vestibular support can make the shape of anterior nostrils and nasal cavity normal ventilation function recover well, its clinical application prospect is worth looking forward to.

Natural polyphenol self-assembled pH-responsive nanoparticles loaded into reversible hydrogel to inhibit oral bacterial activity.

Periodontitis is one of the most prevalent chronic inflammatory diseases and Polyphenols isolated from Turkish gall play a major role in the treatment of inflammatory diseases for their antibacterial, anti-inflammatory and antioxidant activities. In this work, Turkish Galls effective constituent (TGEC, T) was prepared into nanoparticles (T-NPs) by principle of oxidative self-polymerization. The pH-sensitive T-NPs was encapsulated into thermosensitive type in-situ hydrogel, and 42.29 ± 1.12% of effective constituent from T-NPs were continuously released within 96 h under the periodontitis environment. In addition, the weakly alkaline oral micro-environment of patients with periodontitis is more conducive to the sustained release of effective constituent, which is 10.83% more than that of healthy periodontal environment. The bacteriostatic test showed that T-NPs had stronger antibacterial activity on oral pathogens than that of TGEC. Compared with TGEC, the minimum inhibitory concentration (MIC) of T-NPs against P. gingivalis and A. viscosus was reduced by 50% and 25%, respectively. Interestingly, T-NPs induced bacteria lysis by promoting the excessive production of ROS without periodontal tissue damage caused by excessive oxidation reaction. In conclusion, a simple method of preparing microspheres with natural polyphenols was developed, which provides beneficial reference for one-step prepared drug carriers from effective components of natural product, likewise the method offers a green and effective solution to synthesis a new adjuvant therapy drugs for treatment of gingivitis associated with periodontal pockets.

Enhancing the Permselectivity of Thin-Film Composite Membranes Interlayered with MoS2 Nanosheets via Precise Thickness Control.

The demand for highly permeable and selective thin-film composite (TFC) nanofiltration membranes, which are essential for seawater and brackish water softening and resource recovery, is growing rapidly. However, improving and tuning membrane permeability and selectivity simultaneously remain highly challenging owing to the lack of thickness control in polyamide films. In this study, we fabricated a high-performance interlayered TFC membrane through classical interfacial polymerization on a MoS2-coated polyethersulfone substrate. Due to the enhanced confinement effect on the interface degassing and the improved adsorption of the amine monomer by the MoS2 interlayer, the MoS2-interlayered TFC membrane exhibited enhanced roughness and crosslinking. Compared to the control TFC membrane, MoS2-interlayered TFC membranes have a thinner polyamide layer, with thickness ranging from 60 to 85 nm, which can be tuned by altering the MoS2 interlayer thickness. A multilayer permeation model was developed to delineate and analyze the transport resistance and permeability of the MoS2 interlayer and polyamide film through the regression of experimental data. The optimized MoS2-interlayered TFC membrane (0.3-inter) had a 96.8% Na2SO4 rejection combined with an excellent permeability of 15.9 L m-2 h-1 bar-1 (LMH/bar), approximately 2.4 times that of the control membrane (6.6 LMH/bar). This research provides a feasible strategy for the rational design of tunable, high-performance NF membranes for environmental applications.

Rich edge-hosted single-atomic Cu-N4 sites for highly efficient oxygen reduction reaction performance.

Single-atom electrocatalysts with metal-nitrogen-carbon (MNC SACs) moieties in carbon support display outstanding electrocatalytic performance towards oxygen reduction reaction (ORR) and have received widespread attentions. Only active sites on the edges of pores in carbon support are electrochemically accessible and contribute to ORR. Herein, we report a combined hydroxyl-functionalized and NH4Cl-assisted etching strategy to effectively promote the yield of edge-hosted Cu SAs. Thus, well-defined SAs with Cu-N4 configuration are generated into the defect of carbonaceous nanospheres (CuSAs@DCSs). Impressively, the obtained SACs renders outstanding electrocatalytic ORR activity with onset, half-wave potentials of 1.02 V, 0.90 V, and extremely high stability, which transcends the noble-metals and most of the previously reported catalysts. When used in rechargeable Zn-air batteries, CuSAs@DCSs achieves ultralong cycle life at the large current density of 10 mA cm-2 (over 260 h) with low charge-discharge potential gap. Our study demonstrates that the creation of abundant micropores enriches the electrochemically accessible SAs, which locate at the edge-defects and are responsible for the remarkable ORR performance. This work sheds a facile strategy for designing and developing efficient electrocatalyst for various energy-related electrocatalytic reactions.

Tuning phase compositions of MoS2 nanomaterials for enhanced heavy metal removal: performance and mechanism.

Two-dimensional MoS2 nanosheets have shown great potential in heavy metal remediation due to their unique properties. MoS2 has two primary phases: 1T and 2H. Each has different physiochemical properties, but the impact of these differences on the overall material's heavy metal removal performance and associated mechanisms is rarely reported. In this study, we synthesized morphologically similar but phase-distinct MoS2 samples via hydrothermal synthesis, which comprised dominantly either a metallic 1T phase or a semiconducting 2H phase. 1T-MoS2 samples exhibited higher removal capacities for Ag+ and Pb2+ cations relative to 2H-MoS2. In particular, an eight-fold increase in the Pb2+ adsorption capacity was observed in the 1T-MoS2 samples (i.e. ∼632.9 mg g-1) compared to the 2H-MoS2 samples (∼81.6 mg g-1). The mechanisms driving the enhanced performance of 1T-MoS2 were investigated through detailed characterization of metal-laden MoS2 samples and DFT modelling. We found that 1T-MoS2 intrinsically had a larger interlayer spacing than 2H-MoS2 because water molecules were retained between the hydrophilic 1T nanosheets during hydrothermal synthesis. The widened interlayer spacing in 1T-MoS2 allowed the diffusion of heavy metal ions into the nanochannels, increasing the number of adsorption sites and total removal capacities. On the other hand, DFT modelling revealed the energy-favorable adsorption complex of Ag+ and Pb2+ for 1T-MoS2, in which each metal atom was bonded with three S atoms leading to much higher adsorption energies relative to 2H-MoS2 for Ag+ and Pb2+. This study unravels the underlying mechanisms of phase-dependent heavy metal remediation by MoS2 nanosheets, providing an important guide for the use of 2D nanomaterials in environmental applications which include heavy metal removal, contaminant sensing, and membrane separation.