Langmuir最新文献

{"title":"Photocatalytic Degradation of Organic Pollutants by Sulfate Radicals Activated by Defective NH2-MIL-88B","authors":"Zeping Qin, Mingming Sun, Runjie Wu, Pengkun Li, Ran Tai, Hongfei Su, John Tressel, Bicheng Ji, Qiang Wang, Shaowei Chen","doi":"10.1021/acs.langmuir.5c01201","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01201","url":null,"abstract":"Photocatalysis has been recognized as a viable technology for pollutant degradation in wastewater, owing to its ability to generate reactive radicals under photoirradiation. Among these, sulfate radicals <i></i><math display=\"inline\"><mo stretchy=\"false\">(</mo><mi>S</mi><msubsup><mrow><mi>O</mi></mrow><mrow><mn>4</mn></mrow><mrow><mrow><mo lspace=\"0.03em\" rspace=\"0.03em\">·</mo></mrow><mrow><mo>−</mo></mrow></mrow></msubsup><mo stretchy=\"false\">)</mo></math> have been attracting significant attention due to their strong oxidizing properties; yet the specific mechanism of action has remained elusive thus far. In this study, defective NH₂-MIL-88B (DNMB) is prepared via a facile hydrothermal procedure in the presence of potassium sodium tartrate and found to facilitate the production of sulfate radicals from sulfate anions under visible light irradiation, due to partial reduction of Fe³⁺ to Fe²⁺ in the NMB skeleton by the added tartrate that enriches the Fe³⁺/Fe²⁺ redox couples, in addition to other reactive species like superoxide radicals and hydroxy radicals. This effectively improves the degradation efficiency toward a variety of organic pollutants, including antibiotics such as tetracycline (TC), sulfamethoxazole (SMX), and levofloxacin (LEV), as well as common organic contaminants like bisphenol A (BPA) and rhodamine B (RhB), as compared to pristine NMB. Specifically, after 40 minutes of visible light irradiation, the degradation rate increases from 61.5% to 92.1% for TC, from 76.1% to 89.4% for SMX, from 60.5% to 75.2% for LEV, from 61.7% to 91.2% for BPA, and from 78.4% to 94.8% for RhB. The primary active species are identified to be sulfate radicals, with minor contributions from holes, superoxide radicals, and hydroxyl radicals, as demonstrated in quenching experiments and electron spin resonance measurements, and further confirmed by theoretical studies. Degradation pathways for the various pollutants are then proposed based on results from Fukui index calculations and liquid chromatography–mass spectrometry analysis. These results underscore the crucial role of structural engineering in driving the advancement of green and sustainable technologies for environmental engineering.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"110 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921148","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Identification of Topological Metal g-C2N with High Activity and Selectivity for Versatile Oxygen Electrocatalysis","authors":"Rui Tan, Zehou Li, Zhe Xue, Longhui Li, Xueqing Chen, Zhenkun Tang, Xiaolin Wei","doi":"10.1021/acs.langmuir.4c05171","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c05171","url":null,"abstract":"Two-dimensional (2D) carbon nitride materials are emerging as ideal supports for single-atom catalysts (SACs) due to their excellent physicochemical stability, abundant active sites, and ample capacity for metal loading. However, their intrinsic semiconducting properties constrain electrical conductivity, thereby hindering charge transfer during catalytic processes. Herein, we propose a graphene-like 2D carbon nitride structure, g-C₂N, derived from first-principles calculations and theoretical analysis. This structure is identified as a topological metal, featuring a symmetry-protected Dirac cone. Its topologically nontrivial nature is evidenced by distinct edge states, nonzero Berry curvature, and quantized Zak phase. Remarkably, g-C₂N exhibits a Fermi velocity exceeding that of graphene. Furthermore, the constructed Co@C₂N₂ structure is identified as a highly active and selective catalyst for hydrogen peroxide (H₂O₂) electrosynthesis, with a low thermodynamic overpotential of 0.08 V. Additionally, the Co@C₂N₂–N catalyst developed through N-doping strategies demonstrates outstanding bifunctional 4e^– OER/ORR activity with low overpotentials of 0.27 and 0.32 V, respectively. These findings not only broaden the scope of 2D carbon nitride materials but also offer foundational insights for the rational design of highly active catalysts for oxygen electrocatalysis.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"284 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143916007","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Serine-Grafted Cu2O Electrode Enabling Specific β-Hydroxybutyrate Detection by Surface Sensitization-Promoted Electrolysis in Amperometry","authors":"Ting-Chi Lo, Wen-Jyun Wang, Chih-Yen Chen, Jui-Cheng Chang, Wei-Peng Li","doi":"10.1021/acs.langmuir.5c00591","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00591","url":null,"abstract":"As the global prevalence of diabetes continues to rise, the home health testing market has experienced rapid growth. Although blood glucose monitoring is widespread among diabetic patients, there remains a significant lack of testing methods for diabetic ketoacidosis. The present study developed a feasible electrochemical technique for ketoacid detection using serine-immobilized copper(I) oxide nanoparticles (Cu₂O NPs) as the primary electrode material. Given that the serine on the nanoparticle surface enables conjugation with β-hydroxybutyrate (β-HBA) through an esterification reaction between the hydroxyl group of serine and carboxylic acid of β-HBA and another intramolecular nucleophilic acyl substitution between amine and ester groups to form irreversible amide bonding, thus resulting in the β-HBA deposition on the surface of the Cu₂O NP-coated electrode. The quantification of β-HBA can be determined through current variations in amperometry measurement. The results showed a highly linear relationship between reductive current and β-HBA concentration at 0–20 mM, with a reasonable detection limit of 0.1 mM. Moreover, a reasonable mechanism involving the NP surface covering-mediated electrolysis enhancement was proposed. The present method reveals a promising direction in developing sensors for small molecule detection with high specificity and sensitivity.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"41 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143916013","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhancing Monazite Flotation Performance by Introducing Fe3+ to the Solution.","authors":"Tingting Wang,Hongli Fan,Dongyu Yang,Qihuan Zheng,Yuqiao Yang,Yubo Peng,Wei Sun,Hao Lu","doi":"10.1021/acs.langmuir.5c00354","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00354","url":null,"abstract":"Despite the dominance of octyl hydroxamic acid (OHA) in promoting monazite flotation, its limited adsorption on monazite surfaces requires enhancement. This work stands as a systematic study of how the innovative practice of introducing Fe3+ to the solution boosted monazite flotation and examines its underlying mechanism. The initial microflotation tests found that at pH 8, the addition of Fe3+ drives up the flotation recovery rate of monazite to 72.65%, proving that Fe3+ greatly enhanced monazite floatability with OHA. Further analyses revealed that the adsorption of Fe hydrolyzing species onto the surfaces of monazite particles led to an increase in active sites for OHA chemisorption. Through an integrated characterization approach including ζ-potentials, Fourier transform infrared analysis (FTIR), and X-ray photoelectron spectroscopy (XPS), we elucidated the mechanism of how OHA reacted with both Fe3+ species and rare earth (RE) active sites and created Ce/La-O-Fe complexes on the surfaces of monazite particles. This process further generates hydrophobic OHA-Fe chelates, thereby boosting the flotation recoveries.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"48 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921098","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Minimalist Model Lipid System Mimicking the Biophysical Properties of Escherichia coli’s Inner Membrane","authors":"Nicolo Tormena, Teuta Pilizota, Kislon Voïtchovsky","doi":"10.1021/acs.langmuir.5c01138","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01138","url":null,"abstract":"Biological membranes are essential for the development and survival of organisms. They can be highly complex, usually comprising a variety of lipids, proteins, and other biomolecules organized around a lipid bilayer structure. This complexity makes studying specific features of biological membranes difficult, with many research studies relying on simplified models, such as artificial vesicles or supported lipid bilayers. Here, we search for a minimal, lipid-only model system of the <i>Escherichia coli</i> inner membrane. We aim to retain the main lipidomic components in their native ratio while mimicking the membrane’s thermal and mechanical properties. Based on previous studies, we identify 18 potential model systems reflecting key aspects of the known lipidomic composition and progressively narrow down our selection based on the systems’ phase transition temperature and mechanical properties. We identify three ternary model systems able to form stable bilayers that can be made of the commercially available synthetic lipids 16:0–18:1 phosphatidylethanolamine (POPE), 16:0–18:1 phosphatidylglycerol (POPG), and 16:0–18:1 cardiolipin (CL). We anticipate our results to be of interest for future studies making use of <i>E. coli</i> models, for example, investigating membrane proteins’ function or macromolecule–membrane interactions.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"69 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921152","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Novel Formulation of Ionic Liquid-Based Ferrofluids: Investigation of the Magnetic Properties.","authors":"Alessandro Talone,Pierfrancesco Maltoni,Michael Casale,Maryam Abdolrahimi,Sawssen Slimani,Diego Colombara,Luca Leoncino,Patrizia Imperatori,Sara Laureti,Gaspare Varvaro,Davide Peddis","doi":"10.1021/acs.langmuir.5c00403","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00403","url":null,"abstract":"This study establishes a viable process to prepare hybrid nanomaterials comprising stable ionic liquid-based ferrofluids (IL-FFs) with tunable magnetic anisotropy and reduced water contamination, where the latter strongly decreases the colloidal stability of the system. Spinel iron oxide magnetic nanoparticles (MNPs) with different compositions (γ-Fe2O3, Co0.5Zn0.5Fe2O4, and CoFe2O4) and different magnetic anisotropies were synthesized by the polyol method. The particles were coated with dihydrocaffeic acid (DHCA) in tetrahydrofuran (THF) and subsequently transferred directly to 3-ethyl-1-methylimidazolium acetate (EMIMAc), exploring the synergy between intermolecular and covalent bonding to obtain stable dispersions. The evolution of magnetic properties from powder to IL-FFs systems was investigated, allowing us to highlight the synergistic influence of interparticle interaction and magnetic anisotropy on the magnetization dynamics of the nanoparticles.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"20 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921099","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Transparent Janus Nanofibers for Use in Blood-Contact Applications","authors":"Muzammil Kuddushi, Aishwarya S. Pawar, Mehdi Ghaffari Sharaf, Larry D. Unsworth, Xuehua Zhang","doi":"10.1021/acs.langmuir.5c00648","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00648","url":null,"abstract":"Kidney failure occurs when the kidneys can no longer effectively filter waste compounds from the blood, leading to a systemic accumulation of uremic toxins that disrupt hemostasis. Non-specific protein adsorption at the blood–material interface is well-known to direct subsequent host responses. Thus, to develop blood-contacting materials that may become an alternative to traditional dialysis membranes, we explored the effect that uremic toxins have on the adsorption of plasma proteins to Janus membranes. A human plasma system infused with 26 major uremic toxins was designed to replicate the concentrations found in kidney failure patients. This system allowed for the analysis of adsorbed human plasma proteins and clot formation in normal and toxin-treated plasma in the presence of polycaprolactone (PCL)/ethylene vinyl alcohol (EVOH) nanofibers. The findings revealed that uremic toxins significantly increased protein adsorption on PCL/EVOH nanofiber meshes without causing increased clot formation, indicating a lack of enzymatic activation despite higher protein adsorption. Furthermore, the study suggested that unmodified PCL/EVOH surfaces have the potential to trigger a strong humoral immune response, emphasizing the need to understand these interactions for the development of personalized treatment strategies for patients with kidney failure.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"16 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143916009","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Environmentally Sustainable Hydrous Zirconium Oxide–Inulin as an Efficient Adsorbent for Ciprofloxacin Removal: Mechanistic and Thermodynamic Insights via Statistical Physics and Fractal-like Kinetic Modeling","authors":"Mohd Nasir, Monika Bharti, Nafisur Rahman, Mohammad Shahzad Samdani, Mahboob Alam","doi":"10.1021/acs.langmuir.5c00986","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00986","url":null,"abstract":"Pharmaceutical pollutants like ciprofloxacin (CPF) pose environmental risks due to their persistence and limited removal by conventional treatment methods. To address this, a hydrous zirconium oxide–inulin (HZO–inulin) biomaterial was synthesized via wet precipitation and characterized using Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction, thermogravimetric analysis-difference thermal analysis, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller surface area analysis, scanning electron microscopy–energy dispersive X-ray spectroscopy, and transmission electron microscopy. HZO–inulin exhibited high chemical stability under various aquatic conditions. CPF adsorption was optimized using the Box–Behnken design with a desirability function approach, achieving 99.28% removal and a maximum adsorption capacity of 181.46 mg/g under optimal conditions (adsorbent dose = 0.01 g, concentration = 85 mg/L, contact time = 35 min). Isotherm analysis using classical and statistical physics models revealed that the Freundlich model best fit the data, suggesting multilayer adsorption, while statistical physics model 2 indicated monolayer adsorption with two energy levels (<i>R</i>² = 0.9994–0.9997). Adsorption energies (<i>E</i>₁: 28.65–38.62 kJ/mol, <i>E</i>₂: 42.58–54.87 kJ/mol) suggested hydrogen bonding and electrostatic interactions. Thermodynamic studies confirmed spontaneous endothermic adsorption. Kinetic studies at 300 K for CPF concentrations (55, 65, 75 mg/L) followed a fractal-like pseudo-second-order model (<i>R</i>² &gt; 0.998), while diffusion modeling identified boundary-layer diffusion dominance, transitioning to intraparticle diffusion. CPF removal from real water samples was 98.9% (tap water), 99.10% (river water), and 99.15% (wastewater). HZO–inulin retained high adsorption efficiency after eight cycles, confirming its reusability. These findings establish HZO–inulin as an efficient, stable, and sustainable material for water purification applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"76 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143916010","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dynamics of Ferrofluid Droplet Impact on Slippery Liquid-Infused Porous Surfaces.","authors":"Xuan Liu,Yuhang Dai,Haibo Zhao,Cheng Li,Peng Yu","doi":"10.1021/acs.langmuir.5c00814","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00814","url":null,"abstract":"In this study, the impact of ferrofluid droplets on slippery liquid-infused porous surfaces (SLIPS) is explored. A model is proposed to take account of the reduction in the initial volume of the ferrofluid droplet caused by the nonuniform external magnetic field. Five modes are identified based on the distinctive postimpact characteristics, and the corresponding phase diagram is summarized. In the low Weber number range (We ≤ 50), the low energy dissipation caused by the low friction characteristics of the SLIPS, combined with the suppression effect of magnetic field on the lateral expansion of the droplet, accumulates the kinetic energy in the vertical direction. Consequently, the bounce height of the ferrofluid droplet on the SLIPS increases with We, which is contrary to that for the superhydrophobic surfaces. The results offer deeper insights into the magnetic controlled droplet rebound and the impact dynamics across diverse surface types.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"8 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143914974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Integrating Radiative Cooling and Solar Heating for On-Demand Thermal Management.","authors":"Hongmei Zhong,Jiahao Zhang,Ming Sun,Zuankai Wang","doi":"10.1021/acs.langmuir.5c01532","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01532","url":null,"abstract":"Passive radiative cooling has been extensively explored as a sustainable alternative to traditional cooling systems. However, relying solely on this cooling mode restricts their application in temperature-fluctuating environments and may cause overcooling on cold days. To address this challenge, researchers are increasingly developing dual-mode devices that integrate radiative cooling with solar heating, utilizing the Sun's continuous heat source for passive heating. In this perspective, we summarize the latest advancements in this field and highlight specific strategies for switchable dual-mode devices. These strategies generally fall into two categories: Janus design and all-in-one design. Finally, we discuss future challenges and opportunities in on-demand radiative cooling and solar heating, intending to advance this technology toward practical applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"67 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143914976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}