Langmuir最新文献

{"title":"Reusable SnS2-Based Cotton Fabric Composites for Efficient Decontamination of Water from Lead Ions under Continuous Flow Conditions","authors":"Vasiliki I. Karagianni, Efthymia Toti, Christos Dimitriou, Yiannis Deligiannakis, Alexios P. Douvalis, Manolis J. Manos","doi":"10.1021/acs.langmuir.5c01540","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01540","url":null,"abstract":"Lead is a toxic heavy metal that pollutes the environment and accumulates in the human body, causing many severe health issues. Metal sulfides have emerged as promising sorbents for rapidly decontaminating Pb²⁺-containing wastewater, showing exceptional sorption kinetics, capacities, and selectivity against common competitive ionic species. In this study, we present modified SnS₂ phases, namely, SnS₂(DMA)_0.7(H₂O)_0.3 (<b>SnS</b>_<b>2</b><b>/DMA</b>, DMA = dimethylamine) and Sn_1–<i>x</i>S₂·<i>y</i>H₂O (<b>SnS</b>_<b>2</b><b>/acid</b>), which demonstrated efficient removal of Pb²⁺ ions from aqueous solutions. Both materials exhibited fast kinetics (≤4 min), high sorption capacities (838.0 mg g^–1 for <b>SnS</b>_<b>2</b><b>/DMA</b> and 190.0 mg g^–1 for <b>SnS</b>_<b>2</b><b>/acid</b>), remarkable selectivity toward Pb²⁺ over several competing cations and in various pH values, because of strong Pb–S covalent interactions. Aiming for practical wastewater treatment, we immobilized <b>SnS</b>_<b>2</b><b>/DMA</b> and <b>SnS</b>_<b>2</b><b>/acid</b> on cotton fabrics, marking this as the initial application of metal sulfides immobilized onto cotton substrates. The metal sulfide-fabric composites were utilized to remove Pb²⁺ under continuous flow conditions, showing significant Pb²⁺ sorption properties. Significantly, the metal sulfide-based composites can be regenerated and reused over several Pb²⁺ sorption cycles. This feature, demonstrated for the first time in metal sulfide materials, constitutes a breakthrough for this class of sorbents.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"134 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165742","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":"Quantifying the Driving Force for the Surface Reconstruction of Copper under Electrochemical Reduction of CO2 by First-Principles Simulations.","authors":"Yixin Yang,Ming Jiang,Shu Xiao,Siyang Tang,Shan Zhong,Hongjiao Li,Bin Liang","doi":"10.1021/acs.langmuir.5c00887","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00887","url":null,"abstract":"Cu is one of the most widely used catalysts in the electrochemical CO2 reduction reaction (CO2RR) due to its unique ability to convert CO2 to C2+ products. However, surface reconstruction of Cu significantly affects the activity and stability of Cu catalyst. In this work, density functional theory (DFT) coupled with implicit solvation ab initio molecular dynamics (AIMD) was employed to unveil the possible migration pathways of surface Cu atoms during the structural evolution processes under CO2RR. Surface energy, as the intrinsic thermodynamic driving force of surface reconstruction, is distributed to individual surface Cu atoms and shows a quasi-linear relationship with their generalized coordination number (GCN), demonstrating a maximum driving force of ∼1.10 eV under the applied electric field. The *CO adsorbate weakens the binding of surface Cu atoms, resulting in a maximum vertical displacement of Cu atoms of up to 0.8 Å. In contrast, *H on Cu(100) at high coverage induces a horizontal extruding effect on the surface Cu atoms, causing them to move up to 2 Å. The observable migration of surface Cu atoms in the AIMD run occurs only on Cu adatoms, with the adsorption of pure *H or coadsorption of *CO and *H.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"59 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146110","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":"Tuning the Mesopore Network in Meso-Macroporous Silica Monoliths by Hydrothermal Treatment – A Physisorption Study","authors":"Usman Ali, Rafael Meinusch, Kevin Turke, Peter R. Schreiner, Bernd M. Smarsly","doi":"10.1021/acs.langmuir.5c00572","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00572","url":null,"abstract":"Macro-mesoporous silica monolith columns, prepared by a sol–gel procedure developed by K. Nakanishi, show beneficial flow and separation properties due to their 3D-interconnected macropores in combination with mesopores, providing a high surface area. Building on this, they are routinely used in analytical liquid chromatography. Within the synthetic process, fine-tuning of the mesopore dimension and interconnection is achieved by an etching step involving hydrothermal treatment under basic conditions, typically in the range of 80 °C–100 °C. The present study aims to unravel details of this harsh procedure by a comprehensive analysis of the resulting mesoporous network. Thus, a series of silica monoliths was prepared across a range of hydrothermal treatment temperatures (HTT) between 80 and 110 °C, thereby tuning the mesoporosity. Mercury intrusion porosimetry confirmed that enhanced HTT does not alter the macropore dimension and only affects the mesopore space. The study employed state-of-the-art physisorption analysis applying two adsorptives, Ar (87 K) and N₂ (77 K), to identify changes in the mesopore size and network connectivity as a function of HTT. Also, advanced hysteresis scanning was performed on the same materials, providing independent insights into pore network effects. These analyses indicate that increasing HTT systematically enhances the average mesopore size from 8 nm (80 °C) to approximately 25 nm (110 °C) and widens the pore size distribution, pointing to pronounced dissolution of SiO₂ at higher HTT. Surprisingly, the total mesopore volume remains constant upon increasing the HTT, implying a dissolution-reprecipitation mechanism for SiO₂, rather than mere etching. Importantly, the in-depth porosity analysis reveals an increase in the size of necks, which reduces restrictions in the mesopore network connectivity. Furthermore, the data are in line with a recently proposed spatial mesopore size gradient in monoliths, which we find to be relevant at lower HTT and to systematically diminish toward higher HTT.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"10 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153654","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":"Q&A with Professor Santanu Bhattacharya","authors":"Greco GonzálezMiera*,&nbsp;","doi":"10.1021/acs.langmuir.4c0435210.1021/acs.langmuir.4c04352","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04352https://doi.org/10.1021/acs.langmuir.4c04352","url":null,"abstract":"","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"41 20","pages":"12385–12387 12385–12387"},"PeriodicalIF":3.7,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144137520","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":"Growth of Gold Dendritic Structures under the Coexistence of Hexadecyltrimethylammonium Ions (CTA+) and Ethanol.","authors":"Kenta Iida,Nobuyuki Takeyasu","doi":"10.1021/acs.langmuir.5c01118","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01118","url":null,"abstract":"We investigated the growth of gold nano/micro-structures by reducing gold ions with ascorbic acid in a mixed solvent of ethanol and water containing hexadecyltrimethylammonium bromide (CTAB). The geometries of the gold structures were influenced by the ratio of ethanol to water and the concentrations of CTAB and NaBr. We observed gold dendrites exceeding 10 μm in size, which were composed of numerous needles of varying sizes, some as small as a few tens of nanometers. The gold dendrites were grown within 20 min, a shorter duration compared to previous reports. The overall size of the gold dendrites exhibited dependence on the concentration of Br-, allowing for smaller sizes of less than 10 μm. The micelles of CTA+ were essential for the growth of gold dendrites. The ethanol ratio altered the viscosity and surface tension of the solution, resulting in a variety of geometries. We measured the extinction spectra of the gold dendrites, which revealed that they exhibited a broadband optical response. Observations using a dark-field optical microscope showed that their plasmon resonances were predominantly in the red region. The Raman spectrum of para-aminothiophenol (p-ATP) was measured using the gold dendrites under 785 nm, which revealed field enhancement at the surface of the gold dendrites.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"5 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146133","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":"Acid-Etched Self-Assembled Carbonyl Interface toward Dendrite-Free and Long-Cycling Aqueous Zinc Metal Batteries","authors":"Jian Li, Xingyun Yang, Miaomiao Zhao, Yaping Wang, Yifang Zhang","doi":"10.1021/acs.langmuir.5c01556","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01556","url":null,"abstract":"Uncontrolled dendrite growth, severe parasitic reactions, and sluggish interfacial kinetics at the Zn electrode–electrolyte interface critically impede the commercialization of zinc metal batteries. Herein, an in situ acid-etching strategy was used to automatically fabricate a multifunctional interfacial coating enriched with carbonyl oxygen moieties on zinc foils through aqueous adipic acid treatment (denoted as the AZ@Zn-8 electrode). This engineered surface layer demonstrates enhanced zincophilic characteristics, which significantly improve ion transport kinetics while ensuring a uniform zinc deposition/dissolution behavior during electrochemical processes. The firmly bonded AZ coating on zinc substrates, combined with the strategically oriented (002)_Zn planes, synergistically ensures superior corrosion resistance. Consequently, the AZ@Zn-8 electrodes display an ultralong cycle stability over 4800 h at 2 mA cm^–2. Furthermore, the full cells assembled incorporating LiFePO₄/C and NH₄V₄O₁₀ cathode materials demonstrate an enhanced electrochemical performance. Therefore, the stabilized Zn anode enabled by acid etching to spontaneously form a functional interfacial layer offers a straightforward and efficient approach for aqueous zinc metal batteries.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"45 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153657","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":"Pioneers in Applied and Fundamental Interfacial Chemistry (PAFIC): Santanu Bhattacharya.","authors":"Nilanjan Dey","doi":"10.1021/acs.langmuir.5c00589","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00589","url":null,"abstract":"","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"3 1","pages":"12381-12384"},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146106","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":"Numerical Investigations of Translocation Characteristics of Paired Nonspherical Silica Nanoparticles across Pulmonary Surfactant Monolayer","authors":"Kailiang Tang, Wen Gao, Dongxing Tao, Honglin Hang, Haiwen Ge, Xinguang Cui","doi":"10.1021/acs.langmuir.5c01124","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01124","url":null,"abstract":"To understand and prevent the toxic effects of lunar dust on astronauts’ health in future manned lunar exploration missions, the translocation characteristics of paired nonspherical silica nanoparticles (P-NS-SiNPs) across a pulmonary surfactant (PS) monolayer are studied using a coarse-grained molecular dynamics method considering both ellipsoidal and cubic SiNPs with/without bugles. The key findings are as follows: (1) Compared with an individual SiNP, the translocation times for 4 and 6 nm ellipsoidal P-SiNPs decrease by 25–50% and 7.7–30.7% respectively, while those for 4 and 6 nm cubic P-SiNPs increase by 428.6% and 44.4% respectively, due to cooperative effects. (2) As initial minimum distance increases, the crossing times for ellipsoidal P-SiNPs first decrease and then increase, while embedding times for cubic P-SiNPs first increase and then decrease, due to different local curvature. (3) In the combinations of ellipsoidal-coupled cubic P-SiNPs, the translocation times for the 4 nm combination decrease by 25% and 14.3% respectively, while those for the 6 nm combination increase by 30.8% and 88.9%, respectively. (4) As the number of bulges on P-SiNPs increases, the average crossing times for 4 and 6 nm ellipsoidal-type P-SiNPs increase by 40%, 20%, as well as 14.3% and 219.1% respectively, while the embedding times for 4 nm cubic-type P-SiNPs decrease by 60.8% and 68.9% respectively, and those for 6 nm cubic-type P-SiNPs increase by 80.8% and 46.2%, respectively. In conclusion, due to the differences in contact area and local curvature, the translocation characteristics of ellipsoidal and cubic P-SiNPs exhibit two opposite trends under varying situations.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"28 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153656","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":"Structure-Function Relationship of the Most Abundant Ceramide Subspecies Studied on Monolayer Models Using GIXD and Langmuir Isotherms.","authors":"Gerald Brezesinski, Lukáš Opálka, Chen Shen, Carolin Groetzsch, Emanuel Schneck, Adina Eichner","doi":"10.1021/acs.langmuir.5c01340","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01340","url":null,"abstract":"<p><p>The main lipid compounds of the outermost layer of human skin are ceramides (CERs), free fatty acids, and cholesterol. Although numerous studies performed in the past could demonstrate the importance of these lipids for an intact skin barrier function, knowledge about the impact of each single component on the lamellar lipid films is still lacking. Especially, the CERs are a very heterogeneous group with high relevance for a proper barrier. It was found that the reason for the high stability of the lamellae is related to the lipid structure and function, with the type and extent of interactions between the head groups of the individual CER subspecies being particularly important. Elucidating these at the molecular level could help us to understand CER phase behavior in general. Using grazing incidence X-ray diffraction and measurements of Langmuir isotherms, the current work investigated the lateral packing of the monolayers of different subclasses of C18:0 CERs at air-water interfaces, including phytosphingosine, sphingosine, and dihydrosphingosine CERs, all with either α-hydroxy and nonhydroxy <i>N</i>-acylated fatty acyl. We were able to observe clear effects of the minimal differences in the polar headgroup structures of the sphingoid bases, with respect to the number and position of hydroxyl groups and double bonds, on the CER arrangement regarding the compressibility and structure of the films they formed, revealing that the hydroxyl group at the C4 of the phytosphingosine CERs leads not only to the formation of a hydrogen bond network but also to a stable suprastructure, which might be of high benefit for the barrier properties of intact skin.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":" ","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144155279","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":"Deciphering Zn(II)-Carboxylic Acid Interactions: Tailoring Oil/Water Interfaces and Surfactant Efficiency","authors":"Mohammed K. Al-Sakkaf, A. H. M. Emon Ali, Steven Baldelli, Ali Binabdi, Martin P. Andersson, Theis I. Sølling, Ahmed M. El Zohry","doi":"10.1021/acs.langmuir.5c01055","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01055","url":null,"abstract":"This study elucidates the synergistic interactions between dodecanoic acid (C12) and zinc ions (Zn²⁺) at oil/water interfaces, a critical phenomenon for understanding the intricate dynamics of surfactant systems. Interfacial tension (IFT) measurements, performed via pendant drop tensiometry, reveal that the pronounced affinity of C12 for the oil/water interface causes an approximate 35% reduction in the IFT (from 50 to about 32 mN/m). However, introducing Zn²⁺ ions with C12 created an IFT decrease to approximately 22 mN/m, representing an overall reduction of nearly 55%, indicative of their interactions that substantially enhance interfacial adsorption and promote molecular ordering. The stoichiometric relationship between C12 and Zn²⁺ exhibits a marked concentration dependency. This phenomenon underscores the complex nature of the involved interfacial assembly and the dual role of both C12 and Zn²⁺ in modulating the physicochemical properties of the interface, which has been supported by the complementary density functional theory (DFT) and COSMO-RS calculations. Moreover, vibrational sum frequency generation (VSFG) spectroscopy corroborates the experimental findings by detecting high-order alkane chain arrangements induced by the Zn²⁺ ions. These integrated methodologies demonstrate that the Zn²⁺ ion’s role varies, depending on the surface coverage by C12, and causes a more ordered interfacial film under controlled conditions, optimizing the reduction of IFT. Our research introduces a promising approach for creating advanced surfactant systems, emphasizing the intricate role of metal cations like Zn²⁺ at interfaces in various chemical engineering and environmental management applications.applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"133 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153655","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}