Langmuir最新文献

{"title":"Construction of Cu2MoS4/ZnO Heterostructures and Mechanism of Photocatalytic Hydrogen Production","authors":"Yanli Zhuang, Hao Cheng, Shuo Tian, Yancheng Hao, Jikun Pan, Zihuan Zhang, Dan Li, Limin Dong, Jian Li, You Li, Xinxin Jin","doi":"10.1021/acs.langmuir.4c04325","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04325","url":null,"abstract":"Constructing wide and narrow band gap heterogeneous semiconductors is a method to improve the activity of photocatalysts. In this paper, CMS/ZnO heterojunctions were prepared by solvothermal loading of ZnO particles on the surface of Cu₂MoS₄ nanosheets. The photocatalytic H₂ precipitation rate is about 545 μmol·g^–1·h^–1, which is 6.8 times that of Cu₂MoS₄ and 3 times that of ZnO without any cocatalyst. After etching modification of CMS, the photocatalytic hydrogen production efficiency of the ECMS/ZnO heterojunction is further improved. Its hydrogen production efficiency reaches about 1115 μmol·g^–1·h^–1, which is 9 times that of ECMS and 6 times that of ZnO. The reasons are mainly attributed to the following two factors: (1) the formation of the ECMS/ZnO type-II-type heterojunction facilitates the effective separation of photogenerated electrons and holes; (2) the band structure of Cu₂MoS₄ was optimized by etching modification, which made the ECMS/ZnO heterojunction have lower interfacial charge transfer resistance and improved the photocatalytic hydrogen production activity of the heterojunction.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"77 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975584","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":"Tracking Cholesterol Flip-Flop in Mammalian Plasma Membrane through Coarse-Grained Molecular Dynamics Simulations","authors":"Ayishwarya Dutta, Monika Kumari, Hemant K. Kashyap","doi":"10.1021/acs.langmuir.4c03717","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03717","url":null,"abstract":"Plasma membrane (PM) simulations at longer length and time scales at nearly atomistic resolution can provide invaluable insights into cell signaling, apoptosis, lipid trafficking, and lipid raft formation. We propose a coarse-grained (CG) model of a mammalian PM considering major lipid head groups distributed asymmetrically across the membrane bilayer and validate the model against bilayer structural properties from atomistic simulation. Using the proposed CG model, we identify a recurring pattern in the passive collective cholesterol transbilayer motion and study the individual cholesterol flip-flop events and associated pathways along with lateral ordering in the bilayer during a flip-flop event. We identify two discrete cholesterol flip-flop pathways: (i) a systematic rototranslational pathway and (ii) intraleaflet inversion followed by interleaflet translation (or reverse). We observe a periodic cholesterol enrichment in the exoplasmic leaflet of the PM bilayer and examine the underlying cholesterol–lipid affinities. We observe closer association between cholesterol and palmitoylsphingomyelin (PSM) lipid, relative to other lipids, and conclude that the cholesterol enrichment in the exoplasmic leaflet can be attributed to higher PSM content in that leaflet, together leading to formation of short-lived PSM–cholesterol-rich domains.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"49 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975582","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":"Zinc Chloride-Doped g-C3N4 Microtubes for Enhanced Photocatalytic Degradation of Tetracycline Hydrochloride","authors":"Xiao-Yu Ye, Yu-Ling Qi, Ying Cheng, Qiang Wang, Guo-Zhi Han","doi":"10.1021/acs.langmuir.4c03912","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03912","url":null,"abstract":"Morphology regulation and element doping are effective means to improving the photocatalytic performance of graphite-phase carbon nitride (g-C₃N₄). In this article, using melamine and zinc chloride as raw materials, a novel kind of Zn/Cl-doped hollow microtubular g-C₃N₄ (Zn-HT-CN) by a hydrothermal method was developed. The structure and morphology of Zn-HT-CN and reference samples were characterized by X-ray diffraction patterns (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), etc. The doping of Zn/Cl narrowed the bandgap width of the hollow microtubular g-C₃N₄, as well as the inhibiting recombination of photogenerated electron and holes. Compared with the pure g-C₃N₄ microtube, Zn-HT-CN showed excellent catalytic performance for the photodegradation of tetracycline hydrochloride (TCH) under irradiation of visible light. The photodegradation rate of TCH reached 94.41% in 40 min, which was about two times as high as that catalyzed by the pure g-C₃N₄ microtube. Moreover, it was also superior to the g-C₃N₄ microtube doped with other typical metal elements. In addition, Zn-HT-CN showed good tolerance to environmental pH, and the catalytic efficiency of the material remained at 78.78% after five cycles.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"29 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975695","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":"Enhanced Efficiency of Anionic Guerbet-Type Amino Acid Surfactants","authors":"Ettiene Hugo Wiese, Daniel P. Otto, Frans Johannes Smit, Johannes H. L. Jordaan, Hermanus Cornelius M. Vosloo","doi":"10.1021/acs.langmuir.4c02687","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c02687","url":null,"abstract":"This study investigates the surfactant properties and efficiency of linear and Guerbet-type amino acid surfactants. Utilizing a Wilhelmy plate method, we assessed the colloidal efficiency of these surfactants, with the lowest observed critical micelle concentration at 0.046 mmol L^–1, significantly reducing surface tension to as low as 25.1 mN·m^–1. Furthermore, the self-diffusion coefficients of the various surfactants have been determined through ¹H pulsed-field gradient nuclear magnetic resonance diffusion-ordered spectroscopy. The self-diffusion coefficients are linked to the surface tension reduction as a function of concentration to determine the characteristic time scale of diffusion. In this work, the characteristic time scale of diffusion of a series of surfactants was calculated to investigate the interfacial coverage efficiency. Our findings indicate an inverse relationship between the characteristic time scale of diffusion and critical micelle concentrations across surfactants with hydrocarbon tail lengths of 8–22 carbons. Shorter tails correspond to lower colloidal efficiencies, but rapid surface tension reduction, resulting in the characteristic time scale of diffusion values ranging from 120 ns to 2.15 s. This property is crucial for applications requiring rapid action, such as enhancing aerosol efficiency, improving dispersion, and wetting materials in products.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"28 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975580","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":"Ptn (n = 1, 3, and 4) Cluster-Modified MoSe2 Nanosheets: A Potential Sensing and Scavenging Candidate for Lithium-Ion Battery State Characteristic Gases","authors":"Zhixian Zhang, Tian-Yi Sang, Chutian Yu, Lintao Ma, Yi Ao, Chengzhi Zhou, Xingang Chen, Zhipeng Ma, Chunyan Li, Weigen Chen","doi":"10.1021/acs.langmuir.4c04573","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04573","url":null,"abstract":"Realizing reliable online detection of characteristic gases (H₂, C₂H₄, CO, and CO₂) in lithium-ion batteries is crucial to maintain the safe and stable operation of power equipment and new energy storage power plants. In this study, transition metal Pt_<i>n</i> (<i>n</i> = 1, 3, and 4) clusters are attached to MoSe₂ nanosheets for the first time based on density functional theory using the perfect crystalline facet modification method, and the adsorption characteristics and electronic behaviors of H₂, C₂H₄, CO, and CO₂ are investigated and enhanced. The results show that Pt_<i>n</i> (<i>n</i> = 1, 3, and 4) is reliably chemically connected to the substrate without any significant deformation of the geometry. The adsorption properties as well as the band gap, DOS, and LUMO–HOMO are optimized for the modified Gas/Pt_<i>n</i> (<i>n</i> = 1, 3, and 4)-MoSe₂ system. The large electronic states near the Fermi level are further activated by the modification process, and Pt-MoSe₂ and Pt₄-MoSe₂ can serve as battery state characteristic gas sensors suitably according to the detection needs of specific target gases, whereas Pt₃-MoSe₂ can be used as a good adsorbent for effective and reliable scavenging of battery state characteristic gases and is further applied to energy and power equipment and new energy storage power plants.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"104 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975587","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":"Shape-Dependent Structural Order of Red Blood Cells","authors":"Logan D. Piegols, Tobias Dwyer, Sharon C. Glotzer, Omolola Eniola-Adefeso","doi":"10.1021/acs.langmuir.4c04335","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04335","url":null,"abstract":"In this work, we show how shape matters for the ordering of red blood cells (RBCs) at a water–air interface for both artificially rigidified and sphered cells as a model system for hereditary spherocytosis. We report enhanced long-range order for spherical RBCs over disk-shaped RBCs arising from the increased local ordering of spheres relative to disks. We show that rigidity has a greater effect on the radial distribution of spherical vs disk-shaped RBCs by slightly increasing the average distance between cells. The onset of local hexatic bond order of spherical RBCs in mixed disc-sphere systems coincides with the appearance of clustering of spherical cells as the number fraction of spherocytes increases. Additionally, the radial distribution function in mixed-shape systems begins to change with the onset of local hexatic order and clustering of spherical RBCs. By analyzing the radial distribution functions of RBCs, local hexatic bond order, and clustering, we show that the structure of settled RBCs is dictated by shape. These shape-dictated structures may provide a basis for future tools for detecting RBC shape-altering diseases and disorders.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"6 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975585","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 Density Functional Theory (DFT) Modeling Study of NO Reduction by CO over Graphene-Supported Single-Atom Ni Catalysts in the Presence of CO2, SO2, O2, and H2O","authors":"Huanran Wang, Yan Zhao, Zhezi Zhang, Yaming Zhu, Xianchun Li, Dongke Zhang","doi":"10.1021/acs.langmuir.4c03571","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03571","url":null,"abstract":"The mechanisms of NO reduction by CO over nitrogen-doped graphene (N-graphene)-supported single-atom Ni catalysts in the presence of O₂, H₂O, CO₂, and SO₂ have been studied via density functional theory (DFT) modeling. The catalyst is represented by a single Ni atom bonded to four N atoms on N-graphene. Several alternative reaction pathways, including adsorption of NO on the Ni site, direct reduction of NO by CO, decomposition of NO to N₂O followed by reduction of N₂O to N₂, formation of active oxygen radical O*, and reduction of O* by CO, were hypothesized and the energy barrier corresponding to each of the reaction steps was calculated using DFT. The most probable pathway was found to be that NO adsorbed on the Ni site decomposes via the Langmuir–Hinshelwood mechanism to form N₂O and subsequently N₂, leaving an active oxygen radical (O*) on the surface, which is then reduced by CO. The large adsorption energy of NO on the Ni site results in strong resistance to CO₂, SO₂, O₂, and water vapor. The activation energy of N₂O reduction to N₂ was found to be larger than those of NO decomposition to N₂O and active oxygen radical reduction by CO, illustrating that the step of N₂O reduced to N₂ is the rate-controlling step.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"74 6 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975581","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":"Imidazolium-Based Ionic Liquid Exhibiting Dual Hydrophilic and Oleophobic Properties without Polar End Groups","authors":"Alan Tirado, Lei Li","doi":"10.1021/acs.langmuir.4c04319","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04319","url":null,"abstract":"Simultaneously hydrophilic and oleophobic surfaces offer substantial advantages for applications such as antifogging, self-cleaning, and oil–water separation. It remains challenging to engineer such surfaces without requiring polar functional groups. This study introduces HFIL, a novel ionic liquid (IL) coating that achieves simultaneous hydrophilic and oleophobic properties via a one-step dip-coating process without relying on polar functional groups. Key findings show that, despite the bulk form of HFIL having a high hexadecane contact angle (HCA) of 74.1° and an even higher water contact angle (WCA) of 87.6°, the IL forms a stable monolayer on high-energy surfaces exhibiting a much lower WCA of approximately 40° with minimal change to the HCA. Washing tests demonstrate that, even without the polar functional groups, there is a non-zero bonded thickness upon which the oleophobicity is comparable to polytetrafluorethylene (PTFE). These properties highlight HFIL’s potential for durable applications in antifouling, antifogging, and environmental separation technologies, where selective liquid interactions are essential. This work contributes to a broader understanding of IL-based surface modifications, advancing the development of high-performance coatings.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"16 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975588","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":"An Adsorbent for Efficient and Rapid Gold Recovery from Solution: Adsorption Properties and Mechanisms","authors":"Yu-Juan Xie, Tang-Ming Li, Zhao-Ting Shang, Wang-Ting Lu, Fan Yu","doi":"10.1021/acs.langmuir.4c04094","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04094","url":null,"abstract":"Adsorption is an efficient and highly selective method for gold recovery. Introducing rich N/S organic groups to combine with metal–organic frameworks (MOFs) as adsorbents is regarded as a practical and efficient approach to enhance gold recovery. Herein, a MOF (zirconium isothiocyanatobenzenedicarboxylate MOF, UiO-66-NCS) was designed to combine with amidinothiourea (AT) to form UiO-66-AT (zirconium amidothiourea-benzenedicarboxylate MOF) for efficient and rapid adsorption. The prepared UiO-66-AT delivers an improved adsorption capacity (about 903.02 mg/g at 1000 mg·L^–1 of the initial Au³⁺) and an impressive adsorption rate within minutes (about 10 min for 200 mg·L^–1 Au³⁺). Meanwhile, it exhibits sustainable stability after 5 cycles with a retention rate of 99.52% and excellent adsorption selectivity of 98.76% in actual wastewater. According to advanced characterizations and Density Functional Theory (DFT) simulation, the mechanism might be elaborated as electrostatic adsorption, chelating coordination, and chemical reduction. The modified active groups of the MOF provide the adsorption sites for Au(III) and the rapid reduction of Au(0). UiO-66-AT maintains a large adsorption capacity and high surface reduction activity while realizing stable application in multiple cycles, which is of good practical application value.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"36 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981746","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":"Enhanced Prediction of CO2–Brine Interfacial Tension at Varying Temperature Using a Multibranch-Structure-Based Neural Network Approach","authors":"Jiarui Fan, Yimin Jiang, Zhiqiang Fan, Chunlong Yang, Kun He, Dayong Wang","doi":"10.1021/acs.langmuir.4c03366","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03366","url":null,"abstract":"Interfacial tension (<i>IFT</i>_<i>C–B</i>) between CO₂ and brine depends on chemical components in multiphase systems, intricately evolving with a change in temperature. In this study, we developed a convolutional neural network with a multibranch structure (MBCNN), which, in combination with a compiled data set containing measurement data of 1716 samples from 13 available literature sources at wide temperature and pressure ranges (273.15–473.15 K and 0–70 MPa), was used to quantitatively explore the correlation of various chemical components with <i>IFT</i>_<i>C–B</i> at varying temperature, aiming to achieve accurate predictions of <i>IFT</i>_<i>C–B</i> under complex conditions. Our multibranch neural network analysis yielded some important insights: (1) Leveraging the convolutional and multibranch structure, MBCNN effectively mitigates the adverse effects of sparse matrices resulting from the absence of certain basic components, exhibiting higher prediction accuracy particularly for low <i>IFT</i>_<i>C–B</i> scenarios (MAE = 0.47, and R² = 0.9921) than other AI models. (2) The multibranch structure allows MBCNN to additionally capture the interattribute relationship between temperature and each chemical component. Such interattribute relationships are quantitatively correlated with <i>IFT</i>_<i>C–B</i>, demonstrating that varying temperature significantly influences the dependence of <i>IFT</i>_<i>C–B</i> on chemical components in gas and brine by causing the variation in their solubility. Specifically, the ratio of <i>IFT</i>_<i>C–B</i> to the molality of monovalent cations (Na⁺ and K⁺) and bivalent cations (Ca²⁺ and Mg²⁺) in brine, as well as to the mole fraction of non-CO₂ components (CH₄ and N₂) in the gas phase, varies with increasing temperature, approximately following a quadratic function. (3) By formulating the effect of each attribute on <i>IFT</i>_<i>C–B</i> and quantifying their respective weight, we derived a new piecewise function for predicting <i>IFT</i>_<i>C–B</i> at three temperature intervals (<i>T</i> ≤ 293.15 K, 293.15 K &lt; <i>T</i> ≤ 324.4 K, and <i>T</i> &gt; 324.4 K), with high prediction performance (MAE = 2.3672, R² = 0.9263) across a wide temperature range in saline aquifers.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"53 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981745","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}