{"title":"Unusual Temperature-Dependent Thermal Conductivity in Monolayer NCCN: Role of Phonon Hydrodynamics.","authors":"Sheng Wang,Zhong-Xiang Xie,Geng-Hua Liu,Si-Jie Chen,Xue-Kun Chen","doi":"10.1021/acs.langmuir.5c02215","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02215","url":null,"abstract":"Seeking high-thermal-conductivity materials is a route to enhancing the efficiency of heat dissipation in Ga-based high-power-density devices. In this work, we use first-principles calculations with the Boltzmann transport equation to predict the thermal conductivity of nitrogen-substituted diamane (NCCN). It is found that the thermal conductivity (κ) of NCCN is as high as 1800 W/mK at room temperature, which is 13.7% smaller compared to that before considering four-phonon scattering. Moreover, there is an anomalous temperature dependence of κ, inconsistent with the typical κ ∼ 1/T trend. This unusual phonon transport behavior stems from the significant hydrodynamic phonon transport in NCCN, where momentum-conserving N-scattering is a dominant scattering mechanism. More importantly, NCCN demonstrates promising potential for hydrodynamic phonon transport above room temperature and over a broader temperature window compared to that of graphene. With the application of tensile strain, the anomalous temperature dependence of κ is subject to change, as longitudinal acoustic and transverse acoustic phonon softening offsets the effects of flexural acoustic-mode linearization, resulting in a decrease in κ with increased strain. Our conclusion could assist the future exploration of hydrodynamic thermal transport behaviors in 2D materials.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"14 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701386","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}
LangmuirPub Date : 2025-07-25DOI: 10.1021/acs.langmuir.5c01956
Bashar M Al-Zghoul,William P Johnson,Luis Ullauri,Diogo Bolster
{"title":"Parameters Driving Anomalous Transport in Colloids: Dimensional Analysis.","authors":"Bashar M Al-Zghoul,William P Johnson,Luis Ullauri,Diogo Bolster","doi":"10.1021/acs.langmuir.5c01956","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01956","url":null,"abstract":"The anomalous transport of identical colloids, characterized by multiexponential and nonmonotonic retention profiles, under unfavorable conditions, has been the subject of significant interest over the past few decades. This study conducts a dimensional analysis of the governing equations for colloid transport to explore the impact of various dimensionless groups on colloid attachment efficiency (α), defined as the ratio of the number of attached colloids to the number intercepted (i.e., those that enter the near-surface zone). The primary objective of this article is to identify the dimensionless groups responsible for explaining potential variation in α. Our analysis revealed that 15 dimensionless groups govern colloid transport in porous media, which we categorized into three groups: (i) hydrodynamic, (ii) DLVO, and (iii) surface charge heterogeneity dimensionless groups. We assessed the impact of each category on the magnitude of α via pore-assembly colloid trajectory simulations. Our findings indicate that the surface charge heterogeneity dimensionless groups exert a dramatic influence on the value of α compared to the mean-field DLVO or hydrodynamic groups. In particular, the surface charge heterogeneity dimensionless group, Hr (the ratio of the heterodomain radius to the radius of the colloid-surface zone of interaction), significantly impacts α in the approximate range of 0.6 < Hr < 2. As a result, within this range, even a slight variation in Hr causes a marked change in α, facilitating the transition between multiexponential and nonmonotonic retention profiles under unfavorable conditions.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"25 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701383","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}
LangmuirPub Date : 2025-07-24DOI: 10.1021/acs.langmuir.5c01926
Xiumei Xie,Zhongfu Ling,Dehui Li,Hua Zou
{"title":"Revisiting the Preparation of Disc-Like Polymer Particles Based on Seeded Dispersion Polymerization: Multihollow Particles Achieved over a Wide Range of Conditions.","authors":"Xiumei Xie,Zhongfu Ling,Dehui Li,Hua Zou","doi":"10.1021/acs.langmuir.5c01926","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01926","url":null,"abstract":"The preparation of disc-like polystyrene (PS) particles via seeded dispersion polymerization of 2-ethylhexyl methacrylate (EHMA) was previously demonstrated using a shaker with the PS particles as seeds in methanol/water medium in the presence of decane and subsequent removal of PEHMA and decane, but only under restrictive conditions. Moreover, no structural visualization of the disc-like particles by transmission electron microscope (TEM) was conducted. In this work, we revisit this synthesis using a conventional magnetic stirring apparatus, significantly broadening the range of feasible conditions (i.e., methanol/water mass ratios of 10/0-5/5, stirring rates of 80-360 rpm, and polymerization times of 2-24 h). Systematic studies reveal that disc-like morphology can be achieved even with smaller PS seed particles (>730 nm) or alternative hydrocarbons (e.g., hexadecane). Crucially, we recognize for the first time that these disc-like particles exhibit a multihollow structure with compartmentalized voids (50-300 nm), formed via phase separation between PS and decane during polymerization and subsequent decane removal. A mechanism for this unique structure is proposed based on experimental evidence. This work is expected to provide useful insights into the preparation of polymer particles with both disc-like shape and multihollow structure.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"23 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693577","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":"Construction of Di- and Tricarboxylic Acid Facilitated Lanthanum-Based Organic Frameworks on Agricultural Waste Biomass for Adsorption and Removal of Phosphorus from Aqueous Solution.","authors":"Xingqun Li,Junjie Yuan,Yao Zhu,Ke Wang,Jizhang Wang,Tao Zhang,Fengxian Qiu","doi":"10.1021/acs.langmuir.5c02547","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02547","url":null,"abstract":"Agricultural advancement boosts food production and economic growth but also causes solid waste and phosphorus pollution. Using agricultural waste to tackle pollution is a sustainable way to reduce environmental harm and promote resource recycling. In this study, lanthanum (La)-based metal-organic frameworks (MOFs) utilizing terephthalic acid (BDC) and 1,3,5-benzenetricarboxylic acid (BTC) as linkers─referred to as La-BDC MOF and La-BTC MOF, respectively─were synthesized on agricultural waste in the form of rapeseed pollen (PL) biomass, resulting in a refined support with enhanced functionality. A variety of advanced instrumental techniques were employed to investigate the formation of PL@La-BDC MOF and PL@La-BTC MOF. The maximum adsorption densities of PO43- achieved under optimal conditions were recorded at 35.8 mg/g for PL@La-BDC MOF (pH 6.0, 25 °C) and 39.4 mg/g for PL@La-BTC MOF (pH 9.0, 35 °C). These values significantly surpass those reported for previously developed La-based adsorbents. The adsorption processes are best described by the pseudo-second-order model, indicating that chemisorption is the predominant mechanism. The presence of PO43- on both the PL@La-BDC MOF and PL@La-BTC MOF following the adsorption process was verified through FT-IR and XPS analyses. In the case of PL@La-BDC MOF, the primary mechanism involves phosphorus anions in solution displacing hydroxyl groups that are coordinated to the central metal, La, through a ligand exchange process coupled with electrostatic attraction. For PL@La-BTC MOF, the main mechanisms involve electrostatic interactions and the chemisorption of carboxyl groups associated with the phosphorus. Moreover, both materials possess enhanced selective adsorption capabilities for phosphorus and exhibit robust anti-interference properties. This work presents an effective and eco-friendly biomass adsorbent for efficient phosphorus adsorption in solutions. It provides insights for utilizing agricultural waste in environmental remediation, enhancing the practical application of natural waste materials.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"26 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693578","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}
LangmuirPub Date : 2025-07-24DOI: 10.1021/acs.langmuir.5c02354
Ning Yan,Jiamin Wu,Li Hua,Ting Gao,Ruixin Liu,Zhaoqing Lu
{"title":"Fabrication of Highly Dispersed Aramid Nanofibers Based on Cation-Exchange Resin as a Proton Donor: Low Energy Consumption, Solvent Closed-Loop Recovery.","authors":"Ning Yan,Jiamin Wu,Li Hua,Ting Gao,Ruixin Liu,Zhaoqing Lu","doi":"10.1021/acs.langmuir.5c02354","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02354","url":null,"abstract":"Aramid nanofibers (ANFs), as novel high-performance organic nanomaterials, face challenges in conventional preparation processes where liquid water as a proton donor induces fiber entanglement and cross-linking, leading to poor dispersion stability, while dimethyl sulfoxide (DMSO) solvent remains difficult to recover due to inefficient separation. This study proposes using weakly acidic solid cation-exchange resins as H+ donors instead of water. Their slow-release characteristics effectively inhibit gelation and eliminate mechanical post-treatment. The resulting ANFs exhibit reduced fiber diameters (9.6 ± 1.49 nm) with more uniform size distribution, corresponding to a film tensile strength of 231 MPa, representing 42.07% enhancement compared to traditional water-based methods. Innovatively, the introduction of solid proton donors enables closed-loop DMSO solvent recovery, maintaining a 90% recovery rate after three cycles, significantly reducing production costs. This dual-functional strategy combining fiber structure regulation with green solvent recycling advantages provides new insights for the large-scale production of high-performance nanomaterials.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"143 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693580","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":"Dual-Functional Antifouling and Antibacterial Coating for Medical PVC Based on Hyaluronic Acid and a Quaternary Ammonium Salt.","authors":"Kaidi Ding,Yaocheng Zhang,Ying Liu,Chuntai Liu,Yuhong Ma,Changyu Shen","doi":"10.1021/acs.langmuir.5c02384","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02384","url":null,"abstract":"Bacteria adhesion, which forms biofilms with multicellular structures on the surfaces of various medical devices, can result in severe infections and even patient mortality. Here, we develop an effective antifouling and antibacterial coating for poly(vinyl chloride) (PVC) substrates. Specifically, the coating is fabricated with anionic polysaccharide hyaluronic acid (HA) and cationic quaternized N,N-dimethylethylenediamine (QDED). The strong hydration capacity of HA significantly reduces the water contact angle of the modified PVC surfaces from 101.4° to 25.4°, enhancing their antifouling performance, while QDED provides direct bactericidal effects. This synergistic combination exhibits robust resistance to both bacterial adhesion and biofilm formation, as demonstrated by extracorporeal circulation and static biofilm resistance assays, better aligning with long-term clinical requirements. This study presents a simple and effective method for modifying PVC surfaces to achieve antifouling and antibacterial properties without compromising biocompatibility, thereby offering potential applications in biomedical devices.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"704 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701206","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}
LangmuirPub Date : 2025-07-24DOI: 10.1021/acs.langmuir.5c02378
Yong Liu,Kangjie Zhou,Zhuo Huang,Heng Luo,Zhengping Fang,Shuaiyuan Wang,Huiyu Yang,Hai Liu
{"title":"Biomimetic Organohydrogels with Tunable Architectures via Controlled Evaporation-Freeze/Thaw Self-Assembly.","authors":"Yong Liu,Kangjie Zhou,Zhuo Huang,Heng Luo,Zhengping Fang,Shuaiyuan Wang,Huiyu Yang,Hai Liu","doi":"10.1021/acs.langmuir.5c02378","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02378","url":null,"abstract":"Conventional hydrogels often face inherent limitations such as dehydration sensitivity, mechanical brittleness, and optical opacity, which severely restrict their advanced applications. In this study, we report a controlled evaporation-freeze/thaw self-assembly strategy for fabricating biomimetic poly(vinyl alcohol)/graphene oxide nanosheet (PG) organohydrogels with tunable architectures. Inspired by natural nacre, homogeneous layered PG organohydrogels are engineered to simultaneously achieve superior mechanical properties and optical transparency, enabled by a nacre-mimetic \"brick-and-mortar\" microstructure with aligned polymer-nanosheet interfaces. Remarkably, post-treatments combining prolonged evaporation and UV-induced reduction synergistically enhance the mechanical performance, yielding a tensile strength of 6.3 MPa and toughness of 43.0 MJ/m3, surpassing those of many reported poly(vinyl alcohol) (PVA)-based hydrogels. Furthermore, the humidity-regulated self-assembly process enables the creation of skin-like gradient PG organohydrogels, mimicking epidermal-dermal structural hierarchies to achieve optimized water retention and mechanical stability. This work establishes a universal platform for designing high-performance hydrogels that reconcile traditionally conflicting properties, offering great potential for applications in flexible electronics, soft robotics, and biointegrated devices that require environmental adaptability.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"19 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701209","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":"Adsorption Structure of Protonated Melamine on Single Crystal Pt Surfaces.","authors":"Haruki Shimada,Yuto Ito,Yuto Hanaoka,Nagahiro Hoshi,Masashi Nakamura","doi":"10.1021/acs.langmuir.5c01815","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01815","url":null,"abstract":"Pt electrodes modified with melamine significantly activates the oxygen reduction reaction (ORR). A comprehensive understanding of the activation mechanism by melamine is essential for the identification of organic additives that can further activate the ORR. Herein, we investigated the coadsorption structure of water with melamine on single-crystal Pt surfaces using Infrared spectroscopy under ultrahigh vacuum conditions. Protonated melamine was dosed on the Pt surfaces using the electrospray method to model the adsorption structure under acidic conditions. The orientation of the adsorbed melamine depends on the atomic arrangement of the Pt substrate as well as the coexistence of water. The melamine-modified Pt electrode obtained by the electrospray method was transferred to an electrochemical cell, and its ORR activity was evaluated. The kinetic current density of the ORR on the transferred Pt was comparable to that obtained by the conventional wetting modification method. This result indicates that the adsorption structure of melamine prepared by the electrospray method is similar to that obtained by the wetting modification.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"75 3 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701207","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}
LangmuirPub Date : 2025-07-24DOI: 10.1021/acs.langmuir.5c02271
Ismail Paykar,John R Regalbuto,Christopher T Williams
{"title":"Surface Area Determination with a Laboratory Scale and Room Humidity from Single-Point BET Analysis of Physisorbed Water.","authors":"Ismail Paykar,John R Regalbuto,Christopher T Williams","doi":"10.1021/acs.langmuir.5c02271","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02271","url":null,"abstract":"For decades, nitrogen physisorption and the BET equation have been utilized for the characterization of the specific surface area of porous materials. Quantifying physisorbed nitrogen at cryogenic conditions is not instrumentally challenging nor relatively expensive, as liquid nitrogen is common to many chemical laboratories, and turnkey commercial physisorption units are within the budget of many research laboratories. However, a great simplification in instrumentation and a decrease in measurement cost can be achieved by physisorption experiments performed at room temperature and pressure. In this work, it was hypothesized that single-point BET analysis can be applied to physisorbed water at room pressure and temperature with humidity as the measure of relative pressure. That is, the surface area of porous materials can be determined with a lab balance to measure mass and a hygrometer to measure humidity at ambient temperature and pressure. The hypothesis was tested first in a thermogravimetric analyzer and second with a simple benchtop scale and a common hand-held hygrometer for six types of alumina beads, three with microporous and mesoporous pore size distributions and three predominantly mesoporous samples. The single-point BET equation is used to correlate the monolayer capacity of adsorbed water with the TGA mass loss and laboratory humidity. By correlating water monolayer capacity with N2 BET surface areas, the effective cross-sectional area of H2O was calculated to be approximately 20 Å2. This value was applied to the single-point BET analysis of humidity versus mass of samples made on the benchtop scale. The mean error of the benchtop balance measurements was 8.5%, suggesting the feasibility of using simple instrumentation under ambient conditions for surface area determination. It is in principle possible to extend the ambient humidity BET to other materials.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"47 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693579","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}