Langmuir [JOURNAL]
Sun
200 papers
Prussian Blue Analogue-Derived NiFe Sulfide Enabling Synergistic ORR/OER via Tuned Electronic Structures for Zn-Air Batteries.
Ge H, Zheng T, Li G … +1 more , Liu Q
Langmuir · 2026 Jun · PMID 42343701 · Publisher ↗
Bimetallic sulfides have emerged as promising four-electron oxygen electrocatalysts for Zn-air batteries (ZABs). Herein, we report a Prussian blue analogue-derived NiFe sulfide embedded in carbon nanocages (NiFeS/CNCs) w...
Bimetallic sulfides have emerged as promising four-electron oxygen electrocatalysts for Zn-air batteries (ZABs). Herein, we report a Prussian blue analogue-derived NiFe sulfide embedded in carbon nanocages (NiFeS/CNCs) with a polydopamine-derived carbon coating. The heterostructure and conductive carbon framework endow the catalyst with enhanced charge transfer and mass transport properties. Importantly, the strong electronic coupling between Ni and Fe sulfides, together with the abundant NiS/FeS phase interfaces, creates a high density of accessible active sites and optimizes the oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) kinetics. As a result, NiFeS/CNCs exhibits excellent bifunctional ORR/OER activity, delivering a low OER overpotential of 167 mV at 10 mA cm (superior to commercial IrO) and an ORR half-wave potential better than Pt/C. During OER, surface reconstruction occurs, where NiS transforms into catalytically active NiOOH species, accompanied by the oxidation of Fe to higher valence states, revealing the dynamic nature of the active phase. As a result, NiFeS/CNCs exhibits excellent bifunctional activity toward ORR and OER. The assembled rechargeable Zn-air battery delivers a peak power density of 105.9 mW cm and demonstrates long-term cycling stability over 1000 h at 5 mA cm, highlighting its potential for practical energy applications.
Bouncing-to-Merging Transition during Droplet Impact on Heated Subcooled Liquid Film.
Asai B, Saha A
Langmuir · 2026 Jun · PMID 42343153 · Publisher ↗
Droplet impact on mildly heated liquid films is important in applications such as cooling and printing. However, most previous studies on heated substrates have focused on superheated conditions, in which the substrate t...
Droplet impact on mildly heated liquid films is important in applications such as cooling and printing. However, most previous studies on heated substrates have focused on superheated conditions, in which the substrate temperature exceeds the liquid saturation temperature, and evaporation strongly alters the impact dynamics. In this study, we experimentally investigate droplet impact on heated subcooled films, where the film temperature remains below saturation, with particular emphasis on how heating modifies the critical conditions for the transition from noncoalescence to coalescence outcomes. Regime maps obtained at different temperatures are used to characterize these transitions. We further derive a scaling relation for interfacial gas layer drainage that incorporates phase-change effects. The combined scaling analysis and experiments with different liquids reveal the key physical mechanisms governing the critical impact speed required for achieving complete coalescence on mildly heated films.
Controllable Preparation of Thiol-Silica Particles via Optimized Water-to-Ethanol Volume Ratio.
Hui S, Zhang X, Han Y … +1 more , Yang W
Langmuir · 2026 Jun · PMID 42341222 · Publisher ↗
This study focuses on investigating the effects of the water-to-ethanol volume ratio on the preparation of thiol-functionalized silica (SH-SiO) particles. Using 3-mercaptopropyltrimethoxysilane (MPTMS) as the silane prec...
This study focuses on investigating the effects of the water-to-ethanol volume ratio on the preparation of thiol-functionalized silica (SH-SiO) particles. Using 3-mercaptopropyltrimethoxysilane (MPTMS) as the silane precursor and ammonia as the catalyst, the size, morphology, and chemical composition of the synthesized SH-SiO particles were systematically characterized across a gradient of water-to-ethanol volume ratios. Raman spectroscopy was utilized to quantitatively analyze the variations in the contents of thiol (-SH) and disulfide (S-S) groups within the SH-SiO matrix. In addition to comprehensive material characterizations, the as-prepared SH-SiO particles were evaluated as dual-functional platforms, which act as both adsorbents for Au ions and carriers for the loading and sustained release of doxorubicin (DOX). Notably, the SH-SiO particles fabricated under the condition of 90% (v/v) water content demonstrated a superior DOX loading capacity and well-regulated release kinetics, highlighting the significant regulatory role of the water content in optimizing the functional performance of SH-SiO particles.
Coimmobilized Pyridoxal 5'-Phosphate and Aminotransferase in a Hydrogen-Bonded Organic Framework for Sustainable Synthesis of Sitagliptin.
Zhang S, Liu S, Yu L … +1 more , Sun Y
Langmuir · 2026 Jun · PMID 42341190 · Publisher ↗
Aminotransferases (ATAs), essential enzymes for the synthesis of chiral amine drugs, play a crucial role in the synthesis of sitagliptin. The catalytic process of ATAs relies on the effective synergistic action of the co...
Aminotransferases (ATAs), essential enzymes for the synthesis of chiral amine drugs, play a crucial role in the synthesis of sitagliptin. The catalytic process of ATAs relies on the effective synergistic action of the cofactor pyridoxal 5'-phosphate (PLP). However, practical applications face challenges such as the poor stability of ATAs and the inefficient recovery of the expensive cofactor PLP. To address these issues, this study proposes a high-efficiency and stable catalytic nanoreactor, ATA&PLP@PAH-BioHOF-1, fabricated by polyelectrolyte poly(allylamine hydrochloride) (PAH)-mediated coencapsulation of both ATA and PLP in a hydrogen-bonded organic framework, BioHOF-1, for the synthesis of sitagliptin. This immobilization system overcomes the limitations of traditional single immobilization methods that were unable to simultaneously maintain enzyme activity and sustainably reuse the cofactor. The system exhibits excellent loading capacity and catalytic performance, achieving a sitagliptin yield of over 95% within 4 h. Additionally, the system demonstrates outstanding stability, retaining 78.3% of its initial sitagliptin yield (95%) after 18 consecutive catalytic cycles (4 h each), with a total PLP turnover number of 175. This study has thus provided an efficient nanoreactor system for the sustainable production of sitagliptin with PLP recycling.
A Comprehensive Review on Light-Driven Detoxification of Emerging Pollutants by Scalable Photocatalytic Systems.
Singh J, Khushboo, Uttam B … +8 more , Kathuria R, Jaiswal NK, Tyagi N, Kumar P, Assadi AA, Hoang TLG, Kumar P, Nguyen-Tri P
Langmuir · 2026 Jun · PMID 42340352 · Publisher ↗
In modern society, due to rapid urbanization and industry growth, different types of pollutants are accumulating in the environment and making it polluted. The excessive discharge of organic toxins into water bodies is a...
In modern society, due to rapid urbanization and industry growth, different types of pollutants are accumulating in the environment and making it polluted. The excessive discharge of organic toxins into water bodies is a major contributor to environmental pollution and poses significant health risks to society and the environment. Organic toxins from various chemical and textile industries pollute our water resources, forming breeding centers for different disease pathogens and adversely affecting the natural water cycle. Therefore, to protect and sustain life on the planet, it should be our prime mandate to preserve, manage, and remediate our limited available water resources. Organic pollutant decomposition is a difficult task due to their complex nature; therefore, it is important to understand the structures of different pollutants to decompose them perfectly. This review highlights the classification of various pollutants, their structural properties, and their possible detoxification processes through the advanced photocatalytic processes. In addition, the elaboration for the decomposition mechanism of the different toxins, ranging from azo dyes, phenols, pesticides, and nitrogen-based compounds to halo-compounds, has been explained. This review also briefly explains the underlying charge transfer mechanism used by different photocatalysts, such as metal oxide semiconductors and 2D-layered nanostructures. A brief description of this mechanism is mentioned in the review, along with the fundamental principle, the role of active redox radicals, such as superoxides and hydroxyl ions, in facilitating the photocatalytic degradation process. Lastly, the creation of robust and scalable photocatalytic systems for practical environmental applications is discussed along with the knowledge gaps and future research goals. This review provides invaluable insight into developing the advanced photocatalyst materials for the targeted pollutants.
Water Bonding on Close-Packed Surfaces of Rare-Earth Metals (Sc, Y, La) Renews Existing Water-Metal Bonding Picture.
Wu Q, Guo Y, Li J
Langmuir · 2026 Jun · PMID 42339810 · Publisher ↗
Our knowledge of water bonding on metal surfaces is ruled by the coexistence of covalent and electrostatic nature in water-metal interactions, which leads to the well-known, preferred flat geometry on transition metal su...
Our knowledge of water bonding on metal surfaces is ruled by the coexistence of covalent and electrostatic nature in water-metal interactions, which leads to the well-known, preferred flat geometry on transition metal surfaces. Using density functional theory (DFT) calculations, herein we have shown that this picture has to be modified for water bonding on Sc(0001), Y(0001), and La(0001), where upright water orientation has been surprisingly found to preferentially coexist with the flat geometry on the rare-earth metal surfaces. Our investigations have proved that both water orientations on the rare-earth metal surfaces originate from unique bonding mechanisms that do not exist in water adsorption on any late transition metal surfaces. In this unique bonding picture, covalent components are evidently absent in the water-metal interactions, which are overwhelmingly dominated by the first-order quantum electrostatics featured by two nearly separated potential wells in the water-metal bonds and by the second-order quantum electrostatics featured by alternating charge depletion and accumulation regions in interference. The new picture not only advances our understanding of how water makes bonds with earlier transition metal surfaces but also lays a physical basis for improving catalytic performance of the rare-earth-metal-based green catalysts for clean energy.
Non-Symmetrical Low-Voltage Negative Barrier Height Breast Cancer-Associated VOCs Sensing Different-Sized Gold Nanoflower-Functionalized ZnO Thin Films Prepared by a Low Cost Chemical Method.
Kakarla V, Yadav AB, Dhulipalla VR … +1 more , Checker R
Langmuir · 2026 Jun · PMID 42339806 · Publisher ↗
This work reports a high response (∼90,000) from a sol-gel synthesized ZnO thin film achieved through surface functionalization with gold nanoflowers (AuNFs). The device showed an asymmetric voltage response and exhibite...
This work reports a high response (∼90,000) from a sol-gel synthesized ZnO thin film achieved through surface functionalization with gold nanoflowers (AuNFs). The device showed an asymmetric voltage response and exhibited higher sensitivity at very low voltages than at higher voltages. Previous studies used ZnO functionalized with symmetrical (spherical) gold nanoparticles, but their sensor response was nearly 1000 times lower than what we achieved. While standard gold nanoparticles are symmetrical, AuNFs grown with AgNO are asymmetrical. This structural asymmetry creates an asymmetrical response to applied voltage, significantly boosting the sensor's overall performance. For the first time, detached AuNF petals functionalized on ZnO showed a very high response to volatile organic compounds (VOCs). Thiol-free AuNFs were functionalized to the ZnO surface using a low-cost sol-gel drop coating method instead of expensive physical techniques. X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray, and X-ray diffraction measurements were used to analyze AuNFs on the ZnO surface. These studies revealed that nanoflower size governed the loading, which increased up to a threshold value. Beyond this size, the nanoflowers were sparsely distributed, leaving mainly detached nanopetals on the ZnO surface. These sparse nanopetals were responsible for the exceptionally high response (∼90,000) compared to previously reported values. The nanoflower shape and size were controlled by the silver ion concentration in the gold colloidal solution. We fabricated low power gas sensors using AuNF-functionalized ZnO thin films with patterned aluminum electrodes. These sensors showed exceptionally high response and selectivity toward 2-ethyl-1-hexanol, a VOC associated with breast cancer. The sensor demonstrated high sensitivity at a low applied voltage of 0.05 V. Additionally, a negative contact barrier influenced by the size of the AuNFs and the VOCs was observed, which reflects the inter particle barrier height and conductivity.
Interdiffusion at the Molybdenum-TEOS Interface in Flat and Nanostructured Systems during Graphene CVD.
Zappalà S, Scuderi M, Mirabella S … +7 more , Costantino D, Pellegrino AL, Sciuto A, Compagnini G, Privitera V, Rimini E, D'Arrigo G
Langmuir · 2026 Jun · PMID 42339804 · Publisher ↗
The integration of graphene with metallic layers provides a versatile platform for hybrid materials in electronic and optical technologies. Here, we investigate interdiffusion phenomena at the molybdenum-tetraethyl ortho...
The integration of graphene with metallic layers provides a versatile platform for hybrid materials in electronic and optical technologies. Here, we investigate interdiffusion phenomena at the molybdenum-tetraethyl orthosilicate (TEOS)-derived SiO interface during graphene growth by chemical vapor deposition (CVD). Graphene was grown on a 35 nm thick continuous sputtered molybdenum film and on nanostructured molybdenum patterns defined by electron beam lithography, both supported on a 1.6 μm thick TEOS-derived SiO layer. The samples were characterized by Rutherford backscattering spectrometry, secondary ion mass spectrometry, X-ray diffraction, and scanning and transmission electron microscopy. On the flat molybdenum film, the CVD process leads to the formation of Mo-Si and Mo-C phases and to the growth of approximately 15 graphene layers. In contrast, nanostructured molybdenum undergoes solid-state dewetting, resulting in morphological instability and the formation of only about 5 graphene layers. These results demonstrate that catalyst geometry critically influences graphene thickness: interdiffusion is predominantly unidirectional in planar films, whereas it becomes multidirectional in confined nanostructures, leading to partial carbon loss and enhanced silicon incorporation. The loss of structural homogeneity below a critical lateral dimension highlights the key role of interfacial diffusion and surface morphology in controlling graphene growth on metal-oxide substrates.
Modulation of Exciton Transport in Few-Layer and Bulk Tungsten Disulfide under Hydrostatic Pressure.
Zhang Y, Wu W, Zhang H … +8 more , Wen J, Huang M, Wang J, Ma X, Yang Y, Yu X, Wang Y, Zhang X
Langmuir · 2026 Jun · PMID 42339798 · Publisher ↗
Transition-metal dichalcogenides (TMDs) are atomically thin semiconductors with outstanding optoelectronic properties, but their applications in high-performance optoelectronic devices are often limited by low intrinsic...
Transition-metal dichalcogenides (TMDs) are atomically thin semiconductors with outstanding optoelectronic properties, but their applications in high-performance optoelectronic devices are often limited by low intrinsic mobility. Using a diamond anvil cell (DAC) combined with transient absorption spectroscopy, pressure-dependent exciton transport and relaxation dynamics were systematically investigated in few-layer (5 layers) and bulk WS. Within the pressure range of 0 to 2 GPa, hydrostatic pressure induces a nonmonotonic evolution of exciton mobility, reaching maximum enhancements of approximately 3 times and 5 times in few-layer and bulk WS, respectively. Simultaneously, the exciton lifetimes are reduced by approximately 4 times and 7 times. Complementary photoluminescence (PL) and Raman measurements reveal that pressure-enhanced interlayer coupling and lattice compression jointly modulate the electronic structure and exciton relaxation pathways, leading to accelerated relaxation dynamics. The nonmonotonic variation in exciton mobility can be attributed to a competitive mechanism between pressure-regulated band broadening effects (reduced effective mass and enhanced dielectric shielding) and increased defect scattering and lattice scattering. It is worth noting that after pressure release, the mobility remains higher and the lifetime is slightly shorter than the initial values. These results reveal the correlated evolution of exciton mobility and lifetime in WS, identify an optimal pressure window for exciton transport, and elucidate the mechanism of pressure-regulated exciton dynamics, providing insights into the development of high-mobility, fast-response optoelectronic devices.
Easily Prepared and Performance-Enhanced Superhydrophobic, Photothermal, Nonfluorinated Nanocarbon/Nonmetallic Mineral@Long-Chain Alkyl-Containing Polymer-Coated Surface for Protective Textile and Textile Wastewater Treatment.
Chen C, Wang Y, Liu H … +6 more , Guo Z, Chen Y, Wang T, Hu J, Jia L, Jiang L
Langmuir · 2026 Jun · PMID 42339742 · Publisher ↗
By mixing carbon nanotubes, carbon nanospheres, carborundum, or attapulgite into an ethanol system dissolved with dipentaerythritol penta-/hexa-acrylate, branched polyethylenimine, and tetradecylamine, the uncatalyzed on...
By mixing carbon nanotubes, carbon nanospheres, carborundum, or attapulgite into an ethanol system dissolved with dipentaerythritol penta-/hexa-acrylate, branched polyethylenimine, and tetradecylamine, the uncatalyzed one-step in situ reaction of a long-chain alkyl-containing polymer was produced on the above-blended matrices to construct a superhydrophobic, photothermal, nonfluorinated organic-inorganic hybrid material at room temperature. The optimal hybrid material-coated fabric had 155.0° contact angle and 2.0° sliding angle, and its surface temperature increased to 71.6 °C under irradiation (1 sun, 300 s); meanwhile, complete repellency of such a coating to 95 °C water was also reached (contact angle: 152.6°, sliding angle: 2.1°), affirming that a robust air layer, between the solid and liquid, existed in the coating product; given this, the above-mentioned coated fabric efficiently provided protective benefits, including icing delay, photothermal deicing, snow removal, hot-sewage repellency, and antimicrobial properties. Based on the substrate design idea, the poly(vinyl alcohol) sponge was used for coating with the self-manufactured anti-icing and hot sewage-repellent hybrid product to form a simple photothermal evaporator; its evaporation rates for desalinating simulated seawater and saliferous reactive textile-dyeing wastewater were 2.19 kg/mh and 2.21 kg/mh, respectively. Even when in contact with 95 °C acid dyeing residual liquor and 0 °C azoic dyeing residual liquor, this self-floating evaporator could achieve a remarkable purification treatment effect and always keep its Janus superwetting property. We believe that the easy preparation and performance enhancement strategy for superhydrophobic, photothermal, nonfluorinated organic-inorganic hybrid materials, based on synergy between hot-water repellency and substrate design, coincides with technology trends of cleaner production and function integration, which has important implications for exploiting wide-temperature range antiwetting, multipurpose products.
Ion Transport in Charged Membranes: Linking Electric-Field-Driven Mechanisms to Pore Size via Perturbation Analysis.
Romero Zavala PN, Ganguly A, Vigil-Fowler D … +2 more , Smith WA, Gupta A
Langmuir · 2026 Jun · PMID 42339697 · Publisher ↗
Ion-exchange membranes are a critical component in electrochemical systems. Nevertheless, the understanding and modeling of ion transport within these porous structures have been limited by particular complexity reductio...
Ion-exchange membranes are a critical component in electrochemical systems. Nevertheless, the understanding and modeling of ion transport within these porous structures have been limited by particular complexity reductions, either ignoring the dimensionality of their porous network architecture or imposing geometric assumptions (i.e., overlapping double layers). Before addressing this morphology-transport gap, a framework that relates the driving forces of transport to the geometry of a single pore is required. In this work, our modeling domain consists of a two-dimensional single pore with charged walls, connecting two identical electrolyte reservoirs. Using the Poisson-Nernst-Planck equations and regular perturbation theory, we decouple the electric fields and analyze the driving forces of ion transport, specifically electromigration and induced electroosmosis within the pore. These processes are described as analytical functions of the interaction aspect ratio, κ, defined as the ratio of the pore radius to the Debye length. Using this parameter, our study (i) describes the interplay between electromigrative and electroosmotic mechanisms that set ionic conductivity, (ii) identifies a dimensionless group of intrinsic electrolyte properties that indicates the predominant driving force, and (iii) provides a qualitative, confinement-dependent perspective on selectivity in ion-conducting membranes.
BiOBr/g-CN Planar Heterostructures toward Enhanced Tetracycline Hydrochloride Removal.
Wang S, Wang J, Yang P … +1 more , Zhang X
Langmuir · 2026 Jun · PMID 42339658 · Publisher ↗
The redox ability of photocatalysts is a key to the degradation of tetracycline hydrochloride (TCH) which resulted in serious environmental problems. In this paper, narrow band gap BiOBr nanoplates were grown on superior...
The redox ability of photocatalysts is a key to the degradation of tetracycline hydrochloride (TCH) which resulted in serious environmental problems. In this paper, narrow band gap BiOBr nanoplates were grown on superior thin graphitic carbon nitride (g-CN) nanosheets to increase light absorption and enhance redox ability for TCH removal. Meanwhile, g-CN nanosheets were created by a two-step thermal polymerization at 600 and 700 °C, respectively. The deposition of layered BiOBr was finished along the surface of g-CN nanosheets by a direct wet-chemical precipitation. BiOBr nanoplates were in situ grown on g-CN nanosheets to create a well-developed interface and form S-scheme BiOBr/g-CN heterostructures with enhanced photocatalytic performance. Visible light-derived photocatalytic tests indicated that the heterostructure sample created using optimized conditions revealed excellent performance, in which Rhodamine B of 10 mg/L was completely degraded within 9 min (10 mg catalyst added). TCH (50 mg/L) of 80% was degraded within 60 min with a degradation rate of 2.4 × 10 min, which was 6 and 3.4 times of those of pristine g-CN nanosheets and BiOBr, respectively. The free radical capture test suggested that superoxide radicals dominated TCH degradation, and cyclic stability test indicated the degradation rate was kept 72% after 6 cycles. The S-scheme pathway in the heterostructure-enhanced charge separation and retained high redox ability for photocatalytic degradation of pollutants. These results supplied useful approaches for the photocatalysts with a high redox ability.
Non-Contact Mechanics of Soft and Liquid Interfaces by Hydrodynamic Confinement Using a Frequency-Modulated AFM.
Corral L, Curtil C, Lagaize M … +2 more , Leonetti M, Klein HR
Langmuir · 2026 Jun · PMID 42339599 · Publisher ↗
Measuring the mechanical response of liquid interfaces without direct contact remains a major experimental challenge, particularly in liquid-liquid systems where no solid reference exists. Here, we develop a frequency-mo...
Measuring the mechanical response of liquid interfaces without direct contact remains a major experimental challenge, particularly in liquid-liquid systems where no solid reference exists. Here, we develop a frequency-modulation atomic force microscopy (FM-AFM) method to probe liquid interfaces through the hydrodynamic confinement of a viscous liquid film between an oscillating probe and the interface. This approach provides simultaneous access to the in-phase and dissipative components of the effective mechanical response under confinement. Initially, the method is validated on a liquid-solid interface, where the measured confinement thickness and the evolution of the mechanical impedance are consistent with elastohydrodynamic theory over nearly one decade in elastic modulus. It is then applied to a liquid-liquid interface, which exhibits a predominantly viscous response with a finite in-phase contribution and a confinement thickness in the micrometric range. These results show that hydrodynamic confinement provides a sensitive, noncontact approach to compare the mechanical responses of soft and liquid interfaces, and opens perspectives for investigating complex and highly deformable systems such as polymer films, biological membranes, and rafts of nanoparticles.
Chitosan-Tannic Acid-Encapsulated Polydopamine Nanocontainers for pH-Responsive Self-Healing Waterborne Epoxy Coatings.
Song R, Ma X, Wu Y … +6 more , Ye Z, Chen C, Han W, Liu J, Li W, Li Q
Langmuir · 2026 Jun · PMID 42336798 · Publisher ↗
Waterborne epoxy coatings are distinguished by their eco-friendly properties and low volatile organic compound emissions. However, conventional waterborne epoxy coatings often exhibit insufficient barrier performance and...
Waterborne epoxy coatings are distinguished by their eco-friendly properties and low volatile organic compound emissions. However, conventional waterborne epoxy coatings often exhibit insufficient barrier performance and weak self-healing capability, resulting in poor long-term anticorrosion efficiency. To address these drawbacks, this work synthesized a novel MPDA@8-HQ@CS-TA composite, aiming to fabricate a high-performance coating with improved anticorrosion properties, pH responsiveness, and UV weathering resistance. EIS results revealed that the MPDA@8-HQ@CS-TA composite-modified waterborne epoxy coating exhibited remarkably improved barrier performance and self-healing ability. After 40 days of immersion in a corrosive medium, the impedance modulus of the MPDA@8-HQ@CS-TA composite-modified waterborne epoxy coating remained at 5.75 × 10 Ω·cm, significantly outperforming that of the pure epoxy coating (1.227 × 10 Ω·cm). Driven by the decomposition of the CS-TA encapsulation layer, the MPDA@8-HQ@CS-TA composite-modified waterborne epoxy coating also presents remarkable pH-triggered release behavior under acidic conditions. The results from salt spray and ultraviolet accelerated aging trials validate the outstanding weatherability and sustained anticorrosion properties of the developed coating system. This work proposes a promising method for the preparation of sustainable and eco-friendly intelligent anticorrosion coatings.
A Nonhazardous Alternative to Mercury in Liquid Intrusion Porosimetry: Systematic Study of Intrusion/Extrusion Behavior of a Gallium-Based Liquid Metal (eGaInSn) into Meso- and Macroporous Silica, Alumina, and Carbon Materials.
Schuss A, Söllner J, Thommes M
Langmuir · 2026 Jun · PMID 42335421 · Publisher ↗
Mercury porosimetry is considered the standard method for the characterization of macroporous solids. However, health risks and environmental concerns make a replacement for mercury sought-after. Despite many advances in...
Mercury porosimetry is considered the standard method for the characterization of macroporous solids. However, health risks and environmental concerns make a replacement for mercury sought-after. Despite many advances in various techniques, so far, no alternative method is available. Here, we introduce a novel method using, instead of mercury, eGaInSn (Galinstan), a nonhazardous, eutectic gallium alloy, liquid at ambient temperatures, which is already widely used as a replacement for mercury (e.g., thermometers). We utilize a conventional porosimeter with only minor but necessary modifications in sample cell design and filling procedure. To evaluate its potential for pore characterization, we systematically studied the phase and wetting behavior of eGaInSn via intrusion/extrusion experiments in a series of well-defined meso- and macroporous silica (controlled pore glasses), alumina, and disordered carbon materials, including certified reference materials, exhibiting mode pore sizes from the narrow meso- (<20 nm) to the macropore range (1.7 μm). Our results suggest that the intrusion mechanism of eGaInSn represents, analogue to mercury, a confinement-induced shift of the vapor-liquid phase transition of a nonwetting fluid to pressures larger than the saturation vapor pressure. Comparing the pore size/volume distributions obtained by eGaInSn reveals excellent agreement with mercury porosimetry. Furthermore, we systematically studied the effect of pretreatment conditions of the porous materials, e.g., degassing temperature, on the intrusion/extrusion behavior of eGaInSn and find that the degassing temperature has essentially no influence on the eGaInSn intrusion pressure and curve, but significantly affects the extrusion behavior. We demonstrate that, under certain, well-defined experimental conditions, the intrinsic eGaInSn intrusion-extrusion hysteresis loop is revealed, which contains important additional textural information. In conclusion, our work can be considered the first systematic study of the effect of confinement on the wetting and phase behavior of eGaInSn utilizing intrusion/extrusion measurements with a novel method offering potential to finally replace toxic mercury in the analysis of meso- and macroporous solids.
Hysteresis Phenomenon Coupled with Capillary Phase Transition of N/CH Binary Mixtures in Cylindrical Nanopores.
Qiu X, Liu Y, He X … +1 more , Zheng S
Langmuir · 2026 Jun · PMID 42335401 · Publisher ↗
Capillary condensation/evaporation-induced hysteresis is a fundamental characteristic of confined fluid-phase transitions. Although extensively studied for pure fluids, the hysteresis behavior of confined fluid mixtures...
Capillary condensation/evaporation-induced hysteresis is a fundamental characteristic of confined fluid-phase transitions. Although extensively studied for pure fluids, the hysteresis behavior of confined fluid mixtures remains poorly understood. Here, grand canonical Monte Carlo-molecular dynamics (GCMD) simulations are employed to investigate adsorption-desorption hysteresis of N/CH mixtures in cylindrical carbon nanopores. While pure CH and N exhibit the expected pore-size- and temperature-dependent hysteresis behavior, binary mixtures show strongly composition-dependent phase transition characteristics. Competitive adsorption significantly modifies the hysteresis behavior and can either suppress or enhance the metastable capillary phase transitions. As the N concentration increases, the capillary phase-transition pathway shifts from CH-dominated condensation to co-condensation and co-evaporation of both components. Consequently, the apparent hysteresis critical pore diameter () exhibits a nonmonotonic dependence on composition, whereas the apparent hysteresis critical temperature () decreases monotonically with increasing N content. These findings demonstrate that adsorption-desorption hysteresis in confined fluid mixtures cannot be inferred from pure-fluid behavior alone but instead emerges as a collective phenomenon governed by competitive adsorption and composition redistribution, which fundamentally alters both the capillary phase-transition pathway and the apparent hysteresis criticality.
Thermodynamic Insights into Anoxic Arsenic(III) Oxidation: The Critical Role of Oxygen Vacancies in Regulating Redox Reactivity of Fe(II) Bound to Fe(III) (Oxyhydr)oxide Redox Couples.
Liu J, Hou J, Zheng S … +4 more , Xiong J, Wang M, Kappler A, Tan W
Langmuir · 2026 Jun · PMID 42334957 · Publisher ↗
Ferrous iron (Fe(II)) bound to Fe(III) minerals redox couples are ubiquitous in sediments and groundwater, playing a crucial role in arsenic migration, transformation, and associated risks. Although Fe(III) oxides-Fe(II)...
Ferrous iron (Fe(II)) bound to Fe(III) minerals redox couples are ubiquitous in sediments and groundwater, playing a crucial role in arsenic migration, transformation, and associated risks. Although Fe(III) oxides-Fe(II) couples are well known for their reductive transformation of pollutants, the thermodynamic mechanisms driving anoxic As(III) oxidation observed in these systems remain poorly understood. In this study, we combined high-resolution transmission electron microscopy-selected area electron diffraction mapping, Mössbauer spectroscopy, and density functional theory calculations to investigate whether anoxic As(III) oxidation in hematite-Fe(II) couples is influenced by oxygen vacancies (Ov), an intrinsic characteristic of iron (oxyhydr)oxide minerals. Batch experiments demonstrated that Ov in hematite significantly enhanced the As(III) oxidation efficiency (62.7%) compared to defect-free hematite (45.9%) at pH 6 with 0.2 mM Fe(II). Spectroscopic and microscopic analyses revealed recrystallization processes that generated active metastable iron phases after Fe(II) adsorption, acting as electron acceptors for As(III) oxidation. Notably, the defective hematite-Fe(II) couples generated a higher content of active iron phase compared to their defect-free counterparts, which was attributed to thermodynamically favorable electron transfer between Fe(II) and the defective hematite due to the relatively higher redox potential of defective hematite ( = +1297 mV +670 mV). These findings provide evidence of the thermodynamically driven anoxic transformation of As(III), emphasizing the critical role of oxygen vacancies in regulating redox reactivity in oxide-Fe(II) systems.
Dynamics of Moving Contact Line Influenced by Rotational Forcing.
Raveendar G, Mehta SK, Mondal PK
Langmuir · 2026 Jun · PMID 42334891 · Publisher ↗
The present study explores the influence of surface wettability and viscosity ratio on capillary filling, wetting, and interface evolution of an immiscible binary system in a rotational microfluidic system. A thermodynam...
The present study explores the influence of surface wettability and viscosity ratio on capillary filling, wetting, and interface evolution of an immiscible binary system in a rotational microfluidic system. A thermodynamically consistent phase-field model is used to capture the spatiotemporal evolution of the interface, influenced by the complex interplay among the rotational force, surface tension, and viscous resistance. A comprehensive regime map, characterized by the local Weber number, is developed to classify the distinct interfacial transitions. Unlike classical pressure-driven systems that yield uniform centerline viscous fingering, we demonstrate that rotational forcing introduces velocity-dependent transverse Coriolis momentum. This Coriolis force acts as an active symmetry-breaking mechanism, laterally shifting the advancing fluid and driving a skewed morphological distortion. Under hydrophilic conditions, the interface transitions from a concave shape through weakly and strongly centrifugal force-dominated regimes as the rotational Reynolds number increases. Conversely, hydrophobic conditions maintain a convex meniscus, accelerating these regime transitions. Moreover, increasing the viscosity ratio significantly delays regime transitions because of increased viscous resistance from the displaced fluid. For hydrophobic substrates, overcoming this resistive capillary force requires a critical rotational Reynolds number to initiate flow, which scales with both the contact angle and the fluid properties. We believe that the findings of this study will advance the fundamental understanding of interfacial dynamics in rotational microfluidics and provide a foundation for the rational design of next-generation centrifugal lab-on-chip devices, typically used in diagnostics, sample preparation, and biochemical assays.
Iron(III)-Doped Cuprous Oxide Nanoparticles Are Used for Nonenzymatic Glucose-Sensitive Detection.
Xu X, Qin Y, Wang M … +1 more , Qi Y
Langmuir · 2026 Jun · PMID 42334888 · Publisher ↗
Nonenzymatic glucose sensors utilizing CuO as the active material are characterized by low cost, nontoxicity, and environmental friendliness, yet they suffer from limited electrical conductivity. In this work, a series o...
Nonenzymatic glucose sensors utilizing CuO as the active material are characterized by low cost, nontoxicity, and environmental friendliness, yet they suffer from limited electrical conductivity. In this work, a series of iron(III)-doped cuprous oxide (Fe-CuO) nanomaterials, where "" refers to the nominal doping amount, were synthesized via a mild solution-based approach within a metal ion slow-release system constructed with sodium citrate. The performance of these materials as enzyme-free glucose sensors was systematically investigated. Characterization results indicate that Fe doping effectively modulates the crystal growth of CuO, leading to a morphological evolution from well-defined cubes to truncated cubes with roughened surfaces and abundant edges, accompanied by a shift in partially exposed crystal facets from (100) to (111). Regulated by sodium citrate, the particle size was significantly reduced to approximately 250 nm, with Fe uniformly incorporated into the CuO lattice in the form of Fe. Electrochemical analyses reveal that an optimal level of Fe doping (Fe-CuO) markedly enhances the electron transfer capability and electrochemical active surface area of the material, which can be attributed to the introduction of impurity energy levels and the establishment of complementary redox couples involving Fe/Fe and Cu/Cu. The optimized sample exhibits an extensive linear detection range (0.05-9.65 mM), superior sensitivity (1486 μA·mM·cm), and remarkable stability. This study offers an effective strategy for precisely tailoring the microstructure and enhancing the electrochemical properties of metal oxides through transition metal doping, thereby facilitating the development of high-performance sensing materials.
Identification and Intelligent Prediction of Microscopic Residual Oil Distribution Based on the TransUNet Neural Network.
Bai Y, Li R, Xu X … +5 more , Guo D, Zhang N, Sun Y, Yang Y, Bai M
Langmuir · 2026 Jun · PMID 42334886 · Publisher ↗
The morphological distribution and classification of remaining oil are of great significance to oilfield development. Traditional identification and classification methods are limited by large manual errors, low intellig...
The morphological distribution and classification of remaining oil are of great significance to oilfield development. Traditional identification and classification methods are limited by large manual errors, low intelligence, and insufficient precision, and fail to accurately identify microscale remaining oil below 10 μm. This paper proposes a deep learning-based method for remaining oil recognition and classification using TransUNet as the backbone network, combined with image augmentation and Transformer multihead attention mechanism to enhance feature extraction and classification performance. Results show that the proposed method achieves an overall classification accuracy of 94%, with effective recognition thresholds of 3.09 μm for film-like remaining oil and 1.54 μm for drip-like remaining oil. In addition, different displacement mechanisms result in significantly different occurrence states and dynamic evolution laws of remaining oil: water flooding relies on mechanical scouring, polymer flooding depends on viscosity improvement and profile control, while surfactant flooding achieves efficient displacement by reducing interfacial tension and generating emulsification. Among them, remaining oil formed by surfactant flooding is mainly droplet-shaped and easy to be displaced, which reveals its superior displacement effect from a microscopic perspective and provides a basis for formulating targeted oilfield development measures.
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