Langmuir最新文献

{"title":"Polytriazole Binders Based on Chemical Modification Strategies: Microphase Separation Optimization and Performance Enhancement","authors":"Wenwen Deng, Zhiyuan Zhang, Zeyu Wang, Chengyuan Hua, Runxin Wang, Yousheng Qiu, Chongwei An, Jingyu Wang, Baoyun Ye","doi":"10.1021/acs.langmuir.5c00918","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00918","url":null,"abstract":"A traditional butahydroxy solid propellant is widely used because of its good energy and safety properties, but its isocyanate curing system is easily affected by water and has low combustion efficiency during curing. In this paper, by means of the chemical modification method, toluene 2,4-diisocyanate was first used to seal the hydroxy-terminated polybutadiene (HTPB), and then the alkynyl group was introduced to successfully prepare a new alkyny-terminated polybutadiene adhesive (AT-HTPB), which is not subjected to moisture during the curing process and has better comprehensive properties. The process of reaction heat release was monitored online by a fully automatic chemical reactor, which proved that the synthesis path was safe and efficient. The structure of AT-HTPB was characterized by Fourier infrared spectroscopy (FT-IR), hydrogen nuclear magnetic resonance spectroscopy (¹H NMR), and gel chromatography (GPC). The results showed that the prepared AT-HTPB had a high purity and good consistency. Differential scanning calorimetry (DSC), dynamic thermomechanical analysis (DMA), and thermogravimetric mass spectrometry (TGA-MS) showed that AT-HTPB had better thermal stability and retained the advantages of lower glass transition temperature (<i>T</i>_g) than HTPB. It is observed that AT-HTPB has more obvious microphase separation through an atomic force microscope (AFM), and the mechanical properties of AT-HTPB elastomers are more superior than those of AT-HTPB elastomers. Then, AT-HTPB was applied to the solid propellant and the combustion performance was compared with that of the BUtadiol propellant. The results showed that the AT-HTPB propellant had a more concentrated flame and better bonding effect. This study proves that AT-HTPB as a new adhesive has broad application prospects in solid propellants.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"51 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153571","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":"Photoelectrochemical Pb2+ Analysis Based on the Effective Signal Quenching of CoPP toward Ag@PTCA Schottky Junction","authors":"Jie Zhang, Jiapeng Wang, Guohao Shen, Lingying Xia, Rongxing Zhou, Mengjie Li","doi":"10.1021/acs.langmuir.5c01658","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01658","url":null,"abstract":"In this work, a specific and sensitive photoelectrochemical (PEC) biosensor has been constructed for the lead ion (Pb²⁺) assay by applying a silver nanoparticles@3,4,9,10-perylene tetracarboxylic acid (Ag@PTCA) Schottky junction as the signal substrate and cobalt tetraphenyl porphyrin (CoPP) as the signal quencher integrated with nucleic acid double-amplification strategies. The strong unidirectional conductivity of the Shottky junction and the surface plasmon resonance (SPR) effect of Ag NPs significantly enhanced the charge separation capability within the Ag@PTCA Schottky junction, thus providing a robust signal substrate for this biosensor. CoPP embedded within the double-strand DNA structure acted as the effective quencher. The double-amplification strategies containing rolling circle amplification (RCA) and DNAzyme-assisted Pb²⁺ cycling reaction were exquisitely designed and applied for upgrading the detection characteristics of the biosensor. The experimental findings demonstrated that the PEC signal was progressively recovered as the Pb²⁺ concentration increased from 500 fM to 5 μM, and the detection limit was 166.7 fM under optimal conditions, thus endowing the biosensor with the benefits of strong specificity and high selectivity. This method provides promising opportunities for detecting various heavy-metal ions in the fields of environmental monitoring, biological analysis, and medical research under complex conditions.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"151 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153573","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":"Molecular Dynamics Insights into the Stability of Bulk Hydrogen Nanobubbles in Water and Methanol","authors":"Jianping Yuan, Shiduo Wang, Haiqiao Wei, Gequn Shu, Jiaying Pan","doi":"10.1021/acs.langmuir.5c01659","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01659","url":null,"abstract":"Bulk hydrogen nanobubbles (NBs) play a key role in hydrogen generation and utilization. However, their stabilization mechanisms in different solvents remain not fully understood. This study employs molecular dynamics simulations to investigate the stability and evolution of bulk hydrogen NBs in water and methanol, with experimental measurements providing validation. The results show that NBs in methanol tend to dissolve at lower initial gas densities, indicating a lower stability compared to those in water. Under stable conditions, approximately 80% of hydrogen molecules remain inside NBs in water, while only about 40% remain in methanol, consistent with methanol’s higher hydrogen solubility observed experimentally. Further analysis reveals that hydrogen NBs in water exhibit a thinner gas–liquid interface as well as lower internal pressure and gas density, mainly related to its lower hydrogen solubility. Utilizing mechanical equilibrium and critical radius theory, we identify the hydrogen concentration thresholds for NB stability to be 0.96–1.44 mol/L in water and 2.69–2.88 mol/L in methanol. Additionally, hydrogen molecules in methanol exhibit more vigorous motion, stronger gas–liquid interactions, and a weaker hydrogen bond network. This study provides molecular-level insights into the stabilization of bulk hydrogen NBs in different solvents.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"23 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153651","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":"Superhydrophilic Quaternized Electrospun Nanofibers for Fast and Efficient Removal of Cr(VI) from Metallurgical Wastewater","authors":"Hongxing He, Shunfei Li, Xintao Yang, Ying Xu, Siqing Ye, Haonan Dong, Mengye Yang, Ni Yang, Yi Zhang, Zhifeng Nie","doi":"10.1021/acs.langmuir.5c01799","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01799","url":null,"abstract":"Due to the low adsorption capacity, slow adsorption kinetics, and insufficient selectivity of conventional adsorbents in highly acidic environments, therefore, the removal of highly toxic Cr(VI) from industrial metallurgical wastewater remains a great challenge. Herein, a novel superhydrophilic quaternized nanofiber adsorbent was synthesized using electrospinning technology. The superhydrophilic nanofiber adsorbent facilitated water molecule movement during the adsorption process, which increased the system’s free energy and thus promoted the efficient and rapid selective removal of Cr(VI). The adsorbent was completely wetted within 0.06 s and reached a maximum adsorption capacity of 450.33 mg/g in a Cr(VI) solution with an initial concentration of 400 mg/L and equilibrated within 20 min. Adsorption experiments showed that the correlation coefficients of the pseudo-secondary kinetics and Langmuir model of the process were as high as <i>R</i>₂² = 0.994 and <i>R</i>_L² = 0.971–0.993, respectively, suggesting that the adsorption process is mainly surface adsorption driven by chemisorption. Moreover, the adsorption mechanism by Zeta potential analysis and XPS and DFT simulations revealed that the selective adsorption for Cr(VI) is the synergistic action of ion exchange and coordination by electrostatic attraction. In addition, the dynamic column adsorption test demonstrated that the adsorbent could adsorb 6000 times its own mass of Cr(VI) ions in metallurgical wastewater, the recovery of Cr(VI) by nanofibers could still reach 89.7% after five cycles, and the removal efficiency was as high as 95.64% in real metallurgical wastewater, which highlighted the potential of its practical application.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"4 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153652","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}