Pub Date : 2025-03-27DOI: 10.1021/acs.langmuir.5c00346
Kaixuan Zhang, Dongshuai Hou, Shaochun Li, Muhan Wang
Polymer concrete (PC) has attracted considerable interest for its excellent deformation resistance and durability. However, the mechanical drawbacks of polymers, particularly their limited compressive strength, constrain the wider application and design flexibility of PC. While experimental techniques such as X-ray diffraction and scanning electron microscopy provide insights into nanoparticle interactions within the polymer matrix, they lack the resolution to fully elucidate nanoscale mechanisms. To bridge this gap, this study utilizes molecular dynamics (MD) simulations to analyze the shearing behavior of carbon nanoparticle (CNP)-reinforced PC composites. MD simulations allow for atomic-level insights into the interactions between CNPs and the polymer matrix, providing a more detailed understanding of how surface-modified CNPs enhance mechanical properties. Our results show that surface-modified CNPs influence the distribution and conformation of epoxy within the PC system. Amino-functionalized CNPs strengthen the epoxy and calcium silicate hydrate (C–S–H) interface by facilitating calcium–oxygen bond formation. These interactions play a crucial role in improving the mechanical properties of PC. This study provides a fundamental understanding of how surface-modified CNPs reinforce PC and offers valuable insights for optimizing the performance of CNP-reinforced cementitious composites.
{"title":"Molecular Dynamics Simulation of Polymer Concrete Enhanced by Carbon Nanoparticles: Effect of Surface Functional Groups","authors":"Kaixuan Zhang, Dongshuai Hou, Shaochun Li, Muhan Wang","doi":"10.1021/acs.langmuir.5c00346","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00346","url":null,"abstract":"Polymer concrete (PC) has attracted considerable interest for its excellent deformation resistance and durability. However, the mechanical drawbacks of polymers, particularly their limited compressive strength, constrain the wider application and design flexibility of PC. While experimental techniques such as X-ray diffraction and scanning electron microscopy provide insights into nanoparticle interactions within the polymer matrix, they lack the resolution to fully elucidate nanoscale mechanisms. To bridge this gap, this study utilizes molecular dynamics (MD) simulations to analyze the shearing behavior of carbon nanoparticle (CNP)-reinforced PC composites. MD simulations allow for atomic-level insights into the interactions between CNPs and the polymer matrix, providing a more detailed understanding of how surface-modified CNPs enhance mechanical properties. Our results show that surface-modified CNPs influence the distribution and conformation of epoxy within the PC system. Amino-functionalized CNPs strengthen the epoxy and calcium silicate hydrate (C–S–H) interface by facilitating calcium–oxygen bond formation. These interactions play a crucial role in improving the mechanical properties of PC. This study provides a fundamental understanding of how surface-modified CNPs reinforce PC and offers valuable insights for optimizing the performance of CNP-reinforced cementitious composites.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"30 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723785","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}
Pub Date : 2025-03-27DOI: 10.1021/acs.langmuir.4c04049
Bin Li, Wei Xiang, Xiaohui Dou, Yan Wu, Wei Zhang, Zhentao Wang, Junfeng Wang
With growing concerns over environmental pollution associated with fossil fuels, hydrogen (H2) energy has emerged as a promising alternative. Water electrolysis, a key hydrogen production method, is fundamentally governed by the nucleation and stability of electrochemically generated nanobubbles. This study employs coarse-grained molecular dynamics (MD) simulations incorporating a self-programming gas generation algorithm to investigate the nucleation and growth dynamics of nanobubbles on hydrophilic and hydrophobic electrodes. Key parameters, such as contact angle, electric current, and nanobubble number density, were computed to validate the MD model. The findings reveal a three-stage nucleation process: (i) induction─gas molecules accumulate to form a nucleus, (ii) nucleation and growth─gas nuclei expand into nanobubbles, and (iii) stationary state─nanobubble growth ceases. Increased electrode hydrophilicity resulted in larger nanobubble contact angles, aligning well with classical nucleation theory (CNT) at the nanoscale. Three distinct nanobubble types─surface, solution, and pancake nanobubbles─were identified, each exhibiting unique interfacial behaviors based on electrode properties. Solution nanobubbles primarily formed on hydrophilic electrodes, pancake nanobubbles adhered to hydrophobic electrodes, and surface nanobubbles appeared as spherical caps. Energy analysis and phase mapping further delineated the critical parameter ranges for these nanobubble modes, providing valuable insights for optimizing electrode materials to enhance hydrogen production efficiency.
{"title":"Coarse-Grained Molecular Dynamics Simulation of Nucleation and Stability of Electrochemically Generated Nanobubbles","authors":"Bin Li, Wei Xiang, Xiaohui Dou, Yan Wu, Wei Zhang, Zhentao Wang, Junfeng Wang","doi":"10.1021/acs.langmuir.4c04049","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04049","url":null,"abstract":"With growing concerns over environmental pollution associated with fossil fuels, hydrogen (H<sub>2</sub>) energy has emerged as a promising alternative. Water electrolysis, a key hydrogen production method, is fundamentally governed by the nucleation and stability of electrochemically generated nanobubbles. This study employs coarse-grained molecular dynamics (MD) simulations incorporating a self-programming gas generation algorithm to investigate the nucleation and growth dynamics of nanobubbles on hydrophilic and hydrophobic electrodes. Key parameters, such as contact angle, electric current, and nanobubble number density, were computed to validate the MD model. The findings reveal a three-stage nucleation process: (i) <i>induction</i>─gas molecules accumulate to form a nucleus, (ii) <i>nucleation and growth</i>─gas nuclei expand into nanobubbles, and (iii) <i>stationary state</i>─nanobubble growth ceases. Increased electrode hydrophilicity resulted in larger nanobubble contact angles, aligning well with classical nucleation theory (<i>CNT</i>) at the nanoscale. Three distinct nanobubble types─surface, solution, and pancake nanobubbles─were identified, each exhibiting unique interfacial behaviors based on electrode properties. Solution nanobubbles primarily formed on hydrophilic electrodes, pancake nanobubbles adhered to hydrophobic electrodes, and surface nanobubbles appeared as spherical caps. Energy analysis and phase mapping further delineated the critical parameter ranges for these nanobubble modes, providing valuable insights for optimizing electrode materials to enhance hydrogen production efficiency.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"15 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713555","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}
Pub Date : 2025-03-27DOI: 10.1021/acs.langmuir.5c00279
Zijin Zhang, Jin Wang, Yongqing He, Feng Jiao
Coalescence-induced droplet jumping, a spontaneous droplet transport phenomenon, holds significant potential in anti-icing, anti-fogging, self-cleaning, and enhancing condensation heat transfer. However, droplet jumping has a low energy efficiency and an uncontrolled jumping orientation, severely restricting its practical use. We demonstrate experimentally that a pillar superhydrophobic surface may achieve dimensionless jumping velocity vj* = 0.72 and outstanding energy efficiency η = 56%. Compared to a flat superhydrophobic surface, the energy efficiency is raised by about 860%. The improvement in jumping efficiency is due to the pillar limitations and regularization of the internal droplet flow by restricting droplet deformation. For the first time, we have accomplished controlled droplet directional jumping within the 45–130° range by adjusting the magnitude and direction of the Laplace pressure. In addition, we thoroughly investigate how directional droplet jumping is affected by pillar geometric dimensions, droplet radius, and droplet size mismatch. This work introduces a new avenue for increasing the jumping velocity while managing the direction, resulting in better droplet jumping performance in applications.
{"title":"Directional Droplet Coalescence-Induced Jumping Regulated by Laplace Pressure","authors":"Zijin Zhang, Jin Wang, Yongqing He, Feng Jiao","doi":"10.1021/acs.langmuir.5c00279","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00279","url":null,"abstract":"Coalescence-induced droplet jumping, a spontaneous droplet transport phenomenon, holds significant potential in anti-icing, anti-fogging, self-cleaning, and enhancing condensation heat transfer. However, droplet jumping has a low energy efficiency and an uncontrolled jumping orientation, severely restricting its practical use. We demonstrate experimentally that a pillar superhydrophobic surface may achieve dimensionless jumping velocity <i>v</i><sub>j</sub><sup>*</sup> = 0.72 and outstanding energy efficiency <i>η</i> = 56%. Compared to a flat superhydrophobic surface, the energy efficiency is raised by about 860%. The improvement in jumping efficiency is due to the pillar limitations and regularization of the internal droplet flow by restricting droplet deformation. For the first time, we have accomplished controlled droplet directional jumping within the 45–130° range by adjusting the magnitude and direction of the Laplace pressure. In addition, we thoroughly investigate how directional droplet jumping is affected by pillar geometric dimensions, droplet radius, and droplet size mismatch. This work introduces a new avenue for increasing the jumping velocity while managing the direction, resulting in better droplet jumping performance in applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"22 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713609","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}
Surface morphology has been widely used to orchestrate multicellular function. However, most studies are mainly based on two-dimensional (2D) surface morphology. Therefore, a new scaffold that could be used to design and obtain controllable internal surface morphology was fabricated to explore the effect of a micropatterned scaffold on bone repair. In this study, through the combination of three-dimensional (2D) printing and soft lithography, a controllable micropatterned poly(ε-caprolactone) scaffold was obtained, which realized the transformation from 2D micropattern research to 3D research. Pit micropatterns with morphology sizes of 0, 25, and 45 μm (Flat, P25, and P45) were constructed. In vitro, the results showed that the P25 micropattern had a better effect on the promotion of M2 polarization, inhibition of the M1 polarization of RAW264.7 cells, and promotion of the osteogenic differentiation of bone marrow stromal stem cells (BMSCs). Direct and indirect coculture models of macrophages and BMSCs were constructed to study the bone immunomodulation of the pit micropatterns. Compared with the Flat and P45 groups, the P25 group could promote the secretion of M2 markers, inhibit the secretion of M1 markers, and immunomodulate the promotion of osteogenic differentiation of BMSCs. In vivo, the results also showed that the P25 group had a lower proinflammatory effect and better performance than scaffolds without micropatterned surfaces and a bigger morphology size (the P45 group), which could regulate the immune function of macrophages, reduce the inflammatory response, and accelerate bone regeneration and repair. This work provides a new strategy for the preparation of scaffolds for bone defect regeneration.
{"title":"Orchestrating Macrophage and Bone Mesenchymal Stem Cells to Promote Bone Regeneration via Modulation of the Internal Surface Morphology inside 3D Printed Scaffolds","authors":"Xiayu Cai, Shaohui Zhang, Chujie Xiao, Zhaohui Dang, Weihua Huang, Weikang Xu, Gang Wu","doi":"10.1021/acs.langmuir.5c00200","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00200","url":null,"abstract":"Surface morphology has been widely used to orchestrate multicellular function. However, most studies are mainly based on two-dimensional (2D) surface morphology. Therefore, a new scaffold that could be used to design and obtain controllable internal surface morphology was fabricated to explore the effect of a micropatterned scaffold on bone repair. In this study, through the combination of three-dimensional (2D) printing and soft lithography, a controllable micropatterned poly(ε-caprolactone) scaffold was obtained, which realized the transformation from 2D micropattern research to 3D research. Pit micropatterns with morphology sizes of 0, 25, and 45 μm (Flat, P25, and P45) were constructed. In vitro, the results showed that the P25 micropattern had a better effect on the promotion of M2 polarization, inhibition of the M1 polarization of RAW264.7 cells, and promotion of the osteogenic differentiation of bone marrow stromal stem cells (BMSCs). Direct and indirect coculture models of macrophages and BMSCs were constructed to study the bone immunomodulation of the pit micropatterns. Compared with the Flat and P45 groups, the P25 group could promote the secretion of M2 markers, inhibit the secretion of M1 markers, and immunomodulate the promotion of osteogenic differentiation of BMSCs. In vivo, the results also showed that the P25 group had a lower proinflammatory effect and better performance than scaffolds without micropatterned surfaces and a bigger morphology size (the P45 group), which could regulate the immune function of macrophages, reduce the inflammatory response, and accelerate bone regeneration and repair. This work provides a new strategy for the preparation of scaffolds for bone defect regeneration.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"26 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713608","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}
Pub Date : 2025-03-27DOI: 10.1021/acs.langmuir.5c00698
Mustafa Erbakan, Muharrem Taşdemir, Fatih Şenaslan, Oğuz Yunus Sarıbıyık
In this study, we investigated the influence of crystal structure, topography, and elemental composition of aluminum oxide surfaces on bacterial adhesion. The structural properties of the surfaces were systematically controlled by varying the current density (1.5, 2.0, and 2.5 A/dm2) and silver doping during the anodization process. The resulting changes in structural and morphological properties were examined by using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FE-SEM), contact angle measurements, and profilometry. Using FE-SEM analysis, we evaluated the adhesion of model bacteria, Escherichia coli and Staphylococcus aureus, to surfaces exhibiting diverse morphologies and elemental compositions. The surface roughness and crystal size of the aluminum oxide increased proportionally with the applied current density and silver doping. According to the XRD results, the slip plane crystal structure of (311) increased proportionally to the current density but decreased with silver doping. Specifically, while stepped atomic alignment of (311) planes facilitates bacterial attachment, smoother (200) planes reduce the adhered bacteria population. Further analysis via XPS revealed that the oxide crystal structure of undoped surfaces shifted from the tetrahedral to octahedral form with increasing current density, while silver-doped surfaces exhibited the opposite trend. Additionally, increasing current density during the preparation of silver-doped surfaces diminished the ratio of ionic silver to metallic silver, suggesting a lowered propensity for bacterial adhesion. S. aureus adhesion to undoped surfaces increased 4.46-fold for surfaces prepared at 2.5 A/dm2 compared to that at 1.5 A/dm2. Moreover, E. coli adhesion was completely inhibited on silver-doped surfaces anodized at 1.5 A/dm2. Reducing the surface roughness and incorporating silver during the anodization of aluminum surfaces decrease the number of bacteria adhering to aluminum oxide surfaces.
{"title":"Influence of Silver Doping and Anodization Current Density on Aluminum Surface Properties and Surface Adhesion of Staphylococcus aureus and Escherichia coli","authors":"Mustafa Erbakan, Muharrem Taşdemir, Fatih Şenaslan, Oğuz Yunus Sarıbıyık","doi":"10.1021/acs.langmuir.5c00698","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00698","url":null,"abstract":"In this study, we investigated the influence of crystal structure, topography, and elemental composition of aluminum oxide surfaces on bacterial adhesion. The structural properties of the surfaces were systematically controlled by varying the current density (1.5, 2.0, and 2.5 A/dm<sup>2</sup>) and silver doping during the anodization process. The resulting changes in structural and morphological properties were examined by using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FE-SEM), contact angle measurements, and profilometry. Using FE-SEM analysis, we evaluated the adhesion of model bacteria, <i>Escherichia coli</i> and <i>Staphylococcus aureus</i>, to surfaces exhibiting diverse morphologies and elemental compositions. The surface roughness and crystal size of the aluminum oxide increased proportionally with the applied current density and silver doping. According to the XRD results, the slip plane crystal structure of (311) increased proportionally to the current density but decreased with silver doping. Specifically, while stepped atomic alignment of (311) planes facilitates bacterial attachment, smoother (200) planes reduce the adhered bacteria population. Further analysis via XPS revealed that the oxide crystal structure of undoped surfaces shifted from the tetrahedral to octahedral form with increasing current density, while silver-doped surfaces exhibited the opposite trend. Additionally, increasing current density during the preparation of silver-doped surfaces diminished the ratio of ionic silver to metallic silver, suggesting a lowered propensity for bacterial adhesion. <i>S. aureus</i> adhesion to undoped surfaces increased 4.46-fold for surfaces prepared at 2.5 A/dm<sup>2</sup> compared to that at 1.5 A/dm<sup>2</sup>. Moreover, <i>E. coli</i> adhesion was completely inhibited on silver-doped surfaces anodized at 1.5 A/dm<sup>2</sup>. Reducing the surface roughness and incorporating silver during the anodization of aluminum surfaces decrease the number of bacteria adhering to aluminum oxide surfaces.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"3 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713612","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}
Due to the exhaustion of fossil fuels and rising concerns about environmental pollution, direct methanol fuel cells (DMFCs) have emerged as one of the prominent green energy solutions in recent decades. However, the commercialization of DMFCs faces a significant challenge due to the dependence on expensive noble-metal-based electrode materials and the issue of methanol crossover. Therefore, there has been growing interest in developing cost-effective, high-performance anode catalysts to enhance the methanol oxidation reaction (MOR). In this work, unexplored non-noble transition metal oxide materials, such as metal–organic framework (MOF)-derived ZnO, ZnCo2O4, and Zn2CoO4, were directly synthesized on Ni foam using a simple solvothermal method, followed by calcination. The MOR activity of all the materials was tested in a 0.5 M methanol solution under alkaline conditions. Due to the synergetic effect of combined metallic composition, mixed metal oxides exhibited superior performance. The order of MOR activity was measured to be ZnO < Zn2CoO4 < ZnCo2O4. Particularly, ZnCo2O4 exhibited the highest mass activity (42.64 mA mg–1) and geometric current density (166.28 mA cm–2), outperforming Zn2CoO4 (27.44 mA mg–1) and ZnO (12.72 mA mg–1). It also demonstrated the lowest onset potential of 1.32 V (vs RHE) compared to Zn2CoO4 (1.35 V) and ZnO (1.39 V) and maintained excellent long-term stability for 12 h at 1.5 V (vs RHE). Additionally, to determine the optimal methanol concentration, all electrocatalysts were tested across a range of methanol concentrations from 0.1 to 1 M, showing 0.5 M methanol as the most suitable concentration. This study aims to develop cost-effective MOF-derived electrode materials and optimize methanol concentration to maximize catalytic activity. Furthermore, it establishes a foundation for the development of various MOF-derived electrocatalysts and the advancement of DMFC technology.
{"title":"Metal–Organic Framework-Derived Zinc–Cobalt Oxide Materials as High-Performance Anodes for Direct Methanol Fuel Cell Application","authors":"Anshu Kumari, Sayani Debnath, Sumit, Apurba Borah, Gaddam Rajeshkhanna","doi":"10.1021/acs.langmuir.5c00116","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00116","url":null,"abstract":"Due to the exhaustion of fossil fuels and rising concerns about environmental pollution, direct methanol fuel cells (DMFCs) have emerged as one of the prominent green energy solutions in recent decades. However, the commercialization of DMFCs faces a significant challenge due to the dependence on expensive noble-metal-based electrode materials and the issue of methanol crossover. Therefore, there has been growing interest in developing cost-effective, high-performance anode catalysts to enhance the methanol oxidation reaction (MOR). In this work, unexplored non-noble transition metal oxide materials, such as metal–organic framework (MOF)-derived ZnO, ZnCo<sub>2</sub>O<sub>4</sub>, and Zn<sub>2</sub>CoO<sub>4</sub>, were directly synthesized on Ni foam using a simple solvothermal method, followed by calcination. The MOR activity of all the materials was tested in a 0.5 M methanol solution under alkaline conditions. Due to the synergetic effect of combined metallic composition, mixed metal oxides exhibited superior performance. The order of MOR activity was measured to be ZnO < Zn<sub>2</sub>CoO<sub>4</sub> < ZnCo<sub>2</sub>O<sub>4</sub>. Particularly, ZnCo<sub>2</sub>O<sub>4</sub> exhibited the highest mass activity (42.64 mA mg<sup>–1</sup>) and geometric current density (166.28 mA cm<sup>–2</sup>), outperforming Zn<sub>2</sub>CoO<sub>4</sub> (27.44 mA mg<sup>–1</sup>) and ZnO (12.72 mA mg<sup>–1</sup>). It also demonstrated the lowest onset potential of 1.32 V (vs RHE) compared to Zn<sub>2</sub>CoO<sub>4</sub> (1.35 V) and ZnO (1.39 V) and maintained excellent long-term stability for 12 h at 1.5 V (vs RHE). Additionally, to determine the optimal methanol concentration, all electrocatalysts were tested across a range of methanol concentrations from 0.1 to 1 M, showing 0.5 M methanol as the most suitable concentration. This study aims to develop cost-effective MOF-derived electrode materials and optimize methanol concentration to maximize catalytic activity. Furthermore, it establishes a foundation for the development of various MOF-derived electrocatalysts and the advancement of DMFC technology.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"36 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723692","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}
Hydrogel microspheres are considered ideal carriers with broad applications in 3D cell culture, drug delivery, and microtissue construction. Although multiple methods have been developed for generating hydrogel microspheres, there is still a lack of a universal approach that combines operability, stability, cost-effectiveness, and biocompatibility. In this work, a novel rotating microfluidic system (RMS) is proposed, which can rapidly fabricate diverse poly(ethylene glycol) diacrylate/sodium alginate (PEGDA/SA) hydrogel microspheres by motor-driven rotation of the oil phase to form a special T-shaped structure with the needle. The main part of the system consists of commercially available motors, a beaker, and needles that do not require precision machining and are user-friendly with low cost. Moreover, by adjusting system parameters such as the needle structure, flow rate, and rotational speed, the platform enables rapid fabrication of hydrogel microspheres with different sizes and diverse cores, including crescent, thick wavy, oval, and spherical. Furthermore, tumor cell-laden hyaluronic acid methacrylate/sodium alginate (HAMA/SA) hydrogel microspheres were fabricated by using this system, which demonstrated good cell viability and proliferation in the subsequent 3D culture. In vitro drug evaluation of tumor models using cisplatin revealed the potential of this system for drug evaluation. These results indicated that RMS has good potential in other 3D cell culture-based biomedical applications.
{"title":"Rapid Fabrication of Diverse Hydrogel Microspheres for Drug Evaluation on a Rotating Microfluidic System","authors":"Yue Cheng, Bing Li, Jianping Wang, Yubin Wang, Linshan Wang, Muling Wei, Yuying Wang, Zhongrong Chen, Gang Zhao","doi":"10.1021/acs.langmuir.5c00365","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00365","url":null,"abstract":"Hydrogel microspheres are considered ideal carriers with broad applications in 3D cell culture, drug delivery, and microtissue construction. Although multiple methods have been developed for generating hydrogel microspheres, there is still a lack of a universal approach that combines operability, stability, cost-effectiveness, and biocompatibility. In this work, a novel rotating microfluidic system (RMS) is proposed, which can rapidly fabricate diverse poly(ethylene glycol) diacrylate/sodium alginate (PEGDA/SA) hydrogel microspheres by motor-driven rotation of the oil phase to form a special T-shaped structure with the needle. The main part of the system consists of commercially available motors, a beaker, and needles that do not require precision machining and are user-friendly with low cost. Moreover, by adjusting system parameters such as the needle structure, flow rate, and rotational speed, the platform enables rapid fabrication of hydrogel microspheres with different sizes and diverse cores, including crescent, thick wavy, oval, and spherical. Furthermore, tumor cell-laden hyaluronic acid methacrylate/sodium alginate (HAMA/SA) hydrogel microspheres were fabricated by using this system, which demonstrated good cell viability and proliferation in the subsequent 3D culture. In vitro drug evaluation of tumor models using cisplatin revealed the potential of this system for drug evaluation. These results indicated that RMS has good potential in other 3D cell culture-based biomedical applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"34 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723947","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}
SiO2/Fe3O4 hybrid wall microcapsules containing a paraffin core were successfully fabricated by Pickering emulsion template self-assembly and sol–gel technologies. The walls of these microcapsules were embedded with different dosages of Fe3O4 nanoparticles due to the effect of Fe3O4 Pickering emulsion of different concentrations. The resultant microcapsules exhibited a regular spherical morphology and a rough outer surface compared with that of the SiO2 wall. Thermal analysis indicated that the encapsulation efficiency (Een), thermal energy-storage efficiency (Ees), and thermal conductivity of paraffin@SiO2/Fe3O4 hybrid wall microcapsules prepared with 0.01 mol/L Fe3O4 Pickering emulsion [Pa@SiO2/Fe3O4-Ms (0.01)] increased by 16.71%, 16.88%, and 28.4% compared with those of paraffin@SiO2 microcapsules (Pa@SiO2-Ms), respectively. The phase-change temperatures and enthalpy of Pa@SiO2/Fe3O4-Ms (0.01) with an 80–100 μm particle size range changed little after 300 thermal cycles. At the same time, these microcapsules were introduced into water-based acrylic resin paint to prepare phase-change composite protective coatings (PCCPCs) and exhibited excellent thermoregulatory performance. The real-time temperature difference and temperature ramp rate of PCCPCs incorporating 5 wt % (80–100 μm) Pa@SiO2/Fe3O4-Ms (0.01) increased by 4.6 °C and decreased by 2.45 °C/min compared to that of the pure coating, respectively. Meanwhile, the fluctuation amplitude and fluctuation frequency of the average temperature on the back side of 5 wt % (80–100 μm) Pa@SiO2/Fe3O4-Ms (0.01)-PCCPCs decreased by 3.8 °C and extended by 395 s compared to that of the pure coating under one heating and cooling cycle, respectively. This study will provide great potential applications for addressing the risk of shrinkage deformation and cracking of the protected concrete substrates under high-frequency and large temperature difference conditions.
{"title":"Robust and Eco-Friendly Waterborne Phase-Change Composite Protective Coatings Containing Paraffin-Loaded SiO2/Fe3O4 Hybrid Wall Microcapsules and Their Application in Long-Term Effective Temperature Regulation of the Protected Substrate","authors":"Yingjie Ma, Baolei Liu, Dewen Sun, Dongfang Wang, Yabin Ma, Qianping Ran","doi":"10.1021/acs.langmuir.5c00236","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00236","url":null,"abstract":"SiO<sub>2</sub>/Fe<sub>3</sub>O<sub>4</sub> hybrid wall microcapsules containing a paraffin core were successfully fabricated by Pickering emulsion template self-assembly and sol–gel technologies. The walls of these microcapsules were embedded with different dosages of Fe<sub>3</sub>O<sub>4</sub> nanoparticles due to the effect of Fe<sub>3</sub>O<sub>4</sub> Pickering emulsion of different concentrations. The resultant microcapsules exhibited a regular spherical morphology and a rough outer surface compared with that of the SiO<sub>2</sub> wall. Thermal analysis indicated that the encapsulation efficiency (<i>E</i><sub>en</sub>), thermal energy-storage efficiency (<i>E</i><sub>es</sub>), and thermal conductivity of paraffin@SiO<sub>2</sub>/Fe<sub>3</sub>O<sub>4</sub> hybrid wall microcapsules prepared with 0.01 mol/L Fe<sub>3</sub>O<sub>4</sub> Pickering emulsion [Pa@SiO<sub>2</sub>/Fe<sub>3</sub>O<sub>4</sub>-Ms (0.01)] increased by 16.71%, 16.88%, and 28.4% compared with those of paraffin@SiO<sub>2</sub> microcapsules (Pa@SiO<sub>2</sub>-Ms), respectively. The phase-change temperatures and enthalpy of Pa@SiO<sub>2</sub>/Fe<sub>3</sub>O<sub>4</sub>-Ms (0.01) with an 80–100 μm particle size range changed little after 300 thermal cycles. At the same time, these microcapsules were introduced into water-based acrylic resin paint to prepare phase-change composite protective coatings (PCCPCs) and exhibited excellent thermoregulatory performance. The real-time temperature difference and temperature ramp rate of PCCPCs incorporating 5 wt % (80–100 μm) Pa@SiO<sub>2</sub>/Fe<sub>3</sub>O<sub>4</sub>-Ms (0.01) increased by 4.6 °C and decreased by 2.45 °C/min compared to that of the pure coating, respectively. Meanwhile, the fluctuation amplitude and fluctuation frequency of the average temperature on the back side of 5 wt % (80–100 μm) Pa@SiO<sub>2</sub>/Fe<sub>3</sub>O<sub>4</sub>-Ms (0.01)-PCCPCs decreased by 3.8 °C and extended by 395 s compared to that of the pure coating under one heating and cooling cycle, respectively. This study will provide great potential applications for addressing the risk of shrinkage deformation and cracking of the protected concrete substrates under high-frequency and large temperature difference conditions.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"59 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713610","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}
Pub Date : 2025-03-27DOI: 10.1021/acs.langmuir.5c00468
Rajesh Khamrui, Arjama Mukherjee, Siddhartha S. Jana, Suhrit Ghosh
This manuscript reports H-bonding regulated morphology control in aqueous supramolecular assemblies of naphthalene-diimide (NDI)-derived sulfated amphiphiles and its direct correlation with antiviral activity. NDI-1 with a hydrazide group produces a polymersome structure with an efficient display of the sulfate groups on the outer surface, resulting in excellent antiviral activity by a fusion mechanism. NDI-3 lacking any H-bonding group or NDI-2 having the amide group produces particle-like or worm-like structures, respectively, with significantly low antiviral activity. Confocal microscopy images show that NDI-1 is able to fully deactivate and stop the entry of the virus to a host cell, indicating its great promise for future medicinal use, especially as it exhibits negligible toxicity toward a mammalian cell.
{"title":"Morphology Control in Supramolecular Assemblies of Sulfated π-Amphiphiles and Impact on the Antiviral Activity","authors":"Rajesh Khamrui, Arjama Mukherjee, Siddhartha S. Jana, Suhrit Ghosh","doi":"10.1021/acs.langmuir.5c00468","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00468","url":null,"abstract":"This manuscript reports H-bonding regulated morphology control in aqueous supramolecular assemblies of naphthalene-diimide (NDI)-derived sulfated amphiphiles and its direct correlation with antiviral activity. NDI-1 with a hydrazide group produces a polymersome structure with an efficient display of the sulfate groups on the outer surface, resulting in excellent antiviral activity by a fusion mechanism. NDI-3 lacking any H-bonding group or NDI-2 having the amide group produces particle-like or worm-like structures, respectively, with significantly low antiviral activity. Confocal microscopy images show that NDI-1 is able to fully deactivate and stop the entry of the virus to a host cell, indicating its great promise for future medicinal use, especially as it exhibits negligible toxicity toward a mammalian cell.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"64 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723786","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}
Pub Date : 2025-03-26DOI: 10.1021/acs.langmuir.5c00208
Jiawen Song, Parisa Bazazi, Seyed Hossein Hejazi
Nanobubbles, when dispersed in a liquid phase, may enhance mass transport, adsorption, and reactions in many industrial applications, such as fabrication of functional materials, drug delivery, water treatment, carbon dioxide capture, and surface decontamination. Here, we experimentally study the early time spreading dynamics of nanobubble-laden surfactant drops on a hydrophilic solid surface submerged in an oil phase. Along with recovering the retarding effects of surfactants on the early time wetting dynamics, we report that nanobubbles can weaken Marangoni stresses and consequently reduce the duration of the retardation regime. Remarkably, we find that the duration of this retardation regime (tr) exponentially decays with the nanobubble concentration in the dispersion (Nb) according to Nb ∼ log(1/tr). The micro-particle imaging velocimetry analysis of the flow field inside the drop indicates a large reduction in the magnitude of velocities in the presence of surface-active materials, confirming the existence of Marangoni flow that opposes droplet spreading. Our research introduces a simple approach to calculate the nanobubble concentrations in liquids and offers guidelines for controlling wetting dynamics.
{"title":"Early Time Spreading Dynamics of Nanobubble-Laden Drops","authors":"Jiawen Song, Parisa Bazazi, Seyed Hossein Hejazi","doi":"10.1021/acs.langmuir.5c00208","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00208","url":null,"abstract":"Nanobubbles, when dispersed in a liquid phase, may enhance mass transport, adsorption, and reactions in many industrial applications, such as fabrication of functional materials, drug delivery, water treatment, carbon dioxide capture, and surface decontamination. Here, we experimentally study the early time spreading dynamics of nanobubble-laden surfactant drops on a hydrophilic solid surface submerged in an oil phase. Along with recovering the retarding effects of surfactants on the early time wetting dynamics, we report that nanobubbles can weaken Marangoni stresses and consequently reduce the duration of the retardation regime. Remarkably, we find that the duration of this retardation regime (<i>t</i><sub>r</sub>) exponentially decays with the nanobubble concentration in the dispersion (<i>N</i><sub>b</sub>) according to <i>N</i><sub>b</sub> ∼ log(1/<i>t</i><sub>r</sub>). The micro-particle imaging velocimetry analysis of the flow field inside the drop indicates a large reduction in the magnitude of velocities in the presence of surface-active materials, confirming the existence of Marangoni flow that opposes droplet spreading. Our research introduces a simple approach to calculate the nanobubble concentrations in liquids and offers guidelines for controlling wetting dynamics.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"9 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703623","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}
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