Pub Date : 2025-01-10DOI: 10.1021/acs.langmuir.4c04663
Naiyue Zhang, Siting Fu, Pengxiao Fu, Xiaowen Xu
The lateral flow assay is a strip-based analytical method for the portable and convenient detection of analytes of interest. It has the advantages of visual observation, autonomous sample flow, fast coloration time, minimal tedious operation procedures, and reliance on specialized instruments. However, the rough surface of the nitrocellulose membrane renders it difficult for the immobilized nucleic acids to remain in an ordered arrangement, and the immobilized nucleic acids are also liable to be digested in a complex matrix, inducing limited sensitivity and anti-interference. In this work, we demonstrate that the decoration of DNA nanostructures on lateral flow strips can improve assay sensitivity and anti-interference in comparison with commonly studied single-stranded DNA-disposed strips. DNA nanostructures enable probes to be more orderly and arranged on the strip and provide protection. Using adenosine 5′-triphosphate (ATP) as an analyte, a DNA tetrahedron reformative lateral flow strip has increased sensitivity and improved reliability in detection. The DNA nanostructure-decorated lateral flow strip is further successfully applied for ATP detection in real samples, such as bacterium testing and tableware cleanliness checking, by detection of the ATP content therein.
{"title":"DNA Tetrahedron Reformative Lateral Flow Assay for Improved Detection Sensitivity and Anti-Interference","authors":"Naiyue Zhang, Siting Fu, Pengxiao Fu, Xiaowen Xu","doi":"10.1021/acs.langmuir.4c04663","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04663","url":null,"abstract":"The lateral flow assay is a strip-based analytical method for the portable and convenient detection of analytes of interest. It has the advantages of visual observation, autonomous sample flow, fast coloration time, minimal tedious operation procedures, and reliance on specialized instruments. However, the rough surface of the nitrocellulose membrane renders it difficult for the immobilized nucleic acids to remain in an ordered arrangement, and the immobilized nucleic acids are also liable to be digested in a complex matrix, inducing limited sensitivity and anti-interference. In this work, we demonstrate that the decoration of DNA nanostructures on lateral flow strips can improve assay sensitivity and anti-interference in comparison with commonly studied single-stranded DNA-disposed strips. DNA nanostructures enable probes to be more orderly and arranged on the strip and provide protection. Using adenosine 5′-triphosphate (ATP) as an analyte, a DNA tetrahedron reformative lateral flow strip has increased sensitivity and improved reliability in detection. The DNA nanostructure-decorated lateral flow strip is further successfully applied for ATP detection in real samples, such as bacterium testing and tableware cleanliness checking, by detection of the ATP content therein.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"48 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940326","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 : 2025-01-09DOI: 10.1021/acs.langmuir.4c04774
Zhixuan Xie, Shengyu Liu
Flotation is an interfacial process involving gas, liquid, and solid phases, where polar ionic promoters significantly influence both gas–liquid and solid–liquid interfaces during low-rank coal (LRC) flotation. This study examines how the structures of hydrophilic groups in cation–anion mixed promoters affect the interfacial flotation performance of LRC pulp using flotation tests, surface tension tests, wetting heat tests, and molecular dynamics simulations. Results indicate that cation–anion mixed promoters enhance the LRC floatability to varying degrees. When the cationic hydrophilic head contains a benzyl group and the anionic head contains an ethoxy group, both the floatability and selectivity improve. These mixed promoters exhibit superior surface activity compared to single ionic solutions, particularly with ethoxy-containing anions, which demonstrate an increased density and viscoelasticity at the gas–liquid interface. The combination of a benzyl cation and an ethoxy anion results in dense adsorption at the solid–liquid interface, maximizing wettability differences between organic matter and mineral surfaces. This is attributed to hydrogen bonds and π–π interactions between the promoter and the coal surface, enhancing adsorption selectivity. Hydrophobic chains shield polar sites on the LRC surface, promoting water molecule diffusion and providing sites for nonpolar oil molecule adsorption, thereby improving LRC flotation performance.
{"title":"Interface Mechanism of Promoting Low-Rank Coal Flotation by Characteristic Groups in Hydrophilic Moieties of Cationic–Anionic Surfactants","authors":"Zhixuan Xie, Shengyu Liu","doi":"10.1021/acs.langmuir.4c04774","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04774","url":null,"abstract":"Flotation is an interfacial process involving gas, liquid, and solid phases, where polar ionic promoters significantly influence both gas–liquid and solid–liquid interfaces during low-rank coal (LRC) flotation. This study examines how the structures of hydrophilic groups in cation–anion mixed promoters affect the interfacial flotation performance of LRC pulp using flotation tests, surface tension tests, wetting heat tests, and molecular dynamics simulations. Results indicate that cation–anion mixed promoters enhance the LRC floatability to varying degrees. When the cationic hydrophilic head contains a benzyl group and the anionic head contains an ethoxy group, both the floatability and selectivity improve. These mixed promoters exhibit superior surface activity compared to single ionic solutions, particularly with ethoxy-containing anions, which demonstrate an increased density and viscoelasticity at the gas–liquid interface. The combination of a benzyl cation and an ethoxy anion results in dense adsorption at the solid–liquid interface, maximizing wettability differences between organic matter and mineral surfaces. This is attributed to hydrogen bonds and π–π interactions between the promoter and the coal surface, enhancing adsorption selectivity. Hydrophobic chains shield polar sites on the LRC surface, promoting water molecule diffusion and providing sites for nonpolar oil molecule adsorption, thereby improving LRC flotation performance.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"28 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937708","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 : 2025-01-09DOI: 10.1021/acs.langmuir.4c03236
Zahed Shami, Seyed Arad Derakhshan, Rezgar Ahmadi
Water splitting by an electrochemical method to generate hydrogen gas is an economic and green approach to resolve the looming energy and environmental crisis. Designing a composite electrocatalyst having integrated multichannel charge separation, robust stability, and low-cost facile scalability could be considered to address the issue of electrochemical hydrogen evolution. Herein, we report a superhydrophilic, noble-metal-free bimetallic nanostructure TiO2/Ni2P coated on graphitic polyacrylonitrile carbon fibers (g-C/TiO2/Ni2P) using a facile hydrothermal method followed by phosphorylation. In an aqueous-based route, PAN is dissolved in water in the presence of ZnCl2, followed by wet-spinning to prepare scalable PAN/ZnCl2 fibers. The nitrogen-contained porous graphitic carbon fibers are prepared via the pyrolysis of PAN/ZnCl2 fibers; now ZnCl2 acts as a volatile porogen to form porous matrix structures. Finally, the as-prepared graphitic carbon fibers are electrochemically activated by incorporating TiO2/Ni2P active sites. The materials formed in this work show excellent electrocatalytic activity for the hydrogen evolution reaction. The as-synthesized g-C/TiO2/Ni2P catalyst shows a low overpotential, its electrocatalytic activity is improved, and its efficiency is better than that of the commercial Pt/C catalyst. At a current density of −10 mA/cm2, the g-C/TiO2/Ni2P catalyst shows an overpotential of 55 mV, while the commercial Pt/C catalyst shows an overpotential of 77 mV. Our work provides a facile aqueous scalable route with no need for noble metals that can be considered as a potential alternative for the commercial Pt/C catalyst.
{"title":"Facile Aqueous Route to Large-Scale Superhydrophilic TiO2-Incorporated Graphitic Carbon Nitride-Coated Ni(OH)2 and Ni2P Nano-Architecture Arrays as Efficient Electrocatalysts for Enhanced Hydrogen Production","authors":"Zahed Shami, Seyed Arad Derakhshan, Rezgar Ahmadi","doi":"10.1021/acs.langmuir.4c03236","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03236","url":null,"abstract":"Water splitting by an electrochemical method to generate hydrogen gas is an economic and green approach to resolve the looming energy and environmental crisis. Designing a composite electrocatalyst having integrated multichannel charge separation, robust stability, and low-cost facile scalability could be considered to address the issue of electrochemical hydrogen evolution. Herein, we report a superhydrophilic, noble-metal-free bimetallic nanostructure TiO<sub>2</sub>/Ni<sub>2</sub>P coated on graphitic polyacrylonitrile carbon fibers (g-C/TiO<sub>2</sub>/Ni<sub>2</sub>P) using a facile hydrothermal method followed by phosphorylation. In an aqueous-based route, PAN is dissolved in water in the presence of ZnCl<sub>2</sub>, followed by wet-spinning to prepare scalable PAN/ZnCl<sub>2</sub> fibers. The nitrogen-contained porous graphitic carbon fibers are prepared via the pyrolysis of PAN/ZnCl<sub>2</sub> fibers; now ZnCl<sub>2</sub> acts as a volatile porogen to form porous matrix structures. Finally, the as-prepared graphitic carbon fibers are electrochemically activated by incorporating TiO<sub>2</sub>/Ni<sub>2</sub>P active sites. The materials formed in this work show excellent electrocatalytic activity for the hydrogen evolution reaction. The as-synthesized g-C/TiO<sub>2</sub>/Ni<sub>2</sub>P catalyst shows a low overpotential, its electrocatalytic activity is improved, and its efficiency is better than that of the commercial Pt/C catalyst. At a current density of −10 mA/cm<sup>2</sup>, the g-C/TiO<sub>2</sub>/Ni<sub>2</sub>P catalyst shows an overpotential of 55 mV, while the commercial Pt/C catalyst shows an overpotential of 77 mV. Our work provides a facile aqueous scalable route with no need for noble metals that can be considered as a potential alternative for the commercial Pt/C catalyst.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"3 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940332","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}
The growing demand for energy storage batteries, driven by the need to alleviate global warming and reduce fossil fuel dependency, has led to environmental concerns surrounding spent batteries. Efficient recycling of these batteries is essential to prevent pollution and recover valuable metal ions such as nickel (Ni2+), cobalt (Co2+), and manganese (Mn2+). Conventional hydrometallurgical methods for battery recycling, while effective, often involve harmful chemicals and processes. Natural polyphenols offer a greener alternative due to their ability to coordinate with metal ions. However, optimizing polyphenol selection for efficient recovery remains a labor-intensive challenge. This study presents a strategy combining natural polyphenols as green precipitants with the power of GPT-4, a large language model (LLM), to enhance the precipitation and recovery of metal ions from spent batteries. By leveraging the capabilities of GPT-4 in natural language processing, we enable a dynamic, iterative collaboration between human researchers and the LLM, optimizing polyphenol selection for different experimental conditions. The results show that tannic acid achieved precipitation rates of 94.8, 96.7, and 96.7% for Ni2+, Co2+, and Mn2+, respectively, outperforming conventional methods. The integration of GPT-4 enhances both the efficiency and accuracy of the process, ensuring environmental sustainability by minimizing secondary pollution and utilizing biodegradable materials. This innovative strategy demonstrates the potential of combining artificial intelligence-driven analysis with green chemistry to address battery recycling challenges, paving the way for more sustainable and efficient methods.
{"title":"Large Language Modeling to Assist Natural Polyphenols as Green Precipitants for Recycling Spent Batteries","authors":"Huijun Huang, Mei Chen, Yajing Zhang, Xiaoling Wang, Qiuping Xie, Yiran Pu, Yuanmeng He, Limin Zhu, Yunxiang He, Junling Guo","doi":"10.1021/acs.langmuir.4c04262","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04262","url":null,"abstract":"The growing demand for energy storage batteries, driven by the need to alleviate global warming and reduce fossil fuel dependency, has led to environmental concerns surrounding spent batteries. Efficient recycling of these batteries is essential to prevent pollution and recover valuable metal ions such as nickel (Ni<sup>2+</sup>), cobalt (Co<sup>2+</sup>), and manganese (Mn<sup>2+</sup>). Conventional hydrometallurgical methods for battery recycling, while effective, often involve harmful chemicals and processes. Natural polyphenols offer a greener alternative due to their ability to coordinate with metal ions. However, optimizing polyphenol selection for efficient recovery remains a labor-intensive challenge. This study presents a strategy combining natural polyphenols as green precipitants with the power of GPT-4, a large language model (LLM), to enhance the precipitation and recovery of metal ions from spent batteries. By leveraging the capabilities of GPT-4 in natural language processing, we enable a dynamic, iterative collaboration between human researchers and the LLM, optimizing polyphenol selection for different experimental conditions. The results show that tannic acid achieved precipitation rates of 94.8, 96.7, and 96.7% for Ni<sup>2+</sup>, Co<sup>2+</sup>, and Mn<sup>2+</sup>, respectively, outperforming conventional methods. The integration of GPT-4 enhances both the efficiency and accuracy of the process, ensuring environmental sustainability by minimizing secondary pollution and utilizing biodegradable materials. This innovative strategy demonstrates the potential of combining artificial intelligence-driven analysis with green chemistry to address battery recycling challenges, paving the way for more sustainable and efficient methods.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"67 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937705","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 : 2025-01-09DOI: 10.1021/acs.langmuir.4c03492
Jin’an Pang, Yu Han, Bo Sun, Wei Zhao
Electrokinetic (EK) flow is a type of flow driven or manipulated by electric body forces, influenced by various factors such as electric field intensity, electric field form, frequency, electric permittivity/conductivity, fluid viscosity, etc. The diversity of dimensionless parameters, such as the electric Rayleigh number, complicates the comparison of the EK flow stability. Consequently, comparing the performance and cost of micromixers or reactors based on EK flow is challenging, posing an obstacle to their industrial and engineering applications. In this investigation, we theoretically derived a new electric Rayleigh number (Rae) that quantifies the relationship among electric body forces, fluid viscosity, and ion diffusivity, based on a tanh model of electric conductivity distribution. The calculation results indicate that the new Rae exhibits richer variation with the control parameters and better consistency with previous experimental reports. We further conducted experimental studies on the critical electric Rayleigh number (Raec) of the AC EK flow of binary fluids in a divergent microchannel. The experimental variations align well with the theoretical predictions, particularly the existence of an optimal AC frequency and electric conductivity ratio, demonstrating that the tanh model can better elucidate the underlying physics of EK flow. With the new electric Rayleigh number, we found that EK flow in the designed divergent microchannel has a much smaller Raec than previously reported, indicating that EK flow is more unstable and thus more suitable for applications in micromixers or reactors in industry and engineering.
{"title":"A Discussion on the Critical Electric Rayleigh Number for AC Electrokinetic Flow of Binary Fluids in a Divergent Microchannel","authors":"Jin’an Pang, Yu Han, Bo Sun, Wei Zhao","doi":"10.1021/acs.langmuir.4c03492","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03492","url":null,"abstract":"Electrokinetic (EK) flow is a type of flow driven or manipulated by electric body forces, influenced by various factors such as electric field intensity, electric field form, frequency, electric permittivity/conductivity, fluid viscosity, etc. The diversity of dimensionless parameters, such as the electric Rayleigh number, complicates the comparison of the EK flow stability. Consequently, comparing the performance and cost of micromixers or reactors based on EK flow is challenging, posing an obstacle to their industrial and engineering applications. In this investigation, we theoretically derived a new electric Rayleigh number (<i>Ra</i><sub>e</sub>) that quantifies the relationship among electric body forces, fluid viscosity, and ion diffusivity, based on a tanh model of electric conductivity distribution. The calculation results indicate that the new <i>Ra</i><sub>e</sub> exhibits richer variation with the control parameters and better consistency with previous experimental reports. We further conducted experimental studies on the critical electric Rayleigh number (<i>Ra</i><sub>ec</sub>) of the AC EK flow of binary fluids in a divergent microchannel. The experimental variations align well with the theoretical predictions, particularly the existence of an optimal AC frequency and electric conductivity ratio, demonstrating that the tanh model can better elucidate the underlying physics of EK flow. With the new electric Rayleigh number, we found that EK flow in the designed divergent microchannel has a much smaller <i>Ra</i><sub>ec</sub> than previously reported, indicating that EK flow is more unstable and thus more suitable for applications in micromixers or reactors in industry and engineering.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"83 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937823","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 : 2025-01-08DOI: 10.1021/acs.langmuir.4c04857
Xu Yan, Zhaoxiang Yang, Antong Ma, Zhiwu Chen, Yapei Wang
Zwitterionic hydrogels exhibit excellent nonfouling and hemocompatibility. However, the practical application of these materials as antifouling coatings for biomedical devices is hindered by several key challenges, including the harsh preparation conditions and the weak coating stability. Here, we present a two-component zwitterionic hydrogel paint for the in situ preparation of robust zwitterionic hydrogel coatings on various substrate surfaces without UV assistance. It is performed by the curing and adhesion of a zwitterionic hydrogel simultaneously through the ring opening reaction of epoxy and amino inspired by the successful commercial two-component epoxy structural glue. The obtained AB-type PSBMA coating can withstand water flow velocities of up to 15 m/s and still maintain its structural integrity and functional stability. It is noteworthy that the coating preparation process does not require the use of any organic solvent, which greatly simplifies the postprocessing steps for its application in medical devices. Moreover, the coating not only resists bacterial and cell adhesion but also exhibits favorable hemocompatibility. This approach offers a novel concept for the design of zwitterionic hydrogel coatings for biomedical devices.
{"title":"AB-Type Zwitterionic Hydrogel Paint","authors":"Xu Yan, Zhaoxiang Yang, Antong Ma, Zhiwu Chen, Yapei Wang","doi":"10.1021/acs.langmuir.4c04857","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04857","url":null,"abstract":"Zwitterionic hydrogels exhibit excellent nonfouling and hemocompatibility. However, the practical application of these materials as antifouling coatings for biomedical devices is hindered by several key challenges, including the harsh preparation conditions and the weak coating stability. Here, we present a two-component zwitterionic hydrogel paint for the in situ preparation of robust zwitterionic hydrogel coatings on various substrate surfaces without UV assistance. It is performed by the curing and adhesion of a zwitterionic hydrogel simultaneously through the ring opening reaction of epoxy and amino inspired by the successful commercial two-component epoxy structural glue. The obtained AB-type PSBMA coating can withstand water flow velocities of up to 15 m/s and still maintain its structural integrity and functional stability. It is noteworthy that the coating preparation process does not require the use of any organic solvent, which greatly simplifies the postprocessing steps for its application in medical devices. Moreover, the coating not only resists bacterial and cell adhesion but also exhibits favorable hemocompatibility. This approach offers a novel concept for the design of zwitterionic hydrogel coatings for biomedical devices.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"7 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935562","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}
Promethazine hydrochloride (PMHC) is a vital drug that is used as an anticholinergic, antipsychotic, antihistaminic, analgesic, sedative, and neuroleptic. However, the overdosage of PMHC also causes reproductive variations, cardiac changes, hypotension, and endocrinal variations. Hence, the detection of PMHC is crucial. Therefore, in this work an electrochemical method for the detection of PMHC is reported. The fabrication for the modified electrode is built with tungsten (W), nickel (N), and strontium (S) ternary oxide (tWNSO). To the best of our knowledge, this tWNSO ternary oxide preparation is reported for the first time in the literature. The prepared ternary oxide is deposited on the polypyrrole nanotubes, and this nanocomposite that is formed is confirmed by various physical characterizations like XRD, SEM, TEM, UV–vis spectroscopy, FTIR spectroscopy, and also DFT studies for PMHC. Thus, the nanocomposite obtained is used as a working electrode for the detection of PMHC. The fabricated tWNSO/PPyNTs/GCE has an effective surface area of 0.0436 cm2. Also, no fouling was observed. The limit of detection of the analyte PMHC is 3.66 nM, the limit of quantification is 11.10 nM, and the sensitivity of the fabricated electrode in identifying the analyte is found to be 20.10 μA μM–1 cm–2. Thus, the modified working electrode effectively detects the analyte PMHC while demonstrating excellent stability and reproducibility.
{"title":"Ternary Metal (W–Ni–Sr) Oxide@Polypyrrole Nanotubes: A New Frontier in the Electrochemical Detection of Promethazine Hydrochloride (PMHC)","authors":"Shilpa Purushothama, Sirisha Subbareddy, Santhosh Arehalli Shivamurthy, Sandeep Shadakshari, Shruthi Chinnakurli Dwarakanath, Venkata Narayana Palakollu","doi":"10.1021/acs.langmuir.4c03820","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03820","url":null,"abstract":"Promethazine hydrochloride (PMHC) is a vital drug that is used as an anticholinergic, antipsychotic, antihistaminic, analgesic, sedative, and neuroleptic. However, the overdosage of PMHC also causes reproductive variations, cardiac changes, hypotension, and endocrinal variations. Hence, the detection of PMHC is crucial. Therefore, in this work an electrochemical method for the detection of PMHC is reported. The fabrication for the modified electrode is built with tungsten (W), nickel (N), and strontium (S) ternary oxide (tWNSO). To the best of our knowledge, this tWNSO ternary oxide preparation is reported for the first time in the literature. The prepared ternary oxide is deposited on the polypyrrole nanotubes, and this nanocomposite that is formed is confirmed by various physical characterizations like XRD, SEM, TEM, UV–vis spectroscopy, FTIR spectroscopy, and also DFT studies for PMHC. Thus, the nanocomposite obtained is used as a working electrode for the detection of PMHC. The fabricated tWNSO/PPyNTs/GCE has an effective surface area of 0.0436 cm<sup>2</sup>. Also, no fouling was observed. The limit of detection of the analyte PMHC is 3.66 nM, the limit of quantification is 11.10 nM, and the sensitivity of the fabricated electrode in identifying the analyte is found to be 20.10 μA μM<sup>–1</sup> cm<sup>–2</sup>. Thus, the modified working electrode effectively detects the analyte PMHC while demonstrating excellent stability and reproducibility.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"24 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937709","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}
Zwitterionic polymers exhibit strong hydration, high biocompatibility, and antifouling properties. Dendrimers are regularly branched polymers, which are used in the drug delivery system (DDS). In this study, we synthesized zwitterionic monomer- and polymer-conjugated dendrimers as a biocompatible nanoparticle to investigate the relation between the hydration property and biodistribution. A sulfobetaine monomer (SBM) was conjugated at the termini of the polyamidoamine (PAMAM) dendrimer. Polysulfobetaines (PSBs) were produced by reversible addition–fragmentation chain transfer polymerization and were also conjugated at the termini. Intermediate water, that is, water molecules loosely bound to the material, can be estimated from the melting peaks at less than 0 °C in differential scanning calorimetry (DSC) measurement. Our DSC results showed that the PSB-conjugated dendrimers (PSM-dens) contained more intermediate water than the SBM-conjugated dendrimer (SBM-den). PSB-dens accumulated in the tumor after intravenous administration, but SBM-den did not. These suggested that the amount of intermediate water, that is, the hydration property, was related to the biodistribution of the zwitterionic dendrimers. This relation is a possible design criterion for drug carriers. PSB-dens accumulated in the tumor even after the second injection, possibly overcoming the accelerated blood clearance observed with poly(ethylene glycol)-modified nanoparticles. Thus, this kind of zwitterionic polymer-conjugated dendrimer is useful for the DDS in cancer treatment.
{"title":"Hydration and Biodistribution of Zwitterionic Dendrimers Conjugating a Sulfobetaine Monomer and Polymers","authors":"Chie Kojima, Rikuto Hirata, Nanako Dei, Hao He, Yuka Ikemoto, Akikazu Matsumoto","doi":"10.1021/acs.langmuir.4c04276","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04276","url":null,"abstract":"Zwitterionic polymers exhibit strong hydration, high biocompatibility, and antifouling properties. Dendrimers are regularly branched polymers, which are used in the drug delivery system (DDS). In this study, we synthesized zwitterionic monomer- and polymer-conjugated dendrimers as a biocompatible nanoparticle to investigate the relation between the hydration property and biodistribution. A sulfobetaine monomer (SBM) was conjugated at the termini of the polyamidoamine (PAMAM) dendrimer. Polysulfobetaines (PSBs) were produced by reversible addition–fragmentation chain transfer polymerization and were also conjugated at the termini. Intermediate water, that is, water molecules loosely bound to the material, can be estimated from the melting peaks at less than 0 °C in differential scanning calorimetry (DSC) measurement. Our DSC results showed that the PSB-conjugated dendrimers (PSM-dens) contained more intermediate water than the SBM-conjugated dendrimer (SBM-den). PSB-dens accumulated in the tumor after intravenous administration, but SBM-den did not. These suggested that the amount of intermediate water, that is, the hydration property, was related to the biodistribution of the zwitterionic dendrimers. This relation is a possible design criterion for drug carriers. PSB-dens accumulated in the tumor even after the second injection, possibly overcoming the accelerated blood clearance observed with poly(ethylene glycol)-modified nanoparticles. Thus, this kind of zwitterionic polymer-conjugated dendrimer is useful for the DDS in cancer treatment.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"83 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937711","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 : 2025-01-08DOI: 10.1021/acs.langmuir.4c03765
Lijia Zhao, Hao Gao, Shaolong Sheng, Wenbin Ma, Haibo Liu, Kai Wang, Qiang Wang
The stick–slip phenomenon as a prevalent friction instability poses significant challenges to industry, including frictional vibration, reduced precision, and noise generation. The interfacial interactions between asperities on the surface of materials are critical in influencing stick–slip behavior. This study focused on modifying the asperities on the surface of zinc-coated steel through temper rolling as a new approach to suppress friction-induced stick–slip vibration and noise. It was revealed that temper rolling effectively suppressed the stick–slip behavior when the deformation of zinc-coated steel exceeded 2.3%. The proposed mechanism suggested that the temper rolling reduced surface asperity density, resulting in diminished potential energy fluctuations and a subsequent decrease in the stick–slip amplitude (the difference between the static and kinetic friction coefficients). In situ observation using the digital image correlation (DIC) technique demonstrated that the decrease in the stick–slip amplitude affected the motion state of the friction pair, effectively suppressing the stick–slip vibration and noise generation. These findings highlight the potential of temper rolling as an effective strategy for tailoring the surface topography to suppress the stick–slip phenomenon along with its related vibration and noise.
{"title":"Suppressing Friction-Induced Stick–Slip Vibration and Noise of Zinc-Coated Steel through Temper Rolling","authors":"Lijia Zhao, Hao Gao, Shaolong Sheng, Wenbin Ma, Haibo Liu, Kai Wang, Qiang Wang","doi":"10.1021/acs.langmuir.4c03765","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03765","url":null,"abstract":"The stick–slip phenomenon as a prevalent friction instability poses significant challenges to industry, including frictional vibration, reduced precision, and noise generation. The interfacial interactions between asperities on the surface of materials are critical in influencing stick–slip behavior. This study focused on modifying the asperities on the surface of zinc-coated steel through temper rolling as a new approach to suppress friction-induced stick–slip vibration and noise. It was revealed that temper rolling effectively suppressed the stick–slip behavior when the deformation of zinc-coated steel exceeded 2.3%. The proposed mechanism suggested that the temper rolling reduced surface asperity density, resulting in diminished potential energy fluctuations and a subsequent decrease in the stick–slip amplitude (the difference between the static and kinetic friction coefficients). <i>In situ</i> observation using the digital image correlation (DIC) technique demonstrated that the decrease in the stick–slip amplitude affected the motion state of the friction pair, effectively suppressing the stick–slip vibration and noise generation. These findings highlight the potential of temper rolling as an effective strategy for tailoring the surface topography to suppress the stick–slip phenomenon along with its related vibration and noise.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"6 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937712","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 : 2025-01-08DOI: 10.1021/acs.langmuir.4c03677
Luoxi Tan, Haden L. Scott, Micholas Dean Smith, Sai Venkatesh Pingali, Xiaolin Cheng, Hugh M. O’Neill, John Katsaras, Jeremy C. Smith, James G. Elkins, Brian H. Davison, Jonathan D. Nickels
Solvent toxicity limits n-butanol fermentation titer, increasing the cost and energy consumption for subsequent separation processes and making biobased production more expensive and energy-intensive than petrochemical approaches. Amphiphilic solvents such as n-butanol partition into the cell membrane of fermenting microorganisms, thinning the transverse structure, and eventually causing a loss of membrane potential and cell death. In this work, we demonstrate the deleterious effects of n-butanol partitioning upon the lateral dimension of the membrane structure, called membrane domains or lipid rafts. Lipid rafts are regions of the cell membrane enriched with certain lipids, providing a reservoir of high melting temperature lipids and a platform for membrane protein partitioning and oligomerization. Neutron scattering experiments and molecular dynamics simulations revealed that n-butanol increased the size of the lipid domains in a model membrane system. The data showed that n-butanol partitions more into the disordered lipid regions than into the raft-like phase, leading to a differential thinning of these coexisting phases in the plane of the membrane and increasing the hydrophobic mismatch. The resulting increase in line tension at the interface favors domain coalescence to minimize the ratio of the interfacial length to domain area. A detailed computational investigation of the lipid domain interface identifies the boundary as a site of membrane disorder and thinning due to an accumulation of n-butanol. Solvent-induced changes to domain morphology and membrane instability at the domain interface are unrecognized modes of solvent-induced stress to fermenting microbes, representing targets for new solvent tolerance strategies to increase the n-butanol titer.
{"title":"Toxic Effects of Butanol in the Plane of the Cell Membrane","authors":"Luoxi Tan, Haden L. Scott, Micholas Dean Smith, Sai Venkatesh Pingali, Xiaolin Cheng, Hugh M. O’Neill, John Katsaras, Jeremy C. Smith, James G. Elkins, Brian H. Davison, Jonathan D. Nickels","doi":"10.1021/acs.langmuir.4c03677","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03677","url":null,"abstract":"Solvent toxicity limits <i>n</i>-butanol fermentation titer, increasing the cost and energy consumption for subsequent separation processes and making biobased production more expensive and energy-intensive than petrochemical approaches. Amphiphilic solvents such as <i>n</i>-butanol partition into the cell membrane of fermenting microorganisms, thinning the transverse structure, and eventually causing a loss of membrane potential and cell death. In this work, we demonstrate the deleterious effects of <i>n</i>-butanol partitioning upon the lateral dimension of the membrane structure, called membrane domains or lipid rafts. Lipid rafts are regions of the cell membrane enriched with certain lipids, providing a reservoir of high melting temperature lipids and a platform for membrane protein partitioning and oligomerization. Neutron scattering experiments and molecular dynamics simulations revealed that <i>n</i>-butanol increased the size of the lipid domains in a model membrane system. The data showed that <i>n</i>-butanol partitions more into the disordered lipid regions than into the raft-like phase, leading to a differential thinning of these coexisting phases in the plane of the membrane and increasing the hydrophobic mismatch. The resulting increase in line tension at the interface favors domain coalescence to minimize the ratio of the interfacial length to domain area. A detailed computational investigation of the lipid domain interface identifies the boundary as a site of membrane disorder and thinning due to an accumulation of <i>n</i>-butanol. Solvent-induced changes to domain morphology and membrane instability at the domain interface are unrecognized modes of solvent-induced stress to fermenting microbes, representing targets for new solvent tolerance strategies to increase the <i>n</i>-butanol titer.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"20 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935558","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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