Langmuir最新文献

{"title":"N/O Co-doped Porous Carbon with Controllable Porosity Synthesized via an All-in-One Step Method for a High-Rate-Performance Supercapacitor.","authors":"Chenweijia He, Guangjie Yang, Liye Ni, Haoqi Yang, Yongshuo Peng, Xiangdong Liu, Ping Li, Cheng Song, Shuijian He, Qian Zhang","doi":"10.1021/acs.langmuir.4c02328","DOIUrl":"10.1021/acs.langmuir.4c02328","url":null,"abstract":"<p><p>A green and economical methodology to fabricate carbon-based materials with suitable pore size distributions is needed to achieve rapid electrolyte diffusion and improve the performance of supercapacitors. Here, a method combining <i>in situ</i> templates with self-activation and self-doping is proposed. By variation of the molar ratio of magnesium folate and potassium folate, the pore size distribution was effectively adjusted. The optimal carbon materials (K<i>x</i>) have a high specific surface area (1021-1676 m² g^-1) and hierarchical pore structure, which significantly promotes its excellent capacitive properties. Notably, K2 shows an excellent mass specific capacitance of 233 F g^-1 at 0.1 A g^-1. It still retained 113 F g^-1 at 55 A g^-1. The assembled symmetric supercapacitor exhibited an outstanding cyclic stability. It maintains 100% capacitance after 100 000 cycles at 10 A g^-1. The symmetric supercapacitor demonstrated a maximum power density of 99.8 kW kg^-1. This study focuses on the preparation of layered pore structures to provide insights into the sustainable design of carbon materials.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142124190","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":"Electrostatically Spun Fabrication of Fe₃O₄@SiO₂/PVA Membranes for Efficient Methyl Orange (MO) Adsorption and Response Surface Optimization of the Processes.","authors":"Heng Li, Chengzhong Zhang, Huanhuan Jin, Shuai Wang, Ruixin Li, Zhen Zhang","doi":"10.1021/acs.langmuir.4c02266","DOIUrl":"10.1021/acs.langmuir.4c02266","url":null,"abstract":"<p><p>The environmental pollution problem caused by azo dyes urgently needs to be solved. Fe₃O₄@SiO₂/poly(vinyl alcohol) (PVA) membranes were prepared via an electrostatic spinning process. By blending the prepared Fe₃O₄@SiO₂ nanoparticles with PVA, a uniform distribution of Fe₃O₄@SiO₂ nanoparticles within the fibers was achieved, effectively preventing the aggregation of the nanoparticles and demonstrating excellent adsorption performance toward the azo anionic dye methyl orange (MO). The adsorption isotherms and kinetic data for Fe₃O₄@SiO₂/PVA adsorbed MO were consistent with Langmuir and the pseudo-second-order model, respectively. Owing to the electrostatic attraction, hydrogen bonding, and pore-filling effect, Fe₃O₄@SiO₂/PVA effectively removed MO from water, with a maximum adsorption amount of 349.896 mg/g at 25 °C. Very importantly, the Fe₃O₄@SiO₂/PVA membrane can be regenerated and reused efficiently, with no significant decrease in adsorption capacity after five adsorption cycles. In addition, response surface methodology (RSM) was used to analyze the effects of various factors on the MO adsorption performance of Fe₃O₄@SiO₂/PVA membranes, as well as the interactions of various factors. This research indicated that Fe₃O₄@SiO₂/PVA membranes are promising adsorbents for MO due to their low cost, ease of regeneration, and environmental friendliness.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142131107","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":"Understanding the Role of Solvent on the Growth of Zinc Oxide: Insight from Experiment and Molecular Dynamics Simulations.","authors":"Sherif Okeil, Sahar Rabet, Gerardo Valadez Huerta, Gabriele Raabe, Georg Garnweitner","doi":"10.1021/acs.langmuir.4c00921","DOIUrl":"10.1021/acs.langmuir.4c00921","url":null,"abstract":"<p><p>The controlled synthesis of nanoparticles with tailored shapes and morphologies has garnered significant attention, driven by the ever-growing demand for advanced materials with defined properties. In nanoparticle formation, various parameters influence the final product, and among these, the solvent plays a pivotal role, as it constitutes the major component of the reaction medium. In this work, the critical role of solvents in controlling the growth of zinc oxide (ZnO) nanoparticles was investigated, with a focus on simple primary alcoholic solvents as the reaction medium. A model reaction based on the direct solvolysis of anhydrous zinc acetylacetonate was employed to probe the influence of different primary alcohols, specifically methanol, ethanol, and their mixture. A substantial difference in the preferential growth direction of the ZnO nanocrystals in methanol and ethanol was observed through XRD and was further proven through TEM. Thereby, in ethanol, a preferential growth in the [001] direction was observed, resulting in short nanorods as primary particles, while this growth was inhibited in methanol, leading to platelet- or sheet-like primary particles. To unravel the underlying mechanisms responsible for the observed solvent-dependent variations, molecular dynamics (MD) simulations were employed using an optimized interface force field to model the ZnO-alcohol interaction. These simulations provide valuable insights into the preferential adsorption of the solvent molecules onto the polar (0001) and (0001̅) and nonpolar (101̅0) ZnO surfaces, shedding light on the fundamental interactions driving the shape control phenomenon. Essentially, the experimental observations on primary particle morphology could be explained well by the adsorption behavior determined by the MD simulations. Furthermore, this report provides an extensive comparison with various similar reaction systems for ZnO synthesis, deriving correlations with the findings from the model system. These insights contribute to a deeper understanding of the intricate interplay between solvent properties and nanoparticle growth, offering a valuable toolkit for designing and optimizing the synthesis of ZnO nanoparticles with specific shapes and functionalities.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11411714/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142118287","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Schottky Interface Enabled Electrospun Rhodium Oxide Doped Gold for Both pH Sensing and Glucose Measurements in Neutral Buffer and Human Serum","authors":"Weiyu Xiao, Mingman Li, Danlei Li, Bo Shi, Runze Zhong, Yiyuan Zhao, Qingliang Tai, Songbing He, Qiuchen Dong","doi":"10.1021/acs.langmuir.4c02999","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c02999","url":null,"abstract":"This study has focused on adjusting sensing environment from basic to neutral pH and improve sensing performance by doping electrodeposited gold (Au) with metal oxide for nonenzymatic glucose measurements in forming a Schottky interface for superior glucose sensing with detailed analysis for the sensing mechanism. The prepared sensor also holds the ability to measure pH with the identical electrospun metal oxide-electrodeposited Au, which composed a dual sensor (glucose and pH sensor) through applying chronoamperometry and open circuit potential methods. The rhodium oxide nanocoral structure was fabricated with an electrospinning precursor solution, followed by a calcination process, and it was mixed with electrodeposited nanocoral gold to form the Schottky interface by constructing a p-n type heterogeneous junction for improved sensitivity in glucose detection. The prepared materials were characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectrometry (XPS), etc. The prepared materials were used for both pH responsive testing and amperometric glucose measurements. The rhodium oxide nanocoral doped gold demonstrated a sensitivity of 3.52 μA mM^–1 cm^–2 and limit of detection of 20 μM with linear range up to 3 mM glucose concentration compared to solely electrodeposited gold for a sensitivity of 0.46 μA mM^–1 cm^–2 and a limit of detection of 450 μM. The Mott–Schottky method was used for the analysis of an electron transfer process from noble metal to metal oxide to electrolyte in demonstrating the improved sensitivity at neutral pH for glucose measurements due to the Schottky barrier adjustment mechanism at an applied flat band potential of 0.3 V. This work opens a new venue in illustrating the metal oxide/metal materials in the glucose neutral response mechanism. In the end, human serum samples were tested against current commercial glucose meter to certify the accuracy of the proposed sensor.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142235448","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":"Zwitterionic Polyelectrolyte Complex Vesicles Assembled from Homopoly(2-Oxazoline)s as Enzyme Catalytic Nanoreactors for Potent Anti-Tumor Efficiency.","authors":"Hepeng Wang, Guojing Zhang, Min Lin, Christian G Hartinger, Jing Sun","doi":"10.1021/acs.langmuir.4c01729","DOIUrl":"10.1021/acs.langmuir.4c01729","url":null,"abstract":"<p><p>Enzymes are known for their remarkable catalytic efficiency across a wide range of applications. Here, we present a novel and convenient nanoreactor platform based on zwitterionic polyelectrolyte complex vesicles (PCVs), assembled from oppositely charged homopoly(2-oxazoline)s, facilitating enzyme immobilization. We show remarkable enhancements in catalytic activity and stability by encapsulation of lipase as a model enzyme. Even as the temperature rises, the performance of the lipase remains robust. Further, the structural characteristics of PCVs, including hollow architecture and semipermeable membranes, endow them with unique advantages for enzyme cascade reactions involving glucose oxidase (GOx) and horseradish peroxidase (HRP). A decline in catalytic efficiency is shown when the enzymes are individually loaded and subsequently mixed, in contrast to the coloaded GOx-HRP-PCV group. We demonstrate that the vesicle structures establish confined environments where precise enzyme-substrate interactions facilitate enhanced catalytic efficiency. In addition, the nanoreactors exhibit excellent biocompatibility and efficient anti-tumor activity, which hold significant promise for biomedical applications within enzyme-based technologies.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141854163","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":"High Capacitance Performance N, O Codoped Carbon Foams Synthesized via an All-In-One Step Carbonization of Molecular Salt Strategy.","authors":"Liye Ni, Guangjie Yang, Chenweijia He, Tiancheng Lan, Shuijian He, Haoqi Yang, Nan Wu, Rulan Chen, Li Liu, Fangdi Wu, Qian Zhang","doi":"10.1021/acs.langmuir.4c02392","DOIUrl":"10.1021/acs.langmuir.4c02392","url":null,"abstract":"<p><p>The preparation of porous carbon is constrained by the extensive use and detrimental impact of activators and dopants. Therefore, developing green and efficient strategies that leverage the intrinsic properties and pretreatment of the materials to achieve self-activation and self-doping is particularly crucial for porous carbon materials. Herein, potassium histidine was utilized as the molecular salt precursor, attaining the efficient and streamlined preparation of porous carbon through a one-step carbonization process that enables self-activation, self-doping, and self-templating. More interestingly, the carbonization temperature significantly impacts the porous structure of the molecular salt precursors, the properties of the heteroatoms, and electrochemical performance. The designed electrodes exhibit high accessibility to electrolyte ions and effective ion-electron transport channels. Therefore, the optimal carbon material (KHis800) has an excellent mass-specific capacitance of 305.2 F g^-1 at 0.2 A g^-1, and a high capacitance retention rate of 115.6% (50,000 cycles at 5 A g^-1). Notably, KHis800 also shows a maximum energy density of 19.6 Wh kg^-1. This research is dedicated to exploring a more efficient preparation method for porous carbon material via molecular salts, offering insights for the sustainable development of carbon materials.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142102208","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":"Gold Nanoparticles in Serum and Milk and Their Effect for Label-Free Colorimetric Sensing of DNA.","authors":"Yiting Wang, Ruinian Hua, Juewen Liu","doi":"10.1021/acs.langmuir.4c02763","DOIUrl":"10.1021/acs.langmuir.4c02763","url":null,"abstract":"<p><p>Label-free gold nanoparticle (AuNP)-based colorimetric biosensors have been widely used for the detection of DNA. However, the effect of the biological sample matrix has not been fully explored. In this work, we investigated the salt-induced aggregation of AuNPs as well as DNA adsorption in serum and milk. AuNPs of 13, 30, and 50 nm were used as probes. The detection was successful only in a clean buffer but failed in serum or milk. Serum and milk exhibited excellent protective properties, even 250 mM NaCl added did not induce the aggregation of AuNPs. After centrifugation of milk, the supernatant did not protect the AuNPs, whereas the redispersed pellet showed protection. The limit concentration of serum to prevent AuNPs from aggregating was 0.04% for 13 nm AuNPs and 0.01% serum for 50 nm AuNPs. In addition, serum reduced DNA adsorption, and the DNA was adsorbed to the protein corona instead of directly to the AuNP surface. These two factors can explain the difficulty of detection in protein-containing samples. This study articulates the adsorption of proteins by AuNPs in biological samples and offers useful insights into the biosensor design.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142118345","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":"Modulating Electrical Double Layers: Facile Approach for Promoting Noncovalent Interactions between Boron Nitride Nanosheets and Gold Nanoparticles.","authors":"Alireza Dibaji, Motilal Mathesh, Srikanth Mateti, Colin J Barrow, Ying Ian Chen, Wenrong Yang","doi":"10.1021/acs.langmuir.4c02587","DOIUrl":"10.1021/acs.langmuir.4c02587","url":null,"abstract":"<p><p>Electrical double layer (EDL) plays a crucial role in colloidal chemistry, which can be modified by changing the pH and ionic strength of a solution. Even though EDL is well-recognized, there are limited studies exploring interactions between two-dimensional (2D) and zero-dimensional nanoparticles. Herein, we demonstrate a simple pH-based approach to control the EDL of boron nitride nanosheets (BNNSs) and gold nanoparticles (AuNPs) that plays a crucial role in their interaction, displaying a one-way gate effect. We observed that as the EDL decreases, AuNPs can come into closer interaction with BNNSs, and this also resulted in a deceleration of the aggregation process of AuNPs when functionalized with l-cysteine. This work provides a fundamental understanding of how modulation of the EDL of 2D nanomaterials can be achieved through functionalizing strategies.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142118348","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":"Amorphous Titanium Dioxide-Based Heterojunction with Locally Enhanced Electron Transport Multipathways for High-Efficient Photodegradation of Tetracycline.","authors":"Mingyue Sun, Fang Zhou, Yin Guan, Huining Liu, Yuren Zhao, Ge Xu","doi":"10.1021/acs.langmuir.4c02082","DOIUrl":"10.1021/acs.langmuir.4c02082","url":null,"abstract":"<p><p>A novel amorphous titanium dioxide (AT)-based heterojunction, composed of AT, silver bromide, and silver nanoparticles (Ag NPs), was synthesized and designated as AgBr/Ag/AT-4%. The band structure and active species of AgBr/Ag/AT-4% composites were investigated, and the existence of multiple electron transport pathways in the composites was determined. The Channel I is an all-solid-state Z-scheme heterostructure formed between AT and AgBr by Ag acting as an electron transport bridge, and Channel II is excited by the localized surface plasmon resonance effect induced by the Ag NPs on the photocatalyst surface. The Channel III is an electronically bridged medium with Ti³⁺/Ti⁴⁺ redox coupling pairs and oxygen vacancy-mediated trap states constructed from defective structures. The activity of the sample was assessed by the photocatalytic degradation of tetracycline. It is hoped that this work will provide a new idea for the preparation of an amorphous titanium dioxide-based heterojunction with locally enhanced electron transport multiple pathways.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142131103","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":"Application of ANN and RSM for Rhodamine B and Safranine-O Decolorization on Zinc-Carbon Battery Waste Derived Ag/CoFe-LDH/rGO Catalyst.","authors":"Ümit Ecer, Berdan Ulaş, Şakir Yılmaz","doi":"10.1021/acs.langmuir.4c02876","DOIUrl":"10.1021/acs.langmuir.4c02876","url":null,"abstract":"<p><p>The present work is first aimed at recovering graphite from carbon rods of waste zinc-carbon (Zn-C) batteries for applications such as wastewater treatment, in order to contribute to the development of a sustainable environment. Then, a composite material, cobalt-iron layered double hydroxide combination with reduced graphene oxide, and with subsequent Ag nanoparticles deposition via NaBH₄ reduction method (Ag/CoFe-LDH/rGO) was prepared for the catalytic activity of Rhodamine B (RhB) and Safranine-O (SO) as model contaminants from aquatic media. The catalytic activity of RhB and SO by Ag/CoFe-LDH/rGO in the presence of NaBH₄ was studied to model and optimize the process parameters (NaBH₄ amount, reaction time, initial dye concentration (<i>C</i>_o), and catalyst dosage) via central composite design (CCD)-response surface methodology (RSM). Also, an artificial neural network (ANN) model was developed to estimate the catalytic activity of each dye using an RSM data set. The catalytic activities of 99.54% and 99.96% were obtained for RhB and SO dyes, respectively, under the optimal conditions: NaBH₄ amount 12.32 mM, reaction time 3.19 min, <i>C</i>_o 33.46 mg/L, and catalyst dosage 1.24 mg/mL for RhB dye; NaBH₄ amount 16.76 mM, reaction time 3.06 min, <i>C</i>_o 15.10 mg/L, and catalyst dosage 1.46 mg/mL for SO dye. The optimum conditions of process parameters by ANN with gray wolf optimizer (GWO) were in good agreement with the points determined the RSM-CCD. These results demonstrate that RSM and ANN approaches can be applied practically and efficiently to maximize the catalytic activity of RhB and SO by Ag/CoFe-LDH/rGO in the existence of NaBH₄. On the other hand, from the kinetic and thermodynamic studies, the positive activation enthalpy, Δ<i>H</i>^# and the negative activation entropy, Δ<i>S</i>^# values for each dye demonstrated that the catalytic performance was endothermic and less random at the solid/liquid interface.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142124161","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}