Pub Date : 2025-02-23DOI: 10.1021/acs.langmuir.4c04952
Junsheng Wang, Gege He, Jinke Shen, Xiaozhen Lv, Hongyu Mi, Shun Lu
Transition metal and nitrogen codoped graphitic carbon materials with Co–N bonds serve as key non-noble-metal catalysts for the oxygen evolution reaction (OER). To enhance catalytic efficiency, we explore the anchoring of Co–N bonds on nitrogen-doped graphitic carbon (NC) substrates with varied phosphorus content. The catalyst is synthesized through a straightforward sintering and phosphating process of ZIF@DCA in a tube furnace. X-ray photoelectron spectroscopy (XPS) demonstrated that the Co–N bonds effectively formed an efficient charge transfer channel, removing the barrier that separated the Co–N active site from the work electrode surface. Phosphorus is uniformly distributed across the Co–N substrate, ensuring the exposure of most Co–N active sites during the electrochemical reaction. With favorable structural and electronic attributes, P/Co–N-2 showcases the lowest overpotentials at 10 and 300 mA cm–2, which are 200 and 300 mV, respectively. Additionally, it demonstrates stable performance over 100 h in 1 M KOH, outperforming other similar materials and RuO2. This study offers critical insights for the rational design of Co–N structures, exploring the interplay between structure, composition, and activity in electrochemical reactions.
{"title":"Phosphorus Incorporation Increases the Oxygen Electrocatalytic Activity of Co–N Catalysts","authors":"Junsheng Wang, Gege He, Jinke Shen, Xiaozhen Lv, Hongyu Mi, Shun Lu","doi":"10.1021/acs.langmuir.4c04952","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04952","url":null,"abstract":"Transition metal and nitrogen codoped graphitic carbon materials with Co–N bonds serve as key non-noble-metal catalysts for the oxygen evolution reaction (OER). To enhance catalytic efficiency, we explore the anchoring of Co–N bonds on nitrogen-doped graphitic carbon (NC) substrates with varied phosphorus content. The catalyst is synthesized through a straightforward sintering and phosphating process of ZIF@DCA in a tube furnace. X-ray photoelectron spectroscopy (XPS) demonstrated that the Co–N bonds effectively formed an efficient charge transfer channel, removing the barrier that separated the Co–N active site from the work electrode surface. Phosphorus is uniformly distributed across the Co–N substrate, ensuring the exposure of most Co–N active sites during the electrochemical reaction. With favorable structural and electronic attributes, P/Co–N-2 showcases the lowest overpotentials at 10 and 300 mA cm<sup>–2</sup>, which are 200 and 300 mV, respectively. Additionally, it demonstrates stable performance over 100 h in 1 M KOH, outperforming other similar materials and RuO<sub>2</sub>. This study offers critical insights for the rational design of Co–N structures, exploring the interplay between structure, composition, and activity in electrochemical reactions.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"128 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477644","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 : 2025-02-23DOI: 10.1021/acs.langmuir.4c04197
Yumnam Gyani Devi, Ajmal Koya Pulikkal
The anticorrosion properties of three amide-linked alkylpyridinium gemini surfactants (ALAPGS), viz., 3,3′-(propanediamide)bis(1-n-dodecylpyridinium) dibromide (ALDPGS), 3,3′-(propanediamide)bis(1-n-tetradecylpyridinium) dibromide (ALTPGS), and 3,3′-(propanediamide)bis(1-n-octadecylpyridinium) dibromide (ALOPGS), were studied on low-carbon steel in 3.5% NaCl through weight loss, electrochemical impedance spectroscopy (EIS), and potentiodynamic polarization (PDP) methods. The anticorrosive efficiency of ALAPGS on low-carbon steel was contingent upon the concentration and length of the alkyl tails. In addition, the corrosion inhibition efficiency was found to be the highest when the concentration of the gemini reaches close to the critical micelle concentration (cmc) and followed the order ALOPGS > ALTPGS > ALDPGS. The results obtained from EIS agreed with the findings of PDP and weight loss experiments. The PDP studies indicated that the studied gemini acts as a mixed-type inhibitor. Furthermore, the morphology of low-carbon steel was studied through scanning electron microscopy and atomic force microscopy. Molecular dynamics simulations were conducted to understand the interaction between ALAPGS and low-carbon steel. The results suggested that ALAPGS are effective corrosion inhibitors for low-carbon steel.
{"title":"Amide-Linked Alkylpyridinium Gemini Surfactants for Corrosion Mitigation of Low-Carbon Steel","authors":"Yumnam Gyani Devi, Ajmal Koya Pulikkal","doi":"10.1021/acs.langmuir.4c04197","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04197","url":null,"abstract":"The anticorrosion properties of three amide-linked alkylpyridinium gemini surfactants (ALAPGS), viz., 3,3′-(propanediamide)bis(1-<i>n</i>-dodecylpyridinium) dibromide (ALDPGS), 3,3′-(propanediamide)bis(1-<i>n</i>-tetradecylpyridinium) dibromide (ALTPGS), and 3,3′-(propanediamide)bis(1-<i>n</i>-octadecylpyridinium) dibromide (ALOPGS), were studied on low-carbon steel in 3.5% NaCl through weight loss, electrochemical impedance spectroscopy (EIS), and potentiodynamic polarization (PDP) methods. The anticorrosive efficiency of ALAPGS on low-carbon steel was contingent upon the concentration and length of the alkyl tails. In addition, the corrosion inhibition efficiency was found to be the highest when the concentration of the gemini reaches close to the critical micelle concentration (cmc) and followed the order ALOPGS > ALTPGS > ALDPGS. The results obtained from EIS agreed with the findings of PDP and weight loss experiments. The PDP studies indicated that the studied gemini acts as a mixed-type inhibitor. Furthermore, the morphology of low-carbon steel was studied through scanning electron microscopy and atomic force microscopy. Molecular dynamics simulations were conducted to understand the interaction between ALAPGS and low-carbon steel. The results suggested that ALAPGS are effective corrosion inhibitors for low-carbon steel.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"22 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477643","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 : 2025-02-22DOI: 10.1021/acs.langmuir.4c04836
Yu Zhao, Jia-Wei Zhang, Fouad Belhora, Abdelowahed Hajjaji, Chen Song
Discharge phenomena, from electrostatic discharges in integrated circuits to lightning in the atmosphere, are pervasive and can lead to economic consequences in the electronic industry. Among these, partial discharge (PD) is a critical factor causing insulation damage in power equipment, significantly impacting power networks. Moreover, due to the trend of digitization, the number of pieces of power equipment has significantly increased. Real-time online monitoring of equipment can alleviate the impact of unavoidable PD events, and its necessity is significantly enhanced. In response, co-designing advanced materials, non-volatile memory (NVM), and software (SW) for discharge monitoring offers a compelling solution. This is achieved through an integrated sensing–memory–computation system. This review thoroughly examines different technologies used for monitoring PD, focusing on how sensing, memory, and computation play a role. It also looks at the possible difficulties and future expectations when SW and hardware technologies are combined in these systems. The solution to the three challenges of energy consumption, dedicated architecture, and circuit aging in integrated systems will greatly improve the energy efficiency, processing speed, and service life of intelligent monitoring systems. Eventually, this provides a feasible strategy for designing systems that can efficiently reduce the negative impacts of PD through smart monitoring and analysis.
{"title":"Intelligent Monitoring Technology of Partial Discharge Based on an Integrated Sensing–Memory–Computation System","authors":"Yu Zhao, Jia-Wei Zhang, Fouad Belhora, Abdelowahed Hajjaji, Chen Song","doi":"10.1021/acs.langmuir.4c04836","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04836","url":null,"abstract":"Discharge phenomena, from electrostatic discharges in integrated circuits to lightning in the atmosphere, are pervasive and can lead to economic consequences in the electronic industry. Among these, partial discharge (PD) is a critical factor causing insulation damage in power equipment, significantly impacting power networks. Moreover, due to the trend of digitization, the number of pieces of power equipment has significantly increased. Real-time online monitoring of equipment can alleviate the impact of unavoidable PD events, and its necessity is significantly enhanced. In response, co-designing advanced materials, non-volatile memory (NVM), and software (SW) for discharge monitoring offers a compelling solution. This is achieved through an integrated sensing–memory–computation system. This review thoroughly examines different technologies used for monitoring PD, focusing on how sensing, memory, and computation play a role. It also looks at the possible difficulties and future expectations when SW and hardware technologies are combined in these systems. The solution to the three challenges of energy consumption, dedicated architecture, and circuit aging in integrated systems will greatly improve the energy efficiency, processing speed, and service life of intelligent monitoring systems. Eventually, this provides a feasible strategy for designing systems that can efficiently reduce the negative impacts of PD through smart monitoring and analysis.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"26 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470538","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 : 2025-02-22DOI: 10.1021/acs.langmuir.4c05139
Xihao Chen, Jiazhuo Wang, Nicolas F. Martins, Julio R. Sambrano, José A. S. Laranjeira
Penta-octagraphene (POG) is a newly suggested two-dimensional carbon allotrope recognized for its distinct configuration and fascinating electronic characteristics. This work presents a new inorganic counterpart of POG, named POG-B4C2N3, designed through density functional theory (DFT) calculations. This new structure exhibits a direct band gap transition at the X-point, measured at 0.32/0.86 eV with PBE/HSE functionals. Mechanical properties were comprehensively assessed, showcasing its Young’s modulus (Ymax/Ymin = 157.12/100.84 N/m) and shear modulus (Gmax/Gmin = 83.03/38.09 N/m), alongside Poisson’s ratio (νmax/νmin = 0.58/-0.09), indicating that POG-B4C2N3 is an auxetic material. Additionally, Li decoration on this monolayer was studied to investigate its potential to enhance hydrogen storage through physisorption. The Li@POG-B4C2N3 system shows robust physisorption (adsorption energies ranging from −0.35 to −0.19 eV), high hydrogen storage capacity (8.35 wt %), and effective hydrogen desorption dynamics, positioning this novel material as a promising platform for reversible hydrogen storage.
{"title":"Penta-Octa B4C2N3: A New 2D Material for High-Performance Energy Applications","authors":"Xihao Chen, Jiazhuo Wang, Nicolas F. Martins, Julio R. Sambrano, José A. S. Laranjeira","doi":"10.1021/acs.langmuir.4c05139","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c05139","url":null,"abstract":"Penta-octagraphene (POG) is a newly suggested two-dimensional carbon allotrope recognized for its distinct configuration and fascinating electronic characteristics. This work presents a new inorganic counterpart of POG, named POG-B<sub>4</sub>C<sub>2</sub>N<sub>3</sub>, designed through density functional theory (DFT) calculations. This new structure exhibits a direct band gap transition at the X-point, measured at 0.32/0.86 eV with PBE/HSE functionals. Mechanical properties were comprehensively assessed, showcasing its Young’s modulus (<i>Y</i><sub><i>max</i></sub>/<i>Y</i><sub><i>min</i></sub> = 157.12/100.84 N/m) and shear modulus (<i>G</i><sub><i>max</i></sub>/<i>G</i><sub><i>min</i></sub> = 83.03/38.09 N/m), alongside Poisson’s ratio (ν<sub><i>max</i></sub>/ν<sub><i>min</i></sub> = 0.58/-0.09), indicating that POG-B<sub>4</sub>C<sub>2</sub>N<sub>3</sub> is an auxetic material. Additionally, Li decoration on this monolayer was studied to investigate its potential to enhance hydrogen storage through physisorption. The Li@POG-B<sub>4</sub>C<sub>2</sub>N<sub>3</sub> system shows robust physisorption (adsorption energies ranging from −0.35 to −0.19 eV), high hydrogen storage capacity (8.35 wt %), and effective hydrogen desorption dynamics, positioning this novel material as a promising platform for reversible hydrogen storage.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"17 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470541","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 vapor-phase polymerization of pyrrole in the presence of polystyrene (PS) particles adsorbed at the air–water interface successfully leads to the formation of PS/polypyrrole (PPy) Janus particles where only the surface in contact with the air phase is regioselectively covered with the PPy nanolayer. The coverage area of the PPy nanolayer on the Janus particles, and therefore the contact angle of Janus particles at the air–liquid interface, decreases with a decrease in surface tension of liquid by the addition of isopropanol. The contact angle of particles at the interface decreases after the polymerization, which should be because the pyrrole monomer dissolved in the water phase from the gas phase promotes the wetting of the liquid to the PS particles by decreasing the surface tension of the liquid. Controlling the PS particle size realizes the formation of PS/PPy Janus particles with sizes ranging between 5 and 1000 μm. Furthermore, the Janus particles are demonstrated to be oriented at the air–water interface with the hydrophilic PS side toward the water phase and the hydrophobic PPy side toward the air phase, realizing stabilization of an armored bubble in the water medium.
{"title":"Janus Particles Synthesized via Vapor-Phase Coupling Polymerization Protocol","authors":"Kazuma Kuroiwa, Kazusa Takeuchi, Tomoyasu Hirai, Yoshinobu Nakamura, Yuya Oaki, Syuji Fujii","doi":"10.1021/acs.langmuir.4c05061","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c05061","url":null,"abstract":"The vapor-phase polymerization of pyrrole in the presence of polystyrene (PS) particles adsorbed at the air–water interface successfully leads to the formation of PS/polypyrrole (PPy) Janus particles where only the surface in contact with the air phase is regioselectively covered with the PPy nanolayer. The coverage area of the PPy nanolayer on the Janus particles, and therefore the contact angle of Janus particles at the air–liquid interface, decreases with a decrease in surface tension of liquid by the addition of isopropanol. The contact angle of particles at the interface decreases after the polymerization, which should be because the pyrrole monomer dissolved in the water phase from the gas phase promotes the wetting of the liquid to the PS particles by decreasing the surface tension of the liquid. Controlling the PS particle size realizes the formation of PS/PPy Janus particles with sizes ranging between 5 and 1000 μm. Furthermore, the Janus particles are demonstrated to be oriented at the air–water interface with the hydrophilic PS side toward the water phase and the hydrophobic PPy side toward the air phase, realizing stabilization of an armored bubble in the water medium.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"47 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470540","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}
Diethylene glycol (DEG)-assisted glycothermal synthesis can yield highly dispersed crystalline YAG (Y3Al5O12) colloidal nanoparticles (NPs). However, the role of the DEG is still unclear. Herein, we have investigated the influence of volume fraction of the cosolvent DEG and metal precursor concentration on phase composition and dispersion property of the glycothermally synthesized cerium(III)-doped YAG NPs. The addition of DEG can significantly improve the solubility of Al(iOPr)3 in glycol solvents, which in turn ensures a better contact between dissolved Al3+ ions and lanthanide ions. This prevents the formation of much larger boehmite or glycol derivative of boehmite particles from the undissolved Al precursor. With an appropriate Al molar concentration and a DEG to Al molar ratio, colloidal cerium-doped YAG NPs with a hydrodynamic diameter of about 10 nm can be obtained with nearly 100% yield by weight. The computational prediction suggests that colloidal YAG NPs can strongly associate with DEG ligands. The resulting NPs exhibit enhanced dispersion, likely due to the increased polarity and additional hydrogen bonding sites introduced by the DEG ligands. The implementation of DEG had a limited effect on the optical properties of the synthesized NPs, as long as it did not excessively compromise the crystalline integrity.
{"title":"Role of Diethylene Glycol in the Glycothermal Synthesis of Highly Dispersed Colloidal YAG:Ce3+ Nanoparticles","authors":"Yige Yan, Frédéric Lerouge, Carine Michel, Stéphane Parola, Frédéric Chaput","doi":"10.1021/acs.langmuir.4c04752","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04752","url":null,"abstract":"Diethylene glycol (DEG)-assisted glycothermal synthesis can yield highly dispersed crystalline YAG (Y<sub>3</sub>Al<sub>5</sub>O<sub>12</sub>) colloidal nanoparticles (NPs). However, the role of the DEG is still unclear. Herein, we have investigated the influence of volume fraction of the cosolvent DEG and metal precursor concentration on phase composition and dispersion property of the glycothermally synthesized cerium(III)-doped YAG NPs. The addition of DEG can significantly improve the solubility of Al(<sup>i</sup>OPr)<sub>3</sub> in glycol solvents, which in turn ensures a better contact between dissolved Al<sup>3+</sup> ions and lanthanide ions. This prevents the formation of much larger boehmite or glycol derivative of boehmite particles from the undissolved Al precursor. With an appropriate Al molar concentration and a DEG to Al molar ratio, colloidal cerium-doped YAG NPs with a hydrodynamic diameter of about 10 nm can be obtained with nearly 100% yield by weight. The computational prediction suggests that colloidal YAG NPs can strongly associate with DEG ligands. The resulting NPs exhibit enhanced dispersion, likely due to the increased polarity and additional hydrogen bonding sites introduced by the DEG ligands. The implementation of DEG had a limited effect on the optical properties of the synthesized NPs, as long as it did not excessively compromise the crystalline integrity.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"128 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470532","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 : 2025-02-22DOI: 10.1021/acs.langmuir.4c05261
Xiang Wu, Wanze Wu, Xinting Han, Xiao Gong
Oil spill accidents on the sea and oily wastewater produced in daily life have posed serious threats to the environment. Therefore, there is an urgent need for a material that can effectively separate these mixtures using simple operations. Herein, an ecofriendly sandwich-structured coating with excellent superhydrophobic/superoleophilic properties was fabricated by in situ growth on copper mesh and cotton fabric substrates. Specifically, using the versatility of tannic acid (TA) film, including chelation and reduction with Cu2+, flower-like Cu2S@CuO can be in situ grown on a copper mesh or fabric surface. Then, the Schiff base reaction between TA and octadecylamine is used to hydrophobically modify the surface. Water contact angle (WCA) of the sandwich-structured TA-Cu2S-TA-ODA-coated copper mesh and fabric can reach 160.8 and 156.3°. The coated copper mesh can be folded into a miniature container to collect oil, with collection efficiency reaching 96.47%. And the collection efficiency can be above 90% even after 10 cycles, and its WCA is still 155°. Besides, it can quickly separate various oils. Even for highly viscous peanut oil, the separation efficiency and flux can reach 90.7% and 0.038 mL·cm–2·s–1, respectively, which are much higher than those reported by other similar studies. Furthermore, the coating can endow cotton fabrics with excellent UV-shielding performance compared to the original cotton fabrics. In particular, even after 100 tape peeling tests, 7 washing cycles, 1 h of continuous strong UV irradiation, or 24 h of organic solvent soaking, the sandwich-structured TA-Cu2S-TA-ODA coating still has superhydrophobic properties.
{"title":"Sandwich-Structured Superhydrophobic Coating for Rapid and Ultrahigh-Efficiency Viscous Oil Separation from Water","authors":"Xiang Wu, Wanze Wu, Xinting Han, Xiao Gong","doi":"10.1021/acs.langmuir.4c05261","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c05261","url":null,"abstract":"Oil spill accidents on the sea and oily wastewater produced in daily life have posed serious threats to the environment. Therefore, there is an urgent need for a material that can effectively separate these mixtures using simple operations. Herein, an ecofriendly sandwich-structured coating with excellent superhydrophobic/superoleophilic properties was fabricated by in situ growth on copper mesh and cotton fabric substrates. Specifically, using the versatility of tannic acid (TA) film, including chelation and reduction with Cu<sup>2+</sup>, flower-like Cu<sub>2</sub>S@CuO can be in situ grown on a copper mesh or fabric surface. Then, the Schiff base reaction between TA and octadecylamine is used to hydrophobically modify the surface. Water contact angle (WCA) of the sandwich-structured TA-Cu<sub>2</sub>S-TA-ODA-coated copper mesh and fabric can reach 160.8 and 156.3°. The coated copper mesh can be folded into a miniature container to collect oil, with collection efficiency reaching 96.47%. And the collection efficiency can be above 90% even after 10 cycles, and its WCA is still 155°. Besides, it can quickly separate various oils. Even for highly viscous peanut oil, the separation efficiency and flux can reach 90.7% and 0.038 mL·cm<sup>–2</sup>·s<sup>–1</sup>, respectively, which are much higher than those reported by other similar studies. Furthermore, the coating can endow cotton fabrics with excellent UV-shielding performance compared to the original cotton fabrics. In particular, even after 100 tape peeling tests, 7 washing cycles, 1 h of continuous strong UV irradiation, or 24 h of organic solvent soaking, the sandwich-structured TA-Cu<sub>2</sub>S-TA-ODA coating still has superhydrophobic properties.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"27 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470542","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 : 2025-02-22DOI: 10.1021/acs.langmuir.4c04890
Arun Sharma, Navneet Kaur, Narinder Singh
Pharmaceutical pollution in wastewater poses significant environmental and public health concerns worldwide. Chloramphenicol (CP), an antibiotic widely used in medical and veterinary applications, is among the active pharmaceutical ingredients (APIs) frequently detected in aquatic environments. This study explored the encapsulation of chloramphenicol API in contaminated wastewater using rationally designed fibrations based on the silver metal ion-directed self-assembly of fibrillator-type self-assembling ligand (ANS-3). We further investigated the removal of various commonly prescribed drugs, including antibiotics such as β-lactam (amoxicillin), fluoroquinolone (ciprofloxacin), aminoglycoside (neomycin), and tetracycline; antiparasitic agents with antiprotozoal properties (praziquantel and metronidazole); nonsteroidal anti-inflammatory drugs (NSAIDs) such as phenylbutazone and ketoprofen; the vasodilator isoxsuprine; amphiphilic antidepressants (amitriptyline); and the antiviral drug amantadine. The findings validated the crucial influence of polar multifunctionality and structural complexity in enhancing interactions with Ag.ANS-3 matrix, emphasizing its potential for efficient drug sequestration. First, picolinic acid (PA) and phenylalanine (F) were evaluated for their ability to form fibrillar structures, and their morphological characterization revealed well-defined fibrillar networks with varying degrees of porosity and interconnectivity. Then, the strategic inclusion of leucine in synthesizing ANS-3 facilitated the formation of robust fibrillar networks, employing its hydrophobic interactions to drive the self-assembly process. Finally, the encapsulation of APIs was evaluated using Ag(I) metal ion-driven ANS-3 based self-assembled nanofibrous material. This research contributes to the development of innovative physicochemical wastewater treatment strategies for environmental remediation and validates the importance of rational design in encapsulation-based wastewater remediation technologies.
{"title":"Tailored Fibrils Approach via Ag(I).Peptidomimetic-Based Interface Design: Efficient Encapsulation of Diverse Active Pharmaceutical Ingredients in Wastewater Remediation during Effluent Treatment Plant (ETP) Processing","authors":"Arun Sharma, Navneet Kaur, Narinder Singh","doi":"10.1021/acs.langmuir.4c04890","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04890","url":null,"abstract":"Pharmaceutical pollution in wastewater poses significant environmental and public health concerns worldwide. Chloramphenicol (CP), an antibiotic widely used in medical and veterinary applications, is among the active pharmaceutical ingredients (APIs) frequently detected in aquatic environments. This study explored the encapsulation of chloramphenicol API in contaminated wastewater using rationally designed fibrations based on the silver metal ion-directed self-assembly of fibrillator-type self-assembling ligand (<b>ANS-3</b>). We further investigated the removal of various commonly prescribed drugs, including antibiotics such as β-lactam (amoxicillin), fluoroquinolone (ciprofloxacin), aminoglycoside (neomycin), and tetracycline; antiparasitic agents with antiprotozoal properties (praziquantel and metronidazole); nonsteroidal anti-inflammatory drugs (NSAIDs) such as phenylbutazone and ketoprofen; the vasodilator isoxsuprine; amphiphilic antidepressants (amitriptyline); and the antiviral drug amantadine. The findings validated the crucial influence of polar multifunctionality and structural complexity in enhancing interactions with <b>Ag</b>.<b>ANS-3</b> matrix, emphasizing its potential for efficient drug sequestration. First, picolinic acid (PA) and phenylalanine (F) were evaluated for their ability to form fibrillar structures, and their morphological characterization revealed well-defined fibrillar networks with varying degrees of porosity and interconnectivity. Then, the strategic inclusion of leucine in synthesizing <b>ANS-3</b> facilitated the formation of robust fibrillar networks, employing its hydrophobic interactions to drive the self-assembly process. Finally, the encapsulation of APIs was evaluated using Ag(I) metal ion-driven <b>ANS-3</b> based self-assembled nanofibrous material. This research contributes to the development of innovative physicochemical wastewater treatment strategies for environmental remediation and validates the importance of rational design in encapsulation-based wastewater remediation technologies.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"65 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470539","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 : 2025-02-21DOI: 10.1021/acs.langmuir.4c04842
Fengfeng Feng, Dongcheng Xiao, Fan Yang, Hao Liu, Minghai Qu, Weijie Wang
The self-assembly of giant amphiphilic molecules with diverse topological structures has been widely investigated in bulk, solution, and interfacial environments because it can lead to interesting geometric patterns. However, many giant molecules or their self-assembling units are built by covalent bonds, which may limit the movement of the molecular blocks, affecting the self-assembly process and microstructure. In contrast, the self-assembly of giant units with noncovalent interactions can lead to interesting nanomorphologies and nanostructures. In this study, we built giant amphiphilic molecules (BPOSS&POM) by forming electrostatic interactions between hydrophobic isobutyl polyhedral oligomeric silsesquioxanes (BPOSSs) and hydrophilic polyoxometalates (POMs) to investigate the self-assembly behavior in water/acetone, water/THF, and hexane/acetone cosolvents. By controlling the solvent parameters, BPOSS&POM self-assembled into nanosheet, nanobelt, nanosphere, and nanocrumb structures. The morphology and detailed nanostructure of the different self-assemblies were revealed by performing transmission electron microscopy (TEM), scanning electron microscopy (SEM), and small-angle X-ray scattering (SAXS) measurements. The TEM and SAXS results indicated that the self-assembly microphase exhibited a lamellar structure and an interlayer distance of about 3 nm. The microphase structure of the self-assembly was alternatively organized by layers of BPOSS and POM according to their size and dimension. The polarity of the solvents substantially affected the morphology of the nanoassemblies but not the aggregation behavior of BPOSS and POM. This research offers insights into the preparation of nanomaterials with diverse micromorphologies by simply adjusting the solution components.
{"title":"Self-assembled Nanostructures of Noncovalent Giant Amphiphilic Molecules Composed of Hydrophobic Isobutyl BPOSS and Hydrophilic POM in Different Cosolvents","authors":"Fengfeng Feng, Dongcheng Xiao, Fan Yang, Hao Liu, Minghai Qu, Weijie Wang","doi":"10.1021/acs.langmuir.4c04842","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04842","url":null,"abstract":"The self-assembly of giant amphiphilic molecules with diverse topological structures has been widely investigated in bulk, solution, and interfacial environments because it can lead to interesting geometric patterns. However, many giant molecules or their self-assembling units are built by covalent bonds, which may limit the movement of the molecular blocks, affecting the self-assembly process and microstructure. In contrast, the self-assembly of giant units with noncovalent interactions can lead to interesting nanomorphologies and nanostructures. In this study, we built giant amphiphilic molecules (BPOSS&POM) by forming electrostatic interactions between hydrophobic isobutyl polyhedral oligomeric silsesquioxanes (BPOSSs) and hydrophilic polyoxometalates (POMs) to investigate the self-assembly behavior in water/acetone, water/THF, and hexane/acetone cosolvents. By controlling the solvent parameters, BPOSS&POM self-assembled into nanosheet, nanobelt, nanosphere, and nanocrumb structures. The morphology and detailed nanostructure of the different self-assemblies were revealed by performing transmission electron microscopy (TEM), scanning electron microscopy (SEM), and small-angle X-ray scattering (SAXS) measurements. The TEM and SAXS results indicated that the self-assembly microphase exhibited a lamellar structure and an interlayer distance of about 3 nm. The microphase structure of the self-assembly was alternatively organized by layers of BPOSS and POM according to their size and dimension. The polarity of the solvents substantially affected the morphology of the nanoassemblies but not the aggregation behavior of BPOSS and POM. This research offers insights into the preparation of nanomaterials with diverse micromorphologies by simply adjusting the solution components.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"11 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463200","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 : 2025-02-21DOI: 10.1021/acs.langmuir.4c04428
Liuzhen Ren, Jiangzhuo Ren, Luyao Bao, Jun Wen, Min Ye, Haibao Hu
The liquid–liquid interface (LLI), which is the key to cause flow slippage and thus promote drag reduction of liquid-infused surfaces (LISs), does suffer from the action of flow shear. In the current study, the transverse many-body dissipative dynamics simulation method is applied to explore the shear evolution of LLI and the corresponding slippage over a periodically grooved LIS. Results show that a relatively small shear rate only induces a slight deformation of LLI and the corresponding effective slippage is dependent on the shear rate. With a further increase of the shear rate, LLI deforms apparently and then the downstream three phase contact line depins to move once the balance between the capillary force and the shear force is broken, which results in an apparent increase of the slippage, specifically for a convex LLI. Compared with a convex LLI or a concave LLI, a flat LLI remains relatively stable under the same shear action, and an increase of the viscosity ratio and a decrease of the LLI fraction can both strengthen the shear resistance of an LLI, while they are less effective to promote the slippage. Consequently, the current results not only indicate that the slippage is related to the interface deflection and the shear rate but also suggest that both the shear resistance and the slippage of LLI should be considered when designing an effective LIS.
{"title":"Shear Evolution and Slippage of the Liquid–Liquid Interface over a Liquid-Infused Surface: A Many-Body Dissipative Particle Dynamics Study","authors":"Liuzhen Ren, Jiangzhuo Ren, Luyao Bao, Jun Wen, Min Ye, Haibao Hu","doi":"10.1021/acs.langmuir.4c04428","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04428","url":null,"abstract":"The liquid–liquid interface (LLI), which is the key to cause flow slippage and thus promote drag reduction of liquid-infused surfaces (LISs), does suffer from the action of flow shear. In the current study, the transverse many-body dissipative dynamics simulation method is applied to explore the shear evolution of LLI and the corresponding slippage over a periodically grooved LIS. Results show that a relatively small shear rate only induces a slight deformation of LLI and the corresponding effective slippage is dependent on the shear rate. With a further increase of the shear rate, LLI deforms apparently and then the downstream three phase contact line depins to move once the balance between the capillary force and the shear force is broken, which results in an apparent increase of the slippage, specifically for a convex LLI. Compared with a convex LLI or a concave LLI, a flat LLI remains relatively stable under the same shear action, and an increase of the viscosity ratio and a decrease of the LLI fraction can both strengthen the shear resistance of an LLI, while they are less effective to promote the slippage. Consequently, the current results not only indicate that the slippage is related to the interface deflection and the shear rate but also suggest that both the shear resistance and the slippage of LLI should be considered when designing an effective LIS.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"38 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470543","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：