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α-FeOOH-Modified Sn/N-Codoped TiO2 Bifunctional Composites for As(III) Removal through Photocatalytic Oxidation and Simultaneous Adsorption 通过光催化氧化和同时吸附去除 As(III) 的 α-FeOOH 改性 Sn/N 掺杂 TiO2 双功能复合材料
IF 3.9 2区 化学
Langmuir Pub Date : 2024-07-13 DOI: 10.1021/acs.langmuir.4c01742
Juntao Wang, Wenke Zhu, Hanyu Liu, Wenlei Wang, Ting Yang
{"title":"α-FeOOH-Modified Sn/N-Codoped TiO2 Bifunctional Composites for As(III) Removal through Photocatalytic Oxidation and Simultaneous Adsorption","authors":"Juntao Wang, Wenke Zhu, Hanyu Liu, Wenlei Wang, Ting Yang","doi":"10.1021/acs.langmuir.4c01742","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c01742","url":null,"abstract":"Photocatalytic oxidation technology is one of the most efficient and green methods to convert highly toxic As(III) into lowly toxic As(V) for arsenic-polluted wastewater. However, the obtained As(V) may be reduced to As(III) again in the environment, causing secondary pollution. In order to resolve these issues, a bifunctional composite consisting of needle-like α-FeOOH-modified Sn/N-codoped TiO<sub>2</sub> granules (SNT-FeOOH) has been synthesized. After modifying, the band gap of SNT-FeOOH narrowed from 2.94 eV (SNT) to 2.29 eV. When the composites were applied to As(III) removal, 10 mg of SNT-FeOOH could totally photocatalytically oxidize 40 mL of As(III) solution with a concentration of 10,000 μg/L within 15 min and synchronously achieve complete adsorption of the produced As(V), which is much more efficient than pure Sn/N-codoped TiO<sub>2</sub> [21 min for As(III) photocatalytic oxidation and only 20.01% of total arsenic removal efficiency]. Based on the characterizations, α-FeOOH modification plays a significant role in the promoted performances of photocatalytic oxidation and adsorption of SNT-FeOOH, leading to arsenic removal. On one hand, the Fe–O–Ti interfacial chemical interactions formed between α-FeOOH and Sn/N-codoped TiO<sub>2</sub> can further boost the separation rate of photogenerated carriers, hence increasing the photocatalytic oxidation efficiency. On the other hand, α-FeOOH surface hydroxyl groups adsorb the generated As(V) by forming Fe–O–As bonds. The SNT-FeOOH bifunctional composites, prepared in this paper, with dual performances of photocatalytic oxidation and adsorption provide a new strategy to achieve arsenic removal from wastewater.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602850","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}
引用次数: 0
Poly(Photosensitizer-Prodrug) Unimolecular Micelles for Chemo-Photodynamic Synergistic Therapy of Antitumor and Antibacteria 用于抗肿瘤和抗菌化学光动力协同疗法的聚光敏剂-药物单分子胶束
IF 3.9 2区 化学
Langmuir Pub Date : 2024-07-13 DOI: 10.1021/acs.langmuir.4c00950
Jieheng Zhang, Jianchang Xu, Jiaying Zhang, Yibin Lin, Jiaxin Li, Duoqu Chen, Wenjing Lin, Chufen Yang, Guobin Yi
{"title":"Poly(Photosensitizer-Prodrug) Unimolecular Micelles for Chemo-Photodynamic Synergistic Therapy of Antitumor and Antibacteria","authors":"Jieheng Zhang, Jianchang Xu, Jiaying Zhang, Yibin Lin, Jiaxin Li, Duoqu Chen, Wenjing Lin, Chufen Yang, Guobin Yi","doi":"10.1021/acs.langmuir.4c00950","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c00950","url":null,"abstract":"It is crucial to use simple methods to prepare stable polymeric micelles with multiple functions for cancer treatment. Herein, via a “bottom-up” strategy, we reported the fabrication of β-CD-(PEOSMA-PCPTMA-PPEGMA)<sub>21</sub> (βPECP) unimolecular micelles that could simultaneously treat tumors and bacteria with chemotherapy and photodynamic therapy (PDT). The unimolecular micelles consisted of a 21-arm β-cyclodextrin (β-CD) core as a macromolecular initiator, photosensitizer eosin Y (EOS-Y) monomer EOSMA, anticancer drug camptothecin (CPT) monomer, and a hydrophilic shell PEGMA. Camptothecin monomer (CPTMA) could achieve controlled release of the CPT due to the presence of responsively broken disulfide bonds. PEGMA enhanced the biocompatibility of micelles as a hydrophilic shell. Two βPECP with different lengths were synthesized by modulating reaction conditions and the proportion of monomers, which both were self-assembled to unimolecular micelles in water. βPECP unimolecular micelles with higher EOS-Y/CPT content exhibited more excellent <sup>1</sup>O<sub>2</sub> production, in vitro drug release efficiency, higher cytotoxicity, and superior antibacterial activity. Also, we carried out simulations of the self-assembly and CPT release process of micelles, which agreed with the experiments. This nanosystem, which combines antimicrobial and antitumor functions, provides new ideas for bacteria-mediated tumor clinical chemoresistance.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602833","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}
引用次数: 0
Correlating Nitrate Adsorption with the Local Environments of FeCoNiCuZn High-Entropy Alloy Catalysts Using Machine Learning 利用机器学习将硝酸盐吸附与铁钴镍铜锌高熵合金催化剂的局部环境联系起来
IF 3.9 2区 化学
Langmuir Pub Date : 2024-07-13 DOI: 10.1021/acs.langmuir.4c01071
Xiang He
{"title":"Correlating Nitrate Adsorption with the Local Environments of FeCoNiCuZn High-Entropy Alloy Catalysts Using Machine Learning","authors":"Xiang He","doi":"10.1021/acs.langmuir.4c01071","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c01071","url":null,"abstract":"The electrocatalytic nitrate reduction to ammonia holds significant values for water remediations and energy applications, which quests for the development of highly effective catalysts with considerable stability and selectivity. Recently, high-entropy alloys (HEAs) are attracting growing attention for electrocatalytic processes. Nonetheless, studies of HEA-based nitrate reduction to ammonia are still at the early stage, and it remains unclear how the HEA compositions affect the adsorption and activation of the reaction intermediates. Herein, high-throughput density functional theory (DFT) calculations were integrated with machine learning to investigate the dependence of nitrate adsorption on the FeCoNiCuZn HEA structures. In particular, a total of 1268 different structures were sampled and constructed from the multidimensional configuration space, followed by the DFT calculations to investigate the Gibbs free energy of nitrate adsorption (i.e., Δ<i>G</i><sub>NO<sub>3</sub></sub>) on different surface microstructures. Four regression models were successfully developed, which can accurately predict Δ<i>G</i><sub>NO<sub>3</sub></sub> using the HEA structures as the input features. Through the analysis of the feature importance, it was found that the active sites are crucial for nitrate adsorption; meanwhile, the local environments also play a considerable role. The dependence of the Δ<i>G</i><sub>NO<sub>3</sub></sub> and adsorption geometries on the HEA compositions demonstrates that the compositional modulation of the HEA catalysts could be a promising avenue for facile adsorption and activation of reaction intermediates. Overall, this work will contribute to the probabilistic optimization of the HEA microstructures for enhanced electrochemical nitrate reduction.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602849","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}
引用次数: 0
How Molecular Orientation Affects the Static Permittivity Profile of the Polar and Nonpolar Liquid–Liquid Interface 分子取向如何影响极性和非极性液-液界面的静态脆度曲线
IF 3.9 2区 化学
Langmuir Pub Date : 2024-07-13 DOI: 10.1021/acs.langmuir.4c01424
Zhu Liu
{"title":"How Molecular Orientation Affects the Static Permittivity Profile of the Polar and Nonpolar Liquid–Liquid Interface","authors":"Zhu Liu","doi":"10.1021/acs.langmuir.4c01424","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c01424","url":null,"abstract":"The dielectric permittivity across the liquid–liquid interface presents an intrinsic response, with respect to the instantaneous interface reference. We hypothesize that dielectric responses across the nonpolar and polar liquid–liquid interfaces have different behaviors and underlying mechanisms. Molecular dynamics simulations were used to compare and contrast the dielectric response of a nonpolar (1,2-dichloroethane/water) and a polar (1-octanol/water) liquid–liquid interface system. We found that the enhanced dielectric permittivity at the nonpolar interface is attributed to the increased water dipole orientation and polarization density. In the case of the polar interface, strong association of the immiscible solvents inhibits the molecular dipole orientation, counteracting the effect from the enhanced surface water polarization density and resulting in a standard dielectric response. Detailed knowledge of the hydrogen bond networks and molecular dipole orientation with respect to the specific instantaneous interfacial and bulk regions reveals the effect of molecular proximity and the interaction with the opposing interfacial molecules on the mechanism of the dielectric permittivity response across the liquid–liquid interface phase boundary.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602851","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}
引用次数: 0
Corrosion Behavior of Al-Containing CoNiV Medium Entropy Alloy Coating Fabricated by Laser Cladding. 激光熔覆法制造的含铝 CoNiV 中熵合金涂层的腐蚀行为
IF 3.7 2区 化学
Langmuir Pub Date : 2024-07-12 DOI: 10.1021/acs.langmuir.4c02006
Minghao Fei, Peng Xu, Ming Zhang, Jianhua Chen, Chuan Yu
{"title":"Corrosion Behavior of Al-Containing CoNiV Medium Entropy Alloy Coating Fabricated by Laser Cladding.","authors":"Minghao Fei, Peng Xu, Ming Zhang, Jianhua Chen, Chuan Yu","doi":"10.1021/acs.langmuir.4c02006","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c02006","url":null,"abstract":"<p><p>CoNiV medium entropy alloys (MEAs) have been widely recognized for their superior corrosion resistance. Nonetheless, their extensive application has been hindered by high production costs and complex fabrication processes. In this study, CoNiVAl<sub><i>x</i></sub> MEA coatings were synthesized on AISI 304 stainless steel substrates via laser cladding technology. The microstructure, phase composition, corrosion resistance, and corrosion mechanisms of the coatings were systematically investigated by using advanced characterization techniques, including optical microscopy, scanning electron microscopy, transmission electron microscopy, X-ray diffractometry, and electrochemical workstation analysis. The ratio of O<sup>2-</sup>/OH<sup>-</sup> in the passivation film of the coated surface exhibited a gradual increase with the addition of Al. The formation of the Al-containing precipitated phase L2<sub>1</sub> was observed at <i>x</i> = 0.3 and 0.4. The results demonstrated that moderate Al doping (<i>x</i> ≤ 0.2) enhanced corrosion resistance by improving the stability of the passivation film and reducing the thermodynamic tendency toward corrosion. In contrast, excessive Al doping (<i>x</i> > 0.2) led to the formation of the L2<sub>1</sub> phase, which increased the susceptibility to localized corrosion, thus compromising the overall corrosion resistance.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141588981","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}
引用次数: 0
Ab Initio Study of the Graphyne-like γ-SiC Nanoflake for Toxic Gas-Sensing Applications. 用于有毒气体传感应用的类石墨烯 γ-SiC 纳米薄片的 Ab Initio 研究。
IF 3.7 2区 化学
Langmuir Pub Date : 2024-07-12 DOI: 10.1021/acs.langmuir.4c02133
Mohammad Tanvir Ahmed, Debashis Roy, Abdullah Al Roman, Shariful Islam, Farid Ahmed
{"title":"Ab Initio Study of the Graphyne-like γ-SiC Nanoflake for Toxic Gas-Sensing Applications.","authors":"Mohammad Tanvir Ahmed, Debashis Roy, Abdullah Al Roman, Shariful Islam, Farid Ahmed","doi":"10.1021/acs.langmuir.4c02133","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c02133","url":null,"abstract":"<p><p>This study focuses on the geometrical, electronic, and optical properties of the γ-graphyne-like novel γ-SiC nanoflake of the γ-silicon carbide (SiC) monolayer using density functional theory calculations. γ-SiC was revealed to be a stable semiconducting nanoflake confirmed by a negative cohesive energy, real vibrational frequencies, and a 1.749 eV energy gap. The adsorption of COCl<sub>2</sub>, HCN, PH<sub>3</sub>, AsH<sub>3</sub>, CNCl, and C<sub>2</sub>N<sub>2</sub> toxic gases on the γ-SiC nanoflake is also studied, which revealed an attractive gas-nanoflake interaction with the adsorption energy ranging from -0.21 to -0.38 eV. The adsorption results in a significant charge transfer between gas-adsorbent complexes. A significant variation in the energy gap and electrical conductivity was observed due to gas adsorption. γ-SiC showed maximum sensitivity at room temperature for CNCl gas. The entire process of adsorption is exothermic and thermodynamically stable. γ-SiC showed a high absorption coefficient over 10<sup>4</sup> orders with a significant variation in the absorption peak intensity and blue peak shifting. According to the quantum theory and reduced density gradient analysis, all of the gases are physisorbed on the γ-SiC nanoflake due to van der Waals interactions. The obtained results signify the usability of γ-SiC as a potential toxic gas sensor.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597940","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}
引用次数: 0
Surface Coating of NCM523 Cathode Electrodes by the Difunctional Block Copolymer/Lithium Salt Composites. 使用双官能团嵌段共聚物/锂盐复合材料对 NCM523 阴极电极进行表面涂层
IF 3.7 2区 化学
Langmuir Pub Date : 2024-07-12 DOI: 10.1021/acs.langmuir.4c00776
Qiaoyun Wu, Zhuijun Xu, Ying Yu, Meilan Peng, Jie Gao, Lei Nie, Ya-Jun Cheng, Peter Müller-Buschbaum, Yonggao Xia
{"title":"Surface Coating of NCM523 Cathode Electrodes by the Difunctional Block Copolymer/Lithium Salt Composites.","authors":"Qiaoyun Wu, Zhuijun Xu, Ying Yu, Meilan Peng, Jie Gao, Lei Nie, Ya-Jun Cheng, Peter Müller-Buschbaum, Yonggao Xia","doi":"10.1021/acs.langmuir.4c00776","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c00776","url":null,"abstract":"<p><p>Nickel-rich layered oxide cathodes, such as LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub> (NCM523), are prevalent in high-power batteries owing to their high energy density. However, these cathodes suffer from undesirable side reactions occurring at the cathode/liquid electrolyte interface, leading to inferior interface stability and poor cycle life. To address these issues, herein, an amphiphilic diblock copolymer poly(dimethylsiloxane)-<i>block</i>-poly(acrylic acid) (PDMS-<i>b</i>-PAA) along with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is utilized for modifying the electrode surface. This modification causes a thin and stable cathode-electrolyte interface (CEI) on the surface of NCM523 particles, as evidenced by XPS, TEM, and EIS analysis. The introduction of this modified interface successfully suppresses the capacity fading of NCM523. After 200 cycles at a rate of 1.0 C, the capacity of the modified NCM523 cathode is 108.7 mAh g<sup>-1</sup>, with a capacity retention of 82.8%, while the control samples without the polymer modification display a capacity retention of 72.7%. These results outline the distinct advantage of electrode surface modification with diblock copolymers/LiTFSI for the stabilization of Ni-rich layered oxide cathodes.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597942","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}
引用次数: 0
High-Efficiency Photothermal Water Evaporation under Low-Intensity Sunlight Using Wood Biochar Monolith. 利用木质生物炭单体在低强度阳光下进行高效光热蒸发水。
IF 3.7 2区 化学
Langmuir Pub Date : 2024-07-12 DOI: 10.1021/acs.langmuir.4c01385
Mina Mahdian, Shujuan Chen, Jianer Zhang, Donald W Kirk, Moein Shayegannia, Nazir P Kherani, Charles Q Jia
{"title":"High-Efficiency Photothermal Water Evaporation under Low-Intensity Sunlight Using Wood Biochar Monolith.","authors":"Mina Mahdian, Shujuan Chen, Jianer Zhang, Donald W Kirk, Moein Shayegannia, Nazir P Kherani, Charles Q Jia","doi":"10.1021/acs.langmuir.4c01385","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c01385","url":null,"abstract":"<p><p>Utilizing energy directly from the sun, solar water evaporation drives the global hydrological cycle and produces freshwater from saline water in the oceans and on land. As water is a poor solar absorber, a photothermal material is needed to facilitate the conversion of photons to thermal energy and increase the efficiency of solar desalination. However, the current photothermal materials are less efficient and expensive to be manufactured. Inspired by nature, we created a new photothermal material called a wood biochar monolith (WBM) by carbonizing wood using the pyrolysis process at 1000 °C and subsequently steaming at high pressure. Under low light intensity (193 W/m<sup>2</sup>), the light to vapor efficiency of maple WBM is more than 100%. The outstanding performance of WBM is attributed to (1) the facilitated water transport in the hierarchical, open-pore network preserved from the wood precursor in WBM and (2) the reduced evaporation enthalpy of confined water in WBM and the high broadband sunlight absorptivity of WBM. Moreover, the high evaporation rate causes the temperature of WBM to be lower than that of the surrounding water, enabling thermal energy harvesting by WBM from water and making a light-to-vapor efficiency of >100% feasible. This discovery offers opportunities for developing low-cost, high-performance water desalination or humidification devices deployable in remote areas with nonconcentrated natural sunlight.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141588986","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}
引用次数: 0
Surface Hydroxylation-Induced Electrostatic Forces Thicken Water Films on Quartz. 表面羟基化诱导的静电力加厚了石英上的水膜。
IF 3.7 2区 化学
Langmuir Pub Date : 2024-07-12 DOI: 10.1021/acs.langmuir.4c01461
Abdullah Cihan, Piotr Zarzycki, Zhao Hao
{"title":"Surface Hydroxylation-Induced Electrostatic Forces Thicken Water Films on Quartz.","authors":"Abdullah Cihan, Piotr Zarzycki, Zhao Hao","doi":"10.1021/acs.langmuir.4c01461","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c01461","url":null,"abstract":"<p><p>Aqueous films on mineral surfaces control the physical, chemical, and biological transport processes in the atmosphere, soil, and rocks. Despite the importance of thin films for various research and engineering fields, there are still unanswered questions regarding the roles of the different forces affecting the nature of water films. One of these, the focus of this study, is the development of abnormally thick water films on quartz surfaces. In this study, we developed a density-functional-theory-based model to describe the time-dependent evolution of water films and identify the governing forces responsible for thickening films. We simulated the diffusion of water vapor from ambient air toward mineral surfaces and the formation and thickening of water films at various relative humidity values. Our model predicts an abnormal water film thickness on a hydroxylated quartz surface compared to a surface free of hydroxylation, which explains experimental observations. We further used the model to understand the key interaction forces at different stages of water film formation and thickening. Our model suggests that the attractive hydrogen bonding and van der Waals forces initiate a seed layer of water, and the electrostatic forces, generated by the hydroxylated and thus charged surface, lead to the thickening of water films. This generalizable model can provide insights into the peculiarities of water film development on various mineral surfaces.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597943","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}
引用次数: 0
Polypeptoid Monomer Sequence and Chemical Composition as Independent Controls of Interfacial Tension and Elasticity at Air/Fluid Interfaces. 多肽类单体序列和化学组成是空气/流体界面张力和弹性的独立控制因素。
IF 3.7 2区 化学
Langmuir Pub Date : 2024-07-12 DOI: 10.1021/acs.langmuir.4c02195
Michal Roguski, Michael L Davidson, Audra J DeStefano, Rachel A Segalman, Lynn M Walker
{"title":"Polypeptoid Monomer Sequence and Chemical Composition as Independent Controls of Interfacial Tension and Elasticity at Air/Fluid Interfaces.","authors":"Michal Roguski, Michael L Davidson, Audra J DeStefano, Rachel A Segalman, Lynn M Walker","doi":"10.1021/acs.langmuir.4c02195","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c02195","url":null,"abstract":"<p><p>We use sequence-specific polypeptoids to characterize the impact of the monomer sequence on the adsorption of surface-active polymers at fluid/fluid interfaces. Sets of 36 repeat unit polypeptoids with identical chemical composition, but different sequences of hydrophobic moieties along the oligomer chain (taper, inverse taper, blocky, and evenly distributed), are designed and characterized at air/water interfaces. Polypeptoids are driven to the interfaces by decreasing the solvent quality of the aqueous solution. In situ processing of the adsorbed layers causes a collapse of polypeptoids and the formation of irreversibly adsorbed, solvent-avoiding layers at interfaces. Differences in thermodynamic properties, driven by solubility, between the collapsed structures at interfaces are studied with measurements of interfacial tension. The dilatational modulus of polypeptoid-coated interfaces is used as a proxy to probe the extent of the coil-globule collapse at the interface. The role of hydrophobicity is investigated by comparing four sequences of polypeptoids with an increased size of the hydrophilic side chains. In each set of polypeptoids, the composition of molecules, not the sequence, controls the surface concentration. The molecules are described in terms of the distribution of the hydrophobic monomers on the backbone of the polymer. Inverse taper (IT) and blocky (B) sequences of hydrophobic moieties favor the formation of highly elastic interfaces after processing, while taper (T) and distributed (D) showed lower elasticity after processing, which is achieved by replacing good solvent with poor solvent and then nonsolvent. These structures allow for the study of the impact of the chemical composition and sequence of monomers on the properties of polymer-coated interfaces.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141589002","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}
引用次数: 0
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