Langmuir最新文献_第5页

Time-Resolved Electrochemical Kinetics and Pseudocapacitive Charge Storage in Fe-MOF@CoSn-Based Asymmetric Hybrid Supercapacitors. Fe-MOF@CoSn-Based非对称混合超级电容器的时间分辨电化学动力学和假电容电荷存储。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-26 DOI: 10.1021/acs.langmuir.5c02269

Karthick Raja K,Mani Govindasamy,Vivek Kumar

{"title":"Time-Resolved Electrochemical Kinetics and Pseudocapacitive Charge Storage in Fe-MOF@CoSn-Based Asymmetric Hybrid Supercapacitors.","authors":"Karthick Raja K,Mani Govindasamy,Vivek Kumar","doi":"10.1021/acs.langmuir.5c02269","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02269","url":null,"abstract":"Metal-organic frameworks (MOFs) have attracted significant interest as electrode materials for energy storage systems owing to their tunable structures, large surface areas, and adjustable physicochemical properties. In this study, MIL-100(Fe) was successfully grown on CoSn(OH)6 (MOF@CTH), and its electrochemical performance was systematically evaluated for asymmetric hybrid supercapacitors (AHS). The charge storage mechanism was elucidated through Dunn analysis, revealing a significant increase in the distinct capacitive contributions for MOF@CTH2. Additionally, the distribution of relaxation times analysis provided detailed insight into electrochemical kinetics, highlighting a capacitive Faradaic and noncapacitive Faradaic charge transfer process occurring within the relaxation timescale of 0.1-1 s for MOF@CTH2. The MOF@CTH2 electrode attained an outstanding specific capacitance of 1124.6 F/g, corresponding to a specific charge of 562.3 C/g. The hybrid two-electrode system constructed with MOF@CTH2 and reduced graphene oxide as the positive and negative electrode, respectively, delivered an energy density of 36.21 Wh/kg and a power density of 749.98 W/kg. This work advances our understanding of time-resolved electrochemical processes in MOF-based systems and highlights their potential in high-performance AHS applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"63 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140489","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

Strain-Driven Switching of Easy Magnetization Axis in a Ferromagnetic Semiconductor LaBr2 Monolayer. 铁磁半导体LaBr2单层中易磁化轴的应变驱动开关。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-26 DOI: 10.1021/acs.langmuir.5c02790

Jiawen Zhang,Jiaqi Li,Yaxin Pan,He Sun,Chaoran Niu,Shan Wang,Minglei Jia,Fengzhu Ren,Bing Wang

{"title":"Strain-Driven Switching of Easy Magnetization Axis in a Ferromagnetic Semiconductor LaBr2 Monolayer.","authors":"Jiawen Zhang,Jiaqi Li,Yaxin Pan,He Sun,Chaoran Niu,Shan Wang,Minglei Jia,Fengzhu Ren,Bing Wang","doi":"10.1021/acs.langmuir.5c02790","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02790","url":null,"abstract":"The precise manipulation of magnetic anisotropy in spintronic systems exhibits revolutionary potential for next-generation technologies. However, achieving deterministic control at the atomic scale faces critical bottlenecks due to the intricate interplay among spin-orbit coupling, interfacial symmetry breaking, and thermal fluctuations. Here, based on first-principles calculations, we demonstrate effective the control of the easy magnetization axis for the LaBr2 monolayer by using strain engineering. The result shows that the biaxial compressive strain induces a fundamental transition of the easy magnetization axis from in-plane (xy plane) to out-of-plane (z axis). This change in easy magnetization axis stems from the strain-modulated orbital coupling between occupied and unoccupied dxy/dx2-y2 orbital states in La atom, which alters the energy splitting between competing magnetic anisotropy configurations. Our findings establish a viable pathway for engineering magnetic anisotropy in two-dimensional systems through lattice deformation, enabling potential applications in strain-controlled spintronic devices.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"41 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140482","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

Spontaneous Depletion of Valinomycin-Mediated Ion Current in Droplet Interface Bilayers. valinomycin介导的离子电流在液滴界面双层中的自发耗竭。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-26 DOI: 10.1021/acs.langmuir.5c03024

Essraa A Hussein,Stephen A Sarles

{"title":"Spontaneous Depletion of Valinomycin-Mediated Ion Current in Droplet Interface Bilayers.","authors":"Essraa A Hussein,Stephen A Sarles","doi":"10.1021/acs.langmuir.5c03024","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c03024","url":null,"abstract":"Valinomycin (Val) is a selective ion carrier widely used to develop potassium-selective membranes and study carrier-mediated transport across lipid bilayers. Using either black lipid membranes (BLMs) or supported lipid bilayers (SLBs), previous studies explored valinomycin's selectivity and transport mechanism and quantified the amount of potassium ion current per carrier molecule. Herein, we demonstrate that Val-doped membranes exhibit distinct kinetic behavior when incorporated into droplet interface bilayers (DIBs), a platform known for forming highly resistive membranes ideal for studying ion transport and gating phenomena. Specifically, when Val is reconstituted into DIBs to form potassium-selective membranes, we observe a significant decrease in the voltage-driven ion current over time. We investigate this behavior and quantify the effects of applied voltage, Val placement, and oil type on the resulting ionic current response, explain the underlying causes, and propose a strategy to mitigate the current decay challenge. Using a combination of electrophysiology and UV absorbance measurements, our findings reveal that the valinomycin-mediated ion current is diminished due to the loss of Val from the interior of both the lipid membrane and aqueous droplet via its passive diffusion and partitioning into the surrounding oil phase. Increasing the ionophore concentration, applying a DC voltage, and choosing an oil that is readily retained in the bilayer membrane all quicken the onset and increase the rate of Val depletion. Nonetheless, allowing lipid-coated droplets to incubate for extended periods of time in an oil containing Val leads to a Val-doped DIB with a significantly more stable ionic conductance. More broadly, these behaviors demonstrate a challenge to and a possible solution for using DIBs to study hydrophobic membrane-active species.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"89 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140476","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

Inert Center Immobilization of Bromopyrogallol Red on Diazo-Enriched Silica Gel Support via Multipoint Mode: Attune pH Extractor for Sequential Separation of Nd(III), Th(IV), Ce(IV), and Zr(IV) from Aqueous Admixtures. 溴吡咯三酚红在重氮富集硅胶载体上的多点模式惰性中心固定化：调pH萃取器用于从水溶液中连续分离Nd(III), Th(IV), Ce（IV）和Zr（IV）。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-26 DOI: 10.1021/acs.langmuir.5c01934

Tirtha Biswas,Basudev Das,Ankit Ghosh,Tanay K Mondal,Biswajit Hansda,Sambit Bandyopadhyay,Ancy Basumatary,Ilawanbet Tangsong,Bhabatosh Mandal

{"title":"Inert Center Immobilization of Bromopyrogallol Red on Diazo-Enriched Silica Gel Support via Multipoint Mode: Attune pH Extractor for Sequential Separation of Nd(III), Th(IV), Ce(IV), and Zr(IV) from Aqueous Admixtures.","authors":"Tirtha Biswas,Basudev Das,Ankit Ghosh,Tanay K Mondal,Biswajit Hansda,Sambit Bandyopadhyay,Ancy Basumatary,Ilawanbet Tangsong,Bhabatosh Mandal","doi":"10.1021/acs.langmuir.5c01934","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c01934","url":null,"abstract":"In surface functionalization, picric acid was coupled with SG using dimethyldichlorosilane, an efficient silane coupling reagent, resulting in a highly enriched nitro compound. Subsequently, we developed the diazo compound of a densely populated diazo surface to diazo-couple the Bromopyrogallol Red (BPR) using BPR's inert center via multipoint mode: {Si(OSi)4(H2O)x}n{OSi(CH3)2-O-C6H2(N═N+)3(C19H10Br2O8S)1.5}4.yH2O. The parameters x, n, and y have been precisely determined as 0.5, 45, and 20, respectively. The synthesized material is an attune pH extractor comprising appreciable BPR content (40 μmol g-1); BPR's phenolic -OH is involved in extracting Nd(III) as a dimer, while Ce(IV), Th(IV), and Zr(IV) are used as a monomer to attain the respective BTC values of 156, 79, 84, and 88 μmol.g-1. The extractor enhances the solution concentration with enrichment factors 49, 44, 46, and 53 for the respective metal ions Nd(III), Ce(IV), Th(IV), and Zr(IV), respectively, and sequentially separates them from aqueous admixtures. The synthesized material was durable for up to 18 months and may be recycled 200 times without losing extraction capacity.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"19 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140480","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

Effects of Chemical Components and Structure on the Pore Properties of Lignite Treated by Acidification and Tetrahydrofuran. 化学成分和结构对酸化和四氢呋喃处理褐煤孔隙性质的影响。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-26 DOI: 10.1021/acs.langmuir.5c04112

Chunshan Zheng,Jinting Li,Shuaili Liu,Bingyou Jiang,Feilin Han,Mingyun Tang

{"title":"Effects of Chemical Components and Structure on the Pore Properties of Lignite Treated by Acidification and Tetrahydrofuran.","authors":"Chunshan Zheng,Jinting Li,Shuaili Liu,Bingyou Jiang,Feilin Han,Mingyun Tang","doi":"10.1021/acs.langmuir.5c04112","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c04112","url":null,"abstract":"Acid-tetrahydrofuran (THF) treatment could change the soluble components and chemical structure of coal, enhancing the gas extraction performance. Gas chromatography-mass spectrometry (GC-MS) was adopted to analyze the changes in the soluble organic matter in lignite after acid-THF treatment. Based on Fourier transform infrared (FTIR) testing, parameter variations including degrees of hydrogen enrichment (I1), oxygen enrichment (I2), aromatization (I3), and aromatic condensation (I4) of coal were quantitatively analyzed. Meanwhile, the pore structure changes were analyzed through the N2-BET experiment and FHH fractal model. The effects of lignite chemical components and structure on the pore structure were discussed. With the combined acid-THF treatment, lignite extracts are dominated by aliphatic and aromatic compounds, promoting the transformation of micropores and mesopores into macropores. The values of I1, I2, I3, and I4 of the acidified coal are smaller than those of the original coal samples. I1, I2, and I4 further decrease with an increased THF concentration. After the combined treatment, the maximum gas adsorption amount of coal decreases from 14.1439 cm3/g to 9.6635 cm3/g and 6.5026 cm3/g. Acid-THF treatment could lead to a decrease in I1, with a subsequent reduction in the specific surface area (SSA) and pore volume (PV) and an increase in the average pore size (APS). Moreover, significant solubilization of oxygen-containing functional groups results in a decrease in SSA and PV and an increase in APS with decreasing I2. Relationships between I4 and pore structure parameters are similar to those of I1 and I2, reflecting a decrease in aromatic condensation that increases the pore size.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"15 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140483","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

Ice-Template-Assisted Anisotropic Aerogel Monoliths: An Assembly Strategy of Aramid Nanofibers. 冰模板辅助各向异性气凝胶单体：芳纶纳米纤维的组装策略。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-26 DOI: 10.1021/acs.langmuir.5c03624

Chao Qiang,Minming Zou,Wenxing Luo,Jue Wang,Guangyu Zhu,Yifan Huang,Sifan Tan,Jinghui Fan,Baowen Fu,Peng Luo,Yan Ma,Wenjing Chen,Xiongxin Jiang,Qinglin Li,Xiaowu Hu

{"title":"Ice-Template-Assisted Anisotropic Aerogel Monoliths: An Assembly Strategy of Aramid Nanofibers.","authors":"Chao Qiang,Minming Zou,Wenxing Luo,Jue Wang,Guangyu Zhu,Yifan Huang,Sifan Tan,Jinghui Fan,Baowen Fu,Peng Luo,Yan Ma,Wenjing Chen,Xiongxin Jiang,Qinglin Li,Xiaowu Hu","doi":"10.1021/acs.langmuir.5c03624","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c03624","url":null,"abstract":"The manipulation of aramid nanofibers (ANFs) into macroscopic monolithic aerogels with ordered microstructures is critical for enabling their extensive and large-scale practical implementations. This study introduces a top-down strategy utilizing ice templates to prepare aramid aerogel monomers. The process involves dissolving Kevlar fibers in dimethyl sulfoxide (DMSO) under alkaline conditions to produce aramid nanofibers (ANF). Subsequently, the self-assembly of ANF was effectively tailored by using ice templating (referred to as O-ANF) and the nondirectional freezing technique (designated as D-ANF), respectively. The O-ANF aerogel exhibits a distinctive long-range ordered sheet structure with a honeycomb surface pattern, attributed to the low melting point of DMSO (18.4 °C). Axial thermal conductivity of the O-ANF aerogel was 93.5% better compared to the D-ANF aerogel, while its tensile strength in this direction was approximately 5.2 times greater. Molecular dynamics (MD) simulations were utilized to elucidate the mechanisms underlying the enhanced mechanical and thermal properties. Moreover, the O-ANF demonstrated superhydrophilicity, whereas the D-ANF exhibited a contact angle of 67.52°. As an organic aerogel, ANF possesses typical characteristics of low density and high porosity. Additionally, ANF exhibits superior insulation performance from -196 to 200 °C and flame retardancy. Given its exceptional properties and straightforward preparation method, ANF aerogels hold significant potential for applications in aerospace and fire protection.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"52 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140478","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

Supramolecular Polymorphism of an Amphiphilic Boron-Dipyrromethene Dye Mediated by Carbonyl-Aromatic Interactions. 羰基-芳香族相互作用介导的两亲性硼-二吡咯甲烷染料的超分子多态性。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-25 DOI: 10.1021/acs.langmuir.5c03797

Dewang Niu,Baicheng Liu,Zhenhu Zhang,Xiaohan Chu,Yuhuan Yang,Jinglin Shen,Wei Qi,Yongjie Zhang

{"title":"Supramolecular Polymorphism of an Amphiphilic Boron-Dipyrromethene Dye Mediated by Carbonyl-Aromatic Interactions.","authors":"Dewang Niu,Baicheng Liu,Zhenhu Zhang,Xiaohan Chu,Yuhuan Yang,Jinglin Shen,Wei Qi,Yongjie Zhang","doi":"10.1021/acs.langmuir.5c03797","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c03797","url":null,"abstract":"Supramolecular polymorphism is attracting great interest due to its potential for generating versatile functional materials based on the same molecule. Despite the great efforts devoted to manipulating polymorphic aggregation systems, accessible design strategies for such systems are still limited. Herein, we describe the supramolecular polymorphism of an amphiphilic boron-dipyrromethene dye (BODIPY 1) through sophisticated manipulation of noncovalent interactions. In mixed solvents of DMF/H2O, it self-assembles into two different aggregates with distinct structures and optical properties, i.e., kinetically controlled spherical micelles with bathochromically shifted spectra (J-agg) and thermodynamically controlled nanofibers with hypsochromically shifted spectra (H-agg). Notably, these aggregates of BODIPY 1 retain strong fluorescence. Systematic experimental and theoretical studies demonstrate that J-agg is driven simply by hydrophobic interactions, while the formation of H-agg is mediated by a carbonyl-aromatic interaction. The important role of the carbonyl-aromatic interaction in modulating supramolecular polymorphism is demonstrated by various structural characterizations and theoretical calculations. The transformation from J-agg to H-agg can be accelerated by modifying the terminal benzaldehyde group or eliminated by removing the aldehyde C═O. This work can inspire a new strategy for constructing supramolecular polymorphism systems with the desired optical properties.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"89 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140150","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

Glucose-Responsive Superlubricity of a Self-Healing Hydrogel Containing Dynamic Boronic Ester Bonds under Ocular Conditions. 含动态硼酯键的自愈水凝胶在眼部条件下葡萄糖反应性超润滑性的研究。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-25 DOI: 10.1021/acs.langmuir.5c02962

Hongdong Wang,Yuxuan He,Qi Wang,Xiacong Zhang,Yuhong Liu,Jianhua Zhang

{"title":"Glucose-Responsive Superlubricity of a Self-Healing Hydrogel Containing Dynamic Boronic Ester Bonds under Ocular Conditions.","authors":"Hongdong Wang,Yuxuan He,Qi Wang,Xiacong Zhang,Yuhong Liu,Jianhua Zhang","doi":"10.1021/acs.langmuir.5c02962","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c02962","url":null,"abstract":"Dry eye disease (DED) is a widespread ocular disorder that poses a growing threat to global eye health and creates a requirement for stable ocular lubrication. In this study, a strategy for achieving ocular superlubricity is proposed based on the reaction between a P-C2PEGOH hydrogel and glucose in artificial tears. The dynamic boronic ester bonds in the P-C2PEGOH hydrogel undergo a reversible competitive exchange reaction with glucose, leading to the dissociation of original cross-linking points and the release of hydrophilic polyethylene glycol (PEG)-based substrates. Both results of the reaction endow the hydrogel with glucose-responsive superlubricity. Friction tests show that the release of PEG-based substrates reduces the coefficient of friction (COF) of artificial tears from 0.0078 to 0.0037. PEG-based substrates form hydration layers that reduce shear stress of the interface through the hydration lubricating effect. Through varying the glucose concentration, the level of PEG-based substrates in the tears and the hydration capacity on the hydrogel surface can be modulated, thereby enabling glucose-responsive superlubricity. Furthermore, the presence of dynamic boronic esters containing boron-nitrogen coordination bonds endows the hydrogel with a self-healing capability, enabling it to recover its structural integrity after mechanical disruption. Moreover, cytotoxicity assays and in vivo biocompatibility evaluations confirm the biocompatibility of the hydrogel, highlighting its potential for ophthalmic applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"27 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140130","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

Fine-Tuning of Gate Opening in Hybrid Zeolitic Imidazolate Framework-8: Inelastic Neutron Scattering and Density Functional Theory Study. 杂化沸石咪唑盐框架栅开度的微调-8：非弹性中子散射和密度泛函理论研究。

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-25 DOI: 10.1021/acs.langmuir.5c03280

Jaideep Mor,Sandeep K Sharma,Jitendra Bahadur,Srinivasu Kancharlapalli,Jeff Armstrong

{"title":"Fine-Tuning of Gate Opening in Hybrid Zeolitic Imidazolate Framework-8: Inelastic Neutron Scattering and Density Functional Theory Study.","authors":"Jaideep Mor,Sandeep K Sharma,Jitendra Bahadur,Srinivasu Kancharlapalli,Jeff Armstrong","doi":"10.1021/acs.langmuir.5c03280","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c03280","url":null,"abstract":"The gate opening phenomenon observed in zeolitic imidazolate framework-8 (ZIF-8) under gas pressure is attributed to rotation of the 2-methylimidazole (mIm) linker. Gate opening in ZIF-8 has detrimental effects on molecular gas separation selectivity; hence, fine-tuning of the gate opening of ZIF-8 is being explored through controlled linker and metal exchange maintaining the topology. Herein, we present a systematic investigation using in situ inelastic neutron scattering (INS) corroborated with density functional theory (DFT) of fine-tuning of gate opening in hybrid ZIF-8 under N2 pressure. For this study, hybrid ZIF-8 samples, (Co/Zn)ZIF-8 having Co (∼25 mol %) and ZIF-7-8 having benzimidazole, bIm (∼17 mol %), were compared with ZIF-8. Using INS, we confirmed that mIm linker rotation that is responsible for the gate opening in ZIF-8 is significantly hindered by Co or bIm substitutions. INS and DFT results pinpoint the origin of this hindered linker swinging motion to stronger metal-linker bonding and the modified structural configuration of the linker position. This combined experimental and theoretical approach has provided clear evidence of the existence of two control mechanisms for molecular separation and importantly provides a molecular scale explanation. This is a design principle that could be employed in the development of pressure-sensitive separation techniques.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"93 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140128","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

Preparation and Properties of High-Loading Solvent-Free Dry Electrodes in LiFePO4 Lithium-Ion Batteries. LiFePO4锂离子电池高负载无溶剂干电极的制备及性能研究

IF 3.9 2区化学

Langmuir Pub Date : 2025-09-25 DOI: 10.1021/acs.langmuir.5c03698

Hang Xie,Xuemeng Liu,Yunlong Cui,Qinghua Huang,Na Zhang,Longjun Xue,Dawei Song,Hongzhou Zhang,Kai Liu,Xixi Shi,Lianqi Zhang

{"title":"Preparation and Properties of High-Loading Solvent-Free Dry Electrodes in LiFePO4 Lithium-Ion Batteries.","authors":"Hang Xie,Xuemeng Liu,Yunlong Cui,Qinghua Huang,Na Zhang,Longjun Xue,Dawei Song,Hongzhou Zhang,Kai Liu,Xixi Shi,Lianqi Zhang","doi":"10.1021/acs.langmuir.5c03698","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c03698","url":null,"abstract":"In this paper, solvent-free, high-loading graphite (Gr) electrodes (single-sided electrode areal density of 26.8 mg cm-2) and high-loading LiFePO4 (LFP) electrodes (single-sided electrode areal density of 53.8 mg cm-2) are prepared by a dry processing method of powder dry mixing and calendering, whose microstructural homogeneity is optimized to enhance lithium-ion transport in pore channels, thus showing lower tortuosity. Dry electrodes exhibit a cycle stability and rate performance similar to those of low-loading Wet electrodes in half cells. In addition, the Dry LFP electrode exhibits lower polarization and a high Li-ion diffusion coefficient (DLi+), and the Dry LFP electrode (areal capacity: 8.4 mAh cm-2) and Dry Gr electrode (areal capacity: 9.0 mAh cm-2) have good cycling stability in coin and single-layer pouch full cells. The capacity retentions are 68.37 and 75.82% after 200 cycles at 0.2C and after 60 cycles at 0.5C, respectively. This work emphasizes the great potential of the innovative solvent-free dry processing method as a production route for advanced high-capacity LFP lithium-ion batteries due to the advantages of its high-loading ability, good environment, and cost savings.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"37 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140132","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