{"title":"Host–Guest-Driven Sandwich-Like Cyclodextrin Membrane for Instantaneous Diuretics Adsorption in Wastewater","authors":"Lei Zhang, , , Junyi Zhang, , , Tian Tian*, , , Meifang Yang, , , Yu-Xin Chen, , , Qin Xu, , , Peipei Li, , , Ju Wu, , , Wenjing Zhang*, , and , Huan Pang*, ","doi":"10.1021/acsmaterialslett.5c00997","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00997","url":null,"abstract":"<p >The widespread presence of diuretics in wastewater, driven by their growing use in managing hypertension, heart failure, and kidney disorders as well as their chemical stability and bioactivity, poses significant environmental risks. To address these limitations, we developed a host–guest interaction-driven sandwich-like nanocomposite membrane with alternating porous and fibrous layers for rapid diuretic removal. The HPβCD composite membrane (HPβCD CM) demonstrated stable adsorption performance under acid and alkaline conditions. Within 60 s, the HPβCD CM achieved >70% removal of hydrochlorothiazide, exhibiting an adsorption rate constant 2–3 times higher than those of GAC and single-component β-cyclodextrin polymers. The maximum adsorption capacities of the membrane reached 300 mg/g for HCTZ and 200 mg/g for bendroflumethiazide and indapamide. With its outstanding adsorption performance, cost-effectiveness, and ease of regeneration, the HPβCD CM represents a promising solution for advanced water treatment applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3504–3511"},"PeriodicalIF":8.7,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226836","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Eui-Cheol Shin*, , , Rokyeon Kim, , , Sang-Hoon Lee, , and , Hyeon-Deuk Kim*,
{"title":"Hidden Hypernetwork and Homology in Vitrification of Ionic Oxides","authors":"Eui-Cheol Shin*, , , Rokyeon Kim, , , Sang-Hoon Lee, , and , Hyeon-Deuk Kim*, ","doi":"10.1021/acsmaterialslett.5c00848","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00848","url":null,"abstract":"<p >Disorder in complex systems suppresses long-range order, yet correlated motifs can persist at medium-range order (MRO). In dense ionic networks, these patterns often evade conventional diffraction techniques. Here, we elucidate the hidden hypernetwork consisting of MRO and its role in the vitrification of In–Ga–Zn–O─a prototypical ionic oxide─using persistent homology. In the crystal, hypernetworks form two homological classes─<i>D</i><sup>2</sup> (disk) and <i>S</i><sup>1</sup> (loop)─depending on edge-sharing motifs. <i>D</i><sup>2</sup> connectivity recovers after vitrification and governs electronic properties. The diversity of MRO in the amorphous phase converges to ∼10<sup>3</sup> atoms, effectively representing the thermodynamic limit. The topological sensitivity based on the stability theorem indicates that Ga plays a key role in MRO reorganization during densification, accompanied by an increasing mobility gap. Our results demonstrate that glassy ionic oxide behavior is driven not by simple disorder but by a reorganized hypernetwork.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3497–3503"},"PeriodicalIF":8.7,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226834","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Review on Research Progress on Bio-Based Self-Healing Polyurethane","authors":"Hongyu Feng, , , Yuli Wang, , , Ting Zhang, , , Jiangbo Wang, , , Zhixin Jia*, , , Shaohua Jiang*, , and , Xiaoshuai Han*, ","doi":"10.1021/acsmaterialslett.5c01153","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01153","url":null,"abstract":"<p >Self-healing polyurethane (SHPU) shows great potential in enhancing materials’ durability and sustainability, yet balancing robust mechanical properties with efficient self-healing under mild conditions remains challenging. Conventional approaches often sacrifice strength or healing ability. This Review focuses on the key role of biomass-derived materials, including lignin, cellulose, chitosan, and vegetable oils, in resolving this conflict. Acting as dynamic network modifiers, multifunctional enhancers, and microstructural regulators, they enable sacrificial bonding, microphase separation, and improved chain mobility. Biomass-based SHPUs can achieve over 90% self-healing efficiency at room temperature while maintaining strength and toughness and even incorporate additional functions like flame retardancy or conductivity. Moreover, biomass enhances sustainability by reducing fossil resource dependence and promoting recyclability. Despite challenges in performance consistency and raw material variability, molecular engineering offers a promising path toward high-performance, sustainable SHPUs for advanced manufacturing and a circular economy.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3461–3488"},"PeriodicalIF":8.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226826","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Gas-Blowing Medicated Aggregation toward 19% Efficiency in Printed Organic Solar Cell from Nonhalogenated Solvent","authors":"Shang Wen, , , Weiyi Xia, , , Zirui Gan, , , Jingchao Cheng, , , Yuandong Sun, , , Yujie Yang, , , Yunxia Mao, , , Hanyang Chen, , , Dan Liu, , , Wei Li*, , and , Tao Wang*, ","doi":"10.1021/acsmaterialslett.5c01065","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01065","url":null,"abstract":"<p >Doctor-blading is a promising alternative for the large-area printing of organic solar cells (OSCs). However, the power conversion efficiencies (PCEs) of doctor-bladed OSCs are still lower than those of their spin-cast counterparts. This is mainly caused by the prolonged molecular organization time during which excessive aggregation can be encouraged. In this work, a post-treatment using nitrogen gas to blow the backside of the photoactive layer, i.e., the ITO glass side, was utilized to modulate the aggregation growth after blade-coating from a nonhalogenated solvent. A range of morphological measurements reveal that gas-blowing suppresses excessive aggregation of nonfullerene acceptors. As a result, gas-blowing treated PM6:BTP-eC9 OSCs obtained a maximum PCE of 19.0%, which is among the highest values of blade-coated OSCs. Moreover, this morphology transformation also drives the photoactive layer toward the thermodynamic equilibrium state, reducing free volume in the photoactive layer and contributing to better device stabilities.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3489–3496"},"PeriodicalIF":8.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226833","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Gel-Confined Crystallization Unlocks Defect-Minimized Prussian Blue Cathode for High-Performance Sodium-Ion Batteries","authors":"Yonglin Lu, , , Yuheng Chen, , , Wanyi Yuan, , , Jingyi Chen, , , Xin Cao*, , , Yuwei Zhang*, , , Yawen Tang, , and , Ping Wu*, ","doi":"10.1021/acsmaterialslett.5c01093","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01093","url":null,"abstract":"<p >Metal hexacyanoferrates (MHCFs) have emerged as promising cathodes for sodium-ion batteries. However, conventional wet-chemistry-derived MHCFs inevitably contain substantial Fe(CN)<sub>6</sub> vacancies and crystal water, resulting in an undesirable Na-storage performance. Herein, a gel-confined crystallization strategy is developed to prepare highly crystalline MHCFs. In a typical polypyrrole (PPy) gel, the cross-linked network effectively restricts the movement of internal ions through steric hindrance and attractive/repulsive interactions, leading to slow crystal growth and formation of highly crystalline MHCFs. Specifically, iron hexacyanoferrate (FeHCF), with only 1% Fe(CN)<sub>6</sub> vacancy and 2.0 wt% crystal water, has been formed <i>in situ</i> within a PPy gel via this gel-confined crystallization process. The highly crystalline FeHCF coupled with an interconnected PPy framework enables the hybrid cathode to exhibit enhanced activity of low-spin Fe sites, long cycling life, and good rate capability.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3452–3460"},"PeriodicalIF":8.7,"publicationDate":"2025-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Benjamin G. Meyer, , , Guillaume Matthews*, , , Robin Scales, , , Nicole C. Mitchell, , , Ed Darnbrough, , , Robert A. House, , , David E. J. Armstrong, , and , Patrick S. Grant,
{"title":"Deformation and Tensile Properties of Free-Standing Solvent-Free Electrodes for Li-Ion Batteries","authors":"Benjamin G. Meyer, , , Guillaume Matthews*, , , Robin Scales, , , Nicole C. Mitchell, , , Ed Darnbrough, , , Robert A. House, , , David E. J. Armstrong, , and , Patrick S. Grant, ","doi":"10.1021/acsmaterialslett.5c00947","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00947","url":null,"abstract":"<p >Solvent-free (dry-processed) electrodes offer substantial economic and environmental benefits to Li-ion batteries and are manufactured in a way that requires them to withstand tensile loads during roll-to-roll processing. Electrode sheets comprising graphite particles embedded within a polytetrafluoroethylene (PTFE) polymer fibril network were investigated under tension and exhibited viscoelastic behavior: linear loading, plastic deformation, and sheet failure. The degree of PTFE fibrillation during manufacture impacted final sheet properties, and calendering induced fibril alignment and crystallographic texture and macroscopic mechanical anisotropy. Increasing the PTFE fraction by 3.5 wt % led to remarkable improvements in ultimate tensile strength (+900%) and failure strain (+30%). Increasing electrode temperature (>19 °C) delayed sheet failure as PTFE transformed from a triclinic to hexagonal phase, however, higher temperatures (>80 °C) accelerated failure by fibril elongation, pull-out and widespread fibril fracture.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3444–3451"},"PeriodicalIF":8.7,"publicationDate":"2025-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00947","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226822","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Multifunctional Integration of Vanadium-Based Chalcogenides VX (X = S, Se, Te)","authors":"Junlin Luo, , , Haiyu Meng, , , Ruoyan Xu, , , Xingxing Jiang, , , Yu-Qing Zhao, , , Yee Sin Ang*, , and , Xiong-Xiong Xue*, ","doi":"10.1021/acsmaterialslett.5c00908","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00908","url":null,"abstract":"<p >Two-dimensional (2D) ferromagnetic materials integrating multiple functions are promising candidates for building magnetic and electronic nanodevices. Here, we predict a series of stable 2D multifunctional ferromagnetic monolayers VX (X = S, Se, Te) encompassing indirect semiconducting and half-metallic phases with sizable spin gaps. Due to the strong ferromagnetic coupling present in the VX monolayers, the magnetic transition temperatures (<i>Tc</i>) of VS, VSe, and VTe reach 369, 315, and 311 K, respectively. Furthermore, the magnetic and electronic properties of VX monolayers can be sensitively modulated via mechanical strain, while the VS and VSe monolayers further exhibit negative Poisson’s ratios. The VX monolayers thus represent an unusual family of 2D ferromagnetic materials with strong mechano-electromagnetic coupling that may serve as a building block for future multifunctional nanodevices.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3435–3443"},"PeriodicalIF":8.7,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226802","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Madhusudan Chaudhary, , , Muskaan Rawat, , , Elisabeth Springl, , , Daniel Weindl, , , Diganta Sarkar, , , Aiden Yu, , , Dmitry Vrublevskiy, , , Tom Nilges, , , Arthur Mar, , and , Vladimir K. Michaelis*,
{"title":"Entropy-Driven Disorder and Aliovalent Substitution Induce Defects in Na3PnS4 (Pn = P, As, Sb) Solid-State Electrolytes: A Sluice Gate for Sodium Ions","authors":"Madhusudan Chaudhary, , , Muskaan Rawat, , , Elisabeth Springl, , , Daniel Weindl, , , Diganta Sarkar, , , Aiden Yu, , , Dmitry Vrublevskiy, , , Tom Nilges, , , Arthur Mar, , and , Vladimir K. Michaelis*, ","doi":"10.1021/acsmaterialslett.5c00630","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00630","url":null,"abstract":"<p >Sodium-containing chalcogenides are attractive candidates for use as solid-state electrolytes; however, their ionic conductivities remain a challenge. Simultaneously applying isovalent and aliovalent substitution can enhance ionic conductivity by generating substantial site disorder and high vacancy concentrations. To elucidate the mechanism that facilitates sodium ion conduction, a series of mixed-pnicogen solid solutions were prepared from the parent ternary sulfides Na<sub>3</sub><i>Pn</i>S<sub>4</sub> (<i>Pn</i> = P, As, Sb) by high-temperature reactions, including an entropy-driven W-substituted phase, Na<sub>3−δ</sub>P<sub>0.32</sub>As<sub>0.32</sub>Sb<sub>0.32</sub>W<sub>0.04</sub>S<sub>4</sub> (N-PASS-W). N-PASS-W exhibits a very high ionic conductivity of 10 mS cm<sup>–1</sup> and a low activation energy of 0.15 eV. Using PXRD and NMR spectroscopy, an atomic-level model for N-PASS-W was proposed, in which ion hopping occurs over two Na sites within a tetragonal structure (<i>P</i>4̅2<sub>1</sub><i>c</i>). Relationships were also established between the structure and ionic conductivities of the other members to evaluate the influence of crystalline phase, cation size, and site disorder.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3427–3434"},"PeriodicalIF":8.7,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226797","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Direct Visualization of Metastable Charged States in Positive Electrode Materials by Cryo-STEM","authors":"Hinata Fujimura, , , Yosuke Ugata, , , Zhang Xinrui, , , Yoshinobu Miyazaki, , and , Naoaki Yabuuchi*, ","doi":"10.1021/acsmaterialslett.5c01021","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01021","url":null,"abstract":"<p >LiNiO<sub>2</sub> is regarded as an ideal positive electrode material for Li-ion battery applications, offering a large reversible capacity, >200 mA h g<sup>–1</sup>, with a lower cutoff voltage, 4.3 V. The fully charged state, Li<sub>1–<i>x</i></sub>NiO<sub>2</sub> (<i>x</i> ≈ 0.9), is a metastable phase obtained by electrochemical oxidation in Li cells. Due to its instability, atomic-scale imaging of this phase by using scanning transmission electron microscopy (STEM) is particularly challenging, as it readily decomposes under electron beam exposure. In this study, the effect of cryogenic conditions during STEM observation is examined. While as-prepared LiNiO<sub>2</sub> shows strong resistance to beam damage, Li<sub>1–<i>x</i></sub>NiO<sub>2</sub> (<i>x</i> ≈ 0.9) undergoes structural changes under room-temperature beam exposure. In contrast, beam-induced damage is substantially suppressed under cryogenic conditions (−150 °C), enabling successful acquisition of atomic-resolution STEM images. These findings underscore the importance of cryo-STEM techniques for imaging metastable battery materials.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3420–3426"},"PeriodicalIF":8.7,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226796","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hongwei Du, , , Xiang Huang, , , Jian Hui*, , , Lanting Zhang*, , , Yuanxun Zhou*, , and , Hong Wang*,
{"title":"Assessment and Application of Universal Machine Learning Interatomic Potentials in Solid-State Electrolyte Research","authors":"Hongwei Du, , , Xiang Huang, , , Jian Hui*, , , Lanting Zhang*, , , Yuanxun Zhou*, , and , Hong Wang*, ","doi":"10.1021/acsmaterialslett.5c00336","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00336","url":null,"abstract":"<p >High-performance solid-state electrolytes (SSEs) are crucial for next-generation lithium batteries. However, conventional methods like density functional theory and empirical force fields face challenges in computational cost, scalability, and transferability across diverse systems. Machine learning interatomic potentials (MLIPs) offer a promising alternative by balancing accuracy and efficiency. Nevertheless, their performance and applicability for SSEs remain poorly defined, limiting reliable model selection. In this study, we benchmark 12 MLIPs─including GRACE, DPA, MatterSim, MACE, SevenNet, CHGNet, TensorNet, M3GNet, and ORB─across energies, forces, phonons, electrochemical stability, thermodynamic properties, elastic moduli, and Li<sup>+</sup> diffusivity. GRACE-2L-OAM, MACE-MPA, MatterSim, DPA-3.1-3M, and SevenNet-MF-ompa show superior accuracy. Using MatterSim, we study Li<sub>3</sub>YCl<sub>6</sub> and Li<sub>6</sub>PS<sub>5</sub>Cl, revealing that ∼40–50% S/Cl anion disorder enhances Li<sup>+</sup> migration connectivity in Li<sub>6</sub>PS<sub>5</sub>Cl, while higher Li<sup>+</sup> content in Li<sub>3</sub>Ycl<sub>6</sub> expands conduction channels and reduces energy barriers. These insights highlight the power of MLIP-driven simulations for mechanistic understanding and rational design of high-conductivity SSEs.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3403–3412"},"PeriodicalIF":8.7,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226781","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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