{"title":"Spatio-Selective Reconfiguration for Enhanced Ethylene/Ethane Separation in Metal–Organic Framework Membranes","authors":"Ziqi Xu, , , Jia Wang, , , Yuchen Gao, , , Lingchuan Li, , , Wenjiang Zeng, , , Xiangyu Guo*, , and , Qingyuan Yang*, ","doi":"10.1021/acsmaterialslett.5c00935","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00935","url":null,"abstract":"<p >Due to the similar kinetic diameters and physicochemical properties of ethylene and ethane, developing highly efficient C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub> separation membranes remains a huge challenge. In this study, spatio-selective reconfiguration of a Ni-pca-pyz metal–organic framework (MOF) membrane was discovered upon vacuum heat treatment. The progressive migration of the low-boiling-point pyrazine ligands on the coordination unsaturated metal sites in the structure can result in the preferential exposure of the (001) crystal plane, thus the significant increase in C<sub>2</sub>H<sub>4</sub> selectivity due to the optimized diffusion path. The Ni-pca-pyz membrane with preferential (001) crystal plane orientation shows highly competitive C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub> separation performance, with a C<sub>2</sub>H<sub>4</sub> permeance of 351.2 GPU and a C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub> separation factor of 5.6 during mixed-gas permeation, highlighting the promising application of the vacuum heat treatment protocol in structure optimization and performance enhancement of versatile MOF membranes.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3413–3419"},"PeriodicalIF":8.7,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226782","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":"Constructing Charge-Delocalized Polycationic Protective Layer by Chitosan for Zinc-Ion Batteries","authors":"Binbin Ren, , , Yifan Pan, , , Yanchun Xie, , , Yucong Jiao*, , and , Peiyi Wu*, ","doi":"10.1021/acsmaterialslett.5c00839","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00839","url":null,"abstract":"<p >Engineering a polymer-based protective layer on a Zn metal surface can alleviate the side reactions for high Zn reversibility, yet the chain entanglement of the polymer may prolong the pathway and hinder the ion transport for poor battery performance. Here, the Debus-Radziszewski reaction was employed to form an imidazolium cation (IM<sup>+</sup>) structure in chitosan for high-performance protective layers. The protective layer for Zn metal with chitosan connected by IM<sup>+</sup> (ZCIM) owns low entanglement characteristics to facilitate the ion transport channel construction, thus significantly promoting rapid Zn<sup>2+</sup> migration kinetics. Moreover, the IM<sup>+</sup> renders charge delocalization, thereby improving the electric field distribution on the Zn surface to accelerate stable Zn<sup>2+</sup> deposition kinetics. Consequently, the symmetrical Zn battery with ZCIM remains stable at a high depth of discharge of 93.2%, and the Zn/I<sub>2</sub> battery with ZCIM demonstrates a high-capacity retention rate of over 89% at a low N/P ratio of 2.6.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3394–3402"},"PeriodicalIF":8.7,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226817","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}
Nilotpal Deka, , , Supriya Sahoo, , , Vikash Kushwaha, , , Jan K. Zaręba*, , and , Ramamoorthy Boomishankar*,
{"title":"A Highly Electrostrictive A2BX4-Type Hybrid 2D Perovskite Ferroelectric and the Utility of Its Piezoelectric Nanogenerator in Wireless Mat-Sensor Technology","authors":"Nilotpal Deka, , , Supriya Sahoo, , , Vikash Kushwaha, , , Jan K. Zaręba*, , and , Ramamoorthy Boomishankar*, ","doi":"10.1021/acsmaterialslett.5c00713","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00713","url":null,"abstract":"<p >The quasi-spherical theory and ligand halogenation have emerged as effective strategies for promoting polar noncentrosymmetric structures with potential ferroelectric properties. Here, we report a novel two-dimensional (2D) hybrid organic–inorganic perovskite, <b>[</b><i>p</i><b>-ClBnNH</b><sub><b>3</b></sub><b>]</b><sub><b>2</b></sub><b>CdBr</b><sub><b>4</b></sub>, in the polar orthorhombic <i>Ccc</i>2 space group. The structural noncentrosymmetry was confirmed via second harmonic generation (SHG) measurements. Polarization-electric field (<i>P–E</i>) hysteresis measurements revealed a saturation polarization (<i>P</i><sub>s</sub>) of 1.28 μC cm<sup>–2</sup> at room temperature. Furthermore, it exhibits a high electrostrictive coefficient (<i>Q</i><sub>33</sub>) of 3.6 m<sup>4</sup> C<sup>–2</sup>, surpassing those observed in traditional ferroelectrics. For energy harvesting applications, composite films were fabricated by embedding <b>[</b><i>p</i><b>-ClBnNH</b><sub><b>3</b></sub><b>]</b><sub><b>2</b></sub><b>CdBr</b><sub><b>4</b></sub> in thermoplastic polyurethane (TPU) matrix. The 10 wt % device yielded a piezoelectric nanogenerator (PENG) output voltage of 20.0 V and a power density of 67.6 μW cm<sup>–2</sup>. A prototype “mat-sensor”, which is a scalable smart force sensor, was developed, demonstrating rapid response and wireless functionality for real-time applications, including security systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3380–3387"},"PeriodicalIF":8.7,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00713","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226815","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}
Naman Katyal, , , Chunhui Li, , , Martin Kunz, , , Simon J. Teat, , , Piotr Zarzycki, , , Gerbrand Ceder, , and , Michael L. Whittaker*,
{"title":"Defect-Mediated Diffusion Pathways in Spodumene Accelerate Lithium Transport","authors":"Naman Katyal, , , Chunhui Li, , , Martin Kunz, , , Simon J. Teat, , , Piotr Zarzycki, , , Gerbrand Ceder, , and , Michael L. Whittaker*, ","doi":"10.1021/acsmaterialslett.5c00876","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00876","url":null,"abstract":"<p >Lithium extraction from naturally occurring α-spodumene is hindered by poor lithium diffusivity, necessitating high-temperature phase transformation to a low-density β polymorph. Although β spodumene exhibits up to 5 orders of magnitude higher lithium-ion diffusivity, both phases have diffusion activation energies between 0.8 and 1 eV, indicating that polymorph density is not the controlling factor over diffusivity. We show that aluminum vacancies facilitate lithium-ion diffusion in α-spodumene by reducing the migration barrier from 2.4 to 0.9 eV. Bond valence site energy and nudged elastic band calculations show a new lithium local minimum site which promotes a one-dimensional percolation network by reducing the lithium intersite distance from 4.5 Å to 2.9 Å. However, aluminum vacancies are energetically unfavorable to percolate through the whole structure, resulting in very low net lithium diffusivity and highlighting the critical role of nonstoichiometric defects in facilitating lithium transport in rigid aluminosilicate structures.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3388–3393"},"PeriodicalIF":8.7,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00876","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226816","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}
Cariny Polesca, , , Rita Sobreiro-Almeida*, , , Helena Passos, , , João A. P. Coutinho, , , Jason P. Hallett, , , João F. Mano*, , and , Mara G. Freire*,
{"title":"Engineered from Waste: Ionic Liquid Processing of Keratin for 3D Printing Biomedical Scaffolds","authors":"Cariny Polesca, , , Rita Sobreiro-Almeida*, , , Helena Passos, , , João A. P. Coutinho, , , Jason P. Hallett, , , João F. Mano*, , and , Mara G. Freire*, ","doi":"10.1021/acsmaterialslett.5c00629","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00629","url":null,"abstract":"<p >Keratin holds significant potential for biomedical applications due to its superior cytocompatibility and ability to promote cellular migration and differentiation. However, despite these advantages, keratin processing is difficult due to its limited solubility in water and most common organic solvents. Herein, a sustainable and cost-effective approach was used for chicken feather dissolution (a keratin-rich waste) using acetate-based ionic liquids. This method simplifies the development of three-dimensional (3D) structures via directly embedded 3D printing keratin dissolved in ionic liquids (ILs). Using a carbonate-bicarbonate agarose microparticle support bath, we successfully promoted disulfide exchange and direct cross-linking of printed structures with diverse patterns and geometries, exhibiting excellent structural integrity. A comprehensive analysis of the rheological, mechanical, and biological properties was conducted, highlighting their potential biomedical applications. Interestingly, the scaffolds exhibited a dynamic shape-change over time, mediated by cellular traction forces, demonstrating their potential for 4D printing toward innovative bioapplications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3370–3379"},"PeriodicalIF":8.7,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226813","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}
Jonathan H. Gillen, , , My K. Vuong, , , Daniel W. Paley, , and , Christopher M. Bejger*,
{"title":"Conductive Organometallic Polymers from Soluble Superatom Ions","authors":"Jonathan H. Gillen, , , My K. Vuong, , , Daniel W. Paley, , and , Christopher M. Bejger*, ","doi":"10.1021/acsmaterialslett.5c00925","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00925","url":null,"abstract":"<p >Superatomic crystals comprising ligand-capped, metal chalcogenide clusters and fullerenes are modular materials that exhibit enhanced electronic, magnetic, and thermal conductivity properties. We find that neutral, M<sub>4</sub>S<sub>4</sub> (M = Fe, Co) clusters stabilized with <i>N</i>-heterocyclic carbenes (NHCs) can transfer charge to C<sub>60</sub> fullerene to form binary superatomic crystals. Notably, these compounds are soluble in various organic solvents, allowing their properties to be investigated in solution, unlike traditional fullerene-based superatomic crystals. The ion pairs can be further assembled into organometallic polymers using Janus-bis(NHCs) to cross-link the oxidized M<sub>4</sub>S<sub>4</sub> units. We show that the superatomic polymers are more conductive than both the precursor superatomic crystals and the polymers containing only neutral M<sub>4</sub>S<sub>4</sub> clusters. Similar conductivity values can be obtained when neutral M<sub>4</sub>S<sub>4</sub>–NHC polymers are doped with solutions of C<sub>60</sub> fullerene. These findings demonstrate that next generation superatomic materials can be prepared via the combination of charge transfer and polymerization with appropriate cross-linking agents.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3363–3369"},"PeriodicalIF":8.7,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00925","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226814","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":"Covalent Organic Frameworks for Enzyme Immobilization: Synthesis, Pore Structure Modification, and Applications","authors":"Yongheng Shi, , , Lingmei Dai, , , Dehua Liu, , and , Wei Du*, ","doi":"10.1021/acsmaterialslett.5c00905","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00905","url":null,"abstract":"<p >Immobilized enzymes constitute a class of composite biocatalysts whose performance is governed by both enzyme molecules and carrier materials. Recent advances in materials science have yielded diverse novel porous materials, with covalent organic frameworks (COFs) emerging as particularly promising candidates for enzyme immobilization carriers. This review systematically categorizes COF synthesis strategies based on elemental composition, encompassing boron-containing, nitrogen-containing, and novel metal-containing COF variants. Enzyme immobilization techniques on COFs are classified into postsynthesis and presynthesis approaches. Furthermore, methodologies for constructing diverse building blocks and critical linkage structures are summarized, alongside detailed elucidation of pore structure modulation techniques─including topological design, template-assisted methods, and defect engineering─employed to enhance compatibility with enzyme dimensions. Finally, emerging types and application scenarios of immobilized enzyme-COF composite systems are analyzed, emphasizing the critical importance of rational design and recoverability in advancing practical application potential.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3320–3340"},"PeriodicalIF":8.7,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226809","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}
Thiago F. Santos*, , , Felipe Mendonca Fontes Galvão, , , Leônidas Oliveira Neto, , and , Jose H. O. Nascimento*,
{"title":"Emerging Technologies in Wearable Sweat Sensors for Next-Generation Real-Time Health Monitoring","authors":"Thiago F. Santos*, , , Felipe Mendonca Fontes Galvão, , , Leônidas Oliveira Neto, , and , Jose H. O. Nascimento*, ","doi":"10.1021/acsmaterialslett.5c00706","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00706","url":null,"abstract":"<p >Wearable sweat sensors (We-SS) enable noninvasive health monitoring by detecting sweat biomarkers. A bibliometric analysis of 1,006 Scopus-indexed articles (2005–2024) shows 60.9% of publications and 66.5% of citations from 2022–2024, indicating rapid growth. China and the United States lead, with strong global collaboration. We-SS detect electrolytes (Na<sup>+</sup>, K<sup>+</sup>, Cl<sup>–</sup>, 10–120 mM), metabolites (lactate, 2–30 mM; glucose, 10–200 μM; uric acid, 2–200 μM), hormones (cortisol, 0.1–25 ng/mL), and trace metals (Zn<sup>2+</sup>, Cu<sup>2+</sup>, 100–1,000 μg/L) using graphene, MOFs, PEDOT:PSS, and electrochemical methods. AI/IoT integration enhance predictive diagnostics. We-SS market is projected to grow from USD 4.41 billion (2024) to USD 13.47 billion (2034) at a 11.8% CAGR, driven by preventive medicine, sports, and chronic disease management. Challenges include analytical interference, calibration stability, durability, and biocompatibility. Future innovations involve advanced nanomaterials, self-calibrating systems, robust encapsulation, and biocompatible coatings, positioning We-SS for personalized healthcare.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3341–3362"},"PeriodicalIF":8.7,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00706","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226840","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":"Cuproptosis: An Emerging Cell Death Modality for Antitumor Therapy","authors":"Yubin Han, , , Guoqing Zhu, , , Yinuo Jin, , and , Chunxia Li*, ","doi":"10.1021/acsmaterialslett.5c00711","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00711","url":null,"abstract":"<p >Copper plays a critical role in sustaining the activity of enzymes and transcription factors vital to tumor cell proliferation while also regulating signaling networks that preserve cellular homeostasis. However, intracellular copper levels exceeding threshold tolerances can disrupt metabolic processes and trigger cuproptosis, which is a novel, characterized copper-dependent form of regulated cell death. This mechanistically distinct pathway offers a promising therapeutic strategy for selectively targeting malignancies by exploiting mitochondrial copper dysregulation under both physiological and pathological conditions. The burgeoning interest in cuproptosis underscores its broad potential for clinical translation in oncology. In this review, we have synthesized recent advances in the design of antitumor nanomaterials engineered to trigger cuproptosis, while systematically evaluating synergistic therapeutic modalities that could amplify their efficacy. We further discuss unresolved challenges and emerging opportunities to optimize copper-mediated oncologic interventions.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3301–3319"},"PeriodicalIF":8.7,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226808","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}
Biao Fang, , , Lei Wang, , , Zhangyuan Wang, , , Zhipeng Su, , , Feng Zou, , and , Runwei Mo*,
{"title":"Self-Healing Interfacial Cross-Links Enable Supertough Solid Polymer Electrolytes with Eliminating-Dendrite Lithium Metal Battery","authors":"Biao Fang, , , Lei Wang, , , Zhangyuan Wang, , , Zhipeng Su, , , Feng Zou, , and , Runwei Mo*, ","doi":"10.1021/acsmaterialslett.5c01098","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01098","url":null,"abstract":"<p >The integration of solid-state inorganic fillers into polymer matrices can improve the performance of solid lithium metal batteries. However, there is poor interface interaction between the polymer matrix and solid-state inorganic fillers, which has led to the performance of solid lithium metal batteries falling far short of expectations. Here, we constructed a bridging interaction based on borate ester dynamic cross-linking to prepare a supertough and self-healing poly(vinylidene fluoride)-hexafluoropropylene/graphene oxide/borate bonds/Li<sub>6.5</sub>La<sub>3</sub>Zr<sub>1.5</sub>Ta<sub>0.5</sub>O<sub>12</sub> solid polymer electrolyte. The electrolyte exhibits a wide electrochemical window (4.84 V), high elongation at break (205%), outstanding thermal stability (200 °C), and high-capacity retention (90.3% after 900 cycles under 2C). We further revealed the influence of borate ester dynamic cross-linking on the performance of solid polymer electrolyte through density functional theory calculations. This work offers insight into designing high-performance solid polymer electrolytes for solid-state batteries.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3292–3300"},"PeriodicalIF":8.7,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226773","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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