ACS Materials LettersPub Date : 2026-11-02Epub Date: 2026-10-13DOI: 10.1021/acsmaterialslett.6c00598
Kevin A. Stewart, Leonie Cordes, Darya A. Ivannikava, Calvin J. Stevenson, Sophia Q. Vo, Joe J. Brosz, Bhavya S. Rai, Sky D. Cao, Jacob J. Lessard
{"title":"Frontally Fabricated Fluoropolymers","authors":"Kevin A. Stewart, Leonie Cordes, Darya A. Ivannikava, Calvin J. Stevenson, Sophia Q. Vo, Joe J. Brosz, Bhavya S. Rai, Sky D. Cao, Jacob J. Lessard","doi":"10.1021/acsmaterialslett.6c00598","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00598","url":null,"abstract":"<p>Fluoropolymers are ubiquitous in modern technologies owing to their exceptional thermal, chemical, and environmental durability. However, these properties often come at the expense of synthetic severity and recyclability. Here, we report the preparation of semi-fluorinated thermosets and thermoplastics via frontal ring-opening metathesis polymerization (FROMP), enabling rapid synthesis with minimal external energy input and no post-polymerization processing. Fluorinated monomers were prepared from pentafluoropyridine (PFP), whose activated heteroaromatic scaffold enables regioselective nucleophilic aromatic substitution with norbornene-derived nucleophiles. Alcohol-derived monomers intrinsically favored multifunctional reactivity and network formation, whereas 5-norbornene-2-methylamine formed a resonance-stabilized anilide adduct that suppressed further substitution. The resulting amine-linked fluoropolymers displayed linear architectures, favorable mechanical properties despite lacking covalent crosslinks, and improved prospects for reprocessability. Collectively, these studies position FROMP as a promising platform for more sustainable fluoropolymer manufacturing and end-of-life management.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3187–3194"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305701","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}
ACS Materials LettersPub Date : 2026-11-02Epub Date: 2026-10-15DOI: 10.1021/acsmaterialslett.6c00790
Hala E. Soliman, Rhys A. Otten, Amy L. Prieto
{"title":"Direct Contact Presodiation of Na0.67Fe0.5Mn0.5O2 Forms Jahn–Teller Distorted P′2 NaFe0.5Mn0.5O2 Phase","authors":"Hala E. Soliman, Rhys A. Otten, Amy L. Prieto","doi":"10.1021/acsmaterialslett.6c00790","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00790","url":null,"abstract":"<p>The P2-type Na<sub>0.67</sub>Fe<sub>0.5</sub>Mn<sub>0.5</sub>O<sub>2</sub> (NFMO) is an attractive positive electrode for Na-ion batteries. However, NFMO’s capacity is limited by the amount of sodium stored in its initial framework. Here, we show that direct contact presodiation is a facile way to introduce cyclable sodium into NFMO before cycling and increases first cycle desodiation to 241 mAh/g, exceeding its theoretical capacity. We characterize the structural and surface changes that occur during presodiation. We report full conversion to the Jahn–Teller distorted P′2 phase, NaFe<sub>0.5</sub>Mn<sub>0.5</sub>O<sub>2</sub>, before cycling using presodiation. Furthermore, a NaF, PF<sub>5</sub><sup>–</sup>, and Na<sub>2</sub>CO<sub>3</sub>-rich interphase is created on PS-NFMO. With electrochemical impedance spectroscopy and distribution of relaxation times analysis, we show that the charge-transfer impedance contribution is reduced due to differences in interphase speciation of NFMO and PS-NFMO. Lastly, we show that a robust cathode electrolyte interphase is created during presodiation, which enables high coulombic efficiency (>90%).</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3261–3267"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305726","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}
ACS Materials LettersPub Date : 2026-11-02Epub Date: 2026-09-28DOI: 10.1021/acsmaterialslett.6c00691
Sachin Gupta, Pia S. Klee, Ralf Erber, Christoph A. Spiegel, Eva Blasco
{"title":"A Bio-Based and Biocompatible Lipoate-Oil Platform for 3D Digital Light Processing","authors":"Sachin Gupta, Pia S. Klee, Ralf Erber, Christoph A. Spiegel, Eva Blasco","doi":"10.1021/acsmaterialslett.6c00691","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00691","url":null,"abstract":"<p>In the search for alternatives to petrochemically derived monomers for digital light processing (DLP), vegetable oils are an attractive renewable feedstock. However, most reported oil-based inks still rely on acrylate-based cross-linking strategies, limiting the bio-based content and biocompatibility of the resulting printed materials. Here, we present a fully bio-based oil-derived DLP ink that exploits lipoates as photocross-linking units, thereby avoiding the use of acrylates and eliminating the need for photoinitiators. A lipoated triglyceride is synthesized and formulated into a 100% bio-based ink using ethyl lipoate as a reactive diluent and <em>p</em>-cymene as a solvent. The ink exhibits good curing performance and enables the fabrication of complex three-dimensional architectures, which can be depolymerized on demand. Cytocompatibility is demonstrated in a live/dead assay, with cell viability exceeding 97%. These results establish this fully bio-based system as a promising platform for the next generation of sustainable materials for biomedical applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3202–3209"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149306044","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}
ACS Materials LettersPub Date : 2026-11-02Epub Date: 2026-10-08DOI: 10.1021/acsmaterialslett.6c00743
Evelyn C. Peterson, George W. Fritze, Nicholas A. Tomalia, Adam J. Matzger
{"title":"Subverting the Dominant Paradigm in Metal–Organic Framework Activation","authors":"Evelyn C. Peterson, George W. Fritze, Nicholas A. Tomalia, Adam J. Matzger","doi":"10.1021/acsmaterialslett.6c00743","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00743","url":null,"abstract":"<p>The necessity of solvent exchange and evacuation for metal–organic framework (MOF) activation is investigated using HKUST-1, UiO-66, and Zn-MOF-74 as model systems. High surface areas are achieved by simple thermal treatment directly from either the synthesis solvent or the activation solvent. The process requires careful control over time and temperature, as removal of guest solvent molecules competes with linker decomposition. Detailed studies on HKUST-1 reveal the liberation of benzene accompanying material decomposition. NMR spectroscopy data complement TGA-MS data to reveal stepwise linker decarboxylation and an autocatalytic decomposition mechanism. Material collapse, evidenced by a surface area decline upon extended thermal treatment, is found to be accelerated by certain residual solvents, albeit with a mechanism distinct from the commonly invoked mechanism of capillary force-induced collapse.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3237–3242"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305645","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}
ACS Materials LettersPub Date : 2026-11-02Epub Date: 2026-10-03DOI: 10.1021/acsmaterialslett.6c00732
Sheng Li, Chen Kong, Yu Liu, Zhicheng Wang, Chengyao Yang, Qihao Xu, Xin Guo, Xiaoshuang Zhou, Huafei Guo, Sai Jiang, Yi Shi, Lijia Pan
{"title":"SnS2-Based Memristor Arrays for Neuromorphic Computing and Reconfigurable Physical Unclonable Functions","authors":"Sheng Li, Chen Kong, Yu Liu, Zhicheng Wang, Chengyao Yang, Qihao Xu, Xin Guo, Xiaoshuang Zhou, Huafei Guo, Sai Jiang, Yi Shi, Lijia Pan","doi":"10.1021/acsmaterialslett.6c00732","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00732","url":null,"abstract":"<p>The increasing demand for energy-efficient and secure on-device artificial intelligence has stimulated considerable interest in multifunctional memory platforms that combine neuromorphic computing and hardware-level security within a unified architecture. Herein, we present a tin disulfide (SnS<sub>2</sub>)-based memristor array that seamlessly integrates neuromorphic functionalities and reconfigurable physical unclonable functions (PUFs) within a unified hardware platform. The device employs layered SnS<sub>2</sub> as the interlayer material, where intrinsic defect states and stochastic conductive-filament evolution govern the resistive switching behavior. Leveraging tunable analog conductance states and robust nonvolatile switching behavior, the memristor faithfully emulates synaptic plasticity and demonstrates high recognition accuracy in neuromorphic computing tasks. Meanwhile, the stochastic formation of conductive pathways during resistive switching generates unpredictable electrical responses, enabling robust and reconfigurable PUF functionality with strong resilience against machine learning attacks. This work provides a promising pathway toward secure neuromorphic hardware for future edge AI applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3228–3236"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305663","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":"Bioinspired Synthesis of Zeolitic Imidazolate Framework-8 in Giant Unilamellar Vesicles","authors":"Nadia Valletti, Paola Albanese, Masaki Itatani, Norbert Nemet, Gabor Schuszter, Nerith Rocio Elejalde-Cadena, Pietro Lupetti, Eugenio Paccagnini, Annette F. Taylor, Istvan Lagzi, Federico Rossi","doi":"10.1021/acsmaterialslett.6c00099","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00099","url":null,"abstract":"<p>The confined synthesis of functional nanomaterials within biomimetic compartments offers a strategy to address key limitations in biomedical applications, including stability, biocompatibility, and controlled encapsulation. Here, we report the in situ precipitation of zeolitic imidazolate framework-8 (ZIF-8) within phospholipid giant unilamellar vesicles (GUVs). By encapsulating Zn<sup>2+</sup> in the vesicle lumen and triggering crystallization through external addition of membrane-permeable 2-methylimidazole, we establish a bioinspired compartmentalized synthesis approach. Confocal and electron microscopy confirm nanoparticle formation and reveal strong interactions between the precipitated phase and the membrane, leading to poration and selective content release. Crystal-size analysis and comparison with bulk systems show that confinement and the lipid interface modulate nucleation and growth. These results identify GUVs as soft templates for localized nanomaterial synthesis and as modular platforms for drug delivery, bioresponsive systems, and synthetic cell design.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3135–3143"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305671","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":"Microstructure-Induced Anisotropic Elastocaloric Effect and Cyclic Stability in Additively Manufactured NiTi Shape Memory Alloys","authors":"Shuyao Wang, Qiang Zhang, Yongjun Shi, Junyu Chen, Yingbo Liu, Zhaojian Li, Menglu Xi, Yangshu Liu, Chongbo Fu","doi":"10.1021/acsmaterialslett.6c00316","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00316","url":null,"abstract":"<p>NiTi shape memory alloys (SMAs) with semicircular arc-shaped microstructures aligned along the build direction (BD) were fabricated using a customized additive manufacturing scanning strategy. The anisotropic elastocaloric response and cyclic stability were systematically investigated under compressive loading applied perpendicular and parallel to the BD. Loading perpendicular to the BD delivers superior elastocaloric performance and cyclic stability compared to parallel loading. Finite-element simulations incorporating the tailored arc architecture were conducted to analyze stress distribution and transformation behavior. The results reveal that enhanced transformation deformation along the chord-length direction promotes more stress-induced martensitic transformation, thereby amplifying the elastocaloric response. This study elucidates the intrinsic relationship between architected microstructures and anisotropic functional behavior in additively manufactured NiTi SMAs, providing guidance for orientation-dependent design of high-performance elastocaloric materials.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3154–3161"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305718","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}
ACS Materials LettersPub Date : 2026-11-02Epub Date: 2026-07-30DOI: 10.1021/acsmaterialslett.6c00507
Thiago F. Santos, Ihsan Boustani, Jose Heriberto O. Nascimento
{"title":"Borophene beyond Discovery from Fundamental Science to Functional Technologies","authors":"Thiago F. Santos, Ihsan Boustani, Jose Heriberto O. Nascimento","doi":"10.1021/acsmaterialslett.6c00507","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00507","url":null,"abstract":"<p>Borophene (BPh) has quickly gained attention as a highly unusual two-dimensional material, notable for its structural polymorphism, inherent metallic properties, and marked anisotropy. Although recent experimental advances have demonstrated remarkable electronic, catalytic, and mechanical properties, work remains largely confined to ultrahigh-vacuum growth on metallic substrates and small-scale demonstrations. Key hurdles remain before larger-scale adoption, including environmental instability, substrate dependence, and the lack of scalable synthesis methodologies. We outline strategic paths for translating BPh into usable energy, electronic, and catalytic systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3125–3129"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305670","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":"Synergistic Boosting of BiVO4 Photoanode for Photoelectrochemical Water Splitting by Coupling CuSCN with FeCoNiBi","authors":"Pengfei Lv, Zhiru Xie, Guangping Yi, Yiping Zhao, Mengfan Shang, Xiaofan Yang, Sijie Wen, Zhao Jing, Qiang Wang, Dongsheng Song, Pengyi Tang","doi":"10.1021/acsmaterialslett.6c00721","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00721","url":null,"abstract":"<p>Photoelectrochemical (PEC) water splitting offers a sustainable route for solar hydrogen production, but BiVO<sub>4</sub> photoanodes suffer from poor bulk charge separation and sluggish oxygen evolution reaction (OER) kinetics. Herein, a CuSCN hole transport layer and a trimetallic borate FeCoNiB<sub>i</sub> cocatalyst are integrated onto BiVO<sub>4</sub> to synergistically address these bottlenecks. CuSCN forms a PN heterojunction with n-type BiVO<sub>4</sub>, generating a built-in electric field that extracts holes and suppresses bulk recombination. Meanwhile, FeCoNiB<sub>i</sub> accelerates OER kinetics and modulates surface states by passivating recombination centers and increasing intermediate surface states, promoting rapid hole transfer to the electrolyte. The optimized BVO/CuSCN/FeCoNiB<sub>i</sub> photoanode achieves a photocurrent of 5.82 mA cm<sup>–2</sup> at 1.23 V<sub>RHE</sub> and retains 88.7% of its initial activity after 24 h. This work demonstrates that rationally combining a p-type HTL with an OER cocatalyst can simultaneously address bulk recombination and surface transfer limitations, offering a paradigm for designing high-performance and durable PEC water splitting systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3210–3219"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149306047","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":"Advanced Catalytic Materials for Efficient Electrochemical Hydrogen and Oxygen Evolution Reactions in Sustainable Energy Conversion","authors":"Yihao Li, Haiqin Zhang, Rongrong Cui, Ao Wang, Lintao Yang, Hongyao Xue","doi":"10.1021/acsmaterialslett.6c00572","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00572","url":null,"abstract":"<p>Electrochemical water splitting enables renewable hydrogen production, yet laboratory catalyst activity often fails to translate into durable electrolyzer performance. This review integrates interfacial mechanisms, performance evaluation, degradation, and device requirements within a unified framework for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Noble-metal and non-noble-metal catalysts are compared using common criteria encompassing intrinsic activity, conductivity, stability, reconstruction, and resource use. Electronic-structure regulation, defect engineering, heterointerfaces, phase control, and strain are evaluated as interconnected design strategies. Magnetic-field effects are examined by distinguishing spin-dependent kinetics from transport and bubble removal. Density functional theory (DFT) links descriptors and kinetic barriers to electrochemical environments and operando identification of active structures. Translation to proton-exchange-membrane (PEM), alkaline, and anion-exchange-membrane (AEM) electrolyzers highlights catalyst-layer design, realistic current densities, and dynamic operation. This framework guides joint optimization of activity, durability, working-state structure, material utilization, and device-level transport.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 11","pages":"3024–3045"},"PeriodicalIF":8.6,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149305647","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}