ACS Materials Letters最新文献_第6页

Mechanistic Insights into Li+ Transport Enabled by Isolated Sulfur Species in Li3PS4 Glasses Li+在Li3PS4玻璃中的输运机制

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-05-01 DOI: 10.1021/acsmaterialslett.6c00150

Jakub Pawelko, Xavier Rocquefelte, Auguste Tetenoire, David Le Coq, Laurent Calvez, Eric Furet

{"title":"Mechanistic Insights into Li+ Transport Enabled by Isolated Sulfur Species in Li3PS4 Glasses","authors":"Jakub Pawelko, Xavier Rocquefelte, Auguste Tetenoire, David Le Coq, Laurent Calvez, Eric Furet","doi":"10.1021/acsmaterialslett.6c00150","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00150","url":null,"abstract":"All-solid-state lithium-ion batteries have renewed interestinhigh-performance solid electrolytes. Li3PS4 (Li2S–P2S5) glasses are among themost studied due to their high ionic conductivity, traditionally ascribedto rotational motion of polyhedral units facilitating Li+ migration. Using ab initio molecular dynamics, we investigate Li-iondiffusion in Li3PS4 glass, demonstrating thatour structural model reproduces experimental neutron and X-ray diffractionpatterns and conductivity measurements. Importantly, we identify apreviously unrecognized diffusion mechanism: Li+ ions nearisolated sulfur species (Sn with n = 1, 3) display significantly enhanced mobility, withatomic displacements up to 1.7 greater than those associated withbulkier polyhedral units. These results highlight the critical roleof free sulfur species in promoting fast ionic transport, providinginsights for the rational design of glass compositions with optimizedconductivity for solid-state battery applications.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2538–2544"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923875","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}

引用次数: 0

Polyethylene-Based Thermo-Mechanically Recyclable Stretchable Yarns for Circular Sustainable Textiles 用于循环可持续纺织品的聚乙烯基热机械可回收可拉伸纱线

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-07-25 DOI: 10.1021/acsmaterialslett.6c00337

SeongHyeon Kim, Duo Xu, Volodymyr Korolovych, Domingo R. Flores-Hernandez, Kaniz Moriam, Daniel J. Braconnier, Svetlana V. Boriskina

{"title":"Polyethylene-Based Thermo-Mechanically Recyclable Stretchable Yarns for Circular Sustainable Textiles","authors":"SeongHyeon Kim, Duo Xu, Volodymyr Korolovych, Domingo R. Flores-Hernandez, Kaniz Moriam, Daniel J. Braconnier, Svetlana V. Boriskina","doi":"10.1021/acsmaterialslett.6c00337","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00337","url":null,"abstract":"Most high-performance elastic textiles rely on yarns composed of chemically dissimilar polymers, rendering them difficult to recycle. Here, we demonstrate fully thermo-mechanically recyclable stretchable yarns composed of polyethylene (PE) family materials. Inspired by structure–property relationships in natural materials, we engineer a library of melt-spun PE fibers spanning mechanical properties from elastomeric to functional by tuning polymer crystallinity and chain orientation. These fibers are assembled into core–sheath yarns comprising an olefin block copolymer elastic core and a high-strength PE sheath, forming a helical architecture. The resulting yarns exceed mechanical performance of commercial PET–spandex yarns while maintaining full recyclability. We further show that PE homopolymers and copolymers can be jointly melt-processed and recycled without phase separation or loss of performance. This approach enables stretchable recyclable textiles from fibers with previously demonstrated cooling, moisture-wicking, and stain-resistant performance and provides a scalable pathway toward circular garments compatible with existing polyethylene recycling streams.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2545–2554"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923955","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}

引用次数: 0

Achieving Efficient Long-Range Transport in Molecular Devices via Frontier-Orbital Engineering 利用前沿轨道工程实现分子器件的高效远程传输

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-24 DOI: 10.1021/acsmaterialslett.6c00388

Quyen Van Nguyen, Pascal Martin, Thai Anh Do, Jean Christophe Lacroix

{"title":"Achieving Efficient Long-Range Transport in Molecular Devices via Frontier-Orbital Engineering","authors":"Quyen Van Nguyen, Pascal Martin, Thai Anh Do, Jean Christophe Lacroix","doi":"10.1021/acsmaterialslett.6c00388","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00388","url":null,"abstract":"We report highly efficient, long-range hole transport—exhibiting weak dependence on molecular length and temperature—in conjugated molecular devices (<20 nm) fabricated using a bottom-up approach combined with complementary metal-oxide-semiconductor technology. By oxidatively grafting a 2–3 nm thick layer of 3,4-ethylenedioxythiophene (EDOT) moieties onto oligo(bisthienylbenzene) (BTB), we achieve a 0.4 eV upward shift in the HOMO level (from –5.4 to –5.0 eV vs a vacuum). This modest energy adjustment induces dramatic changes in device performance, namely, a ∼104-fold increase in conductance and a 102-fold reduction in rectification, while preserving the intrinsically weak scaling of transport with length and temperature. The resulting BTB-EDOT wires exhibit exceptionally efficient, activationless, long-range transport, characterized by a high extrapolated current density at zero thickness and a low decay constant. This behavior arises from near-resonant hole injection and intrachain multistep polaron tunneling, enabled by strong delocalization.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2555–2562"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923825","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}

引用次数: 0

Advances in the Preparation of Metal–Organic Framework-Derived Pyrolyzed Materials and Their Applications in Enzyme Immobilization 金属-有机骨架衍生热解材料的制备及其在酶固定化中的应用研究进展

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-07-25 DOI: 10.1021/acsmaterialslett.6c00395

Donghui Ji, Zeqing Liu, Lingmei Dai, Dehua Liu, Wei Du

{"title":"Advances in the Preparation of Metal–Organic Framework-Derived Pyrolyzed Materials and Their Applications in Enzyme Immobilization","authors":"Donghui Ji, Zeqing Liu, Lingmei Dai, Dehua Liu, Wei Du","doi":"10.1021/acsmaterialslett.6c00395","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00395","url":null,"abstract":"Metal–organic framework (MOF)-derived pyrolytic materials retain the pristine MOF advantages—high porosity and large surface area—while offering markedly improved stability, making them promising enzyme immobilization carriers. Their pore sizes can be rationally tuned via prepyrolysis modification, in situ activation, or postpyrolysis treatment, thereby enabling the tailored immobilization of bulky enzymes such as lipases. This review is the first to systematically address the use of pyrolyzed MOFs for enzyme immobilization, filling a gap in the literature. We compare derivatives from N-containing, O-containing, and N/O-containing ligands, revealing that N/O-type ligands excel in accommodating large enzymes. Pyrolysis mechanisms under inert, oxidative, reducing, and H2O atmospheres are summarized, linking each atmosphere to material properties. A dedicated section consolidates pore-enlargement strategies—a critical yet underexplored aspect. Finally, we demonstrate the potential of these materials to enhance enzyme stability, activity, and reusability in biocatalysis and biosensing, providing both a practical design guide and broader insights for catalysis, energy storage, and environmental applications.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2401–2416"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923957","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}

引用次数: 0

Beyond Light Harvesting: An Excited-State Perspective on Metal–Organic Framework Photocatalysis 超越光收获：金属-有机框架光催化的激发态视角

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-07-29 DOI: 10.1021/acsmaterialslett.6c00624

Bishnu Das

引用次数: 0

Multiscale Engineered Hydrogels for Adaptive Bioelectronic Interfaces 自适应生物电子界面的多尺度工程水凝胶

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-07-29 DOI: 10.1021/acsmaterialslett.6c00400

Xinyu Qu, Hanjun Sun, Yifan Li, Zhenhua Ni, Qian Wang, Xiaochen Dong

{"title":"Multiscale Engineered Hydrogels for Adaptive Bioelectronic Interfaces","authors":"Xinyu Qu, Hanjun Sun, Yifan Li, Zhenhua Ni, Qian Wang, Xiaochen Dong","doi":"10.1021/acsmaterialslett.6c00400","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00400","url":null,"abstract":"Bioelectronic technology propels medicine toward active perception and closed-loop therapeutic interventions. However, the fundamental mismatches in mechanics, electricity, and environment between rigid devices and soft tissues limit long-term interfacial stability and signal transduction efficiency. While hydrogels offer an ideal interface bridge owing to their biomimetic properties and excellent ion conductivity, traditional single-performance improvements often create functional contradictions, such as the trade-off between conductivity and flexibility, or adhesion and antifouling capability. The precise regulation of hydrogels through multiscale structural engineering transcends these constraints, shifting the leap of bioelectronic interfaces from passive bonding to active self-adaptation. Based on an in-depth analysis of interfacial charge transfer and wet-state adaptation mechanisms, we systematically review the multiscale design strategies for adaptive hydrogels across molecular networks, micro/nanocomposites, and macroscopic heterogeneous architectures. Finally, we evaluate their clinical transformation potential in high-fidelity electrophysiological monitoring and closed-loop therapies, outlining the future of next-generation adaptive bioelectronics.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2417–2437"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923960","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}

引用次数: 0

Origin of the Enhanced Lithium-Ion Conductivity in Lithium-Site Supervalent-Doped Li7La3Zr2O12 Revealed by Machine Learning Molecular Dynamics Simulations 机器学习分子动力学模拟揭示锂位超价掺杂Li7La3Zr2O12中锂离子电导率增强的原因

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-16 DOI: 10.1021/acsmaterialslett.6c00638

Yujie Chen, Ke R. Yang

{"title":"Origin of the Enhanced Lithium-Ion Conductivity in Lithium-Site Supervalent-Doped Li7La3Zr2O12 Revealed by Machine Learning Molecular Dynamics Simulations","authors":"Yujie Chen, Ke R. Yang","doi":"10.1021/acsmaterialslett.6c00638","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00638","url":null,"abstract":"Garnet-type Li7La3Zr2O12 (LLZO) is a promising solid electrolyte, but its highly conductive cubic phase is metastable at room temperature. We investigate lithium-ion migration mechanisms in LLZO using machine-learning molecular dynamics (MLMD), which achieves near-AIMD accuracy while enabling nanosecond-scale simulations at significantly reduced computational cost. Li-site supervalent doping (Fe, Ga, Al, B, and Zn) stabilizes the cubic phase by reducing the energy difference between tetragonal and cubic phases. In tetragonal LLZO, supervalent doping enhances Li-ion transport through vacancy-mediated hopping. In contrast, cubic LLZO possesses a disordered Li sublattice, making transport relatively insensitive to doping and susceptible to migration pathway disruption. Overall, Li-site supervalent doping improves conductivity by stabilizing the cubic phase and activating transport in tetragonal LLZO, rather than increasing intrinsic mobility in cubic LLZO. These results highlight MLMD as a powerful tool for probing ion transport and provide optimal doping strategies to introduce Li vacancies while preserving well-connected migration pathways.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2747–2755"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915841","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}

引用次数: 0

Closed‑Loop Recyclable Water‑Triggered Debond‑on‑Demand Polybenzoxazine Adhesives Enabled by Orthogonal Covalent Adaptable Networks 由正交共价自适应网络实现的闭环可回收水触发的按需脱粘聚苯并恶嗪粘合剂

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-02 DOI: 10.1021/acsmaterialslett.6c00489

Adebayo Isaac Olosho, Prashansa Gupta, Bimlesh Lochab

{"title":"Closed‑Loop Recyclable Water‑Triggered Debond‑on‑Demand Polybenzoxazine Adhesives Enabled by Orthogonal Covalent Adaptable Networks","authors":"Adebayo Isaac Olosho, Prashansa Gupta, Bimlesh Lochab","doi":"10.1021/acsmaterialslett.6c00489","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00489","url":null,"abstract":"Advanced manufacturing requires debond-on-demand (DoD) adhesives that combine strong service adhesion with facile end-of-life disassembly and closed-loop recyclability, yet high adhesion often compromises clean debonding. Herein, we report a mild, scalable, and sustainable route to a water-debondable covalent adaptable network (CAN) adhesive containing orthogonal imine/amine and silyl ether/silanol dynamic covalent linkages, prepared by copolymerizing vanillin-based silyl ether benzoxazine (VBZ) with branched polyethyleneimine (bP). Relative to an imine-deficient guaiacol-based control, the copolymer displays a high glass-transition temperature (70 °C), superior creep recovery, and a fourfold reduction in stress-relaxation activation energy (31 kJ·mol−1), highlighting the key role of imine-mediated bond-exchange kinetics. The adhesive exhibited high lap shear strength (∼8 MPa) and load-bearing capacity (∼100 kg), while complete water-triggered debonding (80 °C, 30 min) enabled clean substrate recovery and reuse. The reclaimed resin was recyclable and reprocessable and retained mechanical properties comparable to the pristine material.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2631–2639"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923731","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}

引用次数: 0

From Ionic Self-Assembly to Polyiodide Trapping: Nitrogen-Site-Rich Organic Single-Crystals for Charge-Transfer Iodine Capture 从离子自组装到多碘化物捕获：用于电荷转移碘捕获的富氮位点有机单晶

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-07-29 DOI: 10.1021/acsmaterialslett.6c00648

Jing He, Xin Li, Huifeng Liu, Shuang Zhang, Yunyun Zhang, Hongdeng Qiu, Jia Chen

{"title":"From Ionic Self-Assembly to Polyiodide Trapping: Nitrogen-Site-Rich Organic Single-Crystals for Charge-Transfer Iodine Capture","authors":"Jing He, Xin Li, Huifeng Liu, Shuang Zhang, Yunyun Zhang, Hongdeng Qiu, Jia Chen","doi":"10.1021/acsmaterialslett.6c00648","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00648","url":null,"abstract":"Radioactive iodine isotopes are volatile fission products with long half-lives, creating persistent risks during nuclear-waste management. Herein, a rational molecular design strategy was employed to assemble a multicarboxylated biphenyltetracarboxylate anion with nitrogen-site-rich cationic ligands. Here, hierarchical ionic self-assembly denotes a stepwise process in which oppositely charged molecular modules first form charge-balanced ion pairs and are subsequently organized through noncovalent packing/stacking into layered single-crystalline ionic frameworks; using this strategy, nitrogen-site-rich ionic organic single-crystals (N-IOCs) were constructed. The developed N-IOCs exhibit exceptional iodine adsorption performance in both vapor and solution phases, reaching 5.16 g/g from vapor and 1079 mg/g from cyclohexane. They also show rapid adsorption kinetics, good moisture resistance, high retention efficiency, and reusability. The highest iodine-capture performance is likely associated with the ordered nitrogen-rich framework environment, in which imidazole-containing sites provide favorable electronic features for host-iodine charge-transfer interactions.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2756–2764"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923961","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}

引用次数: 0

Hydrogels for Sustainable Agriculture: Toward Adaptive Rhizosphere Interfaces 可持续农业的水凝胶：迈向适应性根际界面

IF 8.6 1区化学

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-19 DOI: 10.1021/acsmaterialslett.6c00487

Jungjoon Park, Weixin Guan, Guihua Yu

{"title":"Hydrogels for Sustainable Agriculture: Toward Adaptive Rhizosphere Interfaces","authors":"Jungjoon Park, Weixin Guan, Guihua Yu","doi":"10.1021/acsmaterialslett.6c00487","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00487","url":null,"abstract":"Future sustainable agriculture requires root-zone systems that conserve water, retain nutrients, support beneficial microbes, withstand drought and salinity, and degrade safely in soil. Hydrogels are a promising material platform because their hydrated polymer networks can be tuned in chemistry, mechanics, transport, architecture, and degradation. This viewpoint frames agricultural hydrogels as adaptive rhizosphere interfaces, with exchange at the root-soil interface as the central design target. We organize this opportunity around three directions: water resilience, nutrient efficiency, and biotic integration. Water resilience demands root-zone moisture regulation under soil confinement, salinity, and wet−dry cycling. Nutrient efficiency requires reversible ion retention and synchronized release under plant demand. Biotic integration requires hydrated, permeable, and biodegradable microhabitats that support plant−microbe interactions. We argue that hydrogel design must move beyond swelling capacity and release curves toward the field materials engineering, including soil-confined testing, multifunctional trade-offs, scalable forms, and safe end-of-life behavior for practical climate-resilient and resource-efficient agriculture.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2514–2518"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915746","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}

引用次数: 0