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Potassium-Ion Conducting Amorphous-Based Chlorides KTaCl6 Prepared via Mechanochemistry 机械化学法制备钾离子导电非晶基氯化物KTaCl6
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-07 DOI: 10.1021/acsmaterialslett.6c00441
Kota Motohashi, Hamdi Ben Yahia, Takehiro Nakao, Hiroshi Nakajima, Shigeo Mori, Atsushi Sakuda, Akitoshi Hayashi
{"title":"Potassium-Ion Conducting Amorphous-Based Chlorides KTaCl6 Prepared via Mechanochemistry","authors":"Kota Motohashi,&nbsp;Hamdi Ben Yahia,&nbsp;Takehiro Nakao,&nbsp;Hiroshi Nakajima,&nbsp;Shigeo Mori,&nbsp;Atsushi Sakuda,&nbsp;Akitoshi Hayashi","doi":"10.1021/acsmaterialslett.6c00441","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00441","url":null,"abstract":"<p>All-solid-state potassium batteries have attracted considerable attention as energy storage devices. The development of suitable ionic conductors has received significant attention for the commercialization of the batteries. Here, we report the potassium-ion conductors KTaCl<sub>6</sub> prepared using the mechanochemical method and then heat treatment. The mechanochemically prepared sample comprises the monoclinic crystalline phase embedded within the amorphous component, as revealed by X-ray diffraction and transmission electron microscopy. The mechanochemically prepared sample exhibits an ionic conductivity of 1.8 × 10<sup>−5</sup> S cm<sup>−1</sup> at 30 °C. Upon heat treatment, the sample undergoes crystallization, leading to a decrease in ionic conductivity. It is suggested that the amorphous phase plays a key role in the ion conduction of the KTaCl<sub>6</sub> chlorides.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2580–2585"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915761","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
Perylenediimide Halogen Substitution-Modulated Photochromism and Photocatalytic Activity in Metal−Organic Frameworks 金属-有机骨架中卤素取代调制的光致变色和光催化活性
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-17 DOI: 10.1021/acsmaterialslett.6c00686
Qiuting Yang, Boqin Zi, Xianfu Shen, Yuxiang Zhao, Jian-Jun Liu
{"title":"Perylenediimide Halogen Substitution-Modulated Photochromism and Photocatalytic Activity in Metal−Organic Frameworks","authors":"Qiuting Yang,&nbsp;Boqin Zi,&nbsp;Xianfu Shen,&nbsp;Yuxiang Zhao,&nbsp;Jian-Jun Liu","doi":"10.1021/acsmaterialslett.6c00686","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00686","url":null,"abstract":"<p>Perylenediimides (PDIs), which feature strong visible-light absorption, π-electron-deficient planes, and photochemical characteristics, offer a versatile platform for developing tunable and efficient metal−organic framework (MOF) materials through modulation of their bay-substituent groups. Herein, we report ‌two structurally modified MOFs, MOF-Cl<sub>4</sub> and MOF-Br<sub>2</sub>, whose PDI components feature different halogen substitution patterns in their bay regions, imparting differential halogen-controlled photochromism. Notably, MOF-Cl<sub>4</sub> exhibited high photosensitivity, whereas MOF-Br<sub>2</sub> was found to be almost photochemically inert. Furthermore, both MOFs could be readily photoexcited to generate their respective excited states or radical anions. Interestingly, experimental and theoretical calculations revealed that these excited states or radical anions demonstrated halogen-controlled photocatalytic activities in the oxysulfonylation of alkynes and the aerobic oxidation of enamines. The photocatalytic performance of MOF-Cl<sub>4</sub> proved superior to that of MOF-Br<sub>2</sub>, a difference primarily attributed to the divergent SOMO-1 and optical bandgap of the PDI ligands and MOF materials, induced by the halogen substitution patterns.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2774–2782"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915838","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
Suppressing Reverse Processes in the Perylene Diimide/Strontium Titanate Z-Scheme Heterojunction for Efficient Photocatalytic Overall Water Splitting 抑制聚苝酰二亚胺/钛酸锶z型异质结中逆向过程的高效光催化全水分解
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-20 DOI: 10.1021/acsmaterialslett.6c00509
Xuan Yang, Hang Xu, Yang Guo, Peiyan Chen, Daming Zhao, Zhaohui Tang, Minghao Wang, Liejin Guo
{"title":"Suppressing Reverse Processes in the Perylene Diimide/Strontium Titanate Z-Scheme Heterojunction for Efficient Photocatalytic Overall Water Splitting","authors":"Xuan Yang,&nbsp;Hang Xu,&nbsp;Yang Guo,&nbsp;Peiyan Chen,&nbsp;Daming Zhao,&nbsp;Zhaohui Tang,&nbsp;Minghao Wang,&nbsp;Liejin Guo","doi":"10.1021/acsmaterialslett.6c00509","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00509","url":null,"abstract":"<p>Photocatalytic overall water splitting is promising for sustainable H<sub>2</sub> supply but is hindered by severe charge recombination and the reverse reaction. Herein, we design a novel organic/inorganic heterojunction by coupling π-conjugated perylene diimide polymer (PDIP) with aluminum-doped strontium titanate (SrTiO<sub>3</sub>:Al) to suppress these reverse processes for boosting photocatalytic H<sub>2</sub> evolution. In situ characterizations reveal a direct Z-scheme charge transfer pathway between PDIP and SrTiO<sub>3</sub>:Al, which promotes high‑energy charge carrier separation and suppresses the reverse reaction by spatially segregating the H<sub>2</sub> and O<sub>2</sub> evolution sites onto SrTiO<sub>3</sub>:Al and PDIP, respectively. Further, combined with selective co-catalyst engineering for preventing H<sub>2</sub> and O<sub>2</sub> from contacting on the catalyst surface, these reverse processes are fundamentally suppressed. Consequently, the PDIP/SrTiO<sub>3</sub>:Al heterojunction exhibits substantially enhanced photocatalytic activity for overall water splitting, achieving an H<sub>2</sub> evolution rate 11.8 times higher than that of pristine SrTiO<sub>3</sub>:Al. This dual-suppression strategy provides a validated blueprint for highly efficient solar-to-hydrogen conversion.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2647–2654"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915820","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
Nanoparticle Assembly Drives Magnetic Hyperthermia in Semi-Crystalline Polymers 纳米粒子组装驱动半结晶聚合物的磁热疗
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-27 DOI: 10.1021/acsmaterialslett.6c00501
Laura Ea, Florent Dalmas, Angelo Pommella, Joël Lachambre, Jérôme Adrien, William Chèvremont, Lise-Marie Lacroix, Gildas Coativy, Guilhem P. Baeza
{"title":"Nanoparticle Assembly Drives Magnetic Hyperthermia in Semi-Crystalline Polymers","authors":"Laura Ea,&nbsp;Florent Dalmas,&nbsp;Angelo Pommella,&nbsp;Joël Lachambre,&nbsp;Jérôme Adrien,&nbsp;William Chèvremont,&nbsp;Lise-Marie Lacroix,&nbsp;Gildas Coativy,&nbsp;Guilhem P. Baeza","doi":"10.1021/acsmaterialslett.6c00501","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00501","url":null,"abstract":"<p>We investigate how the assembly of magnetic nanoparticles embedded in a semi-crystalline polymer governs heat generation when submitted to a high-frequency alternating magnetic field by simultaneously monitoring temperature and structural anisotropy through infrared thermography and time-resolved ultra-small-angle X-ray scattering, respectively. A polypropylene matrix is used as a host system to disentangle intrinsic magnetic heating from structural contributions, thereby isolating the additional heat generated by dipolar chain formation above the polymer melting point during successive heating cycles. In contrast, reorienting the chain axis perpendicular to the applied field is found to significantly reduce heat generation. These in situ measurements are complemented by X-ray tomography and scanning electron microscopy experiments, providing a comprehensive view of the underlying mechanisms. Overall, this work establishes a direct relationship between nanoparticle organization and hyperthermia performance, opening new routes for the rational design of functional nanocomposites.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2640–2646"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915827","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
N-Heterocyclic Microenvironment Engineering in Imine Covalent Organic Frameworks: Toward Rational Tuning of Donor–Acceptor Architectures and Nonlinear Optical Performance 亚胺共价有机框架中的n -杂环微环境工程:面向供体-受体结构和非线性光学性能的合理调整
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-22 DOI: 10.1021/acsmaterialslett.6c00575
Mingyan Li, Tingting Li, Yongbing Hu, Jiahao Huang, Ran Yao, Endian Su, Xiangxiang Zhou, Jiahui Chu, Debo Ding, Yun-fang Yang, Jianhong Jia
{"title":"N-Heterocyclic Microenvironment Engineering in Imine Covalent Organic Frameworks: Toward Rational Tuning of Donor–Acceptor Architectures and Nonlinear Optical Performance","authors":"Mingyan Li,&nbsp;Tingting Li,&nbsp;Yongbing Hu,&nbsp;Jiahao Huang,&nbsp;Ran Yao,&nbsp;Endian Su,&nbsp;Xiangxiang Zhou,&nbsp;Jiahui Chu,&nbsp;Debo Ding,&nbsp;Yun-fang Yang,&nbsp;Jianhong Jia","doi":"10.1021/acsmaterialslett.6c00575","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00575","url":null,"abstract":"<p><em>N</em><strong>-</strong>heterocyclic microenvironment engineering is critical for modulating the electronic structure and nonlinear optical (NLO) responses of imine-linked covalent organic frameworks (COFs). Using 5′-(4-aminophenyl)–2′,4′,6′-trimethyl-[1,1′:3′,1″-terphenyl]-4,4″-diamine (ATTD), we synthesized three COFs (<strong>ACOF-1</strong>, <strong>ACOF-2</strong>, and <strong>ACOF-3</strong>) via polycondensation with aldehydes bearing N<sub>0</sub>, N<sub>1</sub>, and N<sub>3</sub> heterocycles, yielding nitrogen contents of 5.25, 6.24, and 8.91%, respectively. Systematic investigation shows that increasing <em>N</em>-content progressively narrows the optical bandgap and strengthens donor–acceptor charge transfer. Open-aperture Z-scan measurements reveal reversible reverse saturable absorption (RSA) to saturable absorption (SA) switching under varying pulse energies for all samples. Closed-aperture Z-scan indicates self-defocusing and RSA for <strong>ACOF-1</strong>, whereas <strong>ACOF-2</strong> and <strong>ACOF-3</strong> exhibit asymmetric twin-peak-valley curves, signifying third- and fifth-order nonlinear refractive contributions. Collectively, the <em>N</em>-heterocyclic microenvironment precisely tailors electronic distribution and charge-transfer dynamics, enabling deliberate NLO performance tuning. This work offers a rational guideline for designing high-performance COF-based NLO materials.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2694–2702"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923695","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
All-in-Waste-Derived Single-Atom Catalysts toward Ultra-Stable Zinc–Air Batteries 用于超稳定锌-空气电池的全废物衍生单原子催化剂
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-24 DOI: 10.1021/acsmaterialslett.6c00626
Xia Li, Hao Wang, Changqing Li, Hui-Min Yan, Jingze Shao, Chongxuan Liu, Shaoqing Chen, Jong-Beom Baek
{"title":"All-in-Waste-Derived Single-Atom Catalysts toward Ultra-Stable Zinc–Air Batteries","authors":"Xia Li,&nbsp;Hao Wang,&nbsp;Changqing Li,&nbsp;Hui-Min Yan,&nbsp;Jingze Shao,&nbsp;Chongxuan Liu,&nbsp;Shaoqing Chen,&nbsp;Jong-Beom Baek","doi":"10.1021/acsmaterialslett.6c00626","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00626","url":null,"abstract":"<p>Developing sustainable electrocatalysts from waste resources offers an attractive route toward clean energy storage and environmental remediation. Herein, an all-in-waste strategy is reported to upcycle sewage sludge and straw into single-atom catalysts for rechargeable zinc–air batteries. High-energy mechanical shearing coupled with self-atmosphere pyrolysis transforms the waste into hierarchical porous carbon hosting Fe<sub>1</sub>–N<sub>4</sub> active sites. The resulting sludge–straw-C catalyst achieves an oxygen reduction reaction kinetic current density of 4.5 mA cm<sup>–2</sup> at 0.75 V, outperforming single-precursor counterparts by 4.1 to 5.6 times. Furthermore, it reduces the oxygen evolution reaction overpotential at 10 mA cm<sup>–2</sup> to 390 mV, a decrease of 120–150 mV. Integrated into rechargeable zinc–air batteries, this catalyst delivers a peak power density of 160 mW cm<sup>–2</sup> and stable cycling over 800 hours. This work provides a scalable and reagent-free route for transforming environmental pollutants into value-added energy materials.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2739–2746"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923757","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
Deep Reinforcement Learning-Guided Design of Broadband Electromagnetic Wave Absorbing Coatings 宽带电磁波吸收涂层的深度强化学习引导设计
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-07 DOI: 10.1021/acsmaterialslett.6c00473
Sirui Fan, Da Wan, Qi Zou, Hongfeng Li, Wenting He, Zhen Li, Yu Liu, Peng Kang, Lei Zheng, Hong-Bo Guo, Huibin Xu
{"title":"Deep Reinforcement Learning-Guided Design of Broadband Electromagnetic Wave Absorbing Coatings","authors":"Sirui Fan,&nbsp;Da Wan,&nbsp;Qi Zou,&nbsp;Hongfeng Li,&nbsp;Wenting He,&nbsp;Zhen Li,&nbsp;Yu Liu,&nbsp;Peng Kang,&nbsp;Lei Zheng,&nbsp;Hong-Bo Guo,&nbsp;Huibin Xu","doi":"10.1021/acsmaterialslett.6c00473","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00473","url":null,"abstract":"<p>Artificial intelligence-assisted design of electromagnetic wave absorbing coatings is often restricted to geometry or topology optimization within fixed materials. Here, we present a modular particle swarm optimization−proximal policy optimization (PSO−PPO) framework for radar-absorbing metastructures that combines a progressive feature fusion surrogate for 8−18 GHz reflection-loss prediction, a ResNet-based empirical filter for low-performance patterns, and reinforcement learning optimization in a mixed discrete-continuous design space. For broadband single-layer optimization, the framework identifies a generated-material M2/Pt metasurface absorber with a 1.30 mm thickness and a CST-validated effective bandwidth of 6.32 GHz, with field simulations indicating absorption from multiple localized resonances and dielectric loss. The same strategy is extended to multilayer inverse design for prescribed single-peak Gaussian spectra, yielding target responses at 10, 12, and 16 GHz with mean absolute errors (MAEs) of 1.64−2.19 dB. This work demonstrates an efficient route for automated absorber optimization and customized spectral regulation.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 9","pages":"2595–2602"},"PeriodicalIF":8.6,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923834","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
Bamboo-Derived Transparent Room-Temperature Phosphorescent Film 竹制室温透明磷光膜
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-07-06 DOI: 10.1021/acsmaterialslett.6c00526
Zijing Pan, Kai Wang, Yujie Bai, Yingxiang Zhai, Min Wang, Min Ge, Xue Liu, Zhijun Chen, Shujun Li
{"title":"Bamboo-Derived Transparent Room-Temperature Phosphorescent Film","authors":"Zijing Pan,&nbsp;Kai Wang,&nbsp;Yujie Bai,&nbsp;Yingxiang Zhai,&nbsp;Min Wang,&nbsp;Min Ge,&nbsp;Xue Liu,&nbsp;Zhijun Chen,&nbsp;Shujun Li","doi":"10.1021/acsmaterialslett.6c00526","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00526","url":null,"abstract":"<p>Fabricating sustainable room‑temperature phosphorescent (RTP) films without relying on intrinsic chromophores constitutes a fundamental objective, yet it remains an enduring challenge. Here, we present an efficient “top‑down” strategy that directly converts natural bamboo into RTP films. Furthermore, delignification was performed on natural bamboo to extract lignin constituents in the first step. After that, the treated bamboo was subjected to carboxymethylation and subsequently dissolved to form a transparent RTP film (B-film). The as-prepared B-film exhibited blue fluorescence and green phosphorescence, with an RTP lifetime reaching 547.77 ms. Moreover, this film possessed favorable processability and could efficiently transfer energy to Rhodamine B (RhB). As a result, a variety of multifunctional afterglow materials were fabricated by employing the B-film. Simultaneously, the luminescent film underwent rapid and complete biodegradation in soil within 15 days. This work is anticipated to provide a convenient strategy for producing sustainable RTP films from biomass resources.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2364–2372"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148666325","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
Interfacially Integrated DNAzyme-Hydrogel Architectures for Eradicating Postoperative Breast Cancer Residual Disease via Tumor-Anchored Pyroptotic Antigen Amplification 界面集成dnazyme -水凝胶结构通过肿瘤锚定的焦噬抗原扩增根除术后乳腺癌残留疾病
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-06-26 DOI: 10.1021/acsmaterialslett.6c00403
Huan He, Yuxin Jin, Shuang Jin, Yunyun Wu, Lin Li, Hongrui Zhu, Jixi Zhang
{"title":"Interfacially Integrated DNAzyme-Hydrogel Architectures for Eradicating Postoperative Breast Cancer Residual Disease via Tumor-Anchored Pyroptotic Antigen Amplification","authors":"Huan He,&nbsp;Yuxin Jin,&nbsp;Shuang Jin,&nbsp;Yunyun Wu,&nbsp;Lin Li,&nbsp;Hongrui Zhu,&nbsp;Jixi Zhang","doi":"10.1021/acsmaterialslett.6c00403","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00403","url":null,"abstract":"<p>Postoperative residual disease and insufficient antigenicity after surgical resection are major causes of breast cancer recurrence and metastasis. Pyroptosis enhances antitumor immunity by releasing intracellular antigens but is limited by tight intracellular Ca<sup>2+</sup> homeostasis and short reactive oxygen species (ROS) lifespan. This study develops a membrane-confined pyroptotic catalytic platform coupling ROS generation with TRP channel-gated Ca<sup>2+</sup> influx to induce pyroptosis and amplify antigenic stimulation in postoperative residual disease. The system comprises a bifunctional DNAzyme (GH) and a CaO<sub>2</sub>-loaded calcium alginate hydrogel (CaO<sub>2</sub>-SA). Preoperatively, GH anchors to tumor membranes via nucleolin recognition; postoperatively, CaO<sub>2</sub>-SA provides sustained H<sub>2</sub>O<sub>2</sub> and Ca<sup>2+</sup> at the resection site. Membrane-localized GH catalyzes H<sub>2</sub>O<sub>2</sub> into hydroxyl radicals to oxidatively damage membranes, activate oxidant-sensitive TRP channels, and drive sustained Ca<sup>2+</sup> influx. This triggers mitochondrial Ca<sup>2+</sup> overload and Caspase-3/GSDME pathway activation, inducing potent pyroptosis. The resultant damage-associated molecular patterns amplify antigenicity, addressing insufficient postoperative immunogenicity in breast cancer.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2264–2273"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148672545","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
Brittle-to-Ductile Transition Temperature Decreases at the Microscale in Muscovite Mica 微尺度下白云母脆性向韧性转变温度降低
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-06-24 DOI: 10.1021/acsmaterialslett.6c00303
Frank W. DelRio, Eric D. Hintsala, Benjamin T. Dankesreiter, Scott J. Grutzik, William M. Mook, Paul G. Kotula, Hasini S. Senanayake, Jeffery A. Greathouse, Anastasia G. Ilgen
{"title":"Brittle-to-Ductile Transition Temperature Decreases at the Microscale in Muscovite Mica","authors":"Frank W. DelRio,&nbsp;Eric D. Hintsala,&nbsp;Benjamin T. Dankesreiter,&nbsp;Scott J. Grutzik,&nbsp;William M. Mook,&nbsp;Paul G. Kotula,&nbsp;Hasini S. Senanayake,&nbsp;Jeffery A. Greathouse,&nbsp;Anastasia G. Ilgen","doi":"10.1021/acsmaterialslett.6c00303","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00303","url":null,"abstract":"<p>Characterizing the structural and chemical transitions of muscovite mica across various scales and thermal profiles is essential for ensuring the reliability of high-voltage power insulation, aerospace thermal barriers, and nanoscale semiconductor substrates under extreme operational stress. Here, we investigate notch fracture toughness <span><span></span><math><msubsup><mi>K</mi><mi>Ic</mi><mi>n</mi></msubsup></math></span> of muscovite mica as a function of feature size <em>w</em> and temperature <em>T</em> with microscale shear testing. <span><span></span><math><msubsup><mi>K</mi><mi>Ic</mi><mi>n</mi></msubsup></math></span> decreased and then stayed constant as <em>w</em> increased, likely from fabrication-induced changes to the microstructure and roughness. Moreover, <span><span></span><math><msubsup><mi>K</mi><mi>Ic</mi><mi>n</mi></msubsup></math></span> initially decreased and then increased as temperature <em>T</em> increased, with the reversal in trend indicative of a brittle-to-ductile transition. Complementary Raman spectroscopy and molecular dynamics showed that the observed trends were due to an increase in bond lengths and a decrease in critical stresses/strains. In comparing the microscale results to macroscale counterparts, it was surmised that the decrease in brittle-to-ductile transition temperature was due to an increase in the dehydroxylation rate.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2178–2185"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148656308","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
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