Electrochromic smart windows demand high optical contrast, fast switching, long-term durability, and charge-storage functionality, yet hydrated tungsten oxides suffer from restricted ion transport and structural degradation during repeated ion insertion/extraction. Here, we present a carbon nitride-driven phase transformation strategy for a durable energy-storing electrochromic hydrated tungsten oxide. Under mild hydrogen annealing, orthorhombic WO3·H2O nanoplates containing an optimized 10 wt % carbon nitride (CNx) selectively transform into predominantly hexagonal WO3·0.33H2O nanorods (∼80%), accompanied by a relatively minor orthorhombic fraction (∼20%). The CNx promotes structural rearrangement while providing nitrogen-rich Li+-interactive sites that regulate interfacial ion transport and improve electrochemical reversibility. Supported by density functional theory, impedance, diffusion, and postcycling analyses, the optimized WHX-CNx10% film shows favorable Li+ insertion, improved charge-transfer kinetics, and excellent structural retention. The air spray-coated film in 3-electrode system delivers 57% optical modulation at 650 nm, coloration/bleaching times of 2.9/0.6 s, stable cycling over 20,000 cycles, and an areal capacitance of 16.9 mF/cm2. A 5 × 5 cm2 device further exhibits optical modulation of 52% at 650 nm with a coloration efficiency of ∼156 cm2/C. These results establish CNx-mediated phase and interface engineering as an effective route toward scalable, durable, and energy-storing electrochromic smart windows.
{"title":"Interface Engineering of Hydrated Tungsten Oxide via Carbon Nitride for Durable Electrochromic Energy Storage","authors":"Himanshu Nath,Alok Kumar,Nikhil Singh,Lavanya Singh Malik,Dibyajyoti Ghosh,Ritu Gupta","doi":"10.1021/acsami.6c15458","DOIUrl":"https://doi.org/10.1021/acsami.6c15458","url":null,"abstract":"Electrochromic smart windows demand high optical contrast, fast switching, long-term durability, and charge-storage functionality, yet hydrated tungsten oxides suffer from restricted ion transport and structural degradation during repeated ion insertion/extraction. Here, we present a carbon nitride-driven phase transformation strategy for a durable energy-storing electrochromic hydrated tungsten oxide. Under mild hydrogen annealing, orthorhombic WO3·H2O nanoplates containing an optimized 10 wt % carbon nitride (CNx) selectively transform into predominantly hexagonal WO3·0.33H2O nanorods (∼80%), accompanied by a relatively minor orthorhombic fraction (∼20%). The CNx promotes structural rearrangement while providing nitrogen-rich Li+-interactive sites that regulate interfacial ion transport and improve electrochemical reversibility. Supported by density functional theory, impedance, diffusion, and postcycling analyses, the optimized WHX-CNx10% film shows favorable Li+ insertion, improved charge-transfer kinetics, and excellent structural retention. The air spray-coated film in 3-electrode system delivers 57% optical modulation at 650 nm, coloration/bleaching times of 2.9/0.6 s, stable cycling over 20,000 cycles, and an areal capacitance of 16.9 mF/cm2. A 5 × 5 cm2 device further exhibits optical modulation of 52% at 650 nm with a coloration efficiency of ∼156 cm2/C. These results establish CNx-mediated phase and interface engineering as an effective route toward scalable, durable, and energy-storing electrochromic smart windows.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"33 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221614","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Spatial proteomics of laser capture microdissection (LCM) specimens is fundamentally constrained by protein loss during processing of ultra-trace samples, limiting proteomic depth and biological insight. Here, we report the integration of a quadruple metal–organic framework (qMOF)-enhanced surfactant-assisted one-pot sample preparation (MSOP) workflow for deep proteomic profiling of micro-scale tissues. The qMOF composite, featuring high-density boronic acid functionalities, acts as a potent protein capture vehicle, drastically minimizing surface adsorption losses. Applied to LCM-isolated mouse myocardial sections as small as 100 × 100 μm (∼20 cells), the MSOP workflow approximately doubled the number of confidently identified proteins, compared to the conventional surfactant-assisted one-pot sample preparation (SOP) method (mean of 2238 vs. 1116), while exhibiting lower quantification variance and preserving unbiased coverage of the proteome’s physicochemical landscape. We further demonstrate the workflow's utility by resolving spatially distinct proteomic signatures in perivascular regions of aged cardiac tissue, identifying molecular hallmarks of aging characterized by impaired cytoskeletal stability and dysregulated mitochondrial functions. Protein–protein interaction network analysis identified Rack1 as a potential key node in cardiac aging, which was further validated by immunohistochemistry. This MSOP-assisted platform provides a robust, cost-effective, and highly sensitive chemical strategy to significantly enhance the depth of discovery-driven spatial proteomics.
激光捕获显微解剖（LCM）样品的空间蛋白质组学从根本上受到超痕量样品处理过程中蛋白质损失的限制，限制了蛋白质组学的深度和生物学洞察力。在这里，我们报道了四金属有机框架（qMOF）增强表面活性剂辅助的一锅样品制备（MSOP）工作流程的集成，用于微尺度组织的深层蛋白质组学分析。qMOF复合材料具有高密度硼酸功能，作为一种有效的蛋白质捕获载体，极大地减少了表面吸附损失。应用于lcm分离的小至100 × 100 μm（~ 20个细胞）的小鼠心肌切片，与传统的表面活性剂辅助的一锅样品制备（SOP）方法（平均2238 vs 1116）相比，MSOP工作流程大约使确定的蛋白质数量增加了一倍，同时表现出更低的定量方差并保持对蛋白质组物理化学环境的无偏覆盖。我们通过解析衰老心脏组织血管周围区域空间上不同的蛋白质组学特征，确定以细胞骨架稳定性受损和线粒体功能失调为特征的衰老分子标志，进一步证明了该工作流程的实用性。蛋白-蛋白相互作用网络分析发现Rack1是心脏衰老的潜在关键节点，并通过免疫组织化学进一步验证。这个msop辅助平台提供了一个强大的、经济高效的、高度敏感的化学策略，显著提高了发现驱动的空间蛋白质组学的深度。
{"title":"Quadruple Boronic Acid-Functionalized Lanthanide MOFs Enable Deep and Unbiased Spatial Proteomics from Ultra-Trace Laser-Captured Microtissues","authors":"Yuankang Zhu,Jiahui Wu,Qi Luo,Shuang Zhang,Qingwen Wang,Lai Jiang,Junli Duan,Alex F. Chen,Xianting Ding","doi":"10.1021/acsami.6c12158","DOIUrl":"https://doi.org/10.1021/acsami.6c12158","url":null,"abstract":"Spatial proteomics of laser capture microdissection (LCM) specimens is fundamentally constrained by protein loss during processing of ultra-trace samples, limiting proteomic depth and biological insight. Here, we report the integration of a quadruple metal–organic framework (qMOF)-enhanced surfactant-assisted one-pot sample preparation (MSOP) workflow for deep proteomic profiling of micro-scale tissues. The qMOF composite, featuring high-density boronic acid functionalities, acts as a potent protein capture vehicle, drastically minimizing surface adsorption losses. Applied to LCM-isolated mouse myocardial sections as small as 100 × 100 μm (∼20 cells), the MSOP workflow approximately doubled the number of confidently identified proteins, compared to the conventional surfactant-assisted one-pot sample preparation (SOP) method (mean of 2238 vs. 1116), while exhibiting lower quantification variance and preserving unbiased coverage of the proteome’s physicochemical landscape. We further demonstrate the workflow's utility by resolving spatially distinct proteomic signatures in perivascular regions of aged cardiac tissue, identifying molecular hallmarks of aging characterized by impaired cytoskeletal stability and dysregulated mitochondrial functions. Protein–protein interaction network analysis identified Rack1 as a potential key node in cardiac aging, which was further validated by immunohistochemistry. This MSOP-assisted platform provides a robust, cost-effective, and highly sensitive chemical strategy to significantly enhance the depth of discovery-driven spatial proteomics.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"29 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218688","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kexin Ma,Lijun Wang,Jie Xu,Tianqi Wang,Yang Liu,Yanyan Liu,Liping Zhou,Zhong Jin,Lin Sun
Intrinsic low conductivity and huge volume expansion severely limit the cycling stability of SiOx anodes. Herein, a 3D crosslinked CNT/SiOx-F@C composite is synthesized via bifunctional fluorosilane crosslinkers and conformal pitch carbon coating. Fluorosilane acts as both a silicon source and a crosslinker to build interconnected, conductive CNT frameworks, while the outer pitch carbon optimizes the pore structure and induces flexible, LixPOyF6-rich SEI layers. Kinetic tests reveal dominant capacitive charge storage and a Li+ diffusion coefficient one-order-of-magnitude higher than that of control electrodes. The half-cell delivers a stable reversible capacity of 672.6 mA h g–1 over 200 cycles at 0.2 A g–1 and retains 86.5% capacity after 600 cycles at 1 A g–1. Pre-lithiation elevates the initial Coulombic efficiency from 47.4 to 84.2%, while the electrode achieves an areal capacity approaching 4 mA h cm–2, far exceeding that of commercial graphite. This dual-carbon synergistic strategy provides a facile route to optimizing silicon oxide anodes.
固有的低电导率和巨大的体积膨胀严重限制了SiOx阳极的循环稳定性。本文通过双功能氟硅烷交联剂和共形沥青碳涂层合成了三维交联CNT/SiOx-F@C复合材料。氟硅烷作为硅源和交联剂构建相互连接的导电碳纳米管框架，而外间距碳优化孔隙结构并诱导柔性的富含lixpoyf6的SEI层。动力学测试表明，电容电荷存储占主导地位，Li+扩散系数比控制电极高一个数量级。这种半电池在0.2 a g-1下循环200次，可提供672.6 mA h g-1的稳定可逆容量，在1 a g-1下循环600次后仍保持86.5%的容量。预锂化将初始库仑效率从47.4提高到84.2%，而电极的面容量接近4 mA h cm-2，远远超过了商用石墨。这种双碳协同策略为优化氧化硅阳极提供了一条简便的途径。
{"title":"Three-Dimensional Crosslinked CNT/SiOx-F Network Encapsulated by Pitch-Derived Carbon as a High-Stable Anode for Lithium-Ion Batteries","authors":"Kexin Ma,Lijun Wang,Jie Xu,Tianqi Wang,Yang Liu,Yanyan Liu,Liping Zhou,Zhong Jin,Lin Sun","doi":"10.1021/acsami.6c14348","DOIUrl":"https://doi.org/10.1021/acsami.6c14348","url":null,"abstract":"Intrinsic low conductivity and huge volume expansion severely limit the cycling stability of SiOx anodes. Herein, a 3D crosslinked CNT/SiOx-F@C composite is synthesized via bifunctional fluorosilane crosslinkers and conformal pitch carbon coating. Fluorosilane acts as both a silicon source and a crosslinker to build interconnected, conductive CNT frameworks, while the outer pitch carbon optimizes the pore structure and induces flexible, LixPOyF6-rich SEI layers. Kinetic tests reveal dominant capacitive charge storage and a Li+ diffusion coefficient one-order-of-magnitude higher than that of control electrodes. The half-cell delivers a stable reversible capacity of 672.6 mA h g–1 over 200 cycles at 0.2 A g–1 and retains 86.5% capacity after 600 cycles at 1 A g–1. Pre-lithiation elevates the initial Coulombic efficiency from 47.4 to 84.2%, while the electrode achieves an areal capacity approaching 4 mA h cm–2, far exceeding that of commercial graphite. This dual-carbon synergistic strategy provides a facile route to optimizing silicon oxide anodes.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"253 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218691","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The introduction of an appropriate passivation layer is considered a viable strategy for improving the long-term stability and electrical performance of thin-film transistors (TFTs). In this study, an additional layer deposition strategy involving the deposition of a single-layer oxygen-related defect control layer on amorphous indium zinc oxide (a-IZO) thin-film transistors is developed. This approach improves the electrical characteristics and negative-bias illumination stress (NBIS) stability of the channel layer. The oxygen-related defect control layer is a hafnium oxynitride (HfON) layer. It functions as an insulating material with a relatively high dielectric constant, high film density, and low surface energy, serving as a protective barrier against environmental degradation such as exposure to ambient air and moisture. In addition, it contributes to the improvement of NBIS-induced stability by passivating the defect sites in a-IZO during the activation annealing process. Furthermore, the number of carriers in the channel layer increased because of the formation of oxygen vacancies in the a-IZO front channel through the oxygen adsorption of the oxygen-related defect control layer, resulting in the fabrication of thin films with better electrical properties. This resulted in field-effect mobility improving from 37.53 to 66.43 cm2/(V s), the on/off current ratio was enhanced from 1.93 × 109 to 5.77 × 1011, and the threshold voltage shift under NBIS at green light (532 nm) flux density of 1 mW/cm2 for 10,000 s decreased from 15.25 to 2.64 V.
{"title":"High-Mobility a-InZnO Thin-Film Transistors Incorporating an Oxygen-Related Defect Control Layer for Improved Illumination Stability and Environmental Reliability","authors":"Jihoon Han,Dong Keun Lee,Shilin Lu,Hyun Jae Kim","doi":"10.1021/acsami.6c17895","DOIUrl":"https://doi.org/10.1021/acsami.6c17895","url":null,"abstract":"The introduction of an appropriate passivation layer is considered a viable strategy for improving the long-term stability and electrical performance of thin-film transistors (TFTs). In this study, an additional layer deposition strategy involving the deposition of a single-layer oxygen-related defect control layer on amorphous indium zinc oxide (a-IZO) thin-film transistors is developed. This approach improves the electrical characteristics and negative-bias illumination stress (NBIS) stability of the channel layer. The oxygen-related defect control layer is a hafnium oxynitride (HfON) layer. It functions as an insulating material with a relatively high dielectric constant, high film density, and low surface energy, serving as a protective barrier against environmental degradation such as exposure to ambient air and moisture. In addition, it contributes to the improvement of NBIS-induced stability by passivating the defect sites in a-IZO during the activation annealing process. Furthermore, the number of carriers in the channel layer increased because of the formation of oxygen vacancies in the a-IZO front channel through the oxygen adsorption of the oxygen-related defect control layer, resulting in the fabrication of thin films with better electrical properties. This resulted in field-effect mobility improving from 37.53 to 66.43 cm2/(V s), the on/off current ratio was enhanced from 1.93 × 109 to 5.77 × 1011, and the threshold voltage shift under NBIS at green light (532 nm) flux density of 1 mW/cm2 for 10,000 s decreased from 15.25 to 2.64 V.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"56 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218680","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Triple-negative breast cancer (TNBC) is characterized by a highly immunosuppressive tumor microenvironment, which severely limits the therapeutic efficacy of current immunotherapies. To address this challenge, we developed a hyaluronic acid-modified tumor-targeted MnO2 nanoreactor (HMGR@HA) for the codelivery of GOx and 20(S)-ginsenoside Rg3 (Rg3), thereby integrating metabolic interference with cascade catalytic therapy and endogenous immune activation. In this system, GOx continuously catalyzed the oxidation of glucose to generate H2O2, which was subsequently converted by MnO2 into highly cytotoxic reactive oxygen species (ROS) while simultaneously producing oxygen. This process established a self-reinforcing catalytic cycle that effectively circumvented the intrinsic limitation of insufficient endogenous H2O2 within the tumor microenvironment. The resulting amplified oxidative stress, in synergy with the chemotherapeutic effect of Rg3, induced profound mitochondrial dysfunction and triggered the cytosolic release of mtDNA. As a potent endogenous danger signal, cytosolic mtDNA robustly activated the cGAS-STING signaling axis, thereby converting localized oxidative damage into strong innate immune activation. In addition, HMGR@HA induced immunogenic cell death (ICD), promoted dendritic cells (DCs) maturation, enhanced infiltration of CD4+ and CD8+ effector T cells, and significantly depleted regulatory T cells (Tregs), collectively leading to extensive remodeling of the tumor immune microenvironment. Ultimately, this self-amplifying catalytic platform effectively drives the transition from localized tumor eradication to systemic antitumor immunity, offering a highly efficient therapeutic strategy for TNBC immunotherapy.
{"title":"Cascade-Catalytic MnO2 Nanoreactor Amplifies Oxidative Stress and Activates cGAS–STING Pathway To Remodel the Immunosuppressive Microenvironment of Triple-Negative Breast Cancer","authors":"Shiman Li,Shuchang Yao,Jingwen Yang,Wenqi Wang,Wenjing Li,Xinzhu Wang,Ke Zhang,Sha Xie,Xiaoyu Peng,Jian Ni,Xiaoxv Dong","doi":"10.1021/acsami.6c15680","DOIUrl":"https://doi.org/10.1021/acsami.6c15680","url":null,"abstract":"Triple-negative breast cancer (TNBC) is characterized by a highly immunosuppressive tumor microenvironment, which severely limits the therapeutic efficacy of current immunotherapies. To address this challenge, we developed a hyaluronic acid-modified tumor-targeted MnO2 nanoreactor (HMGR@HA) for the codelivery of GOx and 20(S)-ginsenoside Rg3 (Rg3), thereby integrating metabolic interference with cascade catalytic therapy and endogenous immune activation. In this system, GOx continuously catalyzed the oxidation of glucose to generate H2O2, which was subsequently converted by MnO2 into highly cytotoxic reactive oxygen species (ROS) while simultaneously producing oxygen. This process established a self-reinforcing catalytic cycle that effectively circumvented the intrinsic limitation of insufficient endogenous H2O2 within the tumor microenvironment. The resulting amplified oxidative stress, in synergy with the chemotherapeutic effect of Rg3, induced profound mitochondrial dysfunction and triggered the cytosolic release of mtDNA. As a potent endogenous danger signal, cytosolic mtDNA robustly activated the cGAS-STING signaling axis, thereby converting localized oxidative damage into strong innate immune activation. In addition, HMGR@HA induced immunogenic cell death (ICD), promoted dendritic cells (DCs) maturation, enhanced infiltration of CD4+ and CD8+ effector T cells, and significantly depleted regulatory T cells (Tregs), collectively leading to extensive remodeling of the tumor immune microenvironment. Ultimately, this self-amplifying catalytic platform effectively drives the transition from localized tumor eradication to systemic antitumor immunity, offering a highly efficient therapeutic strategy for TNBC immunotherapy.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"7 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218686","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aleksandra Pająk,Pavel Pleskunov,Oleg Zabeida,Bill Baloukas,Jolanta Klemberg-Sapieha,Ludvik Martinu
The demand for transparent flexible electrodes (TFEs) with superior simultaneous optical, electrical, and mechanical performance beyond indium tin oxide (ITO) has driven the development of various nanostructured architectures. Metal-based patterned surfaces have become strong contenders in the TFEs field due to their significantly higher mechanical flexibility; however, their current use is, in part, limited by their scattering-induced visibility to the naked eye. Herein, we report polymeric web-assisted two-dimensional nanostructures, fabricated via electrospinning and integrated with gas-phase deposition methods such as magnetron sputtering, yielding thin film nanopatterning with ultra-high luminous transmittance (Tlum) of 98.1% and sheet resistance (Rs) of 17 Ω □–1. The addition of an antireflective coating enhances the Tlum to 99.7%. The designed trilayer, highly absorbing Fabry–Perot stack (Ag/ITO/NiCr) sputtered on patterned nanolines (NLs) leads to backward scattering suppression, rendering them significantly less visible than the “uncloaked” Ag-only NLs. Our findings are confirmed by finite-difference time-domain (FDTD) simulations. These high-performing, near-invisible electrodes allow for adjustable conductivity through thickness control without compromising transparency, while maintaining mechanical robustness under bending. They are also compatible with polymeric substrates, requiring only room-temperature polymer template dissolution, eliminating the need for high-temperature annealing and representing a promising route toward next-generation optoelectronic applications, including displays, photovoltaics, and wearable electronics.
{"title":"Invisible Patterned Silver-Based Transparent Electrodes via Control of Light Scattering and Absorption","authors":"Aleksandra Pająk,Pavel Pleskunov,Oleg Zabeida,Bill Baloukas,Jolanta Klemberg-Sapieha,Ludvik Martinu","doi":"10.1021/acsami.6c09340","DOIUrl":"https://doi.org/10.1021/acsami.6c09340","url":null,"abstract":"The demand for transparent flexible electrodes (TFEs) with superior simultaneous optical, electrical, and mechanical performance beyond indium tin oxide (ITO) has driven the development of various nanostructured architectures. Metal-based patterned surfaces have become strong contenders in the TFEs field due to their significantly higher mechanical flexibility; however, their current use is, in part, limited by their scattering-induced visibility to the naked eye. Herein, we report polymeric web-assisted two-dimensional nanostructures, fabricated via electrospinning and integrated with gas-phase deposition methods such as magnetron sputtering, yielding thin film nanopatterning with ultra-high luminous transmittance (Tlum) of 98.1% and sheet resistance (Rs) of 17 Ω □–1. The addition of an antireflective coating enhances the Tlum to 99.7%. The designed trilayer, highly absorbing Fabry–Perot stack (Ag/ITO/NiCr) sputtered on patterned nanolines (NLs) leads to backward scattering suppression, rendering them significantly less visible than the “uncloaked” Ag-only NLs. Our findings are confirmed by finite-difference time-domain (FDTD) simulations. These high-performing, near-invisible electrodes allow for adjustable conductivity through thickness control without compromising transparency, while maintaining mechanical robustness under bending. They are also compatible with polymeric substrates, requiring only room-temperature polymer template dissolution, eliminating the need for high-temperature annealing and representing a promising route toward next-generation optoelectronic applications, including displays, photovoltaics, and wearable electronics.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"1 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221487","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Husam Walwil,Jonghyun Bae,Seokjun Kim,Dohwan Jung,Nipun Sutradhar,Asad Ali,Sadikul Alam,Robert M. Lavelle,Mohamadali Malakoutian,Kelly Woo,Kaiyan Shan,Hongkun Li,Weidong Zheng,Prakash R. Sultane,Christopher W. Bielawski,Minji Kim,Jiun Oh,Joon Seop Kwak,Srabanti Chowdhury,Jinwoo Hwang,Jae-Hyun Ryou,Jungwoo Oh,Sukwon Choi
Thin film beryllium oxide (BeO) is an emerging material that can potentially be used as a high thermal conductivity gate dielectric and/or passivation layer for high power electronic devices. This study presents the measurement of the thermal conductivity and thermal boundary conductance associated with plasma-enhanced atomic layer deposition (PEALD)-grown polycrystalline BeO films on Si substrates with thicknesses ranging from 25 to 250 nm. The measured out-of-plane thermal conductivities of the 250, 113, 53, and 26 nm-thick BeO films are 13.45 ± 1.45, 8.7 ± 1.35, 7.2 ± 2.1, and 5 ± 2.2 W m–1 K–1, respectively, representing an order-of-magnitude improvement over conventional dielectric materials such as SiN and SiO2. The measured thermal boundary conductance across the BeO/Si interface is ∼200 MW m–2 K–1 at room temperature, which approaches the intrinsic interface limit and suggests that interfacial heat transport is predominantly governed by elastic phonon transmission. The growth of a ∼200 nm-thick polycrystalline diamond film on an AlGaN/GaN-on-Si epitaxial wafer using a 5 nm-thick BeO diamond-seeding is demonstrated, where the structural integrity of the underlying AlGaN/GaN heterostructure is fully preserved. Thermal simulations of AlGaN/GaN high electron mobility transistors (HEMTs) integrated with a top-side polycrystalline diamond heat spreader predict that replacing the conventional SiO2 passivation and nucleation layers with BeO helps reduce the channel temperature rise by an additional 5.2%.
{"title":"Thermal Transport in Atomic Layer Deposition-Grown Beryllium Oxide Thin Films and Implications on Device Cooling","authors":"Husam Walwil,Jonghyun Bae,Seokjun Kim,Dohwan Jung,Nipun Sutradhar,Asad Ali,Sadikul Alam,Robert M. Lavelle,Mohamadali Malakoutian,Kelly Woo,Kaiyan Shan,Hongkun Li,Weidong Zheng,Prakash R. Sultane,Christopher W. Bielawski,Minji Kim,Jiun Oh,Joon Seop Kwak,Srabanti Chowdhury,Jinwoo Hwang,Jae-Hyun Ryou,Jungwoo Oh,Sukwon Choi","doi":"10.1021/acsami.6c16056","DOIUrl":"https://doi.org/10.1021/acsami.6c16056","url":null,"abstract":"Thin film beryllium oxide (BeO) is an emerging material that can potentially be used as a high thermal conductivity gate dielectric and/or passivation layer for high power electronic devices. This study presents the measurement of the thermal conductivity and thermal boundary conductance associated with plasma-enhanced atomic layer deposition (PEALD)-grown polycrystalline BeO films on Si substrates with thicknesses ranging from 25 to 250 nm. The measured out-of-plane thermal conductivities of the 250, 113, 53, and 26 nm-thick BeO films are 13.45 ± 1.45, 8.7 ± 1.35, 7.2 ± 2.1, and 5 ± 2.2 W m–1 K–1, respectively, representing an order-of-magnitude improvement over conventional dielectric materials such as SiN and SiO2. The measured thermal boundary conductance across the BeO/Si interface is ∼200 MW m–2 K–1 at room temperature, which approaches the intrinsic interface limit and suggests that interfacial heat transport is predominantly governed by elastic phonon transmission. The growth of a ∼200 nm-thick polycrystalline diamond film on an AlGaN/GaN-on-Si epitaxial wafer using a 5 nm-thick BeO diamond-seeding is demonstrated, where the structural integrity of the underlying AlGaN/GaN heterostructure is fully preserved. Thermal simulations of AlGaN/GaN high electron mobility transistors (HEMTs) integrated with a top-side polycrystalline diamond heat spreader predict that replacing the conventional SiO2 passivation and nucleation layers with BeO helps reduce the channel temperature rise by an additional 5.2%.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"63 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shen Wang,Maocheng Ji,Yongqi Zhang,Xinzhong Song,Jianyong Li,Jianfeng Li,Jia Man
The abundance of hydrophilic groups and the linear polymer chain structure in waterborne polyurethane (WPU) lead to insufficient water resistance and corrosion protection. These inherent characteristics make it challenging for WPU to be applied in the marine protection field, where high comprehensive performance of coatings is demanded. Herein, a WPU nanocomposite was designed incorporating hydroxyl-terminated polydimethylsiloxane and bifunctionalized nano-silica (modified with 3-aminopropyltriethoxysilane and propyltrimethoxysilane) during prepolymerization. This strategy established an organic–inorganic interpenetrating cross-linked network through covalent bonding and intermolecular interactions. The silica nanoparticles act as interfacial bridges between polymer segments, mitigating phase separation and agglomeration caused by polarity mismatch, thereby enhancing coating compactness and improving stress transfer. Performance tests demonstrate that the properties of the coating have been comprehensively enhanced. The coating exhibits an elongation at break of 254.64% while maintaining a tensile strength of 21.17 MPa. Additionally, the water absorption rate of the coating decreases to approximately 5%, the electrochemical protection efficiency reaches 99.9920%, and no obvious corrosion phenomenon is observed after a 7 day salt spray corrosion test. Additionally, the coating shows excellent drag-reduction performance, with a drag-reduction rate of 6.56% under turbulent flow. By integrating interfacial design with nanocomposite architecture, this work develops a robust WPU coating system suitable for marine engineering applications, and employs molecular dynamics simulations to reveal the microscopic mechanism by which amino and n-propyl silane dual modification inhibits the aggregation of silica nanoparticles as well as the interfacial interaction mechanism, thereby highlighting the role of colloidal and nanomaterial strategies in advancing functional protective coatings.
{"title":"Interfacial Regulation via Organic-Inorganic Interpenetrating Networks for Enhanced Protection in Waterborne Polyurethane Nanocomposites","authors":"Shen Wang,Maocheng Ji,Yongqi Zhang,Xinzhong Song,Jianyong Li,Jianfeng Li,Jia Man","doi":"10.1021/acsami.6c17358","DOIUrl":"https://doi.org/10.1021/acsami.6c17358","url":null,"abstract":"The abundance of hydrophilic groups and the linear polymer chain structure in waterborne polyurethane (WPU) lead to insufficient water resistance and corrosion protection. These inherent characteristics make it challenging for WPU to be applied in the marine protection field, where high comprehensive performance of coatings is demanded. Herein, a WPU nanocomposite was designed incorporating hydroxyl-terminated polydimethylsiloxane and bifunctionalized nano-silica (modified with 3-aminopropyltriethoxysilane and propyltrimethoxysilane) during prepolymerization. This strategy established an organic–inorganic interpenetrating cross-linked network through covalent bonding and intermolecular interactions. The silica nanoparticles act as interfacial bridges between polymer segments, mitigating phase separation and agglomeration caused by polarity mismatch, thereby enhancing coating compactness and improving stress transfer. Performance tests demonstrate that the properties of the coating have been comprehensively enhanced. The coating exhibits an elongation at break of 254.64% while maintaining a tensile strength of 21.17 MPa. Additionally, the water absorption rate of the coating decreases to approximately 5%, the electrochemical protection efficiency reaches 99.9920%, and no obvious corrosion phenomenon is observed after a 7 day salt spray corrosion test. Additionally, the coating shows excellent drag-reduction performance, with a drag-reduction rate of 6.56% under turbulent flow. By integrating interfacial design with nanocomposite architecture, this work develops a robust WPU coating system suitable for marine engineering applications, and employs molecular dynamics simulations to reveal the microscopic mechanism by which amino and n-propyl silane dual modification inhibits the aggregation of silica nanoparticles as well as the interfacial interaction mechanism, thereby highlighting the role of colloidal and nanomaterial strategies in advancing functional protective coatings.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"14 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221608","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Suprobhat Singha Roy,Abhishek Muraleedharan,Vishesh Vishesh,Vidyoth Koka Ruparani,Fajar Dhanish C P,Subrata Kundu
Understanding the dynamic surface reconstruction of precatalyst materials during the oxygen evolution reaction (OER) is a forefront area of research for designing and studying effective electrocatalysts. Here, we report the deliberate engineering of Se vacancies in NiCoSe2 via a facile NaBH4 reduction strategy and systematically investigate how anion vacancies govern surface reconstruction behavior under alkaline OER conditions. The presence of Se vacancies is confirmed via EPR spectroscopy and ICP-MS analysis. Cyclic voltammetry and in situ electrochemical impedance spectroscopy during the electrochemical activation process reveal that the vacancy-enriched NiCoSe2–x undergoes faster and more extensive structural reconstruction than pristine NiCoSe2. Quasi in situ ATR-FTIR and Raman spectroscopy track the dynamic evolution of NiCoOOH during anodic polarization, providing direct spectroscopic evidence for the Se vacancy-promoted NiCoOOH active phase generation with abundant Ni–O–Co synergy. Evaluation of electrochemical surface area and turnover frequency establishes that the generation of abundant Ni–O–Co synergy in NiCoSe2–x simultaneously increases the density of accessible active sites and enhances the intrinsic activity per site. Consequently, the NiCoSe2–x precatalyst delivers significantly improved OER performance relative to bare NiCoSe2, along with high Faradaic selectivity and long-term stability. Post-stability characterizations confirm bulk structural and morphological reconstruction driven by Se vacancies and thus highlight the complete utilization of the available catalytic sites. This work provides a fundamental mechanistic framework linking anion vacancy engineering, surface reconstruction kinetics/mechanism tracking, and intrinsic OER activity enhancement in bimetallic chalcogenide precatalysts, offering rationalized design principles for next-generation earth-abundant OER catalysts.
{"title":"In Situ Tracking of Se Vacancy-Promoted Surface Reconstruction of NiCoSe2 into NiCoOOH during Alkaline Oxygen Evolution","authors":"Suprobhat Singha Roy,Abhishek Muraleedharan,Vishesh Vishesh,Vidyoth Koka Ruparani,Fajar Dhanish C P,Subrata Kundu","doi":"10.1021/acsami.6c15313","DOIUrl":"https://doi.org/10.1021/acsami.6c15313","url":null,"abstract":"Understanding the dynamic surface reconstruction of precatalyst materials during the oxygen evolution reaction (OER) is a forefront area of research for designing and studying effective electrocatalysts. Here, we report the deliberate engineering of Se vacancies in NiCoSe2 via a facile NaBH4 reduction strategy and systematically investigate how anion vacancies govern surface reconstruction behavior under alkaline OER conditions. The presence of Se vacancies is confirmed via EPR spectroscopy and ICP-MS analysis. Cyclic voltammetry and in situ electrochemical impedance spectroscopy during the electrochemical activation process reveal that the vacancy-enriched NiCoSe2–x undergoes faster and more extensive structural reconstruction than pristine NiCoSe2. Quasi in situ ATR-FTIR and Raman spectroscopy track the dynamic evolution of NiCoOOH during anodic polarization, providing direct spectroscopic evidence for the Se vacancy-promoted NiCoOOH active phase generation with abundant Ni–O–Co synergy. Evaluation of electrochemical surface area and turnover frequency establishes that the generation of abundant Ni–O–Co synergy in NiCoSe2–x simultaneously increases the density of accessible active sites and enhances the intrinsic activity per site. Consequently, the NiCoSe2–x precatalyst delivers significantly improved OER performance relative to bare NiCoSe2, along with high Faradaic selectivity and long-term stability. Post-stability characterizations confirm bulk structural and morphological reconstruction driven by Se vacancies and thus highlight the complete utilization of the available catalytic sites. This work provides a fundamental mechanistic framework linking anion vacancy engineering, surface reconstruction kinetics/mechanism tracking, and intrinsic OER activity enhancement in bimetallic chalcogenide precatalysts, offering rationalized design principles for next-generation earth-abundant OER catalysts.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"73 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221473","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shaodong Zhai,Zhenghao Wang,Jing Wang,Xiang Guo,Xiao Tan,Hongnv Zhang,Ruiping Zhang,Nan Hu
Myocardial infarction (MI)-induced cardiac injury is mainly divided into two phases: the acute necrotic phase and the repair phase. Given the distinct therapeutic requirements of each phase—salvaging dying cardiomyocytes and reducing infarct size in the acute phase, while achieving controlled fibrosis to promote effective ventricular remodeling in the repair phase—we designed an ROS-responsive hydrogel co-delivery system (Met/Anti-34a@Gel) loaded with metformin (Met) and Anti-34a liposomes (Anti-34a Lip) to achieve precise regulation of both the acute and repair phases of MI. In the highly oxidative stress microenvironment following MI, the hydrogel gradually degrades and releases Met and Anti-34a Lip in a stage-specific manner. Met improves mitochondrial function, inhibits oxidative stress and ferroptosis, thereby effectively salvaging cardiomyocytes in the acute phase. Anti-34a Lip modulates the differentiation behavior of cardiac fibroblasts, suppressing excessive fibrosis and promoting favorable ventricular remodeling in the repair phase. Echocardiography revealed that Met/Anti-34a@Gel preserved left ventricular ejection fraction (EF) and fractional shortening (FS) at 72 h post-MI, reduced serum MDA levels in the acute phase, and maintained EF at approximately 60.92 ± 8.37% with a lower collagen I/III ratio at 4 weeks, collectively demonstrating both acute cardioprotection and long-term anti-fibrotic remodeling. In this combined therapeutic strategy, the early mitochondrial protection and anti-ferroptosis effects establish a favorable tissue and functional foundation for subsequent precision anti-fibrotic therapy, while the later anti-fibrotic treatment further consolidates the early protective effects. The two actions synergistically form a positive feedback loop, ultimately achieving sustained long-term cardiac functional improvement.
{"title":"ROS-Responsive Hydrogel for Spatiotemporal Cascade Regulation of Ferroptosis and Fibrosis for Myocardial Protection","authors":"Shaodong Zhai,Zhenghao Wang,Jing Wang,Xiang Guo,Xiao Tan,Hongnv Zhang,Ruiping Zhang,Nan Hu","doi":"10.1021/acsami.6c15728","DOIUrl":"https://doi.org/10.1021/acsami.6c15728","url":null,"abstract":"Myocardial infarction (MI)-induced cardiac injury is mainly divided into two phases: the acute necrotic phase and the repair phase. Given the distinct therapeutic requirements of each phase—salvaging dying cardiomyocytes and reducing infarct size in the acute phase, while achieving controlled fibrosis to promote effective ventricular remodeling in the repair phase—we designed an ROS-responsive hydrogel co-delivery system (Met/Anti-34a@Gel) loaded with metformin (Met) and Anti-34a liposomes (Anti-34a Lip) to achieve precise regulation of both the acute and repair phases of MI. In the highly oxidative stress microenvironment following MI, the hydrogel gradually degrades and releases Met and Anti-34a Lip in a stage-specific manner. Met improves mitochondrial function, inhibits oxidative stress and ferroptosis, thereby effectively salvaging cardiomyocytes in the acute phase. Anti-34a Lip modulates the differentiation behavior of cardiac fibroblasts, suppressing excessive fibrosis and promoting favorable ventricular remodeling in the repair phase. Echocardiography revealed that Met/Anti-34a@Gel preserved left ventricular ejection fraction (EF) and fractional shortening (FS) at 72 h post-MI, reduced serum MDA levels in the acute phase, and maintained EF at approximately 60.92 ± 8.37% with a lower collagen I/III ratio at 4 weeks, collectively demonstrating both acute cardioprotection and long-term anti-fibrotic remodeling. In this combined therapeutic strategy, the early mitochondrial protection and anti-ferroptosis effects establish a favorable tissue and functional foundation for subsequent precision anti-fibrotic therapy, while the later anti-fibrotic treatment further consolidates the early protective effects. The two actions synergistically form a positive feedback loop, ultimately achieving sustained long-term cardiac functional improvement.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"12 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221600","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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