The efficient removal of volatile organic compounds (VOCs) with different molecular sizes remains a great challenge in the field of zeolite-based adsorption technology. The conventional composite zeolite systems (e.g., MFI/FAU) suffer from nonuniform crystalline distribution. Herein, a novel synthesis strategy for all-silica MEL zeolites was developed featuring 10-membered ring (10-MR) micropores, extra-large micropores (0.8∼2.0 nm), and small mesopores (2.0∼5.0 nm). The hierarchical pore structure conferred exceptional adsorption capabilities for VOCs across diverse molecular dimensions. The volume and accessibility of extra-large micropores and small mesopores could be tuned by controlling the tetrabutylammonium hydroxide (TBAOH) content in the synthesis gel and crystallization temperature, while prolonged crystallization enhanced framework hydrophobicity due to the decrease of silanol group density. Notably, the optimal sample exhibited a superior m-xylene adsorption capacity of 85.2 mg/g. Meanwhile, high adsorption capacities of acetone, ethyl acetate, and toluene were also obtained, which can be attributed to its high 10-MR micropore volume of 0.178 cm3/g. Importantly, its m-xylene adsorption capacity remained unchanged across multiple regeneration cycles, demonstrating perfect recyclability and structural stability. Low desorption peak temperatures (<115 °C) for all adsorbates were acquired that facilitated regeneration under mild conditions. By integrating hierarchical pore engineering and surface chemistry control within a single zeolite framework, this work overcomes the limitations of traditional composite systems, offering a versatile and efficient system for industrial VOC abatement.
{"title":"Tailored Synthesis of Hierarchical All-Silica MEL Zeolites for Efficient Removal of Versatile VOCs","authors":"Qiang Yu, Zikai Xu, Wei Fan, Junjie Li, Xiangxue Zhu, Xiujie Li","doi":"10.1021/acsami.5c17480","DOIUrl":"https://doi.org/10.1021/acsami.5c17480","url":null,"abstract":"The efficient removal of volatile organic compounds (VOCs) with different molecular sizes remains a great challenge in the field of zeolite-based adsorption technology. The conventional composite zeolite systems (e.g., MFI/FAU) suffer from nonuniform crystalline distribution. Herein, a novel synthesis strategy for all-silica MEL zeolites was developed featuring 10-membered ring (10-MR) micropores, extra-large micropores (0.8∼2.0 nm), and small mesopores (2.0∼5.0 nm). The hierarchical pore structure conferred exceptional adsorption capabilities for VOCs across diverse molecular dimensions. The volume and accessibility of extra-large micropores and small mesopores could be tuned by controlling the tetrabutylammonium hydroxide (TBAOH) content in the synthesis gel and crystallization temperature, while prolonged crystallization enhanced framework hydrophobicity due to the decrease of silanol group density. Notably, the optimal sample exhibited a superior m-xylene adsorption capacity of 85.2 mg/g. Meanwhile, high adsorption capacities of acetone, ethyl acetate, and toluene were also obtained, which can be attributed to its high 10-MR micropore volume of 0.178 cm<sup>3</sup>/g. Importantly, its m-xylene adsorption capacity remained unchanged across multiple regeneration cycles, demonstrating perfect recyclability and structural stability. Low desorption peak temperatures (<115 °C) for all adsorbates were acquired that facilitated regeneration under mild conditions. By integrating hierarchical pore engineering and surface chemistry control within a single zeolite framework, this work overcomes the limitations of traditional composite systems, offering a versatile and efficient system for industrial VOC abatement.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"20 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732094","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}
Yu-Shen Liu, Yu-Hsiang Kuo, Vijay M. Shah, Paul J. A. Kenis, Alexa S. Kuenstler
Carbon dioxide (CO2) capture is critical to mitigating the anthropogenic emissions that contribute to global warming. Polymer membranes can be applied in energy efficient gas separation methods, where chemical and structural features can be tuned to co-optimize selectivity and permeability. In this work, we developed a modular thiol–ene network platform to independently tune cross-link density and functionality to explicitly understand the impact of network architecture and polymer chain functionality on separation performance. By varying the pendant functional groups in the networks, we investigated how molecular substitutions affect the selectivity of CO2/N2 and CO2/O2 selectivity. These membranes were subsequently applied as a selective layer in a thin-film composite membrane system. In pure gas testing, the network with pendant aromatic rings elevated the CO2/N2 selectivity from ≈10 to 34 and CO2/O2 selectivity from ≈5 to 17 compared to bare polydimethylsiloxane (PDMS) membranes, with a CO2 permeability of 1426 barrer. Furthermore, the topologically regular and predictable cross-linking density features in this modular network system allowed us to unravel their effect on CO2 selectivity and permeability. We demonstrate that these functionalized thiol–ene network-based membranes can be used in a pseudomultistage gas separation configuration to concentrate CO2 from gas mixtures of industrially relevant composition.
{"title":"Tailoring Pendant Group Chemistry and Thiol–Ene Network Structure of Thin-Film Composite Membranes to Optimize CO2 Gas Separation","authors":"Yu-Shen Liu, Yu-Hsiang Kuo, Vijay M. Shah, Paul J. A. Kenis, Alexa S. Kuenstler","doi":"10.1021/acsami.5c18327","DOIUrl":"https://doi.org/10.1021/acsami.5c18327","url":null,"abstract":"Carbon dioxide (CO<sub>2</sub>) capture is critical to mitigating the anthropogenic emissions that contribute to global warming. Polymer membranes can be applied in energy efficient gas separation methods, where chemical and structural features can be tuned to co-optimize selectivity and permeability. In this work, we developed a modular thiol–ene network platform to independently tune cross-link density and functionality to explicitly understand the impact of network architecture and polymer chain functionality on separation performance. By varying the pendant functional groups in the networks, we investigated how molecular substitutions affect the selectivity of CO<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub>/O<sub>2</sub> selectivity. These membranes were subsequently applied as a selective layer in a thin-film composite membrane system. In pure gas testing, the network with pendant aromatic rings elevated the CO<sub>2</sub>/N<sub>2</sub> selectivity from ≈10 to 34 and CO<sub>2</sub>/O<sub>2</sub> selectivity from ≈5 to 17 compared to bare polydimethylsiloxane (PDMS) membranes, with a CO<sub>2</sub> permeability of 1426 barrer. Furthermore, the topologically regular and predictable cross-linking density features in this modular network system allowed us to unravel their effect on CO<sub>2</sub> selectivity and permeability. We demonstrate that these functionalized thiol–ene network-based membranes can be used in a pseudomultistage gas separation configuration to concentrate CO<sub>2</sub> from gas mixtures of industrially relevant composition.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"49 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729235","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}
Huan Liu, Duanduan Yin, Ke Li, Yiran Dong, Dan Li, Feng Li, Ying Yang, Xiangjie Bo, Xiangting Dong
Electrochemical water splitting is regarded as an efficient method for hydrogen production. Ru is theoretically deemed as an effective electrocatalyst for hydrogen evolution reactions (HERs) in alkaline media owing to its fast hydrolysis kinetics. Nevertheless, its strong OH– adsorption affinity can lead to active site blockage, often resulting in a suboptimal performance in practical HER applications. In addition, electrocatalytic reactions predominantly take place at surface-active sites. In the case of conventional solid catalysts, the core active material remains largely inaccessible due to mass transfer limitations, significantly reducing the overall utilization of active sites. To address these challenges, the work introduces a competitive adsorption strategy and a hollow structure strategy for constructing Ru–Sn/SnO2 hollow carbon nanofiber electrocatalysts (Ru–Sn/SnO2 HCNFs). The introduction of Sn/SnO2 helps to modulate the intense interaction between Ru and OH–; OH– adsorption on SnO2 is more favorable than Ru, thereby successfully mitigating poisoning on Ru. This process also promotes OH– transfer and Ru active site regeneration. Additionally, the specific surface area of Ru–Sn/SnO2–HCNFs (606.9 m2g–1) is higher than that of the solid fiber of Ru–Sn/SnO2–CNFs (22.7 m2g–1), highlighting the beneficial role of hollow fibers in enhancing the exposure of active sites. Consequently, Ru–Sn/SnO2–HCNFs exhibit an outstanding HER performance, achieving remarkably low overpotentials of only 6.8 mV in 1 M KOH and 23.3 mV in 0.5 M H2SO4 at 10 mA cm–2, respectively. This research offers a novel approach on rational design for high-efficiency HER electrocatalysts.
电化学水分解是一种高效的制氢方法。Ru具有快速的水解动力学,理论上被认为是碱性介质中析氢反应的有效电催化剂。然而,其强大的OH -吸附亲和力可能导致活性位点堵塞,通常导致在实际HER应用中的性能不理想。此外,电催化反应主要发生在表面活性位点。在传统固体催化剂的情况下,由于传质限制,核心活性物质在很大程度上仍然是不可接近的,这大大降低了活性位点的总体利用率。为了解决这些挑战,本研究介绍了一种竞争性吸附策略和一种空心结构策略,用于构建Ru-Sn /SnO2中空碳纳米纤维电催化剂(Ru-Sn /SnO2 HCNFs)。Sn/SnO2的引入有助于调节Ru与OH -之间强烈的相互作用;OH -在SnO2上的吸附比Ru更有利,从而成功地减轻了Ru上的中毒。该过程还促进了OH -转移和Ru活性位点的再生。此外,Ru-Sn / SnO2-HCNFs的比表面积(606.9 m2g-1)高于Ru-Sn / SnO2-CNFs的固体纤维(22.7 m2g-1),突出了中空纤维在增强活性位点暴露方面的有益作用。因此,Ru-Sn / SnO2-HCNFs表现出出色的HER性能,在1 M KOH和10 mA cm-2下,在0.5 M H2SO4中分别获得了6.8 mV和23.3 mV的过电位。本研究为高效HER电催化剂的合理设计提供了一条新途径。
{"title":"Employing Competitive Adsorption and Hollow Nanofiber Strategies toward High-Efficiency Hydrogen Evolution with Ru–Sn/SnO2 Heterojunction Catalysts","authors":"Huan Liu, Duanduan Yin, Ke Li, Yiran Dong, Dan Li, Feng Li, Ying Yang, Xiangjie Bo, Xiangting Dong","doi":"10.1021/acsami.5c18381","DOIUrl":"https://doi.org/10.1021/acsami.5c18381","url":null,"abstract":"Electrochemical water splitting is regarded as an efficient method for hydrogen production. Ru is theoretically deemed as an effective electrocatalyst for hydrogen evolution reactions (HERs) in alkaline media owing to its fast hydrolysis kinetics. Nevertheless, its strong OH<sup>–</sup> adsorption affinity can lead to active site blockage, often resulting in a suboptimal performance in practical HER applications. In addition, electrocatalytic reactions predominantly take place at surface-active sites. In the case of conventional solid catalysts, the core active material remains largely inaccessible due to mass transfer limitations, significantly reducing the overall utilization of active sites. To address these challenges, the work introduces a competitive adsorption strategy and a hollow structure strategy for constructing Ru–Sn/SnO<sub>2</sub> hollow carbon nanofiber electrocatalysts (Ru–Sn/SnO<sub>2</sub> HCNFs). The introduction of Sn/SnO<sub>2</sub> helps to modulate the intense interaction between Ru and OH<sup>–</sup>; OH<sup>–</sup> adsorption on SnO<sub>2</sub> is more favorable than Ru, thereby successfully mitigating poisoning on Ru. This process also promotes OH<sup>–</sup> transfer and Ru active site regeneration. Additionally, the specific surface area of Ru–Sn/SnO<sub>2</sub>–HCNFs (606.9 m<sup>2</sup>g<sup>–1</sup>) is higher than that of the solid fiber of Ru–Sn/SnO<sub>2</sub>–CNFs (22.7 m<sup>2</sup>g<sup>–1</sup>), highlighting the beneficial role of hollow fibers in enhancing the exposure of active sites. Consequently, Ru–Sn/SnO<sub>2</sub>–HCNFs exhibit an outstanding HER performance, achieving remarkably low overpotentials of only 6.8 mV in 1 M KOH and 23.3 mV in 0.5 M H<sub>2</sub>SO<sub>4</sub> at 10 mA cm<sup>–2</sup>, respectively. This research offers a novel approach on rational design for high-efficiency HER electrocatalysts.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"41 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729238","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}
Acute lung injury (ALI) is a serious clinical disease the severe stage of which develops into acute respiratory distress syndrome (ARDS), with a high mortality rate of 35 to 40%. Despite decades of research and development of drugs such as corticosteroids and β-2 adrenergic agonists, treatment efficacy has been limited due to an insufficient drug concentration reaching the lungs. Here, a food-grade γ-cyclodextrin-based metal-organic framework (γCD-MOF) modified with cholesterol (CHS) is developed to load sulfur dioxide (SO2) as a dry powder inhaler (DPI) platform (CHS-CD-MOF@SO2) for ALI treatment. CHS-CD-MOF@SO2 has suitable storage stability and excellent aerodynamic characteristics, with a fine particle fraction (FPF) of 40%, a geometric standard deviation (GSD) value of 1.61, and a mass median aerodynamic diameter (MMAD) of 4.8 μm, which can effectively target the lungs. By employing rhodamine B (RhB) as a fluorescence indicator, in vivo fluorescence imaging confirms the superior lung-targeting capability of CHS-CD-MOFs. CHS-CD-MOF@SO2 can release 92.3 ± 4.4% of SO2 in PBS solution within 5 min. What's more, the permeability of simulated lung fluid within 30 min is as high as 85%, which has the potential for rapid treatment of ALI. In an ALI mouse model, CHS-CD-MOF@SO2 reduces the expression of pro-inflammatory factors tumor necrosis factor-alpha (TNF-α), interleukin-1 beta (IL-1β), and IL-6 by regulating the P38 and nuclear factor kappa B (NF-κB) pathways. It also significantly improves the lung tissue dry/wet ratio and reduces neutrophil infiltration. Importantly, this treatment achieves therapeutic outcomes in key efficacy parameters that was comparable to or better than those of dexamethasone (DXMS), a frontline drug for ALI, underscoring its significant therapeutic potential. This study presents a novel strategy for treating ALI using a DPI-based gas messenger platform. This study provides a novel therapeutic strategy to treat ALI using DPI-loaded gas messengers.
{"title":"Inhalable Food-Grade MOFs Loaded Gas Messenger for Acute Lung Injury Treatment by Pulmonary Delivery.","authors":"Zu-E Hu, Fu-Zhong Zhang, Minfeng Zeng, Ye-Tao Zhang, Jing Li, Yu-Ting Che, Jun-Feng Feng, Bang-Jing Li, Sheng Zhang","doi":"10.1021/acsami.5c20962","DOIUrl":"https://doi.org/10.1021/acsami.5c20962","url":null,"abstract":"<p><p>Acute lung injury (ALI) is a serious clinical disease the severe stage of which develops into acute respiratory distress syndrome (ARDS), with a high mortality rate of 35 to 40%. Despite decades of research and development of drugs such as corticosteroids and β-2 adrenergic agonists, treatment efficacy has been limited due to an insufficient drug concentration reaching the lungs. Here, a food-grade γ-cyclodextrin-based metal-organic framework (γCD-MOF) modified with cholesterol (CHS) is developed to load sulfur dioxide (SO<sub>2</sub>) as a dry powder inhaler (DPI) platform (CHS-CD-MOF@SO<sub>2</sub>) for ALI treatment. CHS-CD-MOF@SO<sub>2</sub> has suitable storage stability and excellent aerodynamic characteristics, with a fine particle fraction (FPF) of 40%, a geometric standard deviation (GSD) value of 1.61, and a mass median aerodynamic diameter (MMAD) of 4.8 μm, which can effectively target the lungs. By employing rhodamine B (RhB) as a fluorescence indicator, in vivo fluorescence imaging confirms the superior lung-targeting capability of CHS-CD-MOFs. CHS-CD-MOF@SO<sub>2</sub> can release 92.3 ± 4.4% of SO<sub>2</sub> in PBS solution within 5 min. What's more, the permeability of simulated lung fluid within 30 min is as high as 85%, which has the potential for rapid treatment of ALI. In an ALI mouse model, CHS-CD-MOF@SO<sub>2</sub> reduces the expression of pro-inflammatory factors tumor necrosis factor-alpha (TNF-α), interleukin-1 beta (IL-1β), and IL-6 by regulating the P38 and nuclear factor kappa B (NF-κB) pathways. It also significantly improves the lung tissue dry/wet ratio and reduces neutrophil infiltration. Importantly, this treatment achieves therapeutic outcomes in key efficacy parameters that was comparable to or better than those of dexamethasone (DXMS), a frontline drug for ALI, underscoring its significant therapeutic potential. This study presents a novel strategy for treating ALI using a DPI-based gas messenger platform. This study provides a novel therapeutic strategy to treat ALI using DPI-loaded gas messengers.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145719995","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}
Hui-Cong Ge, Shengsheng Yu, Jian Zhu, Xiao-Tong Zhan, Shi-Qian Jia, Ling-Bao Xing, Long Yi Jin
The artificial light-harvesting system (LHS) based on the cascade fluorescence resonance energy transfer (FRET) mechanism has ability to widely regulate the luminescent performance, however, it still faces significant challenges to achieve full-color luminescent regulation covering the entire visible spectrum in a single LHS system. In this study, we designed and constructed an artificial LHS with a three-step cascade energy transfer mechanism, achieving effective emission of white light and multicolor fluorescence within the visible light range. A cationic 6-bromobenzo[de]isochromene-1,3-dione derivative (BNI) was prepared, which was able to generate a supramolecular complex with sulfobutylether-β-cyclodextrin (SBE-β-CD) via electrostatic interactions. Given that this complex has excellent dark blue fluorescence performance, it was selected as the energy donor and sequentially participated in FRET process with commercial dyes Fluorescein (Flu), Rhodamine B (RhB) and Sulforhodamine 101 (SR101), thereby constructing an artificial LHS with three-step sequential energy transfer. By precisely regulating the ratios of acceptor molecules, multicolor fluorescence emissions ranging from blue to red bands and white light emission were achieved. Ultimately, the synthesized supramolecular LHS was effectively utilized in the development of multicolor fluorescent light-emitting devices and demonstrated its potential application in information storage.
{"title":"Artificial Light-Harvesting System with Three-Step Cascade Energy Transfer Process for Full-Color Luminescence Modulation","authors":"Hui-Cong Ge, Shengsheng Yu, Jian Zhu, Xiao-Tong Zhan, Shi-Qian Jia, Ling-Bao Xing, Long Yi Jin","doi":"10.1021/acsami.5c20984","DOIUrl":"https://doi.org/10.1021/acsami.5c20984","url":null,"abstract":"The artificial light-harvesting system (LHS) based on the cascade fluorescence resonance energy transfer (FRET) mechanism has ability to widely regulate the luminescent performance, however, it still faces significant challenges to achieve full-color luminescent regulation covering the entire visible spectrum in a single LHS system. In this study, we designed and constructed an artificial LHS with a three-step cascade energy transfer mechanism, achieving effective emission of white light and multicolor fluorescence within the visible light range. A cationic 6-bromobenzo[de]isochromene-1,3-dione derivative (BNI) was prepared, which was able to generate a supramolecular complex with sulfobutylether-β-cyclodextrin (SBE-β-CD) via electrostatic interactions. Given that this complex has excellent dark blue fluorescence performance, it was selected as the energy donor and sequentially participated in FRET process with commercial dyes Fluorescein (Flu), Rhodamine B (RhB) and Sulforhodamine 101 (SR101), thereby constructing an artificial LHS with three-step sequential energy transfer. By precisely regulating the ratios of acceptor molecules, multicolor fluorescence emissions ranging from blue to red bands and white light emission were achieved. Ultimately, the synthesized supramolecular LHS was effectively utilized in the development of multicolor fluorescent light-emitting devices and demonstrated its potential application in information storage.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"11 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718216","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}
Jian Ren, Lin Xu, Xianda Liu, Dongmei Tong, Shujing Wang, Shuxiang Zhang, Ran Wei, Weifeng Zhao, Changsheng Zhao
Hemodialysis membranes would easily accelerate excessive oxidative stress, leading to platelet adhesion and aggregation, which cause exacerbation of hemodialysis-associated thrombocytopenia. Notably, nitric oxide (NO) gas exerts an inhibitory effect on platelet activation by targeting key signaling molecules. Hence, we propose a strategy to inhibit platelet activation and adhesion by turning “harmful reactive oxygen species (ROS)” into “beneficial NO”, thereby preventing hemodialysis-associated thrombocytopenia. In this study, polydopamine-l-arginine (PDA-LA) molecules are coated onto the membrane surface to mainly enhance the mitigation of oxidative stress, while oxidized hyaluronic acid-l-arginine (OHA-LA) molecules are stably cross-linked into the membrane to ensure the sustained NO release for inhibition of platelet adhesion. As a result, the reactive oxygen and nitrogen species (RONS) scavenging capacities are improved to follow: H2O2 (50%), 2,2-diphenyl-1-picrylhydrazyl (DPPH•, 85.60%), 2,2′-azinobis(3-ethylbenzothiazoline-6-sulfonate) radical (ABTS•+, 82.81%), and O2•– (0.125 U/mg). Surprisingly, the concentration of continuously released NO is still approximately 0.590 μM after six cycles (0.557 μM in the first cycle). Importantly, the platelet adhesion experiment demonstrates a sustained inhibition of platelet adhesion, diminished by a factor of 100 per square centimeter (100/cm2). In a simulated sieving experiment, the BSA rejection ratio (97.52%) and urea sieving ratio (98.38%) both meet the basic requirements for hemodialysis membranes. Thus, the obtained PES/PVA/OA@PA membrane is a promising candidate for preventing hemodialysis-associated thrombocytopenia.
{"title":"“Continuously Touching ROS into NO” by Hemodialysis Membranes for Preventing Hemodialysis-Associated Thrombocytopenia","authors":"Jian Ren, Lin Xu, Xianda Liu, Dongmei Tong, Shujing Wang, Shuxiang Zhang, Ran Wei, Weifeng Zhao, Changsheng Zhao","doi":"10.1021/acsami.5c21229","DOIUrl":"https://doi.org/10.1021/acsami.5c21229","url":null,"abstract":"Hemodialysis membranes would easily accelerate excessive oxidative stress, leading to platelet adhesion and aggregation, which cause exacerbation of hemodialysis-associated thrombocytopenia. Notably, nitric oxide (NO) gas exerts an inhibitory effect on platelet activation by targeting key signaling molecules. Hence, we propose a strategy to inhibit platelet activation and adhesion by turning “harmful reactive oxygen species (ROS)” into “beneficial NO”, thereby preventing hemodialysis-associated thrombocytopenia. In this study, polydopamine-<span>l</span>-arginine (PDA-LA) molecules are coated onto the membrane surface to mainly enhance the mitigation of oxidative stress, while oxidized hyaluronic acid-<span>l</span>-arginine (OHA-LA) molecules are stably cross-linked into the membrane to ensure the sustained NO release for inhibition of platelet adhesion. As a result, the reactive oxygen and nitrogen species (RONS) scavenging capacities are improved to follow: H<sub>2</sub>O<sub>2</sub> (50%), 2,2-diphenyl-1-picrylhydrazyl (DPPH<sup>•</sup>, 85.60%), 2,2′-azinobis(3-ethylbenzothiazoline-6-sulfonate) radical (ABTS<sup>•+</sup>, 82.81%), and O<sub>2</sub><sup>•–</sup> (0.125 U/mg). Surprisingly, the concentration of continuously released NO is still approximately 0.590 μM after six cycles (0.557 μM in the first cycle). Importantly, the platelet adhesion experiment demonstrates a sustained inhibition of platelet adhesion, diminished by a factor of 100 per square centimeter (100/cm<sup>2</sup>). In a simulated sieving experiment, the BSA rejection ratio (97.52%) and urea sieving ratio (98.38%) both meet the basic requirements for hemodialysis membranes. Thus, the obtained PES/PVA/OA@PA membrane is a promising candidate for preventing hemodialysis-associated thrombocytopenia.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"16 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729226","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}
To address the challenge of efficient thermal management for lithium-ion batteries across a wide temperature range, we developed a novel dual-temperature composite phase change material (CPCM). The CPCM, constructed with an expanded graphite matrix incorporating paraffin (∼45 °C) and potassium alum (∼90 °C), achieves two distinct phase change platforms and a high total latent heat of 211.4 J/g. Its thermal conductivity was significantly enhanced to 2.53 W/(m·K). In practical battery tests, the CPCM demonstrated superior performance: it reduced the maximum temperature by ∼10 °C across 0.2 to 1C discharge rates and maintained excellent temperature uniformity (ΔT < 2.2 °C). Crucially, under thermal runaway conditions, it lowered the peak temperature of adjacent cells by ∼134 °C, effectively delaying hazardous heat propagation. This work provides a material solution that synergistically combines efficient cooling at normal operating temperatures with robust thermal barrier functionality under extreme conditions.
{"title":"Dual-Temperature Composite Phase Change Material Adapted for Wide-Temperature-Range Applications in Battery Thermal Management","authors":"Shuheng Hu, Liangke Mao, Peng Qin, Zimu Xu, Lijian Ding, Helong Li, Ya Wei, Xiaoli Wang, Zhangyin Li, Zhaozhong Huang","doi":"10.1021/acsami.5c17887","DOIUrl":"https://doi.org/10.1021/acsami.5c17887","url":null,"abstract":"To address the challenge of efficient thermal management for lithium-ion batteries across a wide temperature range, we developed a novel dual-temperature composite phase change material (CPCM). The CPCM, constructed with an expanded graphite matrix incorporating paraffin (∼45 °C) and potassium alum (∼90 °C), achieves two distinct phase change platforms and a high total latent heat of 211.4 J/g. Its thermal conductivity was significantly enhanced to 2.53 W/(m·K). In practical battery tests, the CPCM demonstrated superior performance: it reduced the maximum temperature by ∼10 °C across 0.2 to 1C discharge rates and maintained excellent temperature uniformity (Δ<i>T</i> < 2.2 °C). Crucially, under thermal runaway conditions, it lowered the peak temperature of adjacent cells by ∼134 °C, effectively delaying hazardous heat propagation. This work provides a material solution that synergistically combines efficient cooling at normal operating temperatures with robust thermal barrier functionality under extreme conditions.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"20 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718221","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}
Perovskite photodetectors have emerged as a potential replacement for silicon photodiodes in modern cameras due to their high sensitivity to visible light and ability to be easily integrated into existing electronics. However, the use of perovskite photodetectors in conventional CMOS image sensors requires the application of reverse bias, which can lead to unstable detector performance due to ion migration effects. In this article, we propose a new approach that involves the application of forward voltage pulses to attenuate ion migration while still enabling the capture of photocurrent under reverse bias. Our results show that using this technique after each cycle of signal integration allows for stable operation of perovskite photodetectors for over 180 h, while applying a constant reverse bias leads to degradation within just 10 min. Additionally, we demonstrate stable imaging using alternating voltage and 8 × 8 crossbar arrays of perovskite photodetectors.
{"title":"Mitigating Ion Migration with Alternating Voltage for Stable Perovskite Image Sensors.","authors":"Sergey Tsarev,Yuliia Kominko,Kyuik Cho,Lorenzo J A Ferraresi,Gebhard Matt,Kostiantyn Sakhatskyi,Volodymyr Svintozelskyi,Daria Proniakova,Taekwang Jang,Maksym Kovalenko,Sergii Yakunin","doi":"10.1021/acsami.5c18552","DOIUrl":"https://doi.org/10.1021/acsami.5c18552","url":null,"abstract":"Perovskite photodetectors have emerged as a potential replacement for silicon photodiodes in modern cameras due to their high sensitivity to visible light and ability to be easily integrated into existing electronics. However, the use of perovskite photodetectors in conventional CMOS image sensors requires the application of reverse bias, which can lead to unstable detector performance due to ion migration effects. In this article, we propose a new approach that involves the application of forward voltage pulses to attenuate ion migration while still enabling the capture of photocurrent under reverse bias. Our results show that using this technique after each cycle of signal integration allows for stable operation of perovskite photodetectors for over 180 h, while applying a constant reverse bias leads to degradation within just 10 min. Additionally, we demonstrate stable imaging using alternating voltage and 8 × 8 crossbar arrays of perovskite photodetectors.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"141 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711076","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}
Caitlin D'Ambrosio,Nadim Massad,Amanda L McCahill,William Rears,Pierre Rouviere,Jeffery G Saven,Darrin J Pochan,Christopher J Kloxin,April M Kloxin,Wilfred Chen
Nature's protein sequences dictate structure and function across scales, from the nanometer-scale of viral capsids to micrometer- to millimeter-scale architectures of extracellular matrices and tissues. This multiscale precision underlies diverse functions, including molecular recognition, mechanical support, and dynamic responsiveness. Mimicking this complexity synthetically remains challenging. To address this, we engineered biosynthetic coiled-coil 'bundlemer' peptides as modular building blocks that can be conjugated and assembled into complex, higher-ordered materials. Using recombinant expression, we produced peptides and peptide fusion constructs that are otherwise difficult to achieve via solid-phase peptide synthesis. An N-terminal fusion protein with a pH-cleavable intein-inclusion body facilitated simple, scarless purification directly from insoluble fractions. We further incorporated SpyTag (-VPTIVMVDAYKRYK-) and sortase-recognition motifs (GGG-, -LPETGG) into the bundlemers, enabling precise, programmable assembly using genetically encoded and enzymatic ligation strategies. Using sortase-mediated ligation, we polymerized a single bundlemer into fibrillar structures, which were confirmed via TEM, SEC-MALS, SDS-PAGE, and native gels. Additionally, we constructed multicomponent architectures with a layered bundlemer and EGFP on an E2 nanocage using orthogonal linking chemistries, specifically SpyCatcher-SpyTag ligation and sortase-mediated ligation, and the associated increase in particle size and molecular weight was confirmed via TEM, DLS, and SDS-PAGE. This platform establishes a versatile framework for designing complex, protein-based nanostructures with defined architecture and function, offering possibilities in biomaterials engineering, targeted drug delivery, and synthetic biology.
{"title":"Protein-Based Nanostructures: Column-free Biosynthesis of Bundlemer Peptides with Programmable, Orthogonally Reactive Handles for Nanomaterial Construction.","authors":"Caitlin D'Ambrosio,Nadim Massad,Amanda L McCahill,William Rears,Pierre Rouviere,Jeffery G Saven,Darrin J Pochan,Christopher J Kloxin,April M Kloxin,Wilfred Chen","doi":"10.1021/acsami.5c17204","DOIUrl":"https://doi.org/10.1021/acsami.5c17204","url":null,"abstract":"Nature's protein sequences dictate structure and function across scales, from the nanometer-scale of viral capsids to micrometer- to millimeter-scale architectures of extracellular matrices and tissues. This multiscale precision underlies diverse functions, including molecular recognition, mechanical support, and dynamic responsiveness. Mimicking this complexity synthetically remains challenging. To address this, we engineered biosynthetic coiled-coil 'bundlemer' peptides as modular building blocks that can be conjugated and assembled into complex, higher-ordered materials. Using recombinant expression, we produced peptides and peptide fusion constructs that are otherwise difficult to achieve via solid-phase peptide synthesis. An N-terminal fusion protein with a pH-cleavable intein-inclusion body facilitated simple, scarless purification directly from insoluble fractions. We further incorporated SpyTag (-VPTIVMVDAYKRYK-) and sortase-recognition motifs (GGG-, -LPETGG) into the bundlemers, enabling precise, programmable assembly using genetically encoded and enzymatic ligation strategies. Using sortase-mediated ligation, we polymerized a single bundlemer into fibrillar structures, which were confirmed via TEM, SEC-MALS, SDS-PAGE, and native gels. Additionally, we constructed multicomponent architectures with a layered bundlemer and EGFP on an E2 nanocage using orthogonal linking chemistries, specifically SpyCatcher-SpyTag ligation and sortase-mediated ligation, and the associated increase in particle size and molecular weight was confirmed via TEM, DLS, and SDS-PAGE. This platform establishes a versatile framework for designing complex, protein-based nanostructures with defined architecture and function, offering possibilities in biomaterials engineering, targeted drug delivery, and synthetic biology.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"133 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711045","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}
Modulating the local inflammatory environment and restoring nucleus pulposus cell (NPC) function are essential strategies for mitigating IVDD. In this study, a microgel-based delivery system for microRNA therapeutics, termed POCM@MCCP (PMCCP), was developed. The system employs dual-network hydrogel microspheres composed of chitosan, citric acid, and poly(vinyl alcohol) (CCP), further functionalized with metal-phenolic networks (MPNs) formed from strontium ions (Sr2+) and epigallocatechin gallate (EGCG). This microgel enables dynamic, stimulus-responsive loading of phenylboronic acid-modified oxidized hyaluronic acid (PBA-oHA)-coated miR-155/chito-oligosaccharide (COS) complexes (POCM) through boronate ester linkages. The mechanical elasticity and stability of the CCP microspheres support the consistent and prolonged release of miR-155 even under mechanical compression. Incorporation of MPNs further endows the system with the ability to modulate and suppress the inflammatory microenvironment. In oxidative microenvironments, the boronate bonds cleave, triggering the release of POCM and its subsequent CD44 receptor-mediated internalization by NPCs. Subsequently, miR-155 and COS are released within the acidic intracellular space, modulating the Bcl-2/Bax/Caspase-3 signaling cascade and scavenging intracellular ROS, respectively. Both in vitro and in vivo IVDD models demonstrated that this multifunctional platform effectively suppresses inflammation and restores NPC function, highlighting its potential as a promising therapeutic strategy for IVDD.
{"title":"Enhanced Elastic Multifunctional Dual-Network Hydrogel Microspheres for the Treatment of Intervertebral Disc Degeneration through Inflammation Modulation and Apoptosis Inhibition","authors":"Fei Ma, Chuan Guo, Yuheng Liu, Daqiang Zheng, Walter Munesu Chirume, Dengbo Yao, Weiqiang Lan, Zhen Zhao, Chen Fan, Yu Wang, Qingquan Kong","doi":"10.1021/acsami.5c17783","DOIUrl":"https://doi.org/10.1021/acsami.5c17783","url":null,"abstract":"Modulating the local inflammatory environment and restoring nucleus pulposus cell (NPC) function are essential strategies for mitigating IVDD. In this study, a microgel-based delivery system for microRNA therapeutics, termed POCM@MCCP (PMCCP), was developed. The system employs dual-network hydrogel microspheres composed of chitosan, citric acid, and poly(vinyl alcohol) (CCP), further functionalized with metal-phenolic networks (MPNs) formed from strontium ions (Sr<sup>2</sup><sup>+</sup>) and epigallocatechin gallate (EGCG). This microgel enables dynamic, stimulus-responsive loading of phenylboronic acid-modified oxidized hyaluronic acid (PBA-oHA)-coated miR-155/chito-oligosaccharide (COS) complexes (POCM) through boronate ester linkages. The mechanical elasticity and stability of the CCP microspheres support the consistent and prolonged release of miR-155 even under mechanical compression. Incorporation of MPNs further endows the system with the ability to modulate and suppress the inflammatory microenvironment. In oxidative microenvironments, the boronate bonds cleave, triggering the release of POCM and its subsequent CD44 receptor-mediated internalization by NPCs. Subsequently, miR-155 and COS are released within the acidic intracellular space, modulating the Bcl-2/Bax/Caspase-3 signaling cascade and scavenging intracellular ROS, respectively. Both <i>in vitro</i> and <i>in vivo</i> IVDD models demonstrated that this multifunctional platform effectively suppresses inflammation and restores NPC function, highlighting its potential as a promising therapeutic strategy for IVDD.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"28 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718218","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}