ACS Applied Materials & Interfaces最新文献

{"title":"Nanofiltration Membrane with Enhanced Ion Selectivity Based on a Precision-Engineered Ultrathin Polyethylene Supporting Layer","authors":"Zhenxu Huang, Shiyu Zhang, Jing Liang, Tao Wu, Runnan Zhang, Xinda You, Runlai Li, Xianchun Chen, Qiang Fu","doi":"10.1021/acsami.4c12887","DOIUrl":"https://doi.org/10.1021/acsami.4c12887","url":null,"abstract":"Nanofiltration (NF) technology is increasingly used in the water treatment and separation fields. However, most research has focused on refining the selective layer while overlooking the potential role of the supporting layer. With expertise in ultrathin polymer films, particularly in the production of polyethylene (PE) membranes, we explore the possibility of improving NF membrane performance by precisely controlling the structure and surface properties of the ultrathin supporting layer in this work. Here, we introduced an innovative NF membrane that used a submicrometer ultrathin PE membrane produced through a biaxial stretching process, which is significantly thinner than commercial PE membranes available on the market. The core innovations are as follows: first, we focused on precise control of the supporting layer rather than just the selective layer, achieving significant enhancements in overall NF membrane performance; second, the ultrathin PE supporting layer served as a tunable interface for interfacial polymerization, offering possibilities for structural control of the selective layer and advancing membrane performance innovations. The resulting NF membrane boasts an overall thickness of ∼630 nm, which represents the thinnest NF membrane documented to date. This ultrathin NF membrane showed an ultrahigh Cl^–/SO₄^2– selectivity of 338.03, placing it at the forefront of existing literature. This study sheds light on the important role of the supporting layer in the preparation of selective layers. We believe that this approach has the potential to contribute to the development of ultrathin, high-performance NF membranes.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609873","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}

{"title":"pH and Redox Dual-Responsive Nanoparticle with Enhanced Dendritic Cell Maturation for Cancer Therapy","authors":"Dohyun Yun, Erinn Fagan, Dongik Shin, Woojin Back, Susam Lee, Mun Sik Kim, Heewon Park, Ji-Ho Park, Yeu-Chun Kim","doi":"10.1021/acsami.4c15342","DOIUrl":"https://doi.org/10.1021/acsami.4c15342","url":null,"abstract":"Type I interferons (IFNs) are essential for activating dendritic cells (DCs) and presenting tumor-associated antigens to T cells. IFNs are primarily produced from DCs among immune cells. A combination of chemotherapy and metalloimmunotherapy induces IFN production by activating the cyclic GMP-AMP synthase-stimulator of interferon genes (cGAS-STING) pathway. However, chemotherapeutic agents deplete DC populations, suppressing immunostimulatory activities, despite their potent anticancer activities. Furthermore, an optimal ratio between chemotherapeutic agents and metal for activating DCs at the highest level has not been reported, and evidence for ensuring DC survival is lacking. In this study, we hypothesized that there is an optimal ratio to yield the highest DC maturation and anticancer activity with minimal DC depletion. To demonstrate it, we have designed a pH and redox dual-responsive nanoparticle, MnO₂@BSA@DOX (MD), to prevent DCs from depleting and activate the cGAS-STING pathway both in cancer cells and DCs, inducing considerable levels of IFNs and maturation. MD consists of a core-layer structure, a manganese dioxide (MnO₂) core, and a cross-linked layer with bovine serum albumin (BSA) and doxorubicin (DOX), with a specific ratio of DOX to manganese. MD exhibits structure-based selectivity between cancer cells and DCs by targeting the extracellular pH of the tumor microenvironment and intracellular redox reactions in cancer cells. Among various formulations, the 1:1 ratio shows the highest maturation with no significant depletion. Moreover, it induces distinct cytotoxicity in cancer cells through apoptosis and cGAS-STING activation, leading to increased calreticulin expression and enhanced DC phagocytosis. Consequently, it results in superior tumor suppression and prolonged survival with the high accumulation of MD in the tumor and no observed systemic toxicities, highlighting its potential as a therapeutic agent in cancer treatments.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609875","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}

{"title":"High-Endurance Long-Term Potentiation in Neuromorphic Organic Electrochemical Transistors by PEDOT:PSS Electrochemical Polymerization on the Gate Electrode.","authors":"Federica Mariani, Francesco Decataldo, Filippo Bonafè, Marta Tessarolo, Tobias Cramer, Isacco Gualandi, Beatrice Fraboni, Erika Scavetta","doi":"10.1021/acsami.3c10576","DOIUrl":"10.1021/acsami.3c10576","url":null,"abstract":"<p><p>The brain exhibits extraordinary information processing capabilities thanks to neural networks that can operate in parallel with minimal energy consumption. Memory and learning require the creation of new neural networks through the long-term modification of the structure of the synapses, a phenomenon called long-term plasticity. Here, we use an organic electrochemical transistor to simulate long-term potentiation and depotentiation processes. Similarly to what happens in a synapse, the polymerization of the 3,4-ethylenedioxythiophene (EDOT) on the gate electrode modifies the structure of the device and boosts the ability of the gate potential to modify the conductivity of the channel. Operando AFM measurements were carried out to demonstrate the correlation between neuromorphic behavior and modification of the gate electrode. Long-term enhancement depends on both the number of pulses used and the gate potential, which generates long-term potentiation when a threshold of +0.7 V is overcome. Long-term depotentiation occurs by applying a +3.0 V potential and exploits the overoxidation of the deposited PEDOT:PSS. The induced states are stable for at least 2 months. The developed device shows very interesting characteristics in the field of neuromorphic electronics.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"107589583","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}

{"title":"Biohybrid Energy Storage Circuits Based on Electronically Functionalized Plant Roots.","authors":"Daniela Parker, Abdul Manan Dar, Adam Armada-Moreira, Iwona Bernacka Wojcik, Rajat Rai, Daniele Mantione, Eleni Stavrinidou","doi":"10.1021/acsami.3c16861","DOIUrl":"10.1021/acsami.3c16861","url":null,"abstract":"<p><p>Biohybrid systems based on plants integrate plant structures and processes into technological components targeting more sustainable solutions. Plants' biocatalytic machinery, for example, has been leveraged for the organization of electronic materials directly in the vasculature and roots of living plants, resulting in biohybrid electrochemical devices. Among other applications, energy storage devices were demonstrated where the charge storage electrodes were seamlessly integrated into the plant tissue. However, the capacitance and the voltage output of a single biohybrid supercapacitor are limited. Here, we developed biohybrid circuits based on functionalized conducting roots, extending the performance of plant based biohybrid energy storage systems. We show that root-supercapacitors can be combined in series and in parallel configuration, achieving up to 1.5 V voltage output or up to 11 mF capacitance, respectively. We further demonstrate that the supercapacitors circuit can be charged with an organic photovoltaic cell, and that the stored charge can be used to power an electrochromic display or a bioelectronic device. Furthermore, the functionalized roots degrade in composting similarly to native roots. The proof-of-concept demonstrations illustrate the potential of this technology to achieve more sustainable solutions for powering low consumption devices such as bioelectronics for agriculture or IoT applications.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140026758","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}

{"title":"Laser-Controlled Information Releasing and Hiding Based on Perovskite Phosphors","authors":"Panpan Li, Lifan Shen, Yuhang Zhang, Desheng Li, Edwin Yue Bun Pun, Hai Lin","doi":"10.1021/acsami.4c17038","DOIUrl":"https://doi.org/10.1021/acsami.4c17038","url":null,"abstract":"Laser-active interference with high confidentiality and convenience opens up a cutting-edge path for releasing and hiding key targets; however, its development still faces enormous challenges owing to the difficulty of concealing objects. Herein, a novel conceptual design for laser-controlled information release and hiding (LIRH) is proposed and successfully realized. Cs₂NaInCl₆:Er³⁺, Yb³⁺ (CNIC:Er, Yb) perovskite microcrystal is adopted as a carrier for LIRH implementation, exhibiting excellent up-conversion (UC) emission under NIR (980 and 1530 nm) irradiation due to its ultralow phonon energy. The fluorescence intensity crossover and outstanding photon output capacity are revealed in comparison with Er³⁺/Yb³⁺ codoped and Er³⁺ single-doped CNIC phosphors under different laser sources, and the obvious difference in quantum yields (QY) under 980 and 1530 nm excitation provides theoretical possibility for LIRH. More importantly, the obtained LIRH features high stability at temperatures up to 413 K, showing good adaptability in various potential scenarios. Moreover, CNIC:Er, Yb is further combined with polyacrylonitrile (PAN) polymer to form fluorescent fibers with exceptional crystal stability and composite flexibility, thus making the LIRH code a reality based on perovskite composite phosphors. The laser-active invisibility offers an innovative idea for LIRH, further extending the application of LIRH in the field of information encryption, which has promising prospects in information safety, advanced anticounterfeiting, and smart responsive materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601847","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}

{"title":"Salt-Concentrated Electrolyte Constructing High Elasticity Modulus Interphase for Li-Rich Layered Oxide Cathode","authors":"Zhijie Han, Yuan Liang, Shu Zhao, Qianwen Zhu, Jingteng Zhao, Errui Wang, Shiqi Liu, Boya Wang, Congyu Xu, Bing Yu, Haijun Yu","doi":"10.1021/acsami.4c10787","DOIUrl":"https://doi.org/10.1021/acsami.4c10787","url":null,"abstract":"Stable electrolytes are urgently required for lithium-ion batteries based on lithium-rich layered oxides (LLOs), which generally suffer from fast capacity and voltage decay at high voltages up to 4.8 V. Herein, we report a salt-concentrated electrolyte consisting of 4 M lithium hexafluorophosphate (LiPF₆) salt in ester solvents of fluoroethylene carbonate (FEC) and dimethyl carbonate (DMC) to alleviate the above challenges. The solvent structure in the 4 M electrolyte shows more volatile DMC integrated with Li⁺ and more free antioxidative FEC compared with a 1 M electrolyte, broadening the operation voltage. Simultaneously, this electrolyte endows a thin yet high elasticity modulus LiF-rich interphase on the LLOs surface, which can effectively prevent diverse side reactions and transition metal migration, consequently improving the electrochemical performance with a voltage decay of only 0.46 mV/cycle and capacity retention of 80.3% after 500 cycles. This simple and effective approach boosts the development of high-energy-density batteries using LLOs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609869","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}

{"title":"Toward Commercial-Scale Perovskite Solar Cells: The Role of ALD-SnO2 Buffer Layers in Performance and Stability","authors":"Ai Lan, Hong Lu, Bin Huang, Fei Chen, Zhikuan Chen, Juan Wang, Liqing Li, Hainam Do","doi":"10.1021/acsami.4c14954","DOIUrl":"https://doi.org/10.1021/acsami.4c14954","url":null,"abstract":"Hybrid organic–inorganic perovskite solar cells (PSCs) have shown significant potential in photovoltaic applications due to their superior optoelectronic properties. However, the conventional electron transport layer (ETL) of C₆₀ in PSCs poses challenges such as incomplete coverage and metal diffusion, leading to reduced performance and stability. This work explores the efficacy of atomic layer deposition (ALD) of SnO₂ as an interlayer between C₆₀ and electrode to enhance the performance and stability of devices. Devices with varying SnO₂ thicknesses were fabricated, revealing that a 15 nm ALD-SnO₂ layer optimally improved the power conversion efficiency (PCE) to 23.85%, compared to the 22.86% achieved with a BCP layer. Moreover, the SnO₂-based devices exhibited superior open-circuit voltage (<i>V</i>_OC), short-circuit current density (<i>J</i>_SC), and fill factor (FF). Modules (30 × 30 cm) with ALD-SnO₂ demonstrated notable enhancements in efficiency and uniformity, suggesting the potential for scalable commercial applications. Photoluminescence (PL) and electrochemical impedance spectroscopy (EIS) analyses confirmed the improved charge extraction and reduced recombination with the SnO₂ buffer layer. This research indicates that ALD-SnO₂ is a promising interlayer candidate for PSCs, providing a pathway toward higher efficiency and stability in perovskite solar technology.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609874","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}

{"title":"Tailored Design of a Nanoporous Structure Suitable for Thick Si Electrodes on a Stiff Oxide-Based Solid Electrolyte.","authors":"Kohei Marumoto, Kiyotaka Nakano, Yuki Kondo, Minoru Inaba, Takayuki Doi","doi":"10.1021/acsami.4c15894","DOIUrl":"10.1021/acsami.4c15894","url":null,"abstract":"<p><p>Oxide-based all-solid-state batteries are ideal next-generation batteries that combine high energy density and high safety, but their realization requires the development of interface bonding technology between the stiff solid electrolyte and electrode. Even if the interface could be bonded, it is difficult to hold the interface, because only the electrode expands/contracts unilaterally during charge/discharge reactions. In particular, silicon (Si), which has eagerly awaited as a next-generation negative-electrode material for many years, changes in volume by several hundred percent. To solve these problems, in this work, highly porous silicon oxide (SiO_<i>x</i>) electrodes with different porous structures were fabricated on a stiff garnet-type Li₇La₃Zr₂O₁₂ solid electrolyte, the three-dimensional nanoporous structure was analyzed quantitatively, and the charge/discharge characteristics were investigated. The microscopic observation and electrochemical analysis revealed how we should control the porous structure, such as sizes of pores and SiO_<i>x</i>, size distribution, and porosity, for repeated and stable charge/discharge cycles. In addition, the resultant porous SiO_<i>x</i> electrodes demonstrated superior charge/discharge cycle performance even when it thickened to 5 μm, whereas non-porous SiO_<i>x</i> easily peeled off from the solid electrolyte when its thickness exceeded 0.1 μm. The thick SiO_<i>x</i> films greatly improved the energy density per unit area (mAh cm^-2). Nanosized fine pores with an interconnected open-pore architecture effectively mitigated the internal and interfacial stress upon expansion (charge)/contraction (discharge) of Si, and as a result, the thick and porous SiO_<i>x</i> electrode maintained the interfacial joint with the stiff solid electrolyte after repeated charge/discharge cycles. These results will provide useful insights for effectively designing more practical porous SiO_<i>x</i> powder effectively.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520291","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}

{"title":"Emerging Frontiers in <i>In Situ</i> Forming Hydrogels for Enhanced Hemostasis and Accelerated Wound Healing.","authors":"Sanchita Sarkhel, Amit Jaiswal","doi":"10.1021/acsami.4c07108","DOIUrl":"10.1021/acsami.4c07108","url":null,"abstract":"<p><p>With a surge in the number of accidents and chronic wounds worldwide, there is a growing need for advanced hemostatic and wound care solutions. In this regard, in situ forming hydrogels have emerged as a revolutionary biomaterial due to their inherent properties, which include biocompatibility, biodegradability, porosity, and extracellular matrix (ECM)-like mechanical strength, that render them ideal for biomedical applications. This review demonstrates the advancements of <i>in situ</i> forming hydrogels, tracing their evolution from injectable to more sophisticated forms, such as sprayable and 3-D printed hydrogels. These hydrogels are designed to modulate the pathophysiology of wounds, enhancing hemostasis and facilitating wound repair. The review presents different methodologies for in situ forming hydrogel synthesis, spanning a spectrum of physical and chemical cross-linking techniques. Furthermore, it showcases the adaptability of hydrogels to the dynamic requirements of wound healing processes. Through a detailed discussion, this article sheds light on the multifunctional capabilities of these hydrogels such as their antibacterial, anti-inflammatory, and antioxidant properties. This review aims to inform and inspire continued advancement in the field, ultimately contributing to the development of sophisticated wound care solutions that meet the complexity of clinical needs.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542834","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}

{"title":"Multifunctional Composite Separator Based on NiS₂/NiSe₂ Homologous Heterostructure Polyhedron Promotes Polysulfide Conversion for High Performance Lithium-Sulfur Batteries.","authors":"Bo Zhang, Jiaxin Qie, Jiyuan You, Xiaotong Gao, Yuqian Li, Wenju Wang","doi":"10.1021/acsami.4c13619","DOIUrl":"10.1021/acsami.4c13619","url":null,"abstract":"<p><p>The shuttle effect significantly hinders the industrialization of high-energy-density lithium-sulfur batteries. To address this issue, NiS₂/NiSe₂ homologous heterostructure polyhedron (HHP) composite separators were developed to immobilize polysulfides and promote their swift conversion. An in-situ visualization symmetrical cell was specifically designed to show the rapid polysulfide adsorption capability of NiS₂/NiSe₂ HHP, while the electrolyte-separator interfacial contact behavior was simulated to elucidate the mechanism of action of the composite separator in affecting the homogeneous nucleation of lithium metal surfaces. The electrochemical experimental result highlights the substantial enhancement in the reaction kinetics of polysulfides facilitated by NiS₂/NiSe₂ HHP, owing to its high Li⁺ diffusion coefficient and Li₂S deposition capacity. The NiS₂/NiSe₂ HHP cells demonstrate high initial specific capacity (1224.1 mAh g^-1) at 0.2 C and minimal decay rates (0.073%) at 2 C. The NiS₂/NiSe₂ HHP separator has high electrochemical catalytic activity with multiple adsorption sites, enabling the rapid polysulfide conversion and contributing to the preparation of high-performance lithium-sulfur batteries.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556524","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}