ACS Applied Materials & Interfaces最新文献

{"title":"Triple-Mode Protection with Ln³⁺ Ion-Doped Core-Heptad-Shell Single Nanocrystals for High-Level Security Applications.","authors":"Venkata N K B Adusumalli, Hyeon Jung Yu, Yeongchang Goh, Sang Hwan Nam, Yong Il Park","doi":"10.1021/acsami.4c11798","DOIUrl":"10.1021/acsami.4c11798","url":null,"abstract":"<p><p>In this work, oleic acid (OA)-capped core-heptad-shell (CHS) nanocrystals (NCs) that exhibit multiple emissions achieved through downshifting and orthogonal upconversion are synthesized via layer-by-layer thermal decomposition. This method enables the downshifting process to be accommodated by doping ions in the inert space between two upconversion patterns (the core and fourth shell) and doping Ce/Tb or Ce/Eu ions in the NaGdF₄ layer for the first time. These developed CHS NCs exhibit different emission colors via 980 and 800 nm orthogonal upconversion and downshifting emissions under 256 nm UV excitation in hexane solvent. Furthermore, surface-functionalized OA is removed using mild acid treatment. The resulting bare CHS NCs disperse well in water and exhibit 21.60-fold and 43.59-fold higher Ce/Tb and Ce/Eu luminescence intensities, respectively, than the OA-capped CHS NCs. These NCs are mixed with a carboxymethylcellulose (CMC) polymer in an aqueous medium to form a CMC-CHS NC gel. Invisible patterns and QR codes are printed on nonfluorescent paper using gels and screen-printing techniques. These patterns and QR codes exhibit three different emission colors under three different excitations. This method can be used for high-level anticounterfeiting 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":"142542749","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":"A 3D-Printed Bionic Membrane with Autonomously Passive Unidirectional Liquid Transfer Capability for Water Condensation, Collection, and Purification.","authors":"Sen Meng, Cheng Yao, Gang Liu, Huaifei Chen, Taishan Hu, Zhicheng Zhang, Jie Yang, Wei Yang","doi":"10.1021/acsami.4c11869","DOIUrl":"10.1021/acsami.4c11869","url":null,"abstract":"<p><p>Interfacial solar vapor generation is a promising technology for alleviating the current global water crisis, and the evaporation rate and efficiency have approached the theoretical limit. In a practical interfacial evaporation water purification system, the collection rate of purified water is typically lower than the evaporation rate. Passive collection devices based on gravity are susceptible to environmental influences and exhibit low collection efficiency, while active collection devices consuming external energy suffer from complex device systems and extra energy consumption. Given that both collection devices are nonselective and unable to distinguish contaminants mixed in the vapor, bionic membranes with autonomously passive and unidirectional water transfer capacity are developed through 3D printing for efficient water collection. More importantly, the bionic membranes are capable of high-speed water transportation without the need for external energy or gravity drive and liquid-selective transportation for separating oily pollutants from the collected products. The directional transport property facilitates the modular assembly of the bionic membrane, extending its application to practical large-scale solar-driven seawater desalination systems.</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":"142542827","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":"Correction to \"Photo-Cross-Linkable Methacrylated Gelatin and Hydroxyapatite Hybrid Hydrogel for Modularly Engineering Biomimetic Osteon\".","authors":"Yicong Zuo, Xiaolu Liu, Dan Wei, Jing Sun, Wenqian Xiao, Huan Zhao, Likun Guo, Qingrong Wei, Hongsong Fan, Xingdong Zhang","doi":"10.1021/acsami.4c18156","DOIUrl":"10.1021/acsami.4c18156","url":null,"abstract":"","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":"142542832","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":"Enhancing Hydrogen Evolution Reaction through the Improved Mass Transfer and Charge Transfer by Bimetal Nodes.","authors":"Zhihui Li, Xinyu Zhang, Yiran Teng, Hanming Zhang, Tongguang Xu, Fei Teng","doi":"10.1021/acsami.4c11560","DOIUrl":"10.1021/acsami.4c11560","url":null,"abstract":"<p><p>The high cost of hydrogen production by water electrolysis severely challenges its commercial application. It is highly desirable to develop efficient electrocatalysts and innovative electrolytic cells. Introducing additional metal nodes to form bimetallic metal-organic framework (MOF) is a simple, feasible strategy to overcome the poor electrocatalytic performance of single-metal MOF. In this study, the hydrothermal method is used to synthesize bimetallic Ni<i>_x</i>Co_y-BTC. It is found that for hydrogen evolution reaction (HER), Ni_0.8Co_0.2-BTC merely requires a potential of -0.203 V (vs reverse hydrogen electrode, RHE) to achieve 10 mA cm^-2, which is significantly lower than that of Ni-BTC (-0.341 V vs RHE). Notably, electrochemical impedance spectroscopy (EIS) and distribution of relaxation time (DRT) analysis indicate that Ni<i>_x</i>Co<i>_y</i>-BTC has improved charge transfer and mass transfer process, compared with Ni-BTC. Electron paramagnetic resonance (EPR) confirms that Ni_0.8Co_0.2-BTC has more unpaired electrons than Ni-BTC. Density functional theory (DFT) calculations show that compared with Ni-BTC, Ni<i>_x</i>Co<i>_y</i>-BTC is more thermodynamically favorable for the adsorption of H⁺, OH^-, and H₂O. It demonstrates that the change of mass transfer caused by bimetallic nodes and the delicate variation of MOF surface play an important role in the electrochemical process. Moreover, a novel electrolytic cell was developed using a methanol oxidation reaction (MOR) to replace oxygen evolution reaction (OER). In this MOR-based electrolytic cell, a current density of 50 mA cm^-2 can be achieved at only a cell voltage of 1.85 V, which is lower than the 2.22 V of OER-based electrolytic cell, suggesting that 16.7% electric energy can be saved. At the same time, the Faraday efficiency (FE, 98.2%) of the MOR-based cell is higher than that (94.5%) of the OER-based cell. This research offers a promising strategy for low-cost hydrogen production.</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":"142542836","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":"Human Muscle Inspired Anisotropic and Dynamic Metal Ion-Coordinated Mechanically Robust, Stretchable and Swelling-Resistant Hydrogels for Underwater Motion Sensing and Flexible Supercapacitor Application.","authors":"Ashis Ghosh, Sangita Pandit, Sudhir Kumar, Debabrata Pradhan, Rajat Kumar Das","doi":"10.1021/acsami.4c15018","DOIUrl":"10.1021/acsami.4c15018","url":null,"abstract":"<p><p>Mechanically robust and anisotropic conductive hydrogels have emerged as crucial components in the field of flexible electronic devices, since they possess high mechanical properties and intelligent sensing capabilities. However, the hydrogels often swell on exposure to aqueous medium because of their hydrophilicity, which compromises their mechanical properties. Additionally, the hydrogels' isotropic polymeric networks demonstrate isotropic ion transport, which significantly diminishes the sensing capabilities of electrical devices based on hydrogels. These factors greatly limit their use in flexible and wearable sensors. In this study, we have developed poly(acrylamide-<i>co</i>-maleic acid-<i>co</i>-butyl acrylate) based anisotropic hydrogels by prestretching and drying, followed by ionic cross-linking to fix the alignment. The anisotropic arrangement of the polymer network resulted in significant improvements in mechanical performance and electrical conductivity along the prestretching direction. This anisotropic hydrogel combines hydrophobic and metal ion-ligand interactions, enhancing the maximum tensile strength up to 11 MPa along the prestretching direction, about 3 times higher than in the perpendicular direction. The optimized 200% prestretched hydrogel exhibited high tensile strength (7 MPa), flexibility (fracture strain 370%), high toughness (16 MJ m^-3) and antiswelling behavior in water (equilibrium swelling ratio 2% after 15 days). alongside higher conductivity (3 times higher) and strain sensing ability (4 times higher gauge factor) along the prestretching direction. The hydrogel demonstrated efficient and stable underwater sensing for underwater communication and to monitor human limb position and movement. The anisotropic hydrogel electrolyte-based flexible supercapacitor exhibited 117 Fg^-1 specific capacitance at 0.5 Ag^-1, and maximum energy density 5.85 Whkg^-1, significantly higher than the corresponding values for the isotropic hydrogel-based device (88 F g^-1 and 4.4 Whkg^-1, respectively). This hydrogel mimics the structural design of unidirectionally oriented muscle fibers, showing better direction dependent functional properties than the corresponding isotropic hydrogel. The anti-swelling ability and retention of mechanical and conductive properties of these hydrogels in aqueous environment suggest long-term usage capability of these functional materials.</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":"142563335","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":"Spraying-Deposited Transparent p-Type Sn-Doped CuI Film and Its Ultrahigh-Speed Self-Powered Photodetector.","authors":"Li Xu, Haowei Liu, Jianmei Xu, Wei Zhou, Zhihong Yang, Wei Xu, Jian Sun","doi":"10.1021/acsami.4c11974","DOIUrl":"10.1021/acsami.4c11974","url":null,"abstract":"<p><p>The exploitation of simply processed p-type semiconductors and photodetectors with promising optoelectrical properties remains challenging yet essential for current and future advanced optoelectronic applications. Transparent p-type CuI and Sn-doped CuI (Cu-Sn-I) films and their self-powered photodetectors have been successfully fabricated by the spraying method. It is found that the incorporation of Sn dopants enhances the optical, electrical, and photoelectric properties of CuI thin films as well as their corresponding self-powered heterojunction photodetectors. This improvement of the optoelectrical properties of the Cu-Sn-I film and its photodetector can be attributed to the adjustment of the acceptor defect level and increased hole concentration resulting from Sn doping. The Cu-Sn-I/n-Si photodetector exhibits a responsivity of 10.7 mA/W, a detectivity of 6.79 × 10¹¹ Jones, and a response time of 77 μs/30 μs (0 V bias). The response time exhibits the fastest rise and decay times compared with the other CuI-based self-powered UV photodetectors in recent years, showcasing promising applications in the realm of transparent electronics moving forward. This study also presents an effective strategy for enhancing the electrical properties of p-type semiconductors and devices through effective doping.</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":"142574747","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":"Unravelling the Electrical Field Induced Ion Migration in Flexible OLEDs with PEDOT:PSS Electrodes.","authors":"Chenxi Liu, Mengze Li, Yifan Wang, Zijie Hou, Jian Chen, Kun Cao, Lihui Liu, Shufen Chen","doi":"10.1021/acsami.4c13460","DOIUrl":"10.1021/acsami.4c13460","url":null,"abstract":"<p><p>The development of flexible organic light-emitting didoes (FOLEDs) has spurred the research on flexible transparent electrodes (FTEs). Poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) is one of the most attractive FTEs due to its adjustable conductivity and compatibility with low-cost and large-scale solution processing techniques. Significantly, highly efficient FOLEDs have been achieved with modified PEDOT:PSS FTEs. However, the intrinsic mechanisms that contribute to device degradation of FOLEDs utilizing PEDOT:PSS FTEs have not yet been fully elucidated. In this work, three ionic liquids (ILs) are used to enhance the electrical conductivity and mechanical flexibility of PEDOT:PSS FTEs. Simultaneously, the influence of the electric field induced ion migration from PEDOT:PSS FTEs on the operational stability of FOLEDs is unraveled. We find that the ILs with larger ionic radii and higher steric hindrance are beneficial to suppressing the electrical field induced ion migration and improving the operational stability of FOLEDs. Finally, large-area and high-performance FOLEDs are achieved based on the IL of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide modified PEDOT:PSS FTEs, which demonstrate a high current efficiency of 98.1 cd/A and a longer lifetime of 66.7 min. This finding may promote the practical application of PEDOT:PSS FTEs in flexible optoelectronics.</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":"142574757","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":"A Monte Carlo Approach for Simulating Electrical Conductivity in Highly Porous Ceramic Composites: Impact of Internal Structure.","authors":"Daniel Budáč, Vojtěch Miloš, Michal Carda, Martin Paidar, Karel Bouzek, Jürgen Fuhrmann","doi":"10.1021/acsami.4c08287","DOIUrl":"10.1021/acsami.4c08287","url":null,"abstract":"<p><p>Porous ceramic composites play an important role in several applications. This is due to their unique properties resulting from a combination of various materials. Determination of the composite properties and structure is crucial for their further development and optimization. However, composite analysis often requires complex, expensive, and time-demanding experimental work. Mathematical modeling represents an effective tool to substitute experimental approach. The present study employs a Monte Carlo 3D equivalent electronic circuit network model developed to analyze a highly porous composite on the basis of minimum easily obtainable input parameters. Solid oxide cell electrodes were used as a model example, and this study focuses primarily on materials with a porosity of 55% and higher, characterized by deviation of behavior from those of lower void fraction share. This task is approached by adding to the original Monte Carlo model an additional parameter defining the void phase coalescence phenomenon. The enhanced model accurately simulates electrical conductivity for experimental samples of up to 75% porosity. Using sample composition, single-phase properties, and experimentally determined conductivity, this model allows us to estimate data of the internal structure of the material. This approach offers a rapid and cost-effective method to study material microstructure, providing insights into properties, such as electrical conductivity and heat conductivity. The present research thus contributes to advancing predictive capabilities in understanding and optimizing the performance of composite materials with potential in various technological 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":"142574802","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":"Skeletal Editing of Energetic Materials: Acid-Catalyzed One-Step Synthesis of Bridged Triazoles as High-Energy-Density Materials via the Nef Reaction","authors":"Shreyasi Banik, Navaneet Kumar, Vikas D. Ghule, Srinivas Dharavath","doi":"10.1021/acsami.4c16858","DOIUrl":"https://doi.org/10.1021/acsami.4c16858","url":null,"abstract":"Thermally stable insensitive energetic materials have captivated significant attention from the global research community due to their potential impact. In this study, a series of symmetric and asymmetric nitromethyl-bridged triazole compounds were synthesized from pyrimidine moieties via a skeletal editing approach. Additionally, carbonyl-bridged compounds were synthesized in a single step by using acid-catalyzed Nef reactions from their nitromethyl precursors. Peripheral modifications of pyrimidine resulted in fused energetic moieties. All synthesized compounds were fully characterized by using infrared spectroscopy, high-resolution mass spectrometry, multinuclear magnetic resonance spectroscopy, elemental analysis, and differential scanning calorimetry. Single-crystal X-ray diffraction analysis confirmed the structures of compounds <b>4</b> and <b>10</b>. The newly synthesized moieties exhibit densities ranging from 1.75 to 1.86 g cm^–3, detonation velocities between 8044 and 8608 m s^–1, and detonation pressures between 23.10 and 30.31 GPa. Notably, compounds <b>9</b> and <b>10</b> demonstrate exceptional heat resistance, with decomposition temperatures of 315 and 335 °C, respectively. Computational studies, including density functional theory, quantum theory of atoms in molecules, noncovalent interactions, and electrostatic surface potential analysis, account for hydrogen-bonding and noncovalent interactions. This work highlights the potential of skeletal editing in the development of high-performing, thermally stable energetic 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":"142609753","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":"Chitosan-Based Electronics: The Importance of Acid Strength and Plasticizing Additives on Device Performance","authors":"Bahar Ronnasi, Sophia P. McKillop, May Ourabi, Matthew Perry, Heather A. Sharp, Benoît H. Lessard","doi":"10.1021/acsami.4c10508","DOIUrl":"https://doi.org/10.1021/acsami.4c10508","url":null,"abstract":"A rise in demand for disposable consumer electronics such as smart packaging, wearable electronics, and single-use point-of-source sensors requires the development of eco-friendly and compostable electronic materials. Chitosan is derived from crustacean waste and offers high dielectric constant values without requiring rigorous purification, making it sustainable for large-scale electronic device manufacturing. When processed in acidic media, the protonated backbone of chitosan pairs with counterions from the acid dissociation to form chitosan thin films with electrical double layers (EDLs) and tunable capacitive properties. We report the importance of the choice of acid when processing chitosan by surveying a series of halogenated and biosourced acids with varying p<i>K</i>_a values and solutions with different pH values. Oxalic acid outperforms other acids, with a maximum areal capacitance of 161 nF·mm^–2. Tartaric acid and citric acid, despite lower capacitance values, showed promising results with a stable EDL capacitance and high reproducibility, making them optimal for large-area manufacturing. The incorporation of sorbitol as a plasticizer boosts the EDL formation onset of all chitosan–acid combinations to 1 × 10³–10⁵ Hz and improves reproducibility. High-performing single-walled carbon nanotube thin film transistors were made using chitosan-based dielectrics treated with different acids with and without sorbitol, leading to transconductance as high as ≈5.2 μS and <i>I</i>_on/<i>I</i>_off of 10⁵. The capacitors and transistors remain functional after one year of storage in ambient conditions. Overall, this study demonstrates durable high-performance electronics based on chitosan and stresses the importance of processing acid and the use of plasticizing additives, such as sorbitol.","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":"142609868","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}