960化工网
期刊名称:ACS Nanoscience Au
期刊ISSN:
期刊官方网站:
出版商:
出版周期:
影响因子:0
始发年份:0
年文章数:0
是否OA:
Assembly of Rolled-Up Collagen Constructs on Porous Alumina Textiles
ACS Nanoscience Au ( IF 0 ) Pub Date : 2023-06-01 , DOI: 10.1021/acsnanoscienceau.3c00008
DeepanjaleeDutta,NinaGraupner,JörgMüssig,DorotheaBrüggemann
Developing new techniques to prepare free-standing tubular scaffolds has always been a challenge in the field of regenerative medicine. Here, we report a new and simple way to prepare free-standing collagen constructs with rolled-up architecture by self-assembling nanofibers on porous alumina (Al2O3) textiles modified with different silanes, carbon or gold. Following self-assembly and cross-linking with glutaraldehyde, collagen nanofibers spontaneously rolled up on the modified Al2O3 textiles and detached. The resulting collagen constructs had an inner diameter of approximately 2 to 4 mm in a rolled-up state and could be easily detached from the underlying textiles. Mechanical testing of wet collagen scaffolds following detachment yielded mean values of 3.5 ± 1.9 MPa for the tensile strength, 41.0 ± 20.8 MPa for the Young’s modulus and 8.1 ± 3.7% for the elongation at break. No roll-up was observed on Al2O3 textiles without any modification, where collagen did not assemble into fibers, either. Blends of collagen and chitosan were also found to roll into fibrous constructs on silanized Al2O3 textiles, while fibrinogen nanofibers or blends of collagen and elastin did not yield such structures. Based on these differences, we hypothesize that textile surface charge and protein charge, in combination with the porous architecture of protein nanofibers and differences in mechanical strain, are key factors in inducing a scaffold roll-up. Further studies are required to develop the observed roll-up effect into a reproducible biofabrication process that can enable the controlled production of free-standing collagen-based tubes for soft tissue engineering.
Colloidal Synthesis and Photocatalytic Properties of Cu3NbS4 and Cu3NbSe4 Sulvanite Nanocrystals
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-06-24 , DOI: 10.1021/acsnanoscienceau.2c00021
Chen-YuChang,RobertoPrado-Rivera,MimiLiu,Cheng-YuLai,DanielaRRadu
Niobium sulvanites Cu3NbX4 (X = S, Se) have been theoretically predicted as promising candidates for solar photovoltaics and photocatalytic water splitting. This report outlines the first synthesis of Cu3NbS4 and Cu3NbSe4 in a nanocrystalline form. The crystal structures were investigated by X-ray diffraction, identity was confirmed by Raman spectroscopy, and the optoelectronic properties and morphology of Cu3NbS4 and Cu3NbSe4 nanocrystals were examined by UV–vis spectroscopy and transmission electron microscopy, respectively. To gain insight into the Cu3NbX4 formation, a mechanistic study was conducted for Cu3NbSe4 monitoring the nanoparticles’ formation as a function of reaction time. Methylene blue photodegradation tests were conducted to evaluate the photoactivity of Cu3NbS4 and Cu3NbSe4. The degradation rates, 2.81 × 10–2 min–1 and 1.22 × 10–2 min–1 proved the photocatalysts’ potential of nanoscale Cu3NbX4.
Designer Nanostructures in ACS Nanoscience Au
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-02-16 , DOI: 10.1021/acsnanoscienceau.2c00003
RaymondE.Schaak
We are thrilled to feature a set of outstanding papers in the first issue of Volume 2 of ACS Nanoscience Au! As was also the case in our first issue (DOI: 10.1021/acsnanoscienceau.1c00051), these papers showcase the breadth of the field. When I read this collection, I was struck by the common theme of “design” that was integral throughout the wide range of topics. All of these papers present new knowledge that improves and expands our ability to design nanostructures with precise features, which directly correlate with their functions. A Perspective by Jia Guo, Ting Cheng, and Yan Li from Peking University and Rong Xiang and Shigeo Maruyama from the University of Tokyo discusses one-dimensional (1D) van der Waals (vdW) heterostructures, which offer distinct properties and applications relative to 2D vdW materials that have been extensively studied. The authors emphasize the building-block nature of 1D vdW nanostructures and pathways for synthesizing them, ultimately showcasing a strategy for designing and synthesizing high-quality 1D vdW heterostructures. A Review by Renyun Zhang and Håkan Olin from Mid Sweden University highlights how many different types of inorganic nanomaterials can be used to produce triboelectric nanogenerators that convert mechanical energy to electricity. Zhang and Olin discuss the types and compositions of inorganic nanomaterials that are used in triboelectric nanogenerators, as well as their roles. This comprehensive overview provides design guidelines for how inorganic nanomaterials can be incorporated into triboelectric nanogenerators to achieve unique properties. An Article by Zehua Li, Lei Kang, Robert Lord, Raymond Schaak, Douglas Werner, and Kenneth Knappenberger Jr. from Penn State University and Kyoungweon Park, Andrew Gillman, and Richard Vaia from the Air Force Research Laboratory demonstrates that chiroptical signals can arise from achiral objects due to subtle morphological effects, including atomic-level faceting and asymmetric rounding at nanorod tips. These insights provide new guidelines for designing chiral nanostructures, and I am honored to be a coauthor on this work. An Article by Qing Tang and Fuhua Li from Chongqing University and De-en Jiang from the University of California, Riverside, shows how the structure, bonding, and properties of an atomically precise gold nanocluster evolve with pressure. This computational study provides guidelines for designing cluster-based crystals that have new structures and properties and motivates future experimental studies. An Article by Marcus Tornberg, Robin Sjökvist, Krishna Kumar, Carina Maliakkal, Daniel Jacobsson, and Kimberly Dick from Lund University and Christopher Andersen from Lund University and the Technical University of Denmark provides direct microscopic visualization of twin formation during growth of GaAs nanowires. (The videos provided as Supporting Information are definitely worth viewing! See video 1, video 2, and video 3.) Thermodynamic modeling complements the in situ microscopy to provide new insights and guidelines that will help to enable atomic-level precision during semiconductor nanowire growth. Finally, an Article by Yusuke Sakai, Gerrit Wilkens, Karol Wolski, Szczepan Zapotoczny, and Jonathan Heddle from Jagiellonian University, which is featured on the front cover, reports a general method for producing topologically linked DNA origami. The authors show that catenated single-stranded DNA circles serve as a universal scaffold for catenated DNA origami structures of any design. This approach provides a simple strategy for designing and synthesizing “topogami” DNA nanostructures that are typically challenging to prepare. The research in the second issue of ACS Nanoscience Au provides the nanoscience and nanotechnology communities with knowledge and insights that will be useful for designing new nanostructures with unique features and functions. We are excited about these papers and look forward to seeing more contributions in these and other areas of research! Other research that is available online, which will feature in future issues of ACS Nanoscience Au, describes finite-size effects on energy transfer in nanocrystalline phosphors, photoluminescent lead-free halide perovskite nanocrystals, quantum-confined nanoparticles for photocatalysis, metal-oxide nanomaterials for flexible and wearable sensors, single-molecule sensing of miniproteins with nanopores, and an in vivo imaging platform based on chemically modifiable nanoemulsions. These ASAP publications also highlight the broad topical diversity that defines nanoscience and nanotechnology, and we look forward to featuring these topics, and many others, in future issues! This article has not yet been cited by other publications.
Effects of Immune Cell Heterogeneity and Protein Corona on the Cellular Association and Cytotoxicity of Gold Nanoparticles: A Single-Cell-Based, High-Dimensional Mass Cytometry Study
ACS Nanoscience Au ( IF 0 ) Pub Date : 2023-04-24 , DOI: 10.1021/acsnanoscienceau.3c00001
SeheePark,MyKieuHa,YangsoonLee,JaewooSong,TaeHyunYoon
Understanding how nanoparticles (NPs) interact with biological systems is important in many biomedical research areas. However, the heterogeneous nature of biological systems, including the existence of numerous cell types and multitudes of key environmental factors, makes these interactions extremely challenging to investigate precisely. Here, using a single-cell-based, high-dimensional mass cytometry approach, we demonstrated that the presence of protein corona has significant influences on the cellular associations and cytotoxicity of gold NPs for human immune cells, and those effects vary significantly with the types of immune cells and their subsets. The altered surface functionality of protein corona reduced the cytotoxicity and cellular association of gold NPs in most cell types (e.g., monocytes, dendritic cells, B cells, natural killer (NK) cells, and T cells) and those immune cells selected different endocytosis pathways such as receptor-mediated endocytosis, phagocytosis, and micropinocytosis. However, even slight alterations in the major cell type (phagocytic cells and non-phagocytic cells) and T cell subsets (e.g., memory and naive T cells) resulted in significant protein corona-dependent variations in their cellular dose of gold NPs. Especially, naive T killer cells exhibited additional heterogeneity than memory T killer cells, with clusters exhibiting distinct cellular association patterns in single-cell contour plots. This multi-parametric analysis of mass cytometry data established a conceptual framework for a more holistic understanding of how the human immune system responds to external stimuli, paving the way for the application of precisely engineered NPs as promising tools of nanomedicine under various clinical settings, including targeted drug delivery and vaccine development.
Development of a Preemergent Nanoherbicide: From Efficiency Evaluation to the Assessment of Environmental Fate and Risks to Soil Microorganisms
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-03-08 , DOI: 10.1021/acsnanoscienceau.1c00055
VanessaTakeshita,LucasBragançaCarvalho,JulianaAparecidaGalhardi,GustavoViníciosMunhoz-Garcia,RodrigoFlorianoPimpinato,HalleyCaixetaOliveira,ValdemarLuizTornisielo,LeonardoFernandesFraceto
Nanoparticles based on biodegradable polymers have been shown to be excellent herbicide carriers, improving weed control and protecting the active ingredient in the crop fields. Metribuzin is often found in natural waters, which raises environmental concerns. Nanoencapsulation of this herbicide could be an alternative to reduce its losses to the environment and improve gains in its efficiency. However, there is a paucity of information about the behavior of nanoformulations of herbicides in environmental matrices. In this study, the stability of nanoencapsulated metribuzin in polymeric nanoparticles (nanoMTZ) was verified over time, as well as its dissipation in different soils, followed by the effects on soil enzymatic activity. The physiological parameters and control effects of nanoMTZ on Ipomoea grandifolia plants were investigated. No differences were verified in the half-life of nanoencapsulated metribuzin compared to a commercial formulation of the herbicide. Moreover, no suppressive effects on soil enzymatic activities were observed. The retention of nanoMTZ in the tested soils was lower compared to its commercial analogue. However, the mobility of nanoencapsulated metribuzin was not greatly increased, reflecting a low risk of groundwater contamination. Weed control was effective even at the lowest dose of nanoMTZ (48 g a.i. ha–1), which was consistent with the higher efficiency of nanoMTZ compared to the conventional herbicide in inhibiting PSII activity and decreasing pigment levels. Overall, we verified that nanoMTZ presented a low environmental risk, with increased weed control.
Electron Transfer at Quantum Dot–Metal Oxide Interfaces for Solar Energy Conversion
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-06-22 , DOI: 10.1021/acsnanoscienceau.2c00015
MarcoBallabio,EnriqueCánovas
Electron transfer at a donor–acceptor quantum dot–metal oxide interface is a process fundamentally relevant to solar energy conversion architectures as, e.g., sensitized solar cells and solar fuels schemes. As kinetic competition at these technologically relevant interfaces largely determines device performance, this Review surveys several aspects linking electron transfer dynamics and device efficiency; this correlation is done for systems aiming for efficiencies up to and above the ∼33% efficiency limit set by Shockley and Queisser for single gap devices. Furthermore, we critically comment on common pitfalls associated with the interpretation of kinetic data obtained from current methodologies and experimental approaches, and finally, we highlight works that, to our judgment, have contributed to a better understanding of the fundamentals governing electron transfer at quantum dot–metal oxide interfaces.
Exosomes as Neurological Nanosized Machines
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-04-14 , DOI: 10.1021/acsnanoscienceau.1c00062
ElhamPishavar,MartinaTrentini,FedericaZanotti,FrancescaCamponogara,ElenaTiengo,IlariaZanolla,MassimoBonora,BarbaraZavan
In the past few decades, nanomedicine research has advanced dramatically. In spite of this, traditional nanomedicine faces major obstacles, such as blood–brain barriers, low concentrations at target sites, and rapid removal from the body. Exosomes as natural extracellular vesicles contain special bioactive molecules for cell-to-cell communications and nervous tissue function, which could overcome the challenges of nanoparticles. Most recently, microRNAs, long noncoding RNA, and circulating RNA of exosomes have been appealing because of their critical effect on the molecular pathway of target cells. In this review, we have summarized the important role of exosomes of noncoding RNAs in the occurrence of brain diseases.
Efficient Preparation of a Magnetic Helical Carbon Nanomotor for Targeted Anticancer Drug Delivery
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-11-25 , DOI: 10.1021/acsnanoscienceau.2c00042
YanmingSun,RenjiePan,YuduoChen,YongWang,LeiSun,NengWang,XingMa,GuoPingWang
The applications of nanomotors in the biomedical field have been attracting extensive attention. However, it remains a challenge to fabricate nanomotors in a facile way and effectively load drugs for active targeted therapy. In this work, we combine the microwave heating method and chemical vapor deposition (CVD) to fabricate magnetic helical nanomotors efficiently. The microwave heating method can accelerate intermolecular movement, which converts kinetic energy into heat energy and shortens the preparation time of the catalyst used for carbon nanocoil (CNC) synthesis by 15 times. Fe3O4 nanoparticles are in situ nucleated on the CNC surface by the microwave heating method to fabricate magnetically driven CNC/Fe3O4 nanomotors. In addition, we achieved precise control of the magnetically driven CNC/Fe3O4 nanomotors through remote manipulation of magnetic fields. Anticancer drug doxorubicin (DOX) is then efficiently loaded onto the nanomotors via π–π stacking interactions. Finally, the drug-loaded CNC/Fe3O4@DOX nanomotor can accurately accomplish cell targeting under external magnetic field control. Under short-time irradiation of near-infrared light, DOX can be quickly released onto target cells to effectively kill the cells. More importantly, CNC/Fe3O4@DOX nanomotors allow for single-cell or cell-cluster-targeted anticancer drug delivery, providing a dexterous platform to potentially perform many medically relevant tasks in vivo. The efficient preparation method and application in drug delivery are beneficial for future industrial production and provide inspiration for advanced micro/nanorobotic systems using the CNC as a carrier for a wide range of biomedical applications.
Increase Your Impact: Writing Tips to Reach a Broader Audience
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-07-26 , DOI: 10.1021/acsnanoscienceau.2c00030
RaymondE.Schaak
The scope of ACS Nanoscience Au covers a wide range of scientific and engineering disciplines. (1) Readers of this journal will appreciate that the growing collection of published articles is topically diverse; the same is true for other journals that serve and integrate multiple research fields. The papers that stand out most are those that draw in and engage the largest number of readers across multiple disciplines. Having a paper appeal to this so-called “broad audience” (2) is an important consideration for publication in ACS Nanoscience Au, given the inherently interdisciplinary nature of the field. Certain topics naturally lend themselves to being of interest to a broad audience because they have relevance to society or are particularly timely, such as articles discussing COVID-19 mitigation, testing, and treatment in recent years. Beyond such topics, though, what can authors do to ensure that the widest possible audience notices, engages with, and understands the research described in their papers? Let us consider how readers get their first impressions of an article. Many will begin by looking at the Title and the Table of Contents graphic. If those look interesting, they will then read the Abstract. If the Abstract grabs their attention, they will begin to peruse the paper by skimming the Introduction, browsing the Figures, and perhaps reading the Conclusions. Most readers will only invest in reading the paper in depth if they remain engaged after these initial “triage” steps. Several factors can contribute to whether or not they choose to do so. Some will read it in-depth because they need to; this is typically the case for those in the same or allied research fields who have sought out or come across the paper because of how closely it relates to their own research─this is the so-called “specialized audience.” Others─the broader audience─will desire to read it because it looks interesting, catches their attention or intrigues them in some way, and/or is related to their research but is tangential to their expertise. The latter case is often true for nanoscience and nanoengineering papers, where researchers may be familiar with the various facets of a multidisciplinary field but are not experts in them. In general, specialists will already be hooked because of the topic, so let us consider strategies to help make a paper appeal to this broader audience, as this is what will maximize the impact and reach of the work. Note that many other helpful Editorials have been written on topics relevant to those mentioned below, including Titles and Table of Contents Graphics, (3−8) Abstracts, (9) Figures, (10−14) and Methods sections, (15,16) as well as writing manuscripts in general. (17) Table of Contents Graphic. We visually engage with large amounts of information very quickly, with content scrolling down our smartphones, tablets, and computers at breakneck speed. We make split-second decisions about what content to engage with based on what we see. This is where Table of Contents graphics come into play─it is the visual bait that grabs a reader’s attention and lures them in. For some readers that are part of the broader audience, this graphic is the primary means by which they will decide which articles outside of their specialization to engage with. This is also the key image that will accompany the Title of your work in any promotion from ACS via email or social media. The image should be visually appealing and easy to decipher, highlighting the story and/or key result in the paper. Try to avoid overly technical content, complex plots, large amounts of text, or gimmicky figures and cartoons that obscure the key findings of the work. Title. The Title is the first text-based description of a paper that readers see. Titles that are accurate and descriptive but concise are important; this can be achieved while also maximizing appeal to a broad audience. Consider the following three Titles for a (hypothetical) paper that describes the synthesis of cadmium sulfide quantum dots having different sizes, along with a study of their size-dependent photoluminescent properties: “Synthesis and Properties of Cadmium Sulfide Nanoparticles,” “Synthesis and Optical Properties of Cadmium Sulfide Nanoparticles Having Different Sizes,” and “Synthetic Control of Photoluminescence in Size-Tunable Cadmium Sulfide Quantum Dots.” The first Title is insufficiently descriptive, as “properties” is generic, and the size dependence is not mentioned. The second Title is better, as it mentions that the properties are optical and that different particle sizes are included. The third Title, however, incorporates all of these descriptors (with even greater specificity) while also being more intriguing. The third Title is most likely to appeal to a larger number of readers. Abstract. The Abstract provides a summary of the article and is often limited to 150–250 words. While this may seem like a lot of text, it is actually quite short when considering all aspects of an article that could be summarized! Authors sometimes focus almost exclusively on the technical content so that all of the results are adequately described. It is always important to include the key results in the Abstract, of course, but if one of the goals of a paper is also to appeal to a broader audience, it is important to draw in additional readers by providing context that specialists in the field may not need. Including a one-line summary of the context from the Introduction, along with a brief summary of the Discussion and forward-looking Conclusions, helps make an Abstract well-rounded and appealing to a broad audience. Introduction. The Introduction provides the relevant background information and context that frame the research that the paper is reporting, as well as insights into the significance and novelty of the work. Specialists in the field likely already know much of the literature and may immediately appreciate how this new research fits into the field, but other readers may not. Therefore, it is helpful to begin with the big picture of the work. It is probably not necessary to start at too high of a level, i.e., “Nanoparticles are pieces of matter that have dimensions on the order of 1–100 nm and are used in many applications...,” but rather with something that provides an accurate big-picture introduction to the specific research that will be described, i.e., “Semiconductor nanoparticles have revolutionized applications ranging from biological imaging to display technologies...” It is also helpful to explicitly state why the work is important and what its implications are. For research fields in which there is a dauntingly large number of publications, it is particularly useful to articulate what is unique about the research described in the paper, how it is different from what has been reported before, and why it is significant. This approach makes these key aspects of the research clear to readers, rather than making them guess or presuming they already know. Overall, an effective Introduction has all the information that specialists would want to see, while also having sufficient bigger-picture context and explicit statements defining significance, impact, and implications so that nonspecialists are brought up to speed before diving into the Results and Discussion section. Note that Letters do not have these formal subdivisions, but they should still have these components. Results and Discussion. The Results and Discussion section takes readers on a journey through the data. The Figures show the data, while the Results and Discussion section presents, analyzes, and contextualizes the data. In most cases, specialists in a field will already be very familiar with the type of data─how it was collected, how to interpret it, and what it means. Nonspecialists may have some familiarity with the type of data but generally benefit from some additional insight to fully appreciate its significance. It is often possible to include this extra information without having to write a large amount of additional text. For example, saying “The XRD pattern in Figure 1 indicates that the nanoparticles have an average diameter of 10 nm.” is useful for specialists who know how such information can be obtained from analysis of XRD peak widths. However, a slightly expanded version is more approachable to readers who are new and/or tangential to the field: “The XRD pattern in Figure 1 indicates that the nanoparticles have an average diameter of 10 nm, based on Scherrer analysis of the peak widths.” These minor additions can make a big difference to your readers on the peripheries of your field. It can be helpful to consider aspects of the Results and Discussion to be a form of teaching─clearly and concisely instructing readers in what they need to know (including rationale for experiments and analyses) to understand, appreciate, and learn from the research you are reporting. Figures. Figures should clearly and accurately show the data that is discussed in the paper. Beyond that requirement, the design and layout of the figures can help to draw in readers and make the data easier to follow, analyze, and interpret─or it can make it more difficult! Ensuring that figures are easy to follow, especially when coupled with the text in the Results and Discussion section, is helpful to all readers, but particularly to nonspecialists. Including labels, arrows, and other helpful navigation tools can make a reader’s (and reviewer’s!) job easier. Avoid using font sizes that are too small to easily read and choose colors that have high contrast and can be distinguished by those who have color blindness; this ensures that all readers can see and analyze the Figures. Including schematics and graphics to accompany data can help to show readers how the data fits into the bigger picture and relates to other data. Conclusions. A brief summary of the key results is always helpful in the Conclusions, but it is perhaps even more important to put the new results in context with the field and beyond. Readers, especially nonspecialists, appreciate having an idea of what is (or could be) next as a result of this new research being reported. Forward-looking conclusions set the stage for further work and get readers excited about the future; they can also provide nonspecialists with a greater appreciation and understanding of the field, which can pay long-term dividends in unexpected ways! Readers could be policymakers, grant officers, the media, and─especially for open access articles such as those published in ACS Nanoscience Au─the general public. Methods/Experimental Section. The Methods/Experimental section should always include all information necessary to reproduce the work described in the paper. To make this section more approachable to broader, interdisciplinary audiences, consider briefly mentioning the rationale for choosing certain key reagents, experimental parameters, computational codes, and analytical techniques. Also consider offering troubleshooting tips that would be especially helpful for researchers (including students!) who are new to a field but whose research may depend on reproducing and building upon your work. (16) These and other considerations for helping to make a paper appeal to a broad audience serve several goals, including drawing readers in, allowing them to engage effectively and efficiently with the work described in the paper, and helping them to learn and understand something new─all without making them work too hard to do so. Writing your paper with these goals in mind involves managing first impressions, including the Title and Table of Contents Graphic, and second impressions─the Abstract, Figures, and Conclusions─to encourage readers to read the paper in greater depth. It also involves managing how readers engage with the detailed technical content of the work. Efforts to make a paper more approachable to a broader audience will pay dividends even to researchers in related areas, because increasingly interdisciplinary research relies on the ability to understand, appreciate, and integrate knowledge developing beyond our own field(s). Different writers and readers may have different strategies for doing so, but conscious attention to how the various components of a paper can make it more appealing to a broad audience will expand its reach and impact. When coupled with open access and strategies for expanding a paper’s visibility, (18) authors play a very important and powerful role in shaping the future of their research fields! This article references 18 other publications. This article has not yet been cited by other publications. This article references 18 other publications.
Lanthanides Singing the Blues: Their Fascinating Role in the Assembly of Gigantic Molybdenum Blue Wheels
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-03-02 , DOI: 10.1021/acsnanoscienceau.1c00036
EmirAl-Sayed,AnnetteRompel
Molybdenum blues (MBs) are a distinct class of polyoxometalates, exhibiting versatile/impressive architectures and high structural flexibility. In acidified and reduced aqueous environments, isopolymolybdates generate precisely organizable building blocks, which enable unique nanoscopic molecular systems (MBs) to be constructed and further fine-tuned by hetero elements such as lanthanide (Ln) ions. This Review discusses wheel-shaped MB-based structure types with strong emphasis on the ∼30 Ln-containing MBs as of August 2021, which include both organically hybridized and nonhybridized structures synthesized to date. The spotlight is thereby put on the lanthanide ions and ligand types, which are crucial for the resulting Ln-patterns and alterations in the gigantic structures. Several critical steps and reaction conditions in their synthesis are highlighted, as well as appropriate methods to investigate them both in solid state and in solution. The final section addresses the homogeneous/heterogeneous catalytic, molecular recognition and separation properties of wheel-shaped Ln-MBs, emphasizing their inimitable behavior and encouraging their application in these areas.
Markov State Study of Electrostatic Channeling within the Tricarboxylic Acid Cycle Supercomplex
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-06-07 , DOI: 10.1021/acsnanoscienceau.2c00011
YanXie,ShelleyDMinteer,ScottBanta,ScottCalabreseBarton
The high efficiency of cascade reactions in supramolecular enzyme nanoassemblies, known as metabolons, has attracted substantial attention in various fields ranging from fundamental biochemistry and molecular biology to recent applications in biofuel cells, biosensors, and chemical synthesis. One reason for the high efficiency of metabolons is the structures formed by sequential enzymes that allow the direct transport of intermediates between consecutive active sites. The supercomplex of malate dehydrogenase (MDH) and citrate synthase (CS) is an ideal example of the controlled transport of intermediates via electrostatic channeling. Here, using a combination of molecular dynamics (MD) simulations and a Markov state model (MSM), we examined the transport process of the intermediate oxaloacetate (OAA) from MDH to CS. The MSM enables the identification of the dominant transport pathways of OAA from MDH to CS. Analysis of all pathways using a hub score approach reveals a small set of residues that control OAA transport. This set includes an arginine residue previously identified experimentally. MSM analysis of a mutated complex, where the identified arginine is replaced by alanine, led to a 2-fold decrease in transfer efficiency, also consistent with experimental results. This work provides a molecular-level understanding of the electrostatic channeling mechanism and will enable the further design of catalytic nanostructures utilizing electrostatic channeling.
Inverse-Designed Metaphotonics for Hypersensitive Detection
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-07-25 , DOI: 10.1021/acsnanoscienceau.2c00009
MaximElizarov,YuriSKivshar,AndreaFratalocchi
Controlling the flow of broadband electromagnetic energy at the nanoscale remains a critical challenge in optoelectronics. Surface plasmon polaritons (or plasmons) provide subwavelength localization of light but are affected by significant losses. On the contrary, dielectrics lack a sufficiently robust response in the visible to trap photons similar to metallic structures. Overcoming these limitations appears elusive. Here we demonstrate that addressing this problem is possible if we employ a novel approach based on suitably deformed reflective metaphotonic structures. The complex geometrical shape engineered in these reflectors emulates nondispersive index responses, which can be inverse-designed following arbitrary form factors. We discuss the realization of essential components such as resonators with an ultrahigh refractive index of n = 100 in diverse profiles. These structures support the localization of light in the form of bound states in the continuum (BIC), fully localized in air, in a platform in which all refractive index regions are physically accessible. We discuss our approach to sensing applications, designing a class of sensors where the analyte directly contacts areas of ultrahigh refractive index. Leveraging this feature, we report an optical sensor with sensitivity two times higher than the closest competitor with a similar micrometer footprint. Inversely designed reflective metaphotonics offers a flexible technology for controlling broadband light, supporting optoelectronics’ integration with large bandwidths in circuitry with miniaturized footprints.
Mechanistic Study of the Conductance and Enhanced Single-Molecule Detection in a Polymer–Electrolyte Nanopore
ACS Nanoscience Au ( IF 0 ) Pub Date : 2023-01-10 , DOI: 10.1021/acsnanoscienceau.2c00050
FabioMarcuccio,DimitriosSoulias,ChalmersCCChau,SheenaERadford,EricHewitt,PaoloActis,MartinAndrewEdwards
Solid-state nanopores have been widely employed in the detection of biomolecules, but low signal-to-noise ratios still represent a major obstacle in the discrimination of nucleic acid and protein sequences substantially smaller than the nanopore diameter. The addition of 50% poly(ethylene) glycol (PEG) to the external solution is a simple way to enhance the detection of such biomolecules. Here, we demonstrate with finite-element modeling and experiments that the addition of PEG to the external solution introduces a strong imbalance in the transport properties of cations and anions, drastically affecting the current response of the nanopore. We further show that the strong asymmetric current response is due to a polarity-dependent ion distribution and transport at the nanopipette tip region, leading to either ion depletion or enrichment for few tens of nanometers across its aperture. We provide evidence that a combination of the decreased/increased diffusion coefficients of cations/anions in the bath outside the nanopore and the interaction between a translocating molecule and the nanopore–bath interface is responsible for the increase in the translocation signals. We expect this new mechanism to contribute to further developments in nanopore sensing by suggesting that tuning the diffusion coefficients of ions could enhance the sensitivity of the system.
Interaction of the Staphylococcus aureus Surface Protein FnBPB with Corneodesmosin Involves Two Distinct, Extremely Strong Bonds
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-10-18 , DOI: 10.1021/acsnanoscienceau.2c00036
TelmoOPaiva,AlbertusViljoen,ThainaMdaCosta,JoanAGeoghegan,YvesFDufrêne
Attachment of Staphylococcus aureus to human skin corneocyte cells plays a critical role in exacerbating the severity of atopic dermatitis (AD). Pathogen-skin adhesion is mediated by bacterial cell-surface proteins called adhesins, including fibronectin-binding protein B (FnBPB). FnBPB binds to corneodesmosin (CDSN), a glycoprotein exposed on AD patient corneocytes. Using single-molecule experiments, we demonstrate that CDSN binding by FnBPB relies on a sophisticated two-site mechanism. Both sites form extremely strong bonds with binding forces of ∼1 and ∼2.5 nN albeit with faster dissociation rates than those reported for homologues of the adhesin. This previously unidentified two-binding site interaction in FnBPB illustrates its remarkable variety of adhesive functions and is of biological significance as the high strength and short bond lifetime will favor efficient skin colonization by the pathogen.
Modifying the Molecular Structure of Carbon Nanotubes through Gas-Phase Reactants
ACS Nanoscience Au ( IF 0 ) Pub Date : 2023-02-06 , DOI: 10.1021/acsnanoscienceau.2c00052
MichaelJGiannetto,EricPJohnson,AdamWatson,EdgarDimitrov,AndrewKurth,WenboShi,FrancescoFornasiero,EricRMeshot,DesireeLPlata
Current approaches to carbon nanotube (CNT) synthesis are limited in their ability to control the placement of atoms on the surface of nanotubes. Some of this limitation stems from a lack of understanding of the chemical bond-building mechanisms at play in CNT growth. Here, we provide experimental evidence that supports an alkyne polymerization pathway in which short-chained alkynes directly incorporate into the CNT lattice during growth, partially retaining their side groups and influencing CNT morphology. Using acetylene, methyl acetylene, and vinyl acetylene as feedstock gases, unique morphological differences were observed. Interwall spacing, a highly conserved value in natural graphitic materials, varied to accommodate side groups, increasing systematically from acetylene to methyl acetylene to vinyl acetylene. Furthermore, attenuated total reflectance Fourier-transfer infrared spectroscopy (ATR-FTIR) illustrated the existence of intact methyl groups in the multiwalled CNTs derived from methyl acetylene. Finally, the nanoscale alignment of the CNTs grown in vertically aligned forests differed systematically. Methyl acetylene induced the most tortuous growth while CNTs from acetylene and vinyl-acetylene were more aligned, presumably due to the presence of polymerizable unsaturated bonds in the structure. These results demonstrate that feedstock hydrocarbons can alter the atomic-scale structure of CNTs, which in turn can affect properties on larger scales. This information could be leveraged to create more chemically and structurally complex CNT structures, enable more sustainable chemical pathways by avoiding the need for solvents and postreaction modifications, and potentially unlock experimental routes to a host of higher-order carbonaceous nanomaterials.
Recent Advances in Real-Time Time-Dependent Density Functional Theory Simulations of Plasmonic Nanostructures and Plasmonic Photocatalysis
ACS Nanoscience Au ( IF 0 ) Pub Date : 2023-05-19 , DOI: 10.1021/acsnanoscienceau.2c00061
ConnorJ.Herring,MatthewM.Montemore
Plasmonic catalysis provides a possible means for driving chemical reactions under relatively mild conditions. Rational design of these systems is impeded by the difficulty in understanding the electron dynamics and their interplay with reactions. Real-time, time-dependent density functional theory (RT-TDDFT) can provide dynamic information on excited states in plasmonic systems, including those relevant to plasmonic catalysis, at time scales and length scales that are otherwise out of reach of many experimental techniques. Here, we discuss previous RT-TDDFT studies of plasmonic systems, focusing on recent work that gains insight into plasmonic catalysis. These studies provide insight into plasmon dynamics, including size effects and the role of specific electronic states. Further, these studies provide significant insight into mechanisms underlying plasmonic catalysis, showing the importance of charge transfer between metal and adsorbate states, as well as local field enhancement, in different systems.
Significance of an Electrochemical Sensor and Nanocomposites: Toward the Electrocatalytic Detection of Neurotransmitters and Their Importance within the Physiological System
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-10-28 , DOI: 10.1021/acsnanoscienceau.2c00039
HarjotKaur,SamarjeetSinghSiwal,ReenaVSaini,NirankarSingh,VijayKumarThakur
A prominent neurotransmitter (NT), dopamine (DA), is a chemical messenger that transmits signals between one neuron to the next to pass on a signal to and from the central nervous system (CNS). The imbalanced concentration of DA may cause numerous neurological sicknesses and syndromes, for example, Parkinson’s disease (PD) and schizophrenia. There are many types of NTs in the brain, including epinephrine, norepinephrine (NE), serotonin, and glutamate. Electrochemical sensors have offered a creative direction to biomedical analysis and testing. Researches are in progress to improve the performance of sensors and develop new protocols for sensor design. This review article focuses on the area of sensor growth to discover the applicability of polymers and metallic particles and composite materials as tools in electrochemical sensor surface incorporation. Electrochemical sensors have attracted the attention of researchers as they possess high sensitivity, quick reaction rate, good controllability, and instantaneous detection. Efficient complex materials provide considerable benefits for biological detection as they have exclusive chemical and physical properties. Due to distinctive electrocatalytic characteristics, metallic nanoparticles add fascinating traits to materials that depend on the material’s morphology and size. Herein, we have collected much information on NTs and their importance within the physiological system. Furthermore, the electrochemical sensors and corresponding techniques (such as voltammetric, amperometry, impedance, and chronoamperometry) and the different types of electrodes’ roles in the analysis of NTs are discussed. Furthermore, other methods for detecting NTs include optical and microdialysis methods. Finally, we show the advantages and disadvantages of different techniques and conclude remarks with future perspectives.
Realizing Two-Dimensional Supramolecular Arrays of a Spin Molecule via Halogen Bonding
ACS Nanoscience Au ( IF 0 ) Pub Date : 2022-05-03 , DOI: 10.1021/acsnanoscienceau.2c00005
DingguanWang,ZishenWang,ShaofeiWu,Arramel,XinmaoYin,ChiSinTang,YuanPingFeng,JishanWu,AndrewTSWee
Well-ordered spin arrays are desirable for next-generation molecule-based magnetic devices, yet their synthetic method remains a challenging task. Herein, we demonstrate the realization of two-dimensional supramolecular spin arrays on surfaces via halogen-bonding molecular self-assembly. A bromine-terminated perchlorotriphenylmethyl radical with net carbon spin was synthesized and deposited on Au(111) to achieve two-dimensional supramolecular spin arrays. By taking advantage of the diversity of halogen bonds, five supramolecular spin arrays form and are probed by low-temperature scanning tunneling microscopy at the single-molecule level. First-principles calculations verify that the formation of three distinct types of halogen bonds can be used to tailor supramolecular spin arrays via molecular coverage and annealing temperature. Our work suggests that supramolecular self-assembly can be a promising method to engineer two-dimensional molecular spin arrays.
Sonophotocatalysis with Photoactive Nanomaterials for Wastewater Treatment and Bacteria Disinfection
ACS Nanoscience Au ( IF 0 ) Pub Date : 2023-01-27 , DOI: 10.1021/acsnanoscienceau.2c00058
SinaMoradi,CristinaRodriguez-Seco,FarzanHayati,DonglingMa
Sonophotocatalysis is described as a combination of two individual processes of photocatalysis and sonocatalysis. It has proven to be highly promising in degrading dissolved contaminants in wastewaters as well as bacteria disinfection applications. It eliminates some of the main disadvantages observed in each individual technique such as high costs, sluggish activity, and prolonged reaction times. The review has accomplished a critical analysis of sonophotocatalytic reaction mechanisms and the effect of the nanostructured catalyst and process modification techniques on the sonophotocatalytic performance. The synergistic effect between the mentioned processes, reactor design, and the electrical energy consumption has been discussed due to their importance when implementing this novel technology in practical applications, such as real industrial or municipal wastewater treatment plants. The utilization of sonophotocatalysis in disinfection and inactivation of bacteria has also been reviewed. In addition, we further suggest improvements to promote this technology from the lab-scale to large-scale applications. We hope this up-to-date review will advance future research in this field and push this technology toward widespread adoption and commercialization.
Recent Advances in Site-Specific Lipid Nanoparticles for mRNA Delivery
ACS Nanoscience Au ( IF 0 ) Pub Date : 2023-03-30 , DOI: 10.1021/acsnanoscienceau.2c00062
XiaoXu,TianXia
The success of mRNA vaccines during the COVID-19 pandemic has greatly accelerated the development of mRNA therapy. mRNA is a negatively charged nucleic acid that serves as a template for protein synthesis in the ribosome. Despite its utility, the instability of mRNA requires suitable carriers for in vivo delivery. Lipid nanoparticles (LNPs) are employed to protect mRNA from degradation and enhance its intracellular delivery. To further optimize the therapeutic efficacy of mRNA, site-specific LNPs have been developed. Through local or systemic administration, these site-specific LNPs can accumulate in specific organs, tissues, or cells, allowing for the intracellular delivery of mRNA to specific cells and enabling the exertion of local or systemic therapeutic effects. This not only improves the efficiency of mRNA therapy but also reduces off-target adverse effects. In this review, we summarize recent site-specific mRNA delivery strategies, including different organ- or tissue-specific LNP after local injection, and organ-specific or cell-specific LNP after intravenous injection. We also provide an outlook on the prospects of mRNA therapy.
补充信息
自引率H-indexSCI收录状况PubMed Central (PML)
0
平台客服
平台客服
平台在线客服