ACS Nanoscience Au最新文献

Nanotechnology is vital to many current industries, including electronics, energy, textiles, agriculture, and theranostics. Understanding the chemical mechanisms of nanomaterial synthesis has contributed to the tunability of their unique properties, although studies frequently overlook the potential impact of impurities. Impurities can show adverse effects, clouding the interpretation of results or limiting the practical utility of the nanomaterial. On the other hand, as successful doping has demonstrated, the intentional introduction of impurities can be a powerful tool for enhancing the properties of a nanomaterial. This Review examines the complex role of impurities, unintentionally or intentionally added, during nanoscale synthesis and their effects on the performance and usefulness of the most common classes of nanomaterials: nanocarbons, noble metal and metal oxide nanoparticles, semiconductor quantum dots, thermoelectrics, and perovskites.

Activating the glucagon-like peptide-1 (GLP-1) receptor by oral nucleic acid delivery would be a promising treatment strategy against hyperglycemia due to its various therapeutic actions. However, GLP-1 receptor agonists are effective only in subcutaneous injections because they face multiple barriers due to harsh gastrointestinal tract (GIT) conditions before reaching the site of action. The apical sodium bile acid transporter (ASBT) pathway at the intestinal site could be an attractive target to overcome the problem. Herein, we used our previously established multimodal carrier system utilizing bile salt, protamine sulfate, and calcium phosphate as excipients (PTCA) and the GLP-1 gene as an active ingredient (GENE) to test the effects of different formulation doses against diabetes and obesity. The carrier system demonstrated the ability to protect the GLP-1 model gene encoded within the plasmid at the GIT and transport it via ASBT at the target site. A single oral dose, regardless of quantity, showed the generation of GLP-1 and insulin from the body and maintained the normoglycemic condition by improving insulin sensitivity and blood sugar tolerance for a prolonged period. This oral gene therapy approach shows significantly higher therapeutic efficacy in preclinical studies than currently available US Food and Drug Administration-approved GLP-1 receptor agonists such as semaglutide and liraglutide. Also, a single oral dose of GENE/PTCA is more effective than 20 insulin injections. Our study suggests that oral GENE/PTCA formulation could be a promising alternative to injection-based therapeutics for diabetics, which is effective in long-term treatment and has been found to be highly safe in all aspects of toxicology.

The SARS-CoV-2 pandemic spurred numerous research endeavors to comprehend the virus and mitigate its global severity. Understanding the binding interface between the virus and human receptors is pivotal to these efforts and paramount to curbing infection and transmission. Here we employ atomic force microscopy and steered molecular dynamics simulation to explore SARS-CoV-2 receptor binding domain (RBD) variants and angiotensin-converting enzyme 2 (ACE2), examining the impact of mutations at key residues upon binding affinity. Our results show that the Omicron and Delta variants possess strengthened binding affinity in comparison to the Mu variant. Further, using sera from individuals either vaccinated or with acquired immunity following Delta strain infection, we assess the impact of immunity upon variant RBD/ACE2 complex formation. Single-molecule force spectroscopy analysis suggests that vaccination before infection may provide stronger protection across variants. These results underscore the need to monitor antigenic changes in order to continue developing innovative and effective SARS-CoV-2 abrogation strategies.

A fundamental precept of chemistry is that properties are manifestations of the elements present and their arrangement in space. Controlling the arrangement of atoms in nanocrystals is not well understood in nanocrystal synthesis, especially in the transition metal chalcogenides and pnictides, which have rich phase spaces. This Perspective will cover some of the recent advances and current challenges. The perspective includes introductions to challenges particular to chalcogenide and pnictide chemistry, the often-convoluted roles of bond dissociation energies and mechanisms by which precursors break down, using very organized methods to map the synthetic phase space, a discussion of polytype control, and challenges in characterization, especially for solving novel structures on the nanoscale and time-resolved studies.

Gold nanoparticles (AuNPs) are a promising platform for biomedical applications including therapeutics, imaging, and drug delivery. While much of the literature surrounding the introduction of AuNPs into cellular systems focuses on uptake and cytotoxicity, less is understood about how AuNPs can indirectly affect cells via interactions with the extracellular environment. Previous work has shown that the monocytic cell line THP-1’s ability to undergo chemotaxis in response to a gradient of monocyte chemoattractant protein 1 (MCP-1) was compromised by extracellular polysulfonated AuNPs, presumably by binding to MCP-1 with some preference over other proteins in the media. The hypothesis to be explored in this work is that the degree of sulfonation of the surface would therefore be correlated with the ability of AuNPs to interrupt chemotaxis. Highly sulfonated poly(styrenesulfonate)-coated AuNPs caused strong inhibition of THP-1 chemotaxis; by reducing the degree of sulfonation on the AuNP surface with copolymers [poly(styrenesulfonate-co-maleate) of different compositions], it was found that medium and low sulfonation levels caused weak to no inhibition, respectively. Small, rigid molecular sulfonate surfaces were relatively ineffective at chemotaxis inhibition. Unusually, free poly(styrenesulfonate) caused a dose-dependent reversal of THP-1 cell migration: at low concentrations, free poly(styrenesulfonate) significantly inhibited MCP-1-induced chemotaxis. However, at high concentrations, free poly(styrenesulfonate) acted as a chemorepellent, causing a reversal in the cell migration direction.

Improving charge insertion into intercalation hosts is essential for crucial energy and memory technologies. The layered material TiS₂ provides a promising template for study, but further development of this compound demands improvement to its ion kinetics. Here, we report the incorporation of Se atoms into TiS₂ nanobelts to address barriers related to sluggish ion motion in the material. TiS_1.8Se_0.2 nanobelts are synthesized through a solid-state method, and structural and electrochemical characterizations reveal that solid solutions based on TiS_1.8Se_0.2 nanobelts display increased interlayer spacing and electrical conductivity compared to pure TiS₂ nanobelts. Cyclic voltammetry and electrochemical impedance spectroscopy indicate that the capacitive behavior of the TiS₂ electrode is improved upon Se incorporation, particularly at low depths of discharge in the materials. The presence of Se in the structure can be directly related to an increased pseudocapacitive contribution to electrode behavior at a low Li⁺ content in the material and thus to improved ion kinetics in the TiS_1.8Se_0.2 nanobelts.

Two-dimensional (2D) materials are popular for fundamental physics study and technological applications in next-generation electronics, spintronics, and optoelectronic devices due to a wide range of intriguing physical and chemical properties. Recently, the family of 2D metals and 2D semiconductors has been expanding rapidly because they offer properties once unknown to us. One of the challenges to fully access their properties is poor stability in ambient conditions. In the first half of this Review, we briefly summarize common methods of preparing 2D metals and highlight some recent approaches for making air-stable 2D metals. Additionally, we introduce the physicochemical properties of some air-stable 2D metals recently explored. The second half discusses the air stability and oxidation mechanisms of 2D transition metal dichalcogenides and some elemental 2D semiconductors. Their air stability can be enhanced by optimizing growth temperature, substrates, and precursors during 2D material growth to improve material quality, which will be discussed. Other methods, including doping, postgrowth annealing, and encapsulation of insulators that can suppress defects and isolate the encapsulated samples from the ambient environment, will be reviewed.

In the last two decades, metal–organic frameworks (MOFs) with highly tunable structure and porosity, have emerged as drug nanocarriers in the biomedical field. In particular, nanoscaled MOFs (nanoMOFs) have been widely investigated because of their potential biocompatibility, high drug loadings, and progressive release. To enhance their properties, MOFs have been combined with magnetic nanoparticles (MNPs) to form magnetic nanocomposites (MNP@MOF) with additional functionalities. Due to the magnetic properties of the MNPs, their presence in the nanosystems enables potential combinatorial magnetic targeted therapy and diagnosis. In this Review, we analyze the four main synthetic strategies currently employed for the fabrication of MNP@MOF nanocomposites, namely, mixing, in situ formation of MNPs in presynthesized MOF, in situ formation of MOFs in the presence of MNPs, and layer-by-layer methods. Additionally, we discuss the current progress in bioapplications, focusing on drug delivery systems (DDSs), magnetic resonance imaging (MRI), magnetic hyperthermia (MHT), and theragnostic systems. Overall, we provide a comprehensive overview of the recent advances in the development and bioapplications of MNP@MOF nanocomposites, highlighting their potential for future biomedical applications with a critical analysis of the challenges and limitations of these nanocomposites in terms of their synthesis, characterization, biocompatibility, and applicability.

Surface-catalyzed reactions have been used to synthesize carbon nanomaterials with atomically predefined structures. The recent discovery of a gold surface-catalyzed [3 + 3] cycloaromatization of isopropyl substituted arenes has enabled the on-surface synthesis of arylene-phenylene copolymers, where the surface activates the isopropyl substituents to form phenylene rings by intermolecular coupling. However, the resulting polymers suffered from undesired cross-linking when more than two molecules reacted at a single site. Here we show that such cross-links can be prevented through steric protection by attaching the isopropyl groups to larger arene cores. Upon thermal activation of isopropyl-substituted 8,9-dioxa-8a-borabenzo[fg]tetracene on Au(111), cycloaromatization is observed to occur exclusively between the two molecules. The cycloaromatization intermediate formed by the covalent linking of two molecules is prevented from reacting with further molecules by the wide benzotetracene core, resulting in highly selective one-to-one coupling. Our findings extend the versatility of the [3 + 3] cycloaromatization of isopropyl substituents and point toward steric protection as a powerful concept for suppressing competing reaction pathways in on-surface synthesis.