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我们在纳米技术环境健康与安全和材料表征方面的发展方向是什么？

Where Are We Heading in Nanotechnology Environmental Health and Safety and Materials Characterization?

作者：Andre E. Nel;Wolfgang J. Parak;Warren C. W. Chan;Tian Xia;Mark C. Hersam;C. Jeffrey Brinker;Jeffrey I. Zink;Kent E. Pinkerton;Donald R. Baer;Paul S. Weiss;

DOI：https://doi.org/10.1021/acsnano.5b03496

发表时间：2015年

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Ultrafast Interlayer Charge Transfer Outcompeting Intralayer Valley Relaxation in Few-Layer 2D Heterostructures

While 2D transition metal dichalcogenides (TMDs) feature interesting layer-tunable multivalley band structures, their preeminent role in determining the photoexcitation charge transfer dynamics in 2D heterostructures (HSs) is yet to be unraveled, as previous charge transfer studies on TMD HSs have been mostly focused on monolayers with a direct bandgap at the K valley. By ultrafast transient absorption spectroscopy and deliberately designed few-layer WSe2/WS2 HSs, we have observed an ultrafast interlayer electron transfer from photoexcited few-layer WSe2 to WS2, prior to intralayer relaxation to lower lying dark valleys. More interestingly, we have identified an unconventional ∼0.5 ps electron back-transfer process after the initial interlayer electron transfer in HSs with WSe2 layers ≥ 3, regenerating indirect intralayer excitons. The result reveals an ielectron and valley relaxation pathway mediated by interlayer charge transfer in 2D HSs, faster than intralayer relaxation. It also sheds light on the origin of generally observed robust ultrafast interlayer charge transfer in TMD HSs and provides guidance toward optoelectronic and valleytronic devices using few-layer TMDs.

引用量：0发表时间：2023年
Vanadium Carbide Nanosheets with Broad-Spectrum Antioxidant Activity for Pulmonary Fibrosis Therapy

Idiopathic pulmonary fibrosis is a chronic and highly lethal lung disease that largely results from oxidative stress; however, effective antioxidant therapy by targeting oxidative stress pathogenesis is still lacking. The big challenge is to develop an ideal antioxidant material with superior antifibrotic effects. Herein, we report that V4C3 nanosheets (NSs) can serve as a potential antioxidant for treatment of pulmonary fibrosis by scavenging reactive oxygen and nitrogen species. Interestingly, subtle autoxidation can adjust the valence composition of V4C3 NSs and significantly improve their antioxidant behavior. Valence engineering triggers multiple antioxidant mechanisms including electron transfer, H atom transfer, and enzyme-like catalysis, thus endowing V4C3 NSs with broad-spectrum, high-efficiency, and persistent antioxidant capacity. Benefiting from antioxidant properties and good biocompatibility, V4C3 NSs can significantly prevent myofibroblast proliferation and extracellular matrix abnormality, thus alleviating the progression of bleomycin-induced pulmonary fibrosis in vivo by scavenging ROS, anti-inflammation, and rebuilding antioxidant defenses. This study not only provides an important strategy for designing excellent antioxidant nanomaterials, but also proposes a proof-of-concept demonstration for the treatment of pulmonary fibrosis and other oxidative stress-related diseases.

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“Reaction”-Like Shaping of Self-Delivery Supramolecular Nanodrugs in the Nanoprecipitation Process

Nanoprecipitation, which is achieved through the diffusion and precipitation of drug molecules in blended solvent and antisolvent phases, is a classic route for constructing nanodrugs (NDs) and previously directed by diffusion-controlled theory. However, the diffusion-controlled mechanism is out of date in the recent preparation of self-delivery supramolecular NDs (SDSNDs), characterized by the construction of drug nanoparticles through supramolecular interactions in the absence of carriers and surfactants. Herein, a “reaction”-like complement, contributed from supramolecular interactions, is proposed for the preparation of naphthoquinone SDSNDs. Different from the diffusion-controlled process, the formation rate of SDSNDs via the “reaction”-like process is almost constant and highly dependent on the supramolecular interaction-determined Gibbs free energy of molecular binding. Thus, the formation rate and drug availability of SDSNDs are greatly improved by engineering the supramolecular interactions, which facilitates the preparation of SDSNDs with expected sizes, components, and therapeutic functions. As a deep understanding of supramolecular-interaction-involved nanoprecipitation, the current “reaction”-like protocol not only provides a theoretical supplement for classic nanoprecipitation but also highlights the potential of nanoprecipitation in shaping self-assembled, coassembled, and metal-ion-associated SDSNDs.

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Vanadium Intercalation into Niobium Disulfide to Enhance the Catalytic Activity for Lithium–Sulfur Batteries

Despite their high specific energy and great promise for next-generation energy storage, lithium–sulfur (Li–S) batteries suffer from polysulfide shuttling, slow redox kinetics, and poor cyclability. Catalysts are needed to accelerate polysulfide conversion and suppress the shuttling effect. However, a lack of structure–activity relationships hinders the rational development of efficient catalysts. Herein, we studied the Nb–V–S system and proposed a V-intercalated NbS2 (Nb3VS6) catalyst for high-efficiency Li–S batteries. Structural analysis and modeling revealed that undercoordinated sulfur anions of [VS6] octahedra on the surface of Nb3VS6 may break the catalytic inertness of the basal planes, which are usually the primary exposed surfaces of many 2D layered disulfides. Using Nb3VS6 as the catalyst, the resultant Li–S batteries delivered high capacities of 1541 mAh g–1 at 0.1 C and 1037 mAh g–1 at 2 C and could retain 73.2% of the initial capacity after 1000 cycles. Such an intercalation-induced high activity offers an alternative approach to building better Li–S catalysts.

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Mapping Antibody Domain Exposure on Nanoparticle Surfaces Using DNA-PAINT

Decorating nanoparticles with antibodies (Ab) is a key strategy for targeted drug delivery and imaging. For this purpose, the orientation of the antibody on the nanoparticle is crucial to maximize fragment antibody-binding (Fab) exposure and thus antigen binding. Moreover, the exposure of the fragment crystallizable (Fc) domain may lead to the engagement of immune cells through one of the Fc receptors. Therefore, the choice of the chemistry for nanoparticle-antibody conjugation is key for the biological performance, and methods have been developed for orientation-selective functionalization. Despite the importance of this issue, there is a lack of direct methods to quantify the antibodies’ orientation on the nanoparticle’s surface. Here, we present a generic methodology that enables for multiplexed, simultaneous imaging of both Fab and Fc exposure on the surface of nanoparticles, based on super-resolution microscopy. Fab-specific Protein M and Fc-specific Protein G probes were conjugated to single stranded DNAs and two-color DNA-PAINT imaging was performed. Hereby, we quantitatively addressed the number of sites per particle and highlight the heterogeneity in the Ab orientation and compared the results with a geometrical computational model to validate data interpretation. Moreover, super-resolution microscopy can resolve particle size, allowing the study of how particle dimensions affect antibody coverage. We show that different conjugation strategies modulate the Fab and Fc exposure which can be tuned depending on the application of choice. Finally, we explored the biomedical importance of antibody domain exposure in antibody dependent cell mediated phagocytosis (ADCP). This method can be used universally to characterize antibody-conjugated nanoparticles, improving the understanding of relationships between structure and targeting capacities in targeted nanomedicine.

引用量：0发表时间：2023年
Development of Multifunctional Nanoencapsulatedtrans-Resveratrol/Chitosan Nutraceutical Edible Coating for Strawberry Preservation

Phytochemical nanoencapsulation for nutrient delivery and edible coatings for perishable food preservation are two emerging technologies. Leveraging the strong antimicrobial function of phytochemical nutrients, we propose convergent research to integrate the two technologies by embedding phytochemical-encapsulated nanoparticles in an edible coating on fresh fruits to achieve multiple functions. In particular, we report the study of an edible coating on strawberries that is composited of trans-resveratrol (R)-encapsulated nanoparticles (RNPs) embedded in a chitosan (CS) matrix. The biodegradable and biocompatible RNPs significantly increased the aqueous solubility of R by 150-fold and bioavailability by 3.5-fold after oral administration. Our results demonstrated the abilities of the RNP-embedded CS edible coating to diminish dehydration, prevent nutrient loss, inhibit microbe growth, increase nutraceutical value, preserve strawberry quality, and extend shelf life during storage at both 22 and 4 °C. Such a phytochemical nanoencapsulation-based edible coating is promising for the dual purposes of enhancing nutrient delivery and preserving perishable foods.

引用量：0发表时间：2023年
Solution-Processed Flexible Transparent Electrodes for Printable Electronics

Flexible transparent electrodes (FTEs) have been widely witnessed in various printable electronic devices, especially those involving light. So far, solution processes have demonstrated increasing advantages in preparing FTEs not only in their mild operation conditions and high-throughput but also in the diversity in micropatterning conductive nanomaterials into networks. For the FTEs, both high transparency and high conductivity are desirable, which therefore create requirements for the conductive network by considering the trade-off relationship between the coverage and the micropatterns of the network. In addition, the conductive networks also affect the flexibility of FTEs due to the deformation during bending/stretching. Consequently, solution processes capable of micropatterning conductive nanomaterials including nanoparticles, nanowires/polymers, and graphene/MXene play a crucial role in determining the performance of FTEs. Here, we reviewed recent research progress on solution-processed FTEs, including the solution processes, the solution-processable conductive nanomaterials and the substrates for making FTEs, and applications of FTEs in flexible electronics. Finally, we proposed several perspective outlooks of the FTEs, which aim at not only the enhanced performance but also the performances in extreme conditions and in integration. We believe that the review would offer inspiration for developing functional FTEs.

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Amorphizing Metal Selenides-Based ROS Biocatalysts at Surface Nanolayer toward Ultrafast Inflammatory Diabetic Wound Healing

The microenvironments with high reactive-oxygen-species (ROS) levels, inflammatory responses, and oxidative-stress effects in diabetic ulcer wounds, leading to poor proliferation and differentiation of stem cells, severely inhibit their efficient healing. Here, to overcome the unbalanced multielectron reactions in ROS catalysis, we develop a cobalt selenide-based biocatalyst with an amorphous Ru@CoSe nanolayer for ultrafast and broad-spectrum catalytic ROS-elimination. Owing to the enriched electrons and more unoccupied orbitals of Ru atoms, the amorphous Ru@CoSe nanolayer-equipped biocatalyst displays excellent catalase-like kinetics (maximal reaction velocity, 23.05 μM s–1; turnover number, 2.00 s–1), which exceeds most of the currently reported metal compounds. The theoretical studies show that Ru atoms act as “regulators” to tune the electronic state of the Co sites and modulate the interaction of oxygen intermediates, thus improving the reversible redox properties of active sites. Consequently, the Ru@CoSe can efficiently rescue the proliferation of mesenchymal stem cells and maintain their angiogenic potential in the oxidative stress environment. In vivo experiments reveal the superior ROS-elimination ability of Ru@CoSe on the inflammatory diabetic wound. This study offers an effective nanomedicine for catalytic ROS-scavenging and ultrafast healing of inflammatory wounds and also provides a strategy to design biocatalytic metal compounds via bringing amorphous catalytic structures.

引用量：0发表时间：2023年
Direct Imaging of “Patch-Clasping” and Relaxation in Robust and Flexible Nanoparticle Assemblies

Polymer patching on inorganic nanoparticles (NPs) enables multifunctionality and directed self-assembly into nonclosely packed optical and mechanical metamaterials. However, experimental demonstration of such assemblies has been scant due to challenges in leveraging patch-induced NP–NP attractions and understanding NP self-assembly dynamics. Here we use low-dose liquid-phase transmission electron microscopy to visualize the dynamic behaviors of tip-patched triangular nanoprisms upon patch-clasping, where polymer patches interpenetrate to form cohesive bonds that connect NPs. Notably, these bonds are longitudinally robust but rotationally flexible. Patch-clasping is found to allow highly selective tip–tip assembly, interconversion between dimeric bowtie and sawtooth configurations, and collective structural relaxation of NP networks. The integration of single particle tracking, polymer physics theory, and molecular dynamics simulation reveals the macromolecular origin of patch-clasping-induced NP dynamics. Our experiment–computation integration can aid the design of stimuli-responsive nanomaterials, such as topological metamaterials for chiral sensors, waveguides, and nanoantennas.

引用量：0发表时间：2023年
An Integrated Multilevel Approach Unveils Complex Seed–Nanoparticle Interactions and Their Implications for Seed Priming

Nanotechnology has the potential to revolutionize agriculture with the introduction of engineered nanomaterials. However, their use is hindered by high cost, marginal knowledge of their interactions with plants, and unpredictable effects related to massive use in crop cultivation. Nanopriming is an innovative seed priming technology able to match economic, agronomic, and environmental needs in agriculture. The present study was focused on unveiling, by a multilevel integrated approach, undisclosed aspects of seed priming mediated by iron oxide magnetic nanoparticles in pepper seeds (Capsicum annuum), one of the most economically important crops worldwide. Inductively coupled plasma atomic emission mass spectrometry and scanning electron microscopy were used to quantify the MNP uptake and assess seed surface changes. Magnetic resonance imaging mapped the distribution of MNPs prevalently in the seed coat. The application of MNPs significantly enhanced the root and vegetative growth of pepper plants, whereas seed priming with equivalent Fe concentrations supplied as FeCl3 did not yield these positive effects. Finally, global gene expression by RNA-sequencing identified more than 2,200 differentially expressed genes, most of them involved in plant developmental processes and defense mechanisms. Collectively, these data provide evidence on the link between structural seed changes and an extensive transcriptional reprogramming, which boosts the plant growth and primes the embryo to cope with environmental challenges that might occur during the subsequent developmental and growth stages.

引用量：0发表时间：2023年

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我们在纳米技术环境健康与安全和材料表征方面的发展方向是什么？

Where Are We Heading in Nanotechnology Environmental Health and Safety and Materials Characterization?

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