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24, 51815186 (2012). and L.Z.Z. Thank you for visiting nature.com. Adv. However, the chemical interactions that typically dictate nanoparticle ordering3,4,5 do not inherently provide any means to manipulate structure at larger length scales6,7,8,9. In addition, colitic SD rats receiving Dex-P/NPA2 recovered the expression of tight junction-associated proteins including ZO-1 and occludin-1 and showed significantly reduced local levels of IL-1, IL-6, and TNF compared with the untreated group and Dex-P/PBS group (Fig. 138, 1622816231 (2016). The NPA2 coacervate-bonded porcine skin joints can withstand an applied force five times greater than that of the homolog control groups (NPA1 nanoparticle solution and NPA3 coacervate). Fresh intestinal tissues were bought from Sha Tin Market (Hong Kong), stored on ice, and washed with PBS buffer (1) three times before use. 2c, d, e and Supplementary Fig. 157, 3762 (2020). Science 364, eaav4299 (2019). Khutoryanskiy, V. V. Supramolecular materials: longer and safer gastric residence. Nat. 4d). Anyone you share the following link with will be able to read this content: Sorry, a shareable link is not currently available for this article. Bouten, P. J. et al. Chaim, R., Levin, M., Shlayer, A. The colitic rats received oral gavages of Dex-P-laden NPA2 coacervates (Dex-P/NPA2) or the equivalent amount of Dex-P in PBS (Dex-P/PBS) on days 1, 3, and 5. b Immunohistochemical staining against key macrophage M1/M2 polarization markers iNOS/CD206, c histopathology score, d mRNA levels of tight junction-associated protein ZO-1, e pro-inflammatory cytokines including interleukin IL-1 and IL-6 released by M1 macrophages, and f anti-inflammatory cytokine IL-10 released by M2 macrophages. CAS Nano Today 9, 574589 (2014). Self-assembly of magnetite nanocubes into helical superstructures. Surgical materials: current challenges and nano-enabled solutions. ADS PubMed However, the assembly process between these microscale networks and the co-dispersed nano-objects has not been investigated so far at the microscopic level . Article Love, C. et al. Begley, M. R., Gianola, D. S. & Ray, T. R. Bridging functional nanocomposites to robust macroscale devices. Next, sections were incubated at 4C overnight with primary antibodies directed against ZO-1 conjugated with Alexa Fluor 488 (dilution of 1:200) and occludin-1 conjugated with Alexa Fluor 594 (dilution of 1:200). B. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. Tang, T. D. et al. Crystal structure, Materials, Nanoparticles Nanoparticle assembly enables the synthesis of multiple complex nanoscale structures, but future investigation and application of these materials requires new processing methods to control micro- and macroscale structure as well. Assembly of large-area, highly ordered, crack-free inverse opal films. and JavaScript. The low adhesion energy of the control homologs can be attributed to the weak bulk cohesion (NPA1 solution) or interfacial adhesion (NPA3 coacervate), respectively. Mater. Sci. We suggest that the nanoparticle-assembled coacervate provides a promising drug delivery platform for management and treatment of numerous gastrointestinal diseases where controlled drug release with extended residence time is desired. Clin. Sign up for the Nature Briefing: Translational Research newsletter top stories in biotechnology, drug discovery and pharma. CAS Google Scholar. However, the acquisition of single particles involves complex operation, and the corresponding nanodevices display low-throughput. ADS Finally, a Multiskan microplate reader (Thermo Fisher) was used to collect the absorbance value of each well at 540nm for cell metabolic calculation. In situ deactivation of catechol-containing adhesive using electrochemistry. Therefore, our NPA2 coacervate can mediate sustained release and improve the pharmacokinetics of the preloaded drug in the SD rat model, thereby reducing dosing frequency and systemic drug exposure. Nature Communications Natl Acad. 27). The self-assembly of inorganic nanoparticles to larger structures is of great research interest as it allows the fabrication of novel materials with collective properties correlated to the nanoparticles' individual characteristics. Next sections were incubated at 4C overnight with primary antibody directed against CD206 or iNOS (dilution of 1:200), followed by incubation with a biotinylated secondary antibody (Abcam, ab207995, dilution of 1:500). a Schematic illustration of harsh environmental conditions in the peristaltic GI tract. 3b). However, the complex coacervation process is driven by electrostatic attraction between polyanions and polycations within narrow pH/salt ranges19. Mater. Yang, Y., Wang, X., Yang, F., Shen, H. & Wu, D. A universal soaking strategy to convert composite hydrogels into extremely tough and rapidly recoverable doublenetwork hydrogels. Liquidliquid phase separation of the green mussel adhesive protein Pvfp5 is regulated by the posttranslated dopa amino acid. Appl. The frequency-dependent storage (G) and loss (G) moduli of the liquid NPA2 coacervate as revealed by rheological analysis demonstrates its highly dynamic polymeric structure due to the presence of supramolecular interactions, such as hydrogen bonding derived from the catechol groups (Supplementary Fig. 17). Nanoparticleassembled vacuolated coacervates control macromolecule spatiotemporal distribution to provide a stable segregated cell microenvironment. Birshtein, T. M. & Lyatskaya, Yu. Adv. Rev. 3e) and in vivo conditions (Fig. 33, 2007209 (2021). 3b). Lee, Y. et al. And fresh fecal samples were collected from the above colitic SD rats in each group on day 5 and stored at 80C in autoclaved sterile vials for further analysis of gut microbiota. 19, 391396 (2020). Basts, N. G., Comenge, J. Depriester, D. & Kubler, R. Resolution of the Wicksells equation by minimum distance estimation. Sci. Provided by the Springer Nature SharedIt content-sharing initiative. The polyelectrolyte complex/coacervate continuum. Nature Communications (Nat Commun) Front. i A clustered heatmap of UniFrac values for measuring gut microbiota -diversity illustrated that colitic SD rats receiving Dex-P/NPA2 and healthy SD rats were clustered more closely, suggesting more similar bacterial compositions. In the meantime, to ensure continued support, we are displaying the site without styles Sci. 6). However, most approaches developed for the formation of discrete assemblies are limited to a single and homogeneous system, and incorporation of larger or asymmetrical . A cross-linking approach to stabilizing stimuli-responsive colloidal crystals engineered with DNA. Nat. https://link.springer.com/protocol/10.1007%2F978-1-4939-3139-2_12. Angew. Zhang, J. et al. SD rats (200300g, female, 812 weeks) receiving oral administration of NPA2 coacervate (4g per kg rat) on days 1, 3, 5, 7, and 9 during the 10-day toxicity evaluation and untreated healthy rats were used as the control group. DNA origami is another versatile type of templates for assembly of nanoparticles. Kinetic pathways of crystallization at the nanoscale. The orally administered drug-laden nanoparticle-assembled coacervate significantly mitigates the symptoms of inflammatory bowel disease, restores the diversity of gut microbiota, reduces systemic. For the MTT assay, hMSCs (0.6104 cells/well) were incubated in a 96-well plate in the growth medium. In addition, a heatmap of -diversity distance distribution was generated, and samples with similar -diversity were clustered to reflect the similar compositions of gut microbiota (Fig. Fluid NPA2 coacervate with a solid content of about 15wt% flowed out from a tilted glass bottle and formed a durable adhesive coating on the medical nitrile glove (Fig. The NPA coacervate exhibited: (1) pH and salt-independent stability under the complex environment within the GI tract; (2) effective coating of large intestinal surface and prolonged intestinal retention for several days; and (3) enhanced therapeutic efficacy for IBD and gut microbiota restoration with reduced systemic drug exposure via the controlled release of a loaded drug. Animal experiments were approved by the Animal Experimentation Ethics Committee of the Chinese University of Hong Kong (19-152-MIS) and were carried out in accordance with the guidelines of the Animals Ordinance (Chapter 340), Department of Health, Hong Kong. Nanodevices based on the single nanoparticle represent innovative and promising technology, which could satisfy the increasing requirements of high accuracy, low energy consumption, and small volume. Provided by the Springer Nature SharedIt content-sharing initiative, Chinese Journal of Polymer Science (2023), Chemical Research in Chinese Universities (2023). This robust nanoparticle assembly is achieved by multivalent, self-complementary interactions of the zwitterionic tetrapeptides. The ability to regulate the complex interactions between the individual components is essential in achieving this target. All data are available in the main Article and Supplementary Information, or from the corresponding author upon reasonable request. ADS Deepankumar, K. et al. 5f)66. Open Access articles citing this article. In this study, MALDI-TOF mass spectrometry was used to confirm the successful synthesis of the hydrophobic core (Supplementary Fig. Paintable and rapidly bondable conductive hydrogels as therapeutic cardiac patches. Chem. Histopathology scores of colitic SD rats in the Dex-P/PBS group were not significantly different from the untreated control group (P=0.056, Fig. 2j and Supplementary Fig. Article Nat. Assembly of tailored porous nanofibers from mesoporous MCM41 nanoparticles via electrospinning - Timm - ChemNanoMat - Wiley Online Library If material is not included in the articles Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. Bioresponsive drug delivery systems in intestinal inflammation: State-of-the-art and future perspectives. It operates at the mesoscale where elementary building blocks still feel their atomic nature and can profit from quantum function but at the same time are flexible enough in shape and interaction to permit high structural complexity. Langmuir 27, 1109811105 (2011). Windsor, J. W. & Kaplan, G. G. Evolving epidemiology of IBD. 50, 48084842 (2011). However, solid adhesives with high adhesion energy on wet tissues11,12,13,14 may not be suitable as orally administered intestine-coating drug delivery platforms. In addition, the dried drug-laden NPA2 coacervate that is desirable for oral administration could be prepared via lyophilization, and simply adding dried drug-laden NPA2 coacervate into simulated gastric fluid or water could realize the rehydration to form fluid NPA2 coacervate with sustained-release kinetics of diverse drugs similar to the freshly prepared drug-laden NPA2 coacervate before lyophilization (Supplementary Fig. Mater. We hypothesized that the capability of NPA2 coacervates to mediate the sustained release of water-soluble small molecules such as Dex-P can be ascribed to the relatively hydrophobic environment within the NPA2 coacervate. Endowing oral drug delivery vehicles with wet bioadhesion may prolong intestinal residence time. Liquid-metal nanoparticles were used as reservoirs for mixing with various metal salts (left). Commun. Nat. acknowledge support from the NSF Graduate Research Fellowship Program under grant NSF 1122374. Santos, P. J., Cao, Z., Zhang, J., Alexander-Katz, A. Get the most important science stories of the day, free in your inbox. Get the latest business insights from Dun & Bradstreet. Macromolecules 27, 12561266 (1994). Nature 561, 378382 (2018). Yuan, H. et al. Google Scholar. developed characterization methods, collected microscopy data, designed the experiments and wrote the manuscript. Furthermore, the peak adhesion force of the NPA2 coacervate was achieved at a much larger deformation, indicating the capability to effectively dissipate a large amount of energy under a mechanical challenge (Fig. Nature 466, 474477 (2010). Mater. 141, 1182711831 (2019). Nature 505, 7377 (2014). Adv. 2l). Nanoparticle self-assembly is an efficient bottom-up strategy for the creation of nanostructures. After soaking the NPA2 coacervate-coated intestinal mucosa tissues in simulated gastric fluid (Ga) or simulated intestinal fluid (In) at 37C for 2h, respectively, the adherent coacervate coatings remained undiluted and maintained adhesion on the mucosa surface (Fig. NPA2 coacervates were incubated in simulated gastric fluid (Ga) and simulated intestinal fluid (In) at 37C for 3 days, respectively. Macroscopic materials assembled from nanoparticle superlattices. Internet Explorer). 03 September 2022, JOM Source data are provided as a Source Data file for Fig. Drug Del. Ye, X. et al. Google Scholar. Article Y.D., P.S., H.Z., H.L., and X.P. & Macfarlane, R. J. 2103828 (2021). 3, 891895 (2004). [3] Nat. Anyone you share the following link with will be able to read this content: Sorry, a shareable link is not currently available for this article. The dark spots marked by red circles in the TEM images are supposed to be the hydrophobic cores of the assembled NP2 nanoparticles, while the catechol-functionalized hydrophilic PEG shell acts as a flexible polymer matrix that connects the hydrophobic cores to form the stable NPA2 coacervate dense phase. Google Scholar. Mater. Although orally administered Dex-P may not directly modulate the gut microbiota69, we expected the enhanced gut immune microenvironment by Dex-P/NPA2 treatment can positively regulate the gut microbiota. GPC (Agilent system, 1260 Infinity II) with a refractive index detector was used to detect whether the degraded or dissolved NPA2 coacervate components existed in the simulated body fluids (Ga, In) after 3 days of incubation. The amplified effects of subtle nanoscale anisotropies (such as chirality), collective motion, and non-additivity of their interactions further facilitate their self-organization that can lead to amazingly complex . Adv. Li, L., Yan, B., Yang, J., Chen, L. & Zeng, H. Novel musselinspired injectable selfhealing hydrogel with antibiofouling property. As nanotechnology advances, material scientists are working to improve the efficiency of the manufacturing process. Mater. Auyeung, E. et al. SD rats were allowed unrestricted access to water and a standard laboratory diet before and after oral gavage. 33, 289294 (2001). e The formation of NPA2 coacervate (stained by Fast Green FCF) via NP2 nanoparticle assembly can be visualized by fluidfluid phase separation and further observed by TEM. Article Bio-inspired reversible underwater adhesive. The NPA2 coacervate was chosen as the model for further investigations because hydrogen-bonding interactions provided by the functionalized catechol groups that drive the coacervation of NP2 nanoparticles can mediate adhesion of the NPA2 coacervate to wet tissue surfaces35,36,37,38. Mater. PubMed The nanoparticle solutions then were dialyzed against deionized water (standard regenerated cellulose (RC) dialysis membrane with 3.5kDa cutoff, Spectrum Chemical) at room temperature for 24h to form NPA coacervates via nanoparticle assembly. Adv. Cannarile, L. et al. Google Scholar. Programmable atom equivalents: atomic crystallization as a framework for synthesizing nanoparticle superlattices. Self-assembly is the spontaneous organization of smaller subunits to form larger, well-organized patterns. Zuochen Wang. Transl. Article A DNA-based method for rationally assembling nanoparticles into macroscopic materials. The nanoparticle assembly strategy may be further refined with alternative polyanions and surface stabilizing agents; it may also be applicable to other polycationic antibiotic candidates that encompass a wide range of antimicrobial peptides [50]. Lonely Planet. Nanoparticle Assembly in High Polymer Concentration Solutions Increases Superlattice Stability - Lee - 2021 - Small - Wiley Online Library Research Article Nanoparticle Assembly in High Polymer Concentration Solutions Increases Superlattice Stability Margaret S. Lee, Alfredo Alexander-Katz, Robert J. Macfarlane First published: 28 July 2021 Jeon, O., Wolfson, D. W. & Alsberg, E. Insitu formation of growthfactorloaded coacervate microparticleembedded hydrogels for directing encapsulated stem cell fate. Nanoparticles adsorbed on a membrane can induce deformations of the membrane that give rise to effective interactions between the particles. fi On day 7, colon tissues were analyzed for histopathology score f, MPO activity g, mRNA levels of tight junction-associated proteins including ZO-1 and occludin-1 h, and pro-inflammatory cytokines including interleukin IL-1 and TNF i. DNA-mediated nanoparticle crystallization into Wulff polyhedra. Gut 65, 10611069 (2016). Hepatol. 3). Synthesis of Au nanoparticles; photographs of processing of ANF-Fe 3 O 4 . Karya sastra sebagai cermin kehidupan, dalam tema dan idenya sangat dipengaruhi oleh kondisi lingkungan penyairnya. Commun. Free from electrostatic interactions, our fluid nanoparticle-assembled coacervate demonstrates significant pH- and salt-independent structural stability and forms a physically adhesive coating on a large surface area of intestinal tract with an extended residence time of more than 2 days to mediate the sustained release of preloaded water-soluble small molecule drugs in vivo. Nanoparticle assembly is a complex and versatile method of generating new materials, capable of using thousands of different combinations of particle size, shape, composition, and ligand chemistry to generate a library of unique structures. J. Clin. IBD significantly increases the risk of developing colorectal cancer and imposes a lifelong healthcare burden on millions of patients worldwide2,3,4. 1g and Supplementary Fig. b NPA2 coacervate can glue two ribbons of porcine skin tissue together and hold the weight of the tissues. Liu, J., Tan, C. S. Y. Google Scholar. Sprague Dawley (SD) rats (200300g, female, 812 weeks) were obtained from the Laboratory Animal Services Centre (Chinese University of Hong Kong) and cohoused for a week before being randomly assigned to different groups. Nanoparticle solutions as adhesives for gels and biological tissues. Cite this article. 24,25). The therapeutic efficacy of treatment with NPA2 alone did not show a significant difference compared with that of the non-treated colitic rats (Control) as evidenced by the similar MPO activity, histopathology score, and H&E staining, thus confirming that the NPA2 coacervate only served as a drug delivery vehicle and did not mitigate the colitic symptoms. Nano Lett. a Fluid NPA2 coacervate formed a durable adhesive coating on the medical nitrile glove. Organically linked iron oxide nanoparticle supercrystals with exceptional isotropic mechanical properties. PubMed 2a and Supplementary Fig. Nat. 17, 834 (2018). Chiral superstructures of inorganic nanorods by macroscopic mechanical grinding, Self-sorting in macroscopic supramolecular self-assembly via additive effects of capillary and magnetic forces, Nanoindentation of Supercrystalline Nanocomposites: Linear Relationship Between Elastic Modulus and Hardness, Spherical Packing Superlattices in Self-Assembly of Homogenous Soft Matter: Progresses and Potentials, Transpiration-inspired Capillary for Synchronous Synthesis and Patterning of Silver Nanoparticles, Hierarchically engineered nanostructures from compositionally anisotropic molecular building blocks, Cancel To further test this hypothesis, the capability of NPA coacervates as bioadhesive coatings on the gastrointestinal mucosa was further evaluated in vivo (Fig. The nano- and microstructure of the bulk solids can be tuned as a function of the size, chemical makeup and crystallographic symmetry of the superlattice crystallites, and the micro- and macrostructures can be controlled via subsequent processing steps.

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