30 research outputs found

    Interactive models of communication at the nanoscale using nanoparticles that talk to one another

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    [EN] 'Communication' between abiotic nanoscale chemical systems is an almost-unexplored field with enormous potential. Here we show the design and preparation of a chemical communication system based on enzyme-powered Janus nanoparticles, which mimics an interactive model of communication. Cargo delivery from one nanoparticle is governed by the biunivocal communication with another nanoparticle, which involves two enzymatic processes and the interchange of chemical messengers. The conceptual idea of establishing communication between nanodevices opens the opportunity to develop complex nanoscale systems capable of sharing information and cooperating.A. L.-L. is grateful to 'La Caixa' Banking Foundation for his PhD fellowship. We wish to thank the Spanish Government (MINECO Projects MAT2015-64139-C4-1, CTQ2014-58989-P and CTQ2015-71936-REDT and AGL2015-70235-C2-2-R) and the Generalitat Valenciana (Project PROMETEOII/2014/047) for support. The Comunidad de Madrid (S2013/MIT-3029, Programme NANOAVANSENS) is also gratefully acknowledged.Llopis-Lorente, A.; Díez, P.; Sánchez, A.; Marcos Martínez, MD.; Sancenón Galarza, F.; Martínez-Ruiz, P.; Villalonga, R.... (2017). Interactive models of communication at the nanoscale using nanoparticles that talk to one another. Nature Communications. 8:1-7. https://doi.org/10.1038/ncomms15511S178Tseng, R., Huang, J., Ouyang, J., Kaner, R. & Yang, Y. Polyaniline nanofiber/gold nanoparticle nonvolatile memory. Nano Lett. 5, 1077–1080 (2005).Liu, R. & Sen, A. Autonomous nanomotor based on copper-platinum segmented nanobattery. J. Am. Chem. Soc. 133, 20064–20067 (2011).Valov, I. et al. Nanobatteries in redox-based resistive switches require extension of memristor theory. Nat. Commun. 4, 1771 (2013).Tarn, D. et al. Mesoporous silica nanoparticle nanocarriers: biofunctionality and biocompatibility. Acc. Chem. Res. 46, 792–801 (2013).Kline, T. & Paxton, W. Catalytic nanomotors: remote-controlled autonomous movement of striped metallic nanorods. Angew. Chem. Int. Ed. 117, 754–756 (2005).Akyildiz, I. F., Brunetti, F. & Blázquez, C. Nanonetworks: a new communication paradigm. Comput. Netw. 52, 2260–2279 (2008).Suda, T., Moore, M., Nakano, T., Egashira, R. & Enomoto, A. Exploratory research on molecular communication between nanomachines. Nat. Comput. 25, 1–30 (2005).Malak, D. & Akan, O. B. Molecular communication nanonetworks inside human body. Nano Commun. Netw. 3, 19–35 (2012).Akyildiz, I. F., Jornet, J. M. & Pierobon, M. Nanonetworks: a new frontier in communications. Commun. ACM 54, 84–89 (2011).Nakano, T., Moore, M. J., Wei, F., Vasilakos, A. V. & Shuai, J. Molecular communication and networking: opportunities and challenges. IEEE Trans. Nanobiosci. 11, 135–148 (2012).Waters, C. M. & Bassler, B. L. Quorum sensing: cell-to-cell communication in bacteria. Annu. Rev. Cell Dev. Biol. 21, 319–346 (2005).Dickschat, J. S. Quorum sensing and bacterial biofilms. Nat. Prod. Rep. 27, 343–369 (2010).Kerényi, Á., Bihary, D., Venturi, V. & Pongor, S. Stability of multispecies bacterial communities: signaling networks may stabilize microbiomes. PLoS ONE 8, e57947 (2013).Gotti, C. & Clementi, F. Neuronal nicotinic receptors: from structure to pathology. Prog. Neurobiol. 74, 363–396 (2004).Betke, K. M., Wells, C. A. & Hamm, H. E. GPCR mediated regulation of synaptic transmission. Prog. Neurobiol. 96, 304–321 (2012).Qian, L., Winfree, E. & Bruck, J. Neural network computation with DNA strand displacement cascades. Nature 475, 368–372 (2011).Benenson, Y. Biomolecular computing systems: principles, progress and potential. Nat. Rev. Genet. 13, 455–468 (2012).Ball, P. Chemistry meets computing. Nature 406, 118–120 (2000).de Silva, A. P. & McClenaghan, N. D. Molecular-Scale Logic Gates. Chem. Eur. J. 10, 574–586 (2004).Condon, A. Automata make antisense. Nature 429, 351–352 (2004).Seelig, G., Soloveichik, D., Zhang, D. Y. & Winfree, E. Enzyme-free nucleic acid logic circuits. Science 314, 1585–1588 (2006).Douglas, S. M., Bachelet, I. & Church, G. M. A logic-gated nanorobot for targeted transport of molecular payloads. Science 335, 831–834 (2012).Angelos, S., Yang, Y. W., Khashab, N. M., Stoddart, J. F. & Zink, J. I. Dual-controlled nanoparticles exhibiting AND logic. J. Am. Chem. Soc. 131, 11344–11346 (2009).Liu, H. et al. Dual-responsive surfaces modified with phenylboronic acid-containing polymer brush to reversibly capture and release cancer cells. J. Am. Chem. Soc. 135, 7603–7609 (2013).Lee, J. W. & Klajn, R. Dual-responsive nanoparticles that aggregate under the simultaneous action of light and CO2 . Chem. Commun. 51, 2036–2039 (2015).Liu, D. et al. Resettable, multi-readout logic gates based on controllably reversible aggregation of gold nanoparticles. Angew. Chem. Int. Ed. 50, 4103–4107 (2011).Chitode, J. S. Communication Theory Technical Publications (2010).Wood, J. T. Communication in Our Lives Wadsworth (2009).Guardado-Alvarez, T. M., Sudha Devi, L., Russell, M. M., Schwartz, B. J. & Zink, J. I. Activation of snap-top capped mesoporous silica nanocontainers using two near-infrared photons. J. Am. Chem. Soc. 135, 14000–14003 (2013).Baeza, A., Guisasola, E., Ruiz-Hernández, E. & Vallet-Regí, M. Magnetically triggered multidrug release by hybrid mesoporous silica nanoparticles. Chem. Mater. 24, 517–524 (2012).Zhang, Z. et al. Biocatalytic release of an anticancer drug from nucleic-acids-capped mesoporous SiO2 using DNA or molecular biomarkers as triggering stimuli. ACS Nano 7, 8455–8468 (2013).Tang, F., Li, L. & Chen, D. Mesoporous silica nanoparticles: synthesis, biocompatibility and drug delivery. Adv. Mater. 24, 1504–1534 (2012).Li, Z., Barnes, J. C., Bosoy, A., Stoddart, J. F. & Zink, J. I. Mesoporous silica nanoparticles in biomedical applications. Chem. Soc. Rev. 41, 2590–2605 (2012).Coll, C., Bernardos, A., Martínez-Máñez, R. & Sancenón, F. Gated silica mesoporous supports for controlled release and signaling applications. Acc. Chem. Res. 46, 339–349 (2013).Aznar, E. et al. Gated materials for on-command release of guest molecules. Chem. Rev. 116, 561–718 (2016).Díez, P. et al. Toward the design of smart delivery systems controlled by integrated enzyme-based biocomputing ensembles. J. Am. Chem. Soc. 136, 9116–9123 (2014).Villalonga, R. et al. Enzyme-controlled sensing-actuating nanomachine based on Janus Au-mesoporous silica nanoparticles. Chem. Eur. J. 19, 7889–7894 (2013).Jerez, G., Kaufman, G., Prystai, M., Schenkeveld, S. & Donkor, K. K. Determination of thermodynamic pKa values of benzimidazole and benzimidazole derivatives by capillary electrophoresis. J. Sep. Sci. 32, 1087–1095 (2009).Sheffner, A. L. The reduction in vitro in viscosity of mucoprotein solutions by a new mucolytic agent, N-acetyl-L-cysteine. Ann. N. Y. Acad. Sci. 106, 298–310 (1963).Turkevich, J., Stevenson, P. C. & Hillier, J. A study of the nucleation and growth processes in the synthesis of colloidal gold. Discuss. Faraday Soc. 11, 55–75 (1951).Frens, G. Controlled Nucleation for the Regulation of the Particle Size in Monodisperse Gold Suspensions. Nature 241, 20–22 (1973).Yousef, F. O., Zughul, M. B. & Badwan, A. A. The modes of complexation of benzimidazole with aqueous β-cyclodextrin explored by phase solubility, potentiometric titration, 1H-NMR and molecular modeling studies. J. Incl. Phenom. Macrocycl. Chem. 57, 519–523 (2007).Sánchez, A., Díez, P., Martínez-Ruíz, P., Villalonga, R. & Pingarrón, J. M. Janus Au-mesoporous silica nanoparticles as electrochemical biorecognition-signaling system. Electrochem. Commun. 30, 51–54 (2013).Akyildiz, I. F., Pierobon, M., Balasubramaniam, S. & Koucheryavy, Y. The internet of Bio-Nano things. IEEE Commun. Mag. 53, 32–40 (2015).Sancenón, F., Pascual, L., Oroval, M., Aznar, E. & Martínez-Máñez, R. Gated silica mesoporous materials in sensing applications. ChemistryOpen 4, 418–437 (2015).Akyildiz, I. & Jornet, J. The Internet of nano-things. IEEE Wirel. Commun. 17, 58–63 (2010).Giménez, C. et al. Towards chemical communication between gated nanoparticles. Angew. Chem. Int. Ed. 53, 12629–12633 (2014).Davis, B. G., Lloyd, R. C. & Jones, J. B. Controlled site-selective glycosylation of proteins by a combined site-directed mutagenesis and chemical modification approach. J. Org. Chem. 63, 9614–9615 (1998)

    The worldwide NORM production and a fully automated gamma-ray spectrometer for their characterization

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    Materials containing radionuclides of natural origin, which is modified by human made processes and being subject to regulation because of their radioactivity are known as NORM. We present a brief review of the main categories of non-nuclear industries together with the levels of activity concentration in feed raw materials, products and waste, including mechanisms of radioisotope enrichments. The global management of NORM shows a high level of complexity, mainly due to different degrees of radioactivity enhancement and the huge amount of worldwide waste production. The future tendency of guidelines concerning environmental protection will require both a systematic monitoring based on the ever-increasing sampling and high performance of gamma ray spectroscopy. On the ground of these requirements a new low background fully automated high-resolution gamma-ray spectrometer MCA_Rad has been developed. The design of Pb and Cu shielding allowed to reach a background reduction of two order of magnitude with respect to laboratory radioactivity. A severe lowering of manpower cost is obtained through a fully automation system, which enables up to 24 samples to be measured without any human attendance. Two coupled HPGe detectors increase the detection efficiency, performing accurate measurements on sample volume (180 cc) with a reduction of sample transport cost of material. Details of the instrument calibration method are presented. MCA_Rad system can measure in less than one hour a typical NORM sample enriched in U and Th with some hundreds of Bq/kg, with an overall uncertainty less than 5%. Quality control of this method has been tested. Measurements of certified reference materials RGK-1, RGU-2 and RGTh-1 containing concentrations of K, U and Th comparable to NORM have been performed, resulting an overall relative discrepancy of 5% among central values within the reported uncertainty.Comment: 21 pages, 4 figures, 6 table

    Genome-wide structural variant analysis identifies risk loci for non-Alzheimer's dementias

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    We characterized the role of structural variants, a largely unexplored type of genetic variation, in two non-Alzheimer's dementias, namely Lewy body dementia (LBD) and frontotemporal dementia (FTD)/amyotrophic lateral sclerosis (ALS). To do this, we applied an advanced structural variant calling pipeline (GATK-SV) to short-read whole-genome sequence data from 5,213 European-ancestry cases and 4,132 controls. We discovered, replicated, and validated a deletion in TPCN1 as a novel risk locus for LBD and detected the known structural variants at the C9orf72 and MAPT loci as associated with FTD/ALS. We also identified rare pathogenic structural variants in both LBD and FTD/ALS. Finally, we assembled a catalog of structural variants that can be mined for new insights into the pathogenesis of these understudied forms of dementia

    Clinical phenotypes of acute heart failure based on signs and symptoms of perfusion and congestion at emergency department presentation and their relationship with patient management and outcomes

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    Objective To compare the clinical characteristics and outcomes of patients with acute heart failure (AHF) according to clinical profiles based on congestion and perfusion determined in the emergency department (ED). Methods and results Overall, 11 261 unselected AHF patients from 41 Spanish EDs were classified according to perfusion (normoperfusion = warm; hypoperfusion = cold) and congestion (not = dry; yes = wet). Baseline and decompensation characteristics were recorded as were the main wards to which patients were admitted. The primary outcome was 1-year all-cause mortality; secondary outcomes were need for hospitalisation during the index AHF event, in-hospital all-cause mortality, prolonged hospitalisation, 7-day post-discharge ED revisit for AHF and 30-day post-discharge rehospitalisation for AHF. A total of 8558 patients (76.0%) were warm+ wet, 1929 (17.1%) cold+ wet, 675 (6.0%) warm+ dry, and 99 (0.9%) cold+ dry; hypoperfused (cold) patients were more frequently admitted to intensive care units and geriatrics departments, and warm+ wet patients were discharged home without admission. The four phenotypes differed in most of the baseline and decompensation characteristics. The 1-year mortality was 30.8%, and compared to warm+ dry, the adjusted hazard ratios were significantly increased for cold+ wet (1.660; 95% confidence interval 1.400-1.968) and cold+ dry (1.672; 95% confidence interval 1.189-2.351). Hypoperfused (cold) phenotypes also showed higher rates of index episode hospitalisation and in-hospital mortality, while congestive (wet) phenotypes had a higher risk of prolonged hospitalisation but decreased risk of rehospitalisation. No differences were observed among phenotypes in ED revisit risk. Conclusions Bedside clinical evaluation of congestion and perfusion of AHF patients upon ED arrival and classification according to phenotypic profiles proposed by the latest European Society of Cardiology guidelines provide useful complementary information and help to rapidly predict patient outcomes shortly after ED patient arrival

    Genome-wide structural variant analysis identifies risk loci for non-Alzheimer’s dementias

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    We characterized the role of structural variants, a largely unexplored type of genetic variation, in two non-Alzheimer’s dementias, namely Lewy body dementia (LBD) and frontotemporal dementia (FTD)/amyotrophic lateral sclerosis (ALS). To do this, we applied an advanced structural variant calling pipeline (GATK-SV) to short-read whole-genome sequence data from 5,213 European-ancestry cases and 4,132 controls. We discovered, replicated, and validated a deletion in TPCN1 as a novel risk locus for LBD and detected the known structural variants at the C9orf72 and MAPT loci as associated with FTD/ALS. We also identified rare pathogenic structural variants in both LBD and FTD/ALS. Finally, we assembled a catalog of structural variants that can be mined for new insights into the pathogenesis of these understudied forms of dementia
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