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dc.rights.licenseRoyal Society of Chemistry (RSC)es
dc.contributor.authorDe la Fuente, J. L.es
dc.contributor.authorVega, Jorgees
dc.contributor.authorMateo Martí, Evaes
dc.contributor.authorValles González, M. P.es
dc.contributor.authorRuiz Bermejo, Martaes
dc.contributor.authorPérez Fernández, Cristinaes
dc.date.accessioned2024-01-25T13:04:02Z-
dc.date.available2024-01-25T13:04:02Z-
dc.date.issued2023-06-21-
dc.identifier.citationPhysical Chemistry Chemical Physics 25: 20473-20484 (2023)es
dc.identifier.issn1463-9076-
dc.identifier.otherhttps://pubs.rsc.org/en/content/articlelanding/2023/cp/d3cp00968hes
dc.identifier.urihttp://hdl.handle.net/20.500.12666/920-
dc.description.abstractPrebiotic chemistry one-pot reactions, such as HCN-derived polymerizations, have been used as stimulating starting points for the generation of new multifunctional materials due to the simplicity of the processes, use of water as solvent, and moderate thermal conditions. Slight experimental variations in this special kind of polymerization tune the final properties of the products. Thus, herein, the influence of NH4Cl on the polymerization kinetics of cyanide under hydrothermal conditions and on the macrostructures and properties of this complex system is explored. The kinetics of the process is consistent with an autocatalytic model, but important variations in the polymerization reaction are observed according to a simple empirical model based on a Hill equation. The differences in the kinetic behaviour against NH4Cl were also revealed when the structural, morphological, thermal, electronic and magnetic properties of the synthesized cyanide polymers were compared, and these properties were evaluated by elemental analysis, FTIR, XPS, UV-vis, and ESR spectroscopies, X-ray diffraction, SEM and thermoanalytical techniques. As a result, this hydrothermal prebiotic polymerization is not only pH dependent, as previously thought, but also ammonium subservient. From this result, a hypothetical reaction mechanism was proposed, which involves the active participation of ammonium cations via formamidine and serves as a remarkable point against previous reports. The results discussed here expand the knowledge on HCN wet chemistry, offer an extended view of the relevant parameters during the simulation of hydrothermal scenarios and describe the production of promising paramagnetic and semiconducting materials inspired by prebiotic chemistry.es
dc.description.sponsorshipThe authors used the research facilities of the Centro de Astrobiologı´a (CAB), CSIC-INTA, and were supported by the Instituto Nacional de Te´cnica Aeroespacial ‘‘Esteban Terradas’’ (INTA) and by the project PID2019-104205GB-C21 from the Spanish Ministry of Science and Innovation and the Spanish State Research Agency MCIN/AEI/10.13039/501100011033. Additionally, the authors are grateful to M. Teresa Ferna´ndez for performing the FTIR and XRD measurements, to the Services of Thermal and Chemical Analysis of the Instituto de Ciencias de Materiales de Madrid (ICMM, CSIC) and to the recently closed Service of Electronic Spin Resonance of the Centro de Ayuda a la Investigación of the Universidad Complutense de Madrid (UCM). C. P-F. also thanks the project PRE2018-085781.es
dc.language.isoenges
dc.publisherRoyal Society of Chemistryes
dc.relationinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-104205GB-C21/ES/CICLO DE AEROSOLES EN MARTE Y LA TIERRA, ESTUDIO COMPARATIVO. IMPLICACIONES PARA LA VIDA Y PROTECCION PLANETARIA-ATMOSFERAS (CAMELIA-ATM)/es
dc.relationinfo:eu-repo/grantAgreement/AEI//PRE2018-085781es
dc.titleAmmonium affects the wet chemical network of HCN: feedback between prebiotic chemistry and materials sciencees
dc.typeinfo:eu-repo/semantics/articlees
dc.identifier.doi10.1039/d3cp00968h-
dc.identifier.e-issn1463-9084-
dc.contributor.funderInstituto Nacional de Técnica Aeroespacial (INTA)es
dc.contributor.funderUniversidad Complutense de Madrid (UCM)es
dc.contributor.funderAgencia Estatal de Investigación (AEI)es
dc.contributor.funderConsejo Superior de Investigaciones Científicas (CSIC)es
dc.contributor.funderMinisterio de Ciencia, Innovación y Universidades (MICINN)es
dc.description.peerreviewedPeerreviewes
dc.identifier.funderhttp://dx.doi.org/10.13039/501100011033es
dc.identifier.funderhttp://dx.doi.org/10.13039/501100010687es
dc.identifier.funderhttp://dx.doi.org/10.13039/501100002911es
dc.type.hasVersioninfo:eu-repo/semantics/publishedVersiones
dc.rights.accessRightsinfo:eu-repo/semantics/restrictedAccesses
dc.type.coarhttp://purl.org/coar/resource_type/c_1162es
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