An XPS study of HCN-derived films on pyrite surfaces: a prebiotic chemistry standpoint towards the development of protective coatings

Pérez-Fernández, Cristina; Ruíz-Bermejo, Marta; Gálvez-Martínez, Santos; Mateo‐Martí, Eva

doi:10.1039/d1ra02658e

Cited by 16 publications

(18 citation statements)

References 40 publications

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“…Therefore, the results discussed in this work increase our knowledge about the scarcely studied prebiotic hydrothermal cyanide chemistry 15 , 16 , 20 , 34 , 63 , further demonstrating its relevance in chemical evolution research in the context of the origins of life on the early Earth.…”

Section: Discussionsupporting

confidence: 55%

Prebiotic synthesis of noncanonical nucleobases under plausible alkaline hydrothermal conditions

Pérez-Fernández

Vega

Rayo-Pizarroso

et al. 2022

Sci Rep

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Herein, the potential of alkaline hydrothermal environments for the synthesis of possible ancestral pre-RNA nucleobases using cyanide as a primary source of carbon and nitrogen is described. Water cyanide polymerizations were assisted by microwave radiation to obtain high temperature and a relatively high pressure (MWR, 180 °C, 15 bar) and were also carried out using a conventional thermal system (CTS, 80 °C, 1 bar) to simulate subaerial and aerial hydrothermal conditions, respectively, on the early Earth. For these syntheses, the initial concentration of cyanide and the diffusion effects were studied. In addition, it is well known that hydrolysis conditions are directly related to the amount and diversity of organic molecules released from cyanide polymers. Thus, as a first step, we studied the effect of several hydrolysis procedures, generally used in prebiotic chemistry, on some of the potential pre-RNA nucleobases of interest, together with some of their isomers and/or deamination products, also presumably formed in these complex reactions. The results show that the alkaline hydrothermal scenarios with a relatively constant pH are good geological scenarios for the generation of noncanonical nucleobases using cyanide as a prebiotic precursor.

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Section: Discussionsupporting

confidence: 55%

Prebiotic synthesis of noncanonical nucleobases under plausible alkaline hydrothermal conditions

Pérez-Fernández

Vega

Rayo-Pizarroso

et al. 2022

Sci Rep

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“…Recently, it has been shown that the particle morphology of the known HCN-derived polymers can be tuned by the choice of the synthetic conditions [ 1 , 2 , 3 ]. Some polymers of this heterogeneous family [ 4 ] have been proposed as emergent materials with different applications, such as photocatalysts [ 5 ], semiconductors, nanowires, ferroelectric materials [ 6 ], capacitors [ 1 ], coatings with potential biomedical applications [ 2 , 7 , 8 , 9 ], protective films against corrosion [ 10 , 11 ], or for the development of antimicrobial media for passive filtration [ 12 ].…”

Section: Introductionmentioning

confidence: 99%

Tuning the Morphology in the Nanoscale of NH4CN Polymers Synthesized by Microwave Radiation: A Comparative Study

et al. 2021

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A systematic study is presented to explore the NH4CN polymerization induced by microwave (MW) radiation, keeping in mind the recent growing interest in these polymers in material science. Thus, a first approach through two series, varying the reaction times and the temperatures between 130 and 205 °C, was conducted. As a relevant outcome, using particular reaction conditions, polymer conversions similar to those obtained by means of conventional thermal methods were achieved, with the advantage of a very significant reduction of the reaction times. The structural properties of the end products were evaluated using compositional data, spectroscopic measurements, simultaneous thermal analysis (STA), X-ray diffraction (XRD), and scanning electron microscopy (SEM). As a result, based on the principal component analysis (PCA) from the main experimental results collected, practically only the crystallographic features and the morphologies in the nanoscale were affected by the MW-driven polymerization conditions with respect to those obtained by classical syntheses. Therefore, MW radiation allows us to tune the morphology, size and shape of the particles from the bidimensional C=N networks which are characteristic of the NH4CN polymers by an easy, fast, low-cost and green-solvent production. These new insights make these macromolecular systems attractive for exploration in current soft-matter science.

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“…In addition, recently, HCN-derived polymers have received great attention in materials science [ 18 , 19 ]. Their tunable characteristics provide promising potential applications, such as coating materials of interest in biomedicine [ 19 , 20 , 21 , 22 , 23 , 24 ], as well as effective films against oxidation [ 25 , 26 ] and for the modification of electrodes for the development of biosensors [ 27 ]. Additionally, HCN-derived polymers have been tested as photocatalyzers [ 28 ], capacitors [ 29 ], semiconductors [ 30 ] and passive antimicrobial filters [ 31 ].…”

Section: Introductionmentioning

confidence: 99%

Multivariate Analysis Applied to Microwave-Driven Cyanide Polymerization: A Statistical View of a Complex System

et al. 2023

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For the first time, chemometrics was applied to the recently reported microwave-driven cyanide polymerization. Fast, easy, robust, low-cost, and green-solvent processes are characteristic of these types of reactions. These economic and environmental benefits, originally inspired by the constraints imposed by plausible prebiotic synthetic conditions, have taken advantage of the development of a new generation of HCN-derived multifunctional materials. HCN-derived polymers present tunable properties by temperature and reaction time. However, the apparently random behavior observed in the evolution of cyanide polymerizations, assisted by microwave radiation over time at different temperatures, leads us to study this highly complex system using multivariate analytical tools to have a proper view of the system. Two components are sufficient to explain between 84 and 98% of the total variance in the data in all principal component analyses. In addition, two components explain more than 91% of the total variance in the data in the case of principal component analysis for categorical data. These consistent statistical results indicate that microwave-driven polymerization is a more robust process than conventional thermal syntheses but also that plausible prebiotic chemistry in alkaline subaerial environments could be more complex than in the aerial part of these systems, presenting a clear example of the “messy chemistry” approach of interest in the research about the origins of life. In addition, the methodology discussed herein could be useful for the data analysis of extraterrestrial samples and for the design of soft materials, in a feedback view between prebiotic chemistry and materials science.

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An XPS study of HCN-derived films on pyrite surfaces: a prebiotic chemistry standpoint towards the development of protective coatings

Abstract: Alkaline hydrothermal environment led to a NH4CN-based film with protective corrosion properties on the highly reactive pyrite surface.

Cited by 16 publications

References 40 publications

Prebiotic synthesis of noncanonical nucleobases under plausible alkaline hydrothermal conditions

Prebiotic synthesis of noncanonical nucleobases under plausible alkaline hydrothermal conditions

Tuning the Morphology in the Nanoscale of NH4CN Polymers Synthesized by Microwave Radiation: A Comparative Study

Multivariate Analysis Applied to Microwave-Driven Cyanide Polymerization: A Statistical View of a Complex System

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