<p>The polymerization of hydrogen cyanide (HCN) is considered a central route to molecular complexity in prebiotic chemistry, following the seminal synthesis of adenine reported by Oró. Here, we investigate how mineral identity and mineral loading modulate cyanide reactivity in aqueous aerosols using selected geologically relevant silicate, oxide, carbonate, sulfide, and mixed mineral substrates as simplified analogues of early planetary mineral–water interfaces. Using a target-agnostic, systems-level strategy, we combine complementary spectroscopic and chromatographic techniques, such as FTIR spectroscopy, HPLC–FLD and GC–MS, with multivariate statistical analyses (CATPCA and PCA) to interrogate highly complex reaction mixtures from cyanide polymerizations in the presence of aqueous aerosols. This approach reveals statistically robust, mineral-dependent trends in spectroscopic and chromatographic profiles that are strongly dependent on both mineral abundance and analytical methodologies. Our results demonstrate that minerals could act either as inert matrices or as active modulators of cyanide chemistry, while highlighting the power of untargeted statistical frameworks to extract chemically meaningful information from analytically intractable prebiotic systems, as is the case of the organic complex mixtures from cyanide polymerization reactions.</p>

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Statistical insights into the role of HCN–mineral interactions in aqueous aerosols during chemical evolution

  • Antonio López-García,
  • Elena González-Toril,
  • Fuencisla Cañadas,
  • Marta Ruiz-Bermejo

摘要

The polymerization of hydrogen cyanide (HCN) is considered a central route to molecular complexity in prebiotic chemistry, following the seminal synthesis of adenine reported by Oró. Here, we investigate how mineral identity and mineral loading modulate cyanide reactivity in aqueous aerosols using selected geologically relevant silicate, oxide, carbonate, sulfide, and mixed mineral substrates as simplified analogues of early planetary mineral–water interfaces. Using a target-agnostic, systems-level strategy, we combine complementary spectroscopic and chromatographic techniques, such as FTIR spectroscopy, HPLC–FLD and GC–MS, with multivariate statistical analyses (CATPCA and PCA) to interrogate highly complex reaction mixtures from cyanide polymerizations in the presence of aqueous aerosols. This approach reveals statistically robust, mineral-dependent trends in spectroscopic and chromatographic profiles that are strongly dependent on both mineral abundance and analytical methodologies. Our results demonstrate that minerals could act either as inert matrices or as active modulators of cyanide chemistry, while highlighting the power of untargeted statistical frameworks to extract chemically meaningful information from analytically intractable prebiotic systems, as is the case of the organic complex mixtures from cyanide polymerization reactions.