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Terrestrial hydrothermal systems have been proposed as alternative birthplaces for early life but lacked reasonable scenarios for the supply of biomolecules. Here, we show that elemental sulfur (S 0 ), as the dominant mineral in terrestrial hot springs, can reduce carbon dioxide (CO 2 ) into formic acid (HCOOH) under ultraviolet (UV) light below 280 nm. The semiconducting S 0 is indicated to have a direct bandgap of 4.4 eV. The UV-excited S 0 produces photoelectrons with a highly negative potential of -2.34 V (versus NHE, pH 7), which could reduce CO 2 after accepting electrons from electron donors such as reducing sulfur species. Simultaneously, UV light breaks sulfur bonds, benefiting the adsorption of charged carbonates onto S 0 and assisting their photoreduction. Assuming that terrestrial hot springs covered 1% of primitive Earth's surface, S 0 at 10 μM could have produced maximal 10 9 kg/year HCOOH within 10-cm-thick photic zones, underlying its remarkable contributions to the accumulation of prebiotic biomolecules.

Photoreduction of inorganic carbon(+IV) by elemental sulfur: Implications for prebiotic synthesis in terrestrial hot springs