The emergence of bio-essential nitrogenous molecules like ammonia and urea on early Earth is crucial for the origins of life. Herein, we propose a prebiotic molecular synthesis process involving ammonia and urea on rhodochrosite via a geo-electrochemical mechanism, offering another similar inorganic pathway that produces simple molecules like methane and carbon monoxide in primordial environments. Though long overlooked, Mn element is an essential cofactor in redox enzymes and linked to organic-rich mineral deposits, indicating its role in early biological processes. In this context, the potential of rhodochrosite (the most abundant sedimentary manganese-bearing mineral with naturally doping) to catalyze the conversion of NOx- and CO2 into NH3 and/or urea within a geo-electrochemical system was explore. In situ experiments and theoretical modeling show that dopant modulation of Mn sites optimizes the d-band center, strengthening adsorption of NOx⁻ and CO2 and enabling efficient NH3 and urea production. This finding provides an abiotic pathway for the accumulation of key nitrogenous compounds under prebiotic oceanic conditions, without enzymes or extreme processes, suggesting a compelling mineral-mediated origin for prebiotic nitrogenous molecules.
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Conversion/alloying anode materials exhibiting high K storage capacities suffer from large volume variations and unstable electrode/electrolyte interfaces upon cycling. Herein, taking SnS/reduced graphene oxide (SnS/rGO) anodes as an example, the electrochemical performance of SnS/rGO could significantly be improved via employing potassium bis(fluorosulfonyl)imide (KFSI) salt in electrolytes and ultrathin TiO2 coating. KF-rich inorganic layer was demonstrated to help form robust SEI layer, which could suppress the side reactions to increase the Coulombic efficiency. The formed potassiated KxTiO2 coating layer was constructed to boost charge transfer capability and K-ion diffusion kinetics. The as-prepared SnS/rGO@TiO2-20 electrode in KFSI electrolyte delivers the high CE of 99.1% and 424 mAh·g−1 after 200 cycles with an ultrahigh capacity retention of 98.5%.
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