Ambient ammonia synthesis from air via tandem water microdroplets-driven oxidation and pulsed photoelectrochemical reduction.
basic_science · Level V
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- Record sourced from PubMed, PMID 41802053.
- Also identified by DOI 10.1073/pnas.2529364123 and PMC identifier 12993948.
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Abstract
Artificial N<sub>2</sub> reduction offers a sustainable approach to green NH<sub>3</sub> synthesis, but the practical implementation is challenged by N<sub>2</sub> activation and competing hydrogen evolution. Photoelectrochemical nitrate and nitrite (NO<i><sub>x</sub></i><sup>-</sup>, <i>x</i> = 2 and 3) reduction with favorable thermodynamics represents a promising alternative for NH<sub>3</sub> production, provided that NO<i><sub>x</sub></i><sup>-</sup> can be supplied from the atmosphere. Here, through leveraging water microdroplet chemistry and dynamic photoelectrode-electrolyte interface engineering, we report a tandem air-NO<i><sub>x</sub></i><sup>-</sup>-NH<sub>3</sub> conversion system that integrates catalyst-free N<sub>2</sub> oxidation with pulsed photoelectrochemical NO<i><sub>x</sub></i><sup>-</sup> reduction (mNOR-pPNO<i><sub>x</sub></i>R). The system achieves efficient and selective NH<sub>3</sub> production with a yield rate of 24.5 μmol cm<sup>-2</sup> h<sup>-1</sup> at -0.2 V<sub>RHE</sub>, which are two to three orders of magnitude higher than conventional photo/electrocatalytic N<sub>2</sub> fixation. This study introduces insights for decentralized, on-demand ammonia production from air and water and broadens horizons of microdroplet chemistry and pulse strategy for sustainable chemical manufacturing.